Graphene-based porous silica sheets impregnated with polyethyleneimine for superior CO2 capture.

PubMed

Yang, Shubin; Zhan, Liang; Xu, Xiaoyue; Wang, Yanli; Ling, Licheng; Feng, Xinliang

2013-04-18

It is demonstrated that graphene-based porous silica sheets can serve as an efficient carrier support for PEI via a simple nanocasting technology. The resulting materials possess thin nature, high PEI loading content and high thermal-conductivity. Such features are favorable for the efficient diffusion and adsorption of CO2 as well as the rapid thermal transfer during the CO2 capture process. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Active chemisorption sites in functionalized ionic liquids for carbon capture.

PubMed

Cui, Guokai; Wang, Jianji; Zhang, Suojiang

2016-07-25

Development of novel technologies for the efficient and reversible capture of CO2 is highly desired. In the last decade, CO2 capture using ionic liquids has attracted intensive attention from both academia and industry, and has been recognized as a very promising technology. Recently, a new approach has been developed for highly efficient capture of CO2 by site-containing ionic liquids through chemical interaction. This perspective review focuses on the recent advances in the chemical absorption of CO2 using site-containing ionic liquids, such as amino-based ionic liquids, azolate ionic liquids, phenolate ionic liquids, dual-functionalized ionic liquids, pyridine-containing ionic liquids and so on. Other site-containing liquid absorbents such as amine-based solutions, switchable solvents, and functionalized ionic liquid-amine blends are also investigated. Strategies have been discussed for how to activate the existent reactive sites and develop novel reactive sites by physical and chemical methods to enhance CO2 absorption capacity and reduce absorption enthalpy. The carbon capture mechanisms of these site-containing liquid absorbents are also presented. Particular attention has been paid to the latest progress in CO2 capture in multiple-site interactions by amino-free anion-functionalized ionic liquids. In the last section, future directions and prospects for carbon capture by site-containing ionic liquids are outlined.

Efficacy of Mosquito Traps for Collecting Potential West Nile Mosquito Vectors in a Natural Mediterranean Wetland

PubMed Central

Roiz, David; Roussel, Marion; Muñoz, Joaquin; Ruiz, Santiago; Soriguer, Ramón; Figuerola, Jordi

2012-01-01

Surveillance, research, and control of mosquito-borne diseases such as West Nile virus require efficient methods for sampling mosquitoes. We compared the efficacy of BG-Sentinel and Centers for Disease Control and Prevention (CDC)-CO2 traps in terms of the abundances of host-seeking and blood-fed female mosquitoes and the origin of mosquito bloodmeals. Our results indicate that BG-Sentinel traps that use CO2 and attractants are as effective as CDC-CO2 traps for Culex mosquito species, Ochlerotatus caspius, and they are also highly efficient at capturing Anopheles atroparvus host-seeking and blood-fed females with or without CO2. The CDC-CO2 trap is the least efficient method for capturing blood-fed females. BG-Sentinel traps with attractants and CO2 were significantly better at capturing mosquitoes that had fed on mammals than the unbaited BG-Sentinel and CDC-CO2 traps in the cases of An. atroparvus and Cx. theileri. These results may help researchers to optimize trapping methods by obtaining greater sample sizes and saving time and money. PMID:22492149

Adaptation to high CO2 concentration in an optimal environment: radiation capture, canopy quantum yield and carbon use efficiency

NASA Technical Reports Server (NTRS)

Monje, O.; Bugbee, B.

1998-01-01

The effect of elevated [CO2] on wheat (Triticum aestivum L. Veery 10) productivity was examined by analysing radiation capture, canopy quantum yield, canopy carbon use efficiency, harvest index and daily C gain. Canopies were grown at either 330 or 1200 micromoles mol-1 [CO2] in controlled environments, where root and shoot C fluxes were monitored continuously from emergence to harvest. A rapidly circulating hydroponic solution supplied nutrients, water and root zone oxygen. At harvest, dry mass predicted from gas exchange data was 102.8 +/- 4.7% of the observed dry mass in six trials. Neither radiation capture efficiency nor carbon use efficiency were affected by elevated [CO2], but yield increased by 13% due to a sustained increase in canopy quantum yield. CO2 enrichment increased root mass, tiller number and seed mass. Harvest index and chlorophyll concentration were unchanged, but CO2 enrichment increased average life cycle net photosynthesis (13%, P < 0.05) and root respiration (24%, P < 0.05). These data indicate that plant communities adapt to CO2 enrichment through changes in C allocation. Elevated [CO2] increases sink strength in optimal environments, resulting in sustained increases in photosynthetic capacity, canopy quantum yield and daily C gain throughout the life cycle.

Oxidatively-Stable Linear Poly(propylenimine)-Containing Adsorbents for CO2 Capture from Ultra-Dilute Streams.

PubMed

Pang, Simon H; Lively, Ryan P; Jones, Christopher W

2018-05-29

Aminopolymer-based solid sorbents have been widely investigated for CO2 capture from dilute streams such as flue gas or ambient air. However, the oxidative stability of the most well-studied aminopolymer, poly(ethylenimine) (PEI), is limited, causing it to lose its CO2 capture capacity after exposure to oxygen at elevated temperatures. Here we demonstrate the use of linear poly(propylenimine) (PPI), synthesized via a simple cationic ring-opening polymerization, as a more oxidatively-stable alternative to PEI with high CO2 capacity and amine efficiency. The performance of linear PPI/SBA-15 composites is investigated over a range of CO2 capture conditions (CO2 partial pressure, adsorption temperature) to examine the trade-off between adsorption capacity and sorption site accessibility, which may be expected to be more limited in linear polymers relative to the prototypical hyperbranched PEI. Linear PPI/SBA-15 composites are more efficient at CO2 capture and retain 65-83% of their CO2 capacity after exposure to a harsh oxidative treatment, compared to 20-40% retention for linear PEI. Additionally, we demonstrate long-term stability of linear PPI sorbents over 50 adsorption/desorption cycles with no loss in performance. Combined with other strategies for improving oxidative stability and adsorption kinetics, linear PPI may play a role as a component of stable, solid adsorbents in commercial applications for CO2 capture. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Economic and energetic analysis of capturing CO2 from ambient air

PubMed Central

House, Kurt Zenz; Baclig, Antonio C.; Ranjan, Manya; van Nierop, Ernst A.; Wilcox, Jennifer; Herzog, Howard J.

2011-01-01

Capturing carbon dioxide from the atmosphere (“air capture”) in an industrial process has been proposed as an option for stabilizing global CO2 concentrations. Published analyses suggest these air capture systems may cost a few hundred dollars per tonne of CO2, making it cost competitive with mainstream CO2 mitigation options like renewable energy, nuclear power, and carbon dioxide capture and storage from large CO2 emitting point sources. We investigate the thermodynamic efficiencies of commercial separation systems as well as trace gas removal systems to better understand and constrain the energy requirements and costs of these air capture systems. Our empirical analyses of operating commercial processes suggest that the energetic and financial costs of capturing CO2 from the air are likely to have been underestimated. Specifically, our analysis of existing gas separation systems suggests that, unless air capture significantly outperforms these systems, it is likely to require more than 400 kJ of work per mole of CO2, requiring it to be powered by CO2-neutral power sources in order to be CO2 negative. We estimate that total system costs of an air capture system will be on the order of $1,000 per tonne of CO2, based on experience with as-built large-scale trace gas removal systems. PMID:22143760

Ca-Embedded C2N: an efficient adsorbent for CO2 capture.

PubMed

Liu, Yuzhen; Meng, Zhaoshun; Guo, Xiaojian; Xu, Genjian; Rao, Dewei; Wang, Yuhui; Deng, Kaiming; Lu, Ruifeng

2017-10-25

Carbon dioxide as a greenhouse gas causes severe impacts on the environment, whereas it is also a necessary chemical feedstock that can be converted into carbon-based fuels via electrochemical reduction. To efficiently and reversibly capture CO 2 , it is important to find novel materials for a good balance between adsorption and desorption. In this study, we performed first-principles calculations and grand canonical Monte Carlo (GCMC) simulations, to systematically study metal-embedded carbon nitride (C 2 N) nanosheets for CO 2 capture. Our first-principles results indicated that Ca atoms can be uniformly trapped in the cavity center of C 2 N structure, while the transition metals (Sc, Ti, V, Cr, Mn, Fe, Co) are favorably embedded in the sites off the center of the cavity. The determined maximum number of CO 2 molecules with strong physisorption showed that Ca-embedded C 2 N monolayer is the most promising CO 2 adsorbent among all considered metal-embedded materials. Moreover, GCMC simulations revealed that at room temperature the gravimetric density for CO 2 adsorbed on Ca-embedded C 2 N reached 50 wt% at 30 bar and 23 wt% at 1 bar, higher than other layered materials, thus providing a satisfactory system for the CO 2 capture and utilization.

Process for CO.sub.2 capture using zeolites from high pressure and moderate temperature gas streams

DOEpatents

Siriwardane, Ranjani V [Morgantown, WV; Stevens, Robert W [Morgantown, WV

2012-03-06

A method for separating CO.sub.2 from a gas stream comprised of CO.sub.2 and other gaseous constituents using a zeolite sorbent in a swing-adsorption process, producing a high temperature CO.sub.2 stream at a higher CO.sub.2 pressure than the input gas stream. The method utilizes CO.sub.2 desorption in a CO.sub.2 atmosphere and effectively integrates heat transfers for optimizes overall efficiency. H.sub.2O adsorption does not preclude effective operation of the sorbent. The cycle may be incorporated in an IGCC for efficient pre-combustion CO.sub.2 capture. A particular application operates on shifted syngas at a temperature exceeding 200.degree. C. and produces a dry CO.sub.2 stream at low temperature and high CO.sub.2 pressure, greatly reducing any compression energy requirements which may be subsequently required.

Energy and material balance of CO2 capture from ambient air.

PubMed

Zeman, Frank

2007-11-01

Current Carbon Capture and Storage (CCS) technologies focus on large, stationary sources that produce approximately 50% of global CO2 emissions. We propose an industrial technology that captures CO2 directly from ambient air to target the remaining emissions. First, a wet scrubbing technique absorbs CO2 into a sodium hydroxide solution. The resultant carbonate is transferred from sodium ions to calcium ions via causticization. The captured CO2 is released from the calcium carbonate through thermal calcination in a modified kiln. The energy consumption is calculated as 350 kJ/mol of CO2 captured. It is dominated by the thermal energy demand of the kiln and the mechanical power required for air movement. The low concentration of CO2 in air requires a throughput of 3 million cubic meters of air per ton of CO2 removed, which could result in significant water losses. Electricity consumption in the process results in CO2 emissions and the use of coal power would significantly reduce to net amount captured. The thermodynamic efficiency of this process is low but comparable to other "end of pipe" capture technologies. As another carbon mitigation technology, air capture could allow for the continued use of liquid hydrocarbon fuels in the transportation sector.

Atmospheric CO2 capture by algae: Negative carbon dioxide emission path.

PubMed

Moreira, Diana; Pires, José C M

2016-09-01

Carbon dioxide is one of the most important greenhouse gas, which concentration increase in the atmosphere is associated to climate change and global warming. Besides CO2 capture in large emission point sources, the capture of this pollutant from atmosphere may be required due to significant contribution of diffuse sources. The technologies that remove CO2 from atmosphere (creating a negative balance of CO2) are called negative emission technologies. Bioenergy with Carbon Capture and Storage may play an important role for CO2 mitigation. It represents the combination of bioenergy production and carbon capture and storage, keeping carbon dioxide in geological reservoirs. Algae have a high potential as the source of biomass, as they present high photosynthetic efficiencies and high biomass yields. Their biomass has a wide range of applications, which can improve the economic viability of the process. Thus, this paper aims to assess the atmospheric CO2 capture by algal cultures. Copyright © 2016 Elsevier Ltd. All rights reserved.

Rational construction of a stable Zn4O-based MOF for highly efficient CO2 capture and conversion.

PubMed

Zhou, Hui-Fang; Liu, Bo; Hou, Lei; Zhang, Wen-Yan; Wang, Yao-Yu

2018-01-11

By employing a carboxylate ligand derived from benzene-1,4-dicarboxylate, a chemically stable Zn 4 O-based self-penetrating metal-organic framework has been rationally synthesized, which exhibits high CO 2 adsorption and efficient catalytic conversion for CO 2 cycloaddition.

Predicting the ultimate potential of natural gas SOFC power cycles with CO2 capture - Part A: Methodology and reference cases

NASA Astrophysics Data System (ADS)

Campanari, Stefano; Mastropasqua, Luca; Gazzani, Matteo; Chiesa, Paolo; Romano, Matteo C.

2016-08-01

Driven by the search for the highest theoretical efficiency, in the latest years several studies investigated the integration of high temperature fuel cells in natural gas fired power plants, where fuel cells are integrated with simple or modified Brayton cycles and/or with additional bottoming cycles, and CO2 can be separated via chemical or physical separation, oxy-combustion and cryogenic methods. Focusing on Solid Oxide Fuel Cells (SOFC) and following a comprehensive review and analysis of possible plant configurations, this work investigates their theoretical potential efficiency and proposes two ultra-high efficiency plant configurations based on advanced intermediate-temperature SOFCs integrated with a steam turbine or gas turbine cycle. The SOFC works at atmospheric or pressurized conditions and the resulting power plant exceeds 78% LHV efficiency without CO2 capture (as discussed in part A of the work) and 70% LHV efficiency with substantial CO2 capture (part B). The power plants are simulated at the 100 MW scale with a complete set of realistic assumptions about fuel cell (FC) performance, plant components and auxiliaries, presenting detailed energy and material balances together with a second law analysis.

Promoting Ethylene Selectivity from CO2 Electroreduction on CuO Supported onto CO2 Capture Materials.

PubMed

Yang, Hui-Juan; Yang, Hong; Hong, Yu-Hao; Zhang, Peng-Yang; Wang, Tao; Chen, Li-Na; Zhang, Feng-Yang; Wu, Qi-Hui; Tian, Na; Zhou, Zhi-You; Sun, Shi-Gang

2018-03-09

Cu is a unique catalyst for CO 2 electroreduction, since it can catalyze CO 2 reduction to a series of hydrocarbons, alcohols, and carboxylic acids. Nevertheless, such Cu catalysts suffer from poor selectivity. High pressure of CO 2 is considered to facilitate the activity and selectivity of CO 2 reduction. Herein, a new strategy is presented for CO 2 reduction with improved C 2 H 4 selectivity on a Cu catalyst by using CO 2 capture materials as the support at ambient pressure. N-doped carbon (N x C) was synthesized through high-temperature carbonization of melamine and l-lysine. We observed that the CO 2 uptake capacity of N x C depends on both the microporous area and the content of pyridinic N species, which can be controlled by the carbonization temperature (600-800 °C). The as-prepared CuO/N x C catalysts exhibit a considerably higher C 2 H 4 faradaic efficiency (36 %) than CuO supported on XC-72 carbon black (19 %), or unsupported CuO (20 %). Moreover, there is a good linear relationship between the C 2 H 4 faradaic efficiency and CO 2 uptake capacity of the supports for CuO. The local high CO 2 concentration near Cu catalysts, created by CO 2 capture materials, was proposed to increase the coverage of CO intermediate, which is favorable for the coupling of two CO units in the formation of C 2 H 4 . This study demonstrates that pairing Cu catalysts with CO 2 capture supports is a promising approach for designing highly effective CO 2 reduction electrocatalysts. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Highly Surface-Active Ca(OH)2 Monolayer as a CO2 Capture Material.

PubMed

Özçelik, V Ongun; Gong, Kai; White, Claire E

2018-03-14

Greenhouse gas emissions originating from fossil fuel combustion contribute significantly to global warming, and therefore the design of novel materials that efficiently capture CO 2 can play a crucial role in solving this challenge. Here, we show that reducing the dimensionality of bulk crystalline portlandite results in a stable monolayer material, named portlandene, that is highly effective at capturing CO 2 . On the basis of theoretical analysis comprised of ab initio quantum mechanical calculations and force-field molecular dynamics simulations, we show that this single-layer phase is robust and maintains its stability even at high temperatures. The chemical activity of portlandene is seen to further increase upon defect engineering of its surface using vacancy sites. Defect-containing portlandene is capable of separating CO and CO 2 from a syngas (CO/CO 2 /H 2 ) stream, yet is inert to water vapor. This selective behavior and the associated mechanisms have been elucidated by examining the electronic structure, local charge distribution, and bonding orbitals of portlandene. Additionally, unlike conventional CO 2 capturing technologies, the regeneration process of portlandene does not require high temperature heat treatment because it can release the captured CO 2 by application of a mild external electric field, making portlandene an ideal CO 2 capturing material for both pre- and postcombustion processes.

Technical and Energy Performance of an Advanced, Aqueous Ammonia-Based CO2 Capture Technology for a 500 MW Coal-Fired Power Station.

PubMed

Li, Kangkang; Yu, Hai; Feron, Paul; Tade, Moses; Wardhaugh, Leigh

2015-08-18

Using a rate-based model, we assessed the technical feasibility and energy performance of an advanced aqueous-ammonia-based postcombustion capture process integrated with a coal-fired power station. The capture process consists of three identical process trains in parallel, each containing a CO2 capture unit, an NH3 recycling unit, a water separation unit, and a CO2 compressor. A sensitivity study of important parameters, such as NH3 concentration, lean CO2 loading, and stripper pressure, was performed to minimize the energy consumption involved in the CO2 capture process. Process modifications of the rich-split process and the interheating process were investigated to further reduce the solvent regeneration energy. The integrated capture system was then evaluated in terms of the mass balance and the energy consumption of each unit. The results show that our advanced ammonia process is technically feasible and energy-competitive, with a low net power-plant efficiency penalty of 7.7%.

Techno-economic assessment of polymer membrane systems for postcombustion carbon capture at coal-fired power plants.

PubMed

Zhai, Haibo; Rubin, Edward S

2013-03-19

This study investigates the feasibility of polymer membrane systems for postcombustion carbon dioxide (CO(2)) capture at coal-fired power plants. Using newly developed performance and cost models, our analysis shows that membrane systems configured with multiple stages or steps are capable of meeting capture targets of 90% CO(2) removal efficiency and 95+% product purity. A combined driving force design using both compressors and vacuum pumps is most effective for reducing the cost of CO(2) avoided. Further reductions in the overall system energy penalty and cost can be obtained by recycling a portion of CO(2) via a two-stage, two-step membrane configuration with air sweep to increase the CO(2) partial pressure of feed flue gas. For a typical plant with carbon capture and storage, this yielded a 15% lower cost per metric ton of CO(2) avoided compared to a plant using a current amine-based capture system. A series of parametric analyses also is undertaken to identify paths for enhancing the viability of membrane-based capture technology.

Carbon dioxide capture from atmospheric air using sodium hydroxide spray.

PubMed

Stolaroff, Joshuah K; Keith, David W; Lowry, Gregory V

2008-04-15

In contrast to conventional carbon capture systems for power plants and other large point sources, the system described in this paper captures CO2 directly from ambient air. This has the advantages that emissions from diffuse sources and past emissions may be captured. The objective of this research is to determine the feasibility of a NaOH spray-based contactor for use in an air capture system by estimating the cost and energy requirements per unit CO2 captured. A prototype system is constructed and tested to measure CO2 absorption, energy use, and evaporative water loss and compared with theoretical predictions. A numerical model of drop collision and coalescence is used to estimate operating parameters for a full-scale system, and the cost of operating the system per unit CO2 captured is estimated. The analysis indicates that CO2 capture from air for climate change mitigation is technically feasible using off-the-shelf technology. Drop coalescence significantly decreases the CO2 absorption efficiency; however, fan and pump energy requirements are manageable. Water loss is significant (20 mol H2O/mol CO2 at 15 degrees C and 65% RH) but can be lowered by appropriately designing and operating the system. The cost of CO2 capture using NaOH spray (excluding solution recovery and CO2 sequestration, which may be comparable) in the full-scale system is 96 $/ton-CO2 in the base case, and ranges from 53 to 127 $/ton-CO2 under alternate operating parameters and assumptions regarding capital costs and mass transfer rate. The low end of the cost range is reached by a spray with 50 microm mean drop diameter, which is achievable with commercially available spray nozzles.

Design of Stratified Functional Nanoporous Materials for CO 2 Capture and Conversion

DOE Office of Scientific and Technical Information (OSTI.GOV)

Johnson, J. Karl; Ye, Jingyun

The objective of this project is to develop novel nanoporous materials for CO 2 capture and conversion. The motivation of this work is that capture of CO 2 from flue gas or the atmosphere coupled with catalytic hydrogenation of CO 2 into valuable chemicals and fuels can reduce the net amount of CO 2 in the atmosphere while providing liquid transportation fuels and other commodity chemicals. One approach to increasing the economic viability of carbon capture and conversion is to design a single material that can be used for both the capture and catalytic conversion of CO 2, because suchmore » a material could increase efficiency through process intensification. We have used density functional theory (DFT) methods to design catalytic moieties that can be incorporated into various metal organic framework (MOF) materials. We chose to work with MOFs because they are highly tailorable, can be functionalized, and have been shown to selectively adsorb CO 2 over N 2, which is a requirement for CO 2 capture from flue gas. Moreover, the incorporation of molecular catalytic moieties into MOF, through covalent bonding, produces a heterogeneous catalytic material having activities and selectivities close to those of homogeneous catalysts, but without the draw-backs associated with homogeneous catalysis.« less

Bench Scale Process for Low Cost CO 2 Capture Using a PhaseChanging Absorbent: Techno-Economic Analysis Topical Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Miebach, Barbara; McDuffie, Dwayne; Spiry, Irina

The objective of this project is to design and build a bench-scale process for a novel phase-changing CO 2 capture solvent. The project will establish scalability and technical and economic feasibility of using a phase-changing CO 2 capture absorbent for post-combustion capture of CO 2 from coal-fired power plants with 90% capture efficiency and 95% CO 2 purity at a cost of $40/tonne of CO 2 captured by 2025 and a cost of <$10/tonne of CO 2 captured by 2035. This report presents system and economic analysis for a process that uses a phase changing aminosilicone solvent to remove COmore » 2 from pulverized coal (PC) power plant flue gas. The aminosilicone solvent is a pure 1,3-bis(3-aminopropyl)-1,1,3,3-tetramethyldisiloxane (GAP-0). Performance of the phase-changing aminosilicone technology is compared to that of a conventional carbon capture system using aqueous monoethanolamine (MEA). This analysis demonstrates that the aminosilicone process has significant advantages relative to an MEA-based system. The first-year CO 2 removal cost for the phase-changing CO 2 capture process is $52.1/tonne, compared to $66.4/tonne for the aqueous amine process. The phase-changing CO 2 capture process is less costly than MEA because of advantageous solvent properties that include higher working capacity, lower corrosivity, lower vapor pressure, and lower heat capacity. The phase-changing aminosilicone process has approximately 32% lower equipment capital cost compared to that of the aqueous amine process. However, this solvent is susceptible to thermal degradation at CSTR desorber operating temperatures, which could add as much as $88/tonne to the CO 2 capture cost associated with solvent makeup. Future work is focused on mitigating this critical risk by developing an advanced low-temperature desorber that can deliver comparable desorption performance and significantly reduced thermal degradation rate.« less

In silico discovery of metal-organic frameworks for precombustion CO2 capture using a genetic algorithm

PubMed Central

Chung, Yongchul G.; Gómez-Gualdrón, Diego A.; Li, Peng; Leperi, Karson T.; Deria, Pravas; Zhang, Hongda; Vermeulen, Nicolaas A.; Stoddart, J. Fraser; You, Fengqi; Hupp, Joseph T.; Farha, Omar K.; Snurr, Randall Q.

2016-01-01

Discovery of new adsorbent materials with a high CO2 working capacity could help reduce CO2 emissions from newly commissioned power plants using precombustion carbon capture. High-throughput computational screening efforts can accelerate the discovery of new adsorbents but sometimes require significant computational resources to explore the large space of possible materials. We report the in silico discovery of high-performing adsorbents for precombustion CO2 capture by applying a genetic algorithm to efficiently search a large database of metal-organic frameworks (MOFs) for top candidates. High-performing MOFs identified from the in silico search were synthesized and activated and show a high CO2 working capacity and a high CO2/H2 selectivity. One of the synthesized MOFs shows a higher CO2 working capacity than any MOF reported in the literature under the operating conditions investigated here. PMID:27757420

Important roles of enthalpic and entropic contributions to CO2 capture from simulated flue gas and ambient air using mesoporous silica grafted amines.

PubMed

Alkhabbaz, Mustafa A; Bollini, Praveen; Foo, Guo Shiou; Sievers, Carsten; Jones, Christopher W

2014-09-24

The measurement of isosteric heats of adsorption of silica supported amine materials in the low pressure range (0-0.1 bar) is critical for understanding the interactions between CO2 and amine sites at low coverage and hence to the development of efficient amine adsorbents for CO2 capture from flue gas and ambient air. Heats of adsorption for an array of silica-supported amine materials are experimentally measured at low coverage using a Calvet calorimeter equipped with a customized dosing manifold. In a series of 3-aminopropyl-functionalized silica materials, higher amine densities resulted in higher isosteric heats of adsorption, clearly showing that the density/proximity of amine sites can influence the amine efficiency of adsorbents. In a series of materials with fixed amine loading but different amine types, strongly basic primary and secondary amine materials are shown to have essentially identical heats of adsorption near 90 kJ/mol. However, the adsorption uptakes vary substantially as a function of CO2 partial pressure for different primary and secondary amines, demonstrating that entropic contributions to adsorption may play a key role in adsorption at secondary amine sites, making adsorption at these sites less efficient at the low coverages that are important to the direct capture of CO2 from ambient air. Thus, while primary amines are confirmed to be the most effective amine types for CO2 capture from ambient air, this is not due to enhanced enthalpic contributions associated with primary amines over secondary amines, but may be due to unfavorable entropic factors associated with organization of the second alkyl chain on the secondary amine during CO2 adsorption. Given this hypothesis, favorable entropic factors may be the main reason primary amine based adsorbents are more effective under air capture conditions.

Heat recovery from sorbent-based CO.sub.2 capture

DOEpatents

Jamal, Aqil; Gupta, Raghubir P

2015-03-10

The present invention provides a method of increasing the efficiency of exothermic CO.sub.2 capture processes. The method relates to withdrawing heat generated during the exothermic capture of CO.sub.2 with various sorbents via heat exchange with a working fluid. The working fluid is provided at a temperature and pressure such that it is in the liquid state, and has a vaporization temperature in a range such that the heat arising from the reaction of the CO.sub.2 and the sorbent causes a phase change from liquid to vapor state in whole or in part and transfers heat from to the working fluid. The resulting heated working fluid may subsequently be used to generate power.

Potentiel des méthodes de séparation et stockage du CO2 dans la lutte contre l'effet de serreThe role of CO2 capture and sequestration in mitigation of climate change

NASA Astrophysics Data System (ADS)

Jean-Baptiste, Philippe; Ducroux, René

2003-06-01

Increasing atmospheric level of greenhouse gases are causing global warming and putting at risk the global climate system. The main anthropogenic greenhouse gas is CO 2. Technical solutions exist to reduce CO 2 emission and stabilise atmospheric CO 2 concentration, including energy saving and energy efficiency, switch to lower carbon content fuels like natural gas and to energy sources that operate with zero CO 2 emissions such as renewable or nuclear energy, enhance the natural sinks for CO 2 (forests, soils, etc.), and last but not least, sequester CO 2 from fossil fuels combustion. The purpose of this paper is to provide an overview of the technology and cost for capture and storage of CO 2. Some of the factors that will influence application, including environmental impact, cost and efficiency, are also discussed. Capturing CO 2 and storing it in underground geological reservoirs appears as the best environmentally acceptable option. It can be done with existing technology; however, substantial R&D is needed to improve available technology and to lower the cost. Applicable to large CO 2 emitting industrial facilities such as power plants, cement factories, steel industry, etc., which amount to more than 30% of the global anthropogenic CO 2 emission, it represents a valuable tool in the battle against global warming. To cite this article: P. Jean-Baptiste, R. Ducroux, C. R. Geoscience 335 (2003).

A technical, economic, and environmental assessment of amine-based CO2 capture technology for power plant greenhouse gas control.

PubMed

Rao, Anand B; Rubin, Edward S

2002-10-15

Capture and sequestration of CO2 from fossil fuel power plants is gaining widespread interest as a potential method of controlling greenhouse gas emissions. Performance and cost models of an amine (MEA)-based CO2 absorption system for postcombustion flue gas applications have been developed and integrated with an existing power plant modeling framework that includes multipollutant control technologies for other regulated emissions. The integrated model has been applied to study the feasibility and cost of carbon capture and sequestration at both new and existing coal-burning power plants. The cost of carbon avoidance was shown to depend strongly on assumptions about the reference plant design, details of the CO2 capture system design, interactions with other pollution control systems, and method of CO2 storage. The CO2 avoidance cost for retrofit systems was found to be generally higher than for new plants, mainly because of the higher energy penalty resulting from less efficient heat integration as well as site-specific difficulties typically encountered in retrofit applications. For all cases, a small reduction in CO2 capture cost was afforded by the SO2 emission trading credits generated by amine-based capture systems. Efforts are underway to model a broader suite of carbon capture and sequestration technologies for more comprehensive assessments in the context of multipollutant environmental management.

Comparaison de la performance environnementale de la production thermique d'electricite avec et sans sequestration geologique du dioxyde de carbone

NASA Astrophysics Data System (ADS)

Bellerive, Nathalie

The research project hypothesis is that CO2 capture and sequestration technologies (CSC) leads to a significant decrease in global warming, but increases the impact of all other aspects of the study. This is because other processes used for CO2 capture and sequestration require additional quantities of raw materials and energy. Two other objectives are described in this project. The first is the modeling of an Integrated Gasification Combined Cycle power plant for which there is no known generic data. The second is to select the right hypothesis regarding electrical production technologies, CO2 capture, compression and transportation by pipeline and finally sequestration. "Life Cycle Assessment" (LCA) analyses were chosen for this research project. LCA is an exhaustive quantitative method used to evaluate potential environmental impacts associated with a product, a service or an activity from resource extraction to waste elimination. This tool is governed by ISO 14 040 through ISO 14 049 and is sustained by the Society of Environmental Toxicology and Chemistry (SETAC) and the United Nations Environment Program (UNEP). Two power plants were studied, the Integrated Gasification Combined Cycle (IGCC) power plant and the Natural Gas Combined Cycle (NGCC) power plant. In order to sequester CO2 in geological formation, it is necessary to extract CO2from emission flows. For the IGCC power plant, CO 2 was captured before the burning phase. For the NGCC power plant, the capture was done during the afterburning phase. Once the CO2 was isolated, it was compressed and directed through a transportation pipe 1 000 km in length on the ground surface and in the sea. It is hypothesized that the power plant is 300 km from the shore and the sequestration platform 700 km from France's shore, in the North Sea. The IGCC power plant modeling and data selection regarding CO2 capture and sequestration were done by using primary data from the industry and the Ecoinvent generic database (Version 1.2). This database was selected due to its European source. Finally, technical calculations and literature were used to complete the data inventory. This was validated by electrical experts in order to increase data and modeling precision. Results were similar for IGCC and NGCC power plants using Impact 2002+, an impacts analysis method. Global warming potential decreased by 67% with the implementation of CO2 capture and sequestration compared to systems without CSC. Results for all others impacts categories, demonstrated an increase from 16% to 116% in relative proportions compared to systems without CSC. The main contributor was the additional quantity of energy required to operate CO2 capture and compression facilities. This additional energy negatively affected the power plant's global efficiency because of the increase in the quantity of fossil fuel that needed to be extracted and consumed. The increase in other impacts was mainly due to additional electricity, fossil fuel (for extracting, treatment and transportation) and additional emissions generated during power plant operations. A scenario analysis was done to study the sensitivity and variability of uncertain data during the software modeling process of a power plant. Data on power plant efficiency is the most variable and sensitive during modeling, followed by the length of the transportation pipe and the leaking rate during CO2 sequestration. This result analysis is interesting because it led to the maximum efficiency scenario with capture (with a short CO 2 transportation distance and a low leaking rate) obtaining better results on all impact category indicators, compared to the minimum efficiency scenario without capture. In fact, positive results on all category indicators were possible during the system comparison between the two cases (with and without capture). (Abstract shortened by UMI.)

Room-temperature ionic liquids and composite materials: platform technologies for CO(2) capture.

PubMed

Bara, Jason E; Camper, Dean E; Gin, Douglas L; Noble, Richard D

2010-01-19

Clean energy production has become one of the most prominent global issues of the early 21st century, prompting social, economic, and scientific debates regarding energy usage, energy sources, and sustainable energy strategies. The reduction of greenhouse gas emissions, specifically carbon dioxide (CO(2)), figures prominently in the discussions on the future of global energy policy. Billions of tons of annual CO(2) emissions are the direct result of fossil fuel combustion to generate electricity. Producing clean energy from abundant sources such as coal will require a massive infrastructure and highly efficient capture technologies to curb CO(2) emissions. Current technologies for CO(2) removal from other gases, such as those used in natural gas sweetening, are also capable of capturing CO(2) from power plant emissions. Aqueous amine processes are found in the vast majority of natural gas sweetening operations in the United States. However, conventional aqueous amine processes are highly energy intensive; their implementation for postcombustion CO(2) capture from power plant emissions would drastically cut plant output and efficiency. Membranes, another technology used in natural gas sweetening, have been proposed as an alternative mechanism for CO(2) capture from flue gas. Although membranes offer a potentially less energy-intensive approach, their development and industrial implementation lags far behind that of amine processes. Thus, to minimize the impact of postcombustion CO(2) capture on the economics of energy production, advances are needed in both of these areas. In this Account, we review our recent research devoted to absorptive processes and membranes. Specifically, we have explored the use of room-temperature ionic liquids (RTILs) in absorptive and membrane technologies for CO(2) capture. RTILs present a highly versatile and tunable platform for the development of new processes and materials aimed at the capture of CO(2) from power plant flue gas and in natural gas sweetening. The desirable properties of RTIL solvents, such as negligible vapor pressures, thermal stability, and a large liquid range, make them interesting candidates as new materials in well-known CO(2) capture processes. Here, we focus on the use of RTILs (1) as absorbents, including in combination with amines, and (2) in the design of polymer membranes. RTIL amine solvents have many potential advantages over aqueous amines, and the versatile chemistry of imidazolium-based RTILs also allows for the generation of new types of CO(2)-selective polymer membranes. RTIL and RTIL-based composites can compete with, or improve upon, current technologies. Moreover, owing to our experience in this area, we are developing new imidazolium-based polymer architectures and thermotropic and lyotropic liquid crystals as highly tailorable materials based on and capable of interacting with RTILs.

Novel Silica Nanostructured Platforms with Engineered Surface Functionality and Spherical Morphology for Low-Cost High-Efficiency Carbon Capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lai, Cheng-Yu; Radu, Daniela R.; Pizzi, Nicholas

Carbon capture is an integral part of the CO 2 mitigation efforts, and encompasses, among other measures, the demonstration of effective and inexpensive CO 2 capture technologies. The project demonstrated a novel platform—the amine-functionalized stellate mesoporous silica nanosphere (MSN)—for effective CO 2 absorption. The reported CO 2 absorption data are superior to the performance of other reported silica matrices utilized for carbon capture, featuring an amount of over 4 milimoles CO 2/g sorbent at low temperatures (in the range of 30-45 ºC), selected for simulating the temperature of actual flue gas. The reported platform is highly resilient, showing recyclability andmore » 85 % mass conservation of sorbent upon nine tested cycles. Importantly, the stellate MSNs show high CO 2 selectivity at room temperature, indicating that the presence of nitrogen in flue gas will not impair the CO 2 absorption performance. The results could lead to a simple and inexpensive new technology for CO 2 mitigation which could be implemented as measure of CO 2 mitigation in current fossil-fuel burning plants in the form of solid sorbent.« less

Comparative efficiency of two models of CO2 traps in the collection of free-living stages of ixodides.

PubMed

Guedes, Elizângela; de Azevedo Prata, Márcia Cristina; dos Reis, Eder Sebastião; Cançado, Paulo Henrique Duarte; Leite, Romário Cerqueira

2012-12-01

Traps using carbon dioxide (CO(2)) as a chemical attractant are known to be effective when capturing nymphs and adults of some free-living tick species such as Amblyomma cajennense and Amblyomma parvum. Despite the fact that the main source of CO(2) is dry ice, the chemical trap which uses 20 % lactic acid (C(3)H(6)O(3)) and calcium carbonate (CaCO(3)) has been tested as an alternative source of CO(2) whenever it is difficult to obtain dry ice. The objective of this paper was to test and compare the efficiency of these two models of traps during the study of population dynamics of A. cajennense and Amblyomma dubitatum in Coronel Pacheco, Minas Gerais, Brazil. Within the period comprising May 2006 to April 2008, eight CO(2) traps, of which four were dry ice and four chemical, were put in the pasture every 14 days at preestablished areas over a 1.0-m(2) white cotton flannel cloth with a capture dispositive which constituted of double-sided adhesive tapes fixed onto the four corners of the flannels. On every collection day, a cotton flannel without any chemical attractant was placed in the same area of the pasture to become an instrument to control the traps' capture efficiency. After 1 h, the white flannels were collected and placed in plastic bags for later identification and counting of the ticks. A total of 2,133 nymphs of Amblyomma sp., 328 adults of A. cajennense, and 292 adults of A. dubitatum were collected. Out of this total, the dry ice traps captured 1,087 nymphs (51 %), 188 A. cajennense (58.2 %), and 151 A. dubitatum (53 %), while the chemical traps captured 1,016 nymphs (47.6 %), 133 A. cajennense (41 %), and 133 A. dubitatum (46.5 %); 30 nymphs (1.4 %), 7 A. cajennense (0.8 %), and 8 A. dubitatum (0.5 %) were found on the control flannel. The capture potentials of ticks, nymphs, and adults, by the two models of traps tested, were statistically similar (p > 0.05). These results confirm the efficiency of the chemical trap enabling its use in areas of either difficult access or too distant from a dry ice supplier as is the case of forest areas where studies about ixodological fauna are generally carried out.

Pilot-Scale Silicone Process for Low-Cost Carbon Dioxide Capture. Final Scientific/Technical Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hancu, Dan; Wood, Benjamin; Genovese, Sarah

GE Global Research has developed, over the last 8 years, a platform of cost effective CO 2 capture technologies based on a non-aqueous aminosilicone solvent (GAP-1m). As demonstrated in a previous funded DOE project (DE-FE0007502), the GAP-1m solvent has increased CO 2 working capacity, lower volatility and corrosivity than the benchmark aqueous amine technology. The current report describes the cooperative program between GE Global Research (GE GRC), and the National Carbon Capture Center (NCCC) to design, construct, and operate a pilot-scale process using GAP-1m solvent to demonstrate its performance at 0.5 MWe. (i) Performance of the GAP-1m solvent was demonstratedmore » in a 0.5 MWe pilot with real flue gas for over 900 hrs. of operation using two alternative desorption designs: a Continuous Stirred Tank Reactor (CSTR), and a Steam Stripper Column (SSC). The CSTR is a one-stage separation unit with reduced space requirements, and capital cost. The alternative is a multi-stage separation column, with improved desorption efficiency. Testing the two desorber options allowed us to identify the most cost effective, and space efficient desorber solution. (ii) CSTR Campaign: The CSTR desorber unit was designed, fabricated and integrated with the pilot solvent test unit (PSTU), replacing the PSTU Steam Stripper Column at NCCC. Solvent management and waste water special procedures were implemented to accommodate operation of the non-aqueous solvent in the PSTU. Performance of the GAP-1m solvent with the CSTR was demonstrated for over 500 hrs. while varying temperature of the desorption (230 – 265 oF), solvent circulation rate (GAP-1m : CO 2 (molar) = 1.5 – 4), and flue gas flow rates (0.2 – 0.5 MWe). Solvent carry-over in the CO 2 product was minimized by maintaining water content below 5 wt.%, and desorption pressure at 7 psig. CO 2 capture efficiency achieved was 95% at 0.25 MWe (GAP-1m : CO 2 = 4 (molar), 230 oF desorption), and 65% at 0.5 MWe (GAP-1m : CO 2 (molar) = 1.5, 248 oF). Solvent loss was dominated by thermal degradation of the rich solvent. (iii) Steam Stripper Column Campaign: Higher expected cost of the solvent vs. aqueous amines makes solvent management a top priority to maintain the low cost for the process. During the testing of the GAP-1m solvent with the CSTR, thermal degradation of the rich solvent was found to be the main mechanism in solvent loss. Small amounts of water in the working solution were found to be an effective way to enable steam stripping, thereby lowering desorption temperature, and hence reducing thermal degradation. Steam stripping also increased working capacity by 30% due to a more efficient desorption. The concept was first tested in a glass stripping column (lab scale, GE GRC), optimized in a continuous bench scale system (2 kWe, GE GRC), and demonstrated in a 0.5 MWe PSTU at NCCC. No special system modifications were required to the PSTU to accommodate the testing of the non-aqueous GAP-1 solvent with the regenerator column. SSC was found to be more robust towards solvent entrainment (H 2O < 35 wt.%). 90 – 95% CO 2 capture efficiency was achieved under stoichiometric conditions at 0.5 MWe (235 oF desorption, 2 psig and 19 wt. % H 2O). Both CO 2 capture efficiency and specific duty reached optimum conditions at 18 wt.% H 2O. Low amine degradation (< 0.05 wt.%/day) was recorded over 350 hrs. of operation. Controlled water addition to GAP-1m solvent decreased the desorption temperature, thermal degradation, and improved the CO 2 working capacity due to more efficient absorption and desorption processes. Under these conditions, the GAP-1m solvent exhibited a 25% increased working capacity, and 10% reduction in specific steam duty vs. MEA, at 10 oF lower desorption temperature. (iv) Techno-economic Analysis: The pilot-scale PSTU engineering data were used to update the capture system process models, and the techno-economic analysis was performed for a 550 MW coal fired power plant. The 1st year CO 2 removal cost for the aminosilicone-based carbon-capture process was evaluated at $48/ton CO 2 using the steam stripper column. This is a 20% reduction compared to MEA, primarily due to lower overall capital cost. CO 2 cost using the CSTR desorber is dominated by the economics of the solvent make-up. The steam stripper desorber is the preferred unit operation due to a more efficient desorption, and reduced solvent make-up rate. Further reduction in CO 2 capture cost is expected by lowering the manufacturing cost of the solvent, implementing flowsheet optimization and/or implementing the next generation aminosilicone solvent with improved stability and increased CO 2 working capacity.« less

On the potential for BECCS efficiency improvement through heat recovery from both post-combustion and oxy-combustion facilities.

PubMed

Dowell, N Mac; Fajardy, M

2016-10-20

In order to mitigate climate change to no more than 2 °C, it is well understood that it will be necessary to directly remove significant quantities of CO 2 , with bioenergy CCS (BECCS) regarded as a promising technology. However, BECCS will likely be more costly and less efficient at power generation than conventional CCS. Thus, approaches to improve BECCS performance and reduce costs are of importance to facilitate the deployment of this key technology. In this study, the impact of biomass co-firing rate and biomass moisture content on BECCS efficiency with both post- and oxy-combustion CO 2 capture technologies was evaluated. It was found that post-combustion capture BECCS (PCC-BECCS) facilities will be appreciably less efficient than oxy-combustion capture BECCS (OCC-BECCS) facilities. Consequently, PCC-BECCS have the potential to be more carbon negative than OCC-BECCS per unit electricity generated. It was further observed that the biomass moisture content plays an important role in determining the BECCS facilities' efficiency. This will in turn affect the enthalpic content of the BECCS plant exhaust and implies that exhaust gas heat recovery may be an attractive option at higher rates of co-firing. It was found that there is the potential for the recovery of approximately 2.5 GJ heat per t CO 2 at a temperature of 100 °C from both PCC-BECCS and OCC-BECCS. On- and off-site applications for this recovered heat are discussed, considering boiler feedwater pre-heating, solvent regeneration and district heating cases.

CO₂ carbonation under aqueous conditions using petroleum coke combustion fly ash.

PubMed

González, A; Moreno, N; Navia, R

2014-12-01

Fly ash from petroleum coke combustion was evaluated for CO2 capture in aqueous medium. Moreover the carbonation efficiency based on different methodologies and the kinetic parameters of the process were determined. The results show that petroleum coke fly ash achieved a CO2 capture yield of 21% at the experimental conditions of 12 g L(-1), 363°K without stirring. The carbonation efficiency by petroleum coke fly ash based on reactive calcium species was within carbonation efficiencies reported by several authors. In addition, carbonation by petroleum coke fly ash follows a pseudo-second order kinetic model. Copyright © 2014 Elsevier Ltd. All rights reserved.

Coordination effect-regulated CO2 capture with an alkali metal onium salts/crown ether system

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yang, Zhen-Zhen; Jiang, Deen; Zhu, Xiang

2014-01-01

A coordination effect was employed to realize equimolar CO2 absorption, adopting easily synthesized amino group containing absorbents (alkali metal onium salts). The essence of our strategy was to increase the steric hindrance of cations so as to enhance a carbamic acid pathway for CO2 capture. Our easily synthesized alkali metal amino acid salts or phenolates were coordinated with crown ethers, in which highly sterically hindered cations were obtained through a strong coordination effect of crown ethers with alkali metal cations. For example, a CO2 capacity of 0.99 was attained by potassium prolinate/18-crown-6, being characterized by NMR, FT-IR, and quantum chemistrymore » calculations to go through a carbamic acid formation pathway. The captured CO2 can be stripped under very mild conditions (50 degrees C, N-2). Thus, this protocol offers an alternative for the development of technological innovation towards efficient and low energy processes for carbon capture and sequestration.« less

Ultralow Parasitic Energy for Postcombustion CO 2 Capture Realized in a Nickel Isonicotinate Metal–Organic Framework with Excellent Moisture Stability

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nandi, Shyamapada; Collins, Sean; Chakraborty, Debanjan

2017-01-25

Metal-organic frameworks (MOFs) have attracted significant attention as solid sorbents in gas separation processes for low-energy postcombustion CO 2 capture. The parasitic energy (PE) has been put forward as a holistic parameter that measures how energy efficient (and therefore cost-effective) the CO 2 capture process will be using the material. In this work, we present a nickel isonicotinate based ultramicroporous MOF, 1 [Ni-(4PyC)(2)center dot DMF], that has the lowest PE for postcombustion CO, capture reported to date. We calculate a PE of 655 kJ/kg CO 2, which is lower than that of the best performing material previously reported, Mg-MOF-74. Further,more » 1 exhibits exceptional hydrolytic stability with the CO 2 adsorption isotherm being unchanged following 7 days of steam-treatment (>85% RH) or 6 months of exposure to the atmosphere. The diffusion coefficient of CO 2 in 1 is also 2 orders of magnitude higher than in zeolites currently used in industrial scrubbers. Breakthrough experiments show that 1 only loses 7% of its maximum CO 2 capacity under humid conditions.« less

CO2 capture by ionic liquids - an answer to anthropogenic CO2 emissions?

PubMed

Sanglard, Pauline; Vorlet, Olivier; Marti, Roger; Naef, Olivier; Vanoli, Ennio

2013-01-01

Ionic liquids (ILs) are efficient solvents for the selective removal of CO2 from flue gas. Conventional, offthe-shelf ILs are limited in use to physisorption, which restricts their absorption capacity. After adding a chemical functionality like amines or alcohols, absorption of CO2 occurs mainly by chemisorption. This greatly enhances CO2 absorption and makes ILs suitable for potential industrial applications. By carefully choosing the anion and the cation of the IL, equimolar absorption of CO2 is possible. This paper reviews the current state of the art of CO2 capture by ILs and presents the current research in this field performed at the ChemTech Institute of the Ecole d'Ingénieurs et d'Architectes de Fribourg.

High-Surface-Area CO2 Sponge: High Performance CO2 Scrubbing Based on Hollow Fiber-Supported Designer Ionic Liquid Sponges

DOE Office of Scientific and Technical Information (OSTI.GOV)

None

IMPACCT Project: The team from ORNL and Georgia Tech is developing a new technology that will act like a sponge, integrating a new, alcohol-based ionic liquid into hollow fibers (magnified image, right) to capture CO2 from the exhaust produced by coal-fired power plants. Ionic liquids, or salts that exist in liquid form, are promising materials for carbon capture and storage, but their tendency to thicken when combined with CO2 limits their efficiency and poses a challenge for their development as a cost-effective alternative to current-generation solutions. Adding alcohol to the mix limits this tendency to thicken in the presence ofmore » CO2 but can also make the liquid more likely to evaporate, which would add significantly to the cost of CO2 capture. To solve this problem, ORNL is developing new classes of ionic liquids with high capacity for absorbing CO2. ORNL’s sponge would reduce the cost associated with the energy that would need to be diverted from power plants to capture CO2 and release it for storage.« less

Synthesis of highly efficient CaO-based, self-stabilizing CO2 sorbents via structure-reforming of steel slag.

PubMed

Tian, Sicong; Jiang, Jianguo; Yan, Feng; Li, Kaimin; Chen, Xuejing

2015-06-16

Capturing anthropogenic CO2 in a cost-effective and highly efficient manner is one of the most challenging issues faced by scientists today. Herein, we report a novel structure-reforming approach to convert steel slag, a cheap, abundant, and nontoxic calcium-rich industrial waste, as the only feedstock into superior CaO-based, self-stabilizing CO2 sorbents. The CO2 capture capacity of all the steel slag-derived sorbents was improved more than 10-fold compared to the raw slag, with the maximum uptake of CO2 achieving at 0.50 gCO2 gsorbent(-1). Additionally, the initial steel slag-derived sorbent could retain 0.25 gCO2 gsorbent(-1), that is, a decay rate of only 12% over 30 carbonation-calcination cycles, the excellent self-stabilizing property allowed it to significantly outperform conventional CaO, and match with most of the existing synthetic CaO-based sorbents. A synergistic effect that facilitated CO2 capture by CaO-based sorbents was clearly recognized when Mg and Al, the most common elements in steel slag, coexisted with CaO in the forms of MgO and Al2O3, respectively. During the calcium looping process, MgO served as a well spacer to increase the porosity of sorbents together with Al2O3 serving as a durable stabilizer to coresist the sintering of CaCO3 grains at high temperatures.

Metal-Organic Frameworks as Potential Platforms for Carbon Dioxide Capture and Chemical Transformation

NASA Astrophysics Data System (ADS)

Gao, Wenyang

The anthropogenic carbon dioxide (CO2) emission into the atmosphere, mainly through the combustion of fossil fuels, has resulted in a balance disturbance of the carbon cycle. Overwhelming scientific evidence proves that the escalating level of atmospheric CO2 is deemed as the main culprit for global warming and climate change. It is thus imperative to develop viable CO2 capture and sequestration (CCS) technologies to reduce CO2 emissions, which is also essential to avoid the potential devastating effects in future. The drawbacks of energy-cost, corrosion and inefficiency for amine-based wet-scrubbing systems which are currently used in industry, have prompted the exploration of alternative approaches for CCS. Extensive efforts have been dedicated to the development of functional porous materials, such as activated carbons, zeolites, porous organic polymers, and metal-organic frameworks (MOFs) to capture CO2. However, these adsorbents are limited by either poor selectivity for CO2 separation from gas mixtures or low CO2 adsorption capacity. Therefore, it is still highly demanding to design next-generation adsorbent materials fulfilling the requirements of high CO2 selectivity and enough CO2 capacity, as well as high water/moisture stability under practical conditions. Metal-organic frameworks (MOFs) have been positioned at the forefront of this area as a promising type of candidate amongst various porous materials. This is triggered by the modularity and functionality of pore size, pore walls and inner surface of MOFs by use of crystal engineering approaches. In this work, several effective strategies, such as incorporating 1,2,3-triazole groups as moderate Lewis base centers into MOFs and employing flexible azamacrocycle-based ligands to build MOFs, demonstrate to be promising ways to enhance CO 2 uptake capacity and CO2 separation ability of porous MOFs. It is revealed through in-depth studies on counter-intuitive experimental observations that the local electric field favours more than the richness of exposed nitrogen atoms for the interactions between MOFs and CO2 molecules, which provides a new perspective for future design of new MOFs and other types of porous materials for CO2 capture. Meanwhile, to address the water/moisture stability issue of MOFs, remote stabilization of copper paddlewheel clusters is achieved by strengthening the bonding between organic ligands and triangular inorganic copper trimers, which in turn enhances the stability of the whole MOF network and provides a better understanding of the mechanism promoting prospective suitable MOFs with enhanced water stability. In contrast with CO2 capture by sorbent materials, the chemical transformation of the captured CO2 into value-added products represents an alternative which is attractive and sustainable, and has been of escalating interest. The nanospace within MOFs not only provides the inner porosity for CO2 capture, but also engenders accessible room for substrate molecules for catalytic purpose. It is demonstrated that high catalytic efficiency for chemical fixation of CO2 into cyclic carbonates under ambient conditions is achieved on MOF-based nanoreactors featuring a high-density of well-oriented Lewis active sites. Furthermore, described for the first time is that CO 2 can be successfully inserted into aryl C-H bonds of a MOF to generate carboxylate groups. This proof-of-concept study contributes a different perspective to the current landscape of CO2 capture and transformation. In closing, the overarching goal of this work is not only to seek efficient MOF adsorbents for CO2 capture, but also to present a new yet attractive scenario of CO2 utilization on MOF platforms.

Development of Novel Carbon Sorbents for CO{sub 2} Capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Krishnan, Gopala; Hornbostel, Marc; Bao, Jianer

2013-11-30

An innovative, low-cost, and low-energy-consuming carbon dioxide (CO{sub 2}) capture technology was developed, based on CO{sub 2}adsorption on a high-capacity and durable carbon sorbent. This report describes the (1) performance of the concept on a bench-scale system; (2) results of parametric tests to determine the optimum operating conditions; (3) results of the testing with a flue gas from coal-fired boilers; and (4) evaluation of the technical and economic viability of the technology. The process uses a falling bed of carbon sorbent microbeads to separate the flue gas into two streams: a CO{sub 2} -lean flue gas stream from which >more » 90% of the CP{sub 2} is removed and a pure stream of CO{sub 2} that is ready for compression and sequestration. The carbo sorbent microbeads have several unique properties such as high CO{sub 2} capacity, low heat of adsorption and desorption (25 to 28 kJ/mole), mechanically robust, and rapid adsorption and desorption rates. The capture of CO{sub 2} from the flue gas is performed at near ambient temperatures in whic the sorbent microbeads flow down by gravity counter-current with the up-flow of the flue gas. The adsorbed CO{sub 2} is stripped by heating the CO{sub 2}-loaded sorbent to - 100°C, in contact with low-pressure (- 5 psig) steam in a section at the bottom of the adsorber. The regenerated sorben is dehydrated of adsorbed moisture, cooled, and lifted back to the adsorber. The CO{sub 2} from the desorber is essentially pure and can be dehydrated, compressed, and transported to a sequestration site. Bench-scale tests using a simulated flue gas showed that the integrated system can be operated to provide > 90% CO{sub 2} capture from a 15% CO{sub 2} stream in the adsorber and produce > 98% CO{sub 2} at the outlet of the stripper. Long-term tests ( 1,000 cycles) showed that the system can be operated reliably without sorbent agglomeration or attrition. The bench-scale reactor was also operated using a flue gas stream from a coal-fired boil at the University of Toledo campus for about 135 h, comprising 7,000 cycles of adsorption and desorption using the desulfurized flue gas that contained only 4.5% v/v CO{sub 2}. A capture efficiency of 85 to 95% CO{sub 2} was achieved under steady-state conditi ons. The CO{sub 2} adsorption capacity did not change significantly during the field test, as determined from the CO{sub 2} adsorptio isotherms of fresh and used sorbents. The process is also being tested using the flue gas from a PC-fired power plant at the National Carbon Capture Center (NCCC), Wilsonville, AL. The cost of electricity was calculated for CO{sub 2} capture using the carbon sorbent and compared with the no-CO{sub 2} capture and CO{sub 2} capture with an amine-based system. The increase i the levelized cost of electricity (L-COE) is about 37% for CO{sub 2} capture using the carbon sorbent in comparison to 80% for an amine-based system, demonstrating the economic advantage of C capture using the carbon sorbent. The 37% increase in the L-COE corresponds to a cost of capture of $30/ton of CO{sub 2}, including compression costs, capital cost for the capture system, and increased plant operating and capital costs to make up for reduced plant efficiency. Preliminary sensitivity analyses showed capital costs, pressure drops in the adsorber, and steam requirement for the regenerator are the major variables in determining the cost of CO{sub 2} capture. The results indicate that further long-term testing with a flue gas from a pulverized coal­ fired boiler should be performed to obtain additional data relating to the effects of flue gas contaminants, the ability to reduce pressure drop by using alternate structural packing , and the use of low-cost construction materials.« less

Sorbents with high efficiency for CO2 capture based on amines-supported carbon for biogas upgrading.

PubMed

Pino, Lidia; Italiano, Cristina; Vita, Antonio; Fabiano, Concetto; Recupero, Vincenzo

2016-10-01

Sorbents for CO 2 capture have been prepared by wet impregnation of a commercial active carbon (Ketjen-black, Akzo Nobel) with two CO 2 -philic compounds, polyethylenimine (PEI) and tetraethylenepentamine (TEPA), respectively. The effects of amine amount (from 10 to 70wt.%), CO 2 concentration in the feed, sorption temperature and gas hourly space velocity on the CO 2 capture performance have been investigated. The sorption capacity has been evaluated using the breakthrough method, with a fixed bed reactor equipped with on line gas chromatograph. The samples have been characterized by N 2 adsorption-desorption, scanning electron microscopy and energy dispersive X-ray (SEM/EDX). A promising CO 2 sorption capacity of 6.90 mmol/g sorbent has been obtained with 70wt.% of supported TEPA at 70°C under a stream containing 80vol% of CO 2 . Sorption tests, carried out with simulated biogas compositions (CH 4 /CO 2 mixtures), have revealed an appreciable CO 2 separation selectivity; stable performance was maintained for 20 adsorption-desorption cycles. Copyright © 2016. Published by Elsevier B.V.

Design of Aminopolymer Structure to Enhance Performance and Stability of CO2 Sorbents: Poly(propylenimine) vs Poly(ethylenimine).

PubMed

Pang, Simon H; Lee, Li-Chen; Sakwa-Novak, Miles A; Lively, Ryan P; Jones, Christopher W

2017-03-15

Studies on aminopolymer/oxide composite materials for direct CO 2 capture from air have often focused on the prototypical poly(ethylenimine) (PEI) as the aminopolymer. However, it is known that PEI will oxidatively degrade at elevated temperatures. This degradation has been ascribed to the presence of secondary amines, which, when oxidized, lose their CO 2 capture capacity. Here, we demonstrate the use of small molecule poly(propylenimine) (PPI) in linear and dendritic architectures supported in silica as adsorbent materials for direct CO 2 capture from air. Regardless of amine loading or aminopolymer architecture, the PPI-based sorbents are found to be more efficient for CO 2 capture than PEI-based sorbents. Moreover, PPI is found to be more resistant to oxidative degradation than PEI, even while containing secondary amines, as supported by FTIR, NMR, and ESI-MS studies. These results suggest that PPI-based CO 2 sorbents may allow for longer sorbent working lifetimes due to an increased tolerance to sorbent regeneration conditions and suggest that the presence of secondary amines may not mean that all aminopolymers will oxidatively degrade.

Atmospheric CO2 capture for the artificial photosynthetic system

NASA Astrophysics Data System (ADS)

Nogalska, Adrianna; Zukowska, Adrianna; Garcia-Valls, Ricard

2017-11-01

The scope of these studies is to evaluate the ambient CO2 capture abilities of the membrane contactor system in the same conditions as leaves works during photosynthesis, such as ambient temperature, pressure and low CO2 concentration, where the only driving force is the concentration gradient. The polysulfone membrane was made by phase inversion process and characterized by ESEM micrographs which were used to determine the thickness, asymmetry and pore size. Besides, the porosity of the membrane was measured from the membrane and polysulfone density correlation and hydrophobicity was analyzed by contact angle measurements. Moreover, the compatibility of the membrane and absorbent solution was evaluated, in order to exclude wetting issues. The prepared membranes were introduced in a cross flow module and used as contactor between the CO2 and the potassium hydroxide solution, as absorbing media. The influence of the membrane thickness, absorbent stirring rate and absorption time, on CO2 capture were evaluated. The results show that the efficiency of our CO2 capture system is similar to stomatal carbon dioxide assimilation rate.

Pilot testing of a membrane system for postcombustion CO 2 capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Merkel, Tim; Kniep, Jay; Wei, Xiaotong

2015-09-30

This final report summarizes work conducted for the U.S. Department of Energy, National Energy Technology Laboratory (DOE) to scale up an efficient post-combustion CO 2 capture membrane process to the small pilot test stage (award number DE-FE0005795). The primary goal of this research program was to design, fabricate, and operate a membrane CO 2 capture system to treat coal-derived flue gas containing 20 tonnes CO 2/day (20 TPD). Membrane Technology and Research (MTR) conducted this project in collaboration with Babcock and Wilcox (B&W), the Electric Power Research Institute (EPRI), WorleyParsons (WP), the Illinois Sustainable Technology Center (ISTC), Enerkem (EK), andmore » the National Carbon Capture Center (NCCC). In addition to the small pilot design, build and slipstream testing at NCCC, other project efforts included laboratory membrane and module development at MTR, validation field testing on a 1 TPD membrane system at NCCC, boiler modeling and testing at B&W, a techno-economic analysis (TEA) by EPRI/WP, a case study of the membrane technology applied to a ~20 MWe power plant by ISTC, and an industrial CO 2 capture test at an Enerkem waste-to-biofuel facility. The 20 TPD small pilot membrane system built in this project successfully completed over 1,000 hours of operation treating flue gas at NCCC. The Polaris™ membranes used on this system demonstrated stable performance, and when combined with over 10,000 hours of operation at NCCC on a 1 TPD system, the risk associated with uncertainty in the durability of postcombustion capture membranes has been greatly reduced. Moreover, next-generation Polaris membranes with higher performance and lower cost were validation tested on the 1 TPD system. The 20 TPD system also demonstrated successful operation of a new low-pressure-drop sweep module that will reduce parasitic energy losses at full scale by as much as 10 MWe. In modeling and pilot boiler testing, B&W confirmed the viability of CO 2 recycle to the boiler as envisioned in the MTR process design. The impact of this CO 2 recycle on boiler efficiency was quantified and incorporated into a TEA of the membrane capture process applied to a full-scale power plant. As with previous studies, the TEA showed the membrane process to be lower cost than the conventional solvent capture process even at 90% CO 2capture. A sensitivity study indicates that the membrane capture cost decreases significantly if the 90% capture requirement is relaxed. Depending on the process design, a minimum capture cost is achieved at 30-60% capture, values that would meet proposed CO 2 emission regulations for coal-fired power plants. In summary, this project has successfully advanced the MTR membrane capture process through small pilot testing (technology readiness level 6). The technology is ready for future scale-up to the 10 MWe size.« less

Ability of an alkali-tolerant mutant strain of the microalga Chlorella sp. AT1 to capture carbon dioxide for increasing carbon dioxide utilization efficiency.

PubMed

Kuo, Chiu-Mei; Lin, Tsung-Hsien; Yang, Yi-Chun; Zhang, Wen-Xin; Lai, Jinn-Tsyy; Wu, Hsi-Tien; Chang, Jo-Shu; Lin, Chih-Sheng

2017-11-01

An alkali-tolerant Chlorella sp. AT1 mutant strain was screened by NTG mutagenesis. The strain grew well in pH 6-11 media, and the optimal pH for growth was 10. The CO 2 utilization efficiencies of Chlorella sp. AT1 cultured with intermittent 10% CO 2 aeration for 10, 20 and 30min at 3-h intervals were approximately 80, 42 and 30%, respectively. In alkaline medium (pH=11) with intermittent 10% CO 2 aeration for 30min at 3-, 6- and 12-h intervals, the medium pH gradually changed to 10, and the biomass productivities of Chlorella sp. AT1 were 0.987, 0.848 and 0.710gL -1 d -1 , respectively. When Chlorella sp. AT1 was aerated with 10% CO 2 intermittently for 30min at 3-h intervals in semi-continuous cultivation for 21days, the biomass concentration and biomass productivity were 4.35gL -1 and 0.726gL -1 d -1 , respectively. Our results show that CO 2 utilization efficiency can be markedly increased by intermittent CO 2 aeration and alkaline media as a CO 2 -capturing strategy for alkali-tolerant microalga cultivation. Copyright © 2017 Elsevier Ltd. All rights reserved.

High-efficiency power production from natural gas with carbon capture

NASA Astrophysics Data System (ADS)

Adams, Thomas A.; Barton, Paul I.

A unique electricity generation process uses natural gas and solid oxide fuel cells at high electrical efficiency (74%HHV) and zero atmospheric emissions. The process contains a steam reformer heat-integrated with the fuel cells to provide the heat necessary for reforming. The fuel cells are powered with H 2 and avoid carbon deposition issues. 100% CO 2 capture is achieved downstream of the fuel cells with very little energy penalty using a multi-stage flash cascade process, where high-purity water is produced as a side product. Alternative reforming techniques such as CO 2 reforming, autothermal reforming, and partial oxidation are considered. The capital and energy costs of the proposed process are considered to determine the levelized cost of electricity, which is low when compared to other similar carbon capture-enabled processes.

Membrane thinning for efficient CO2 capture

PubMed Central

Selyanchyn, Roman; Fujikawa, Shigenori

2017-01-01

Abstract Enhancing the fluxes in gas separation membranes is required for utilizing the membranes on a mass scale for CO2 capture. Membrane thinning is one of the most promising approaches to achieve high fluxes. In addition, sophisticated molecular transport across membranes can boost gas separation performance. In this review, we attempt to summarize the current state of CO2 separation membranes, especially from the viewpoint of thinning the selective layers and the membrane itself. The gas permeation behavior of membranes with ultimate thicknesses and their future directions are discussed. PMID:29152016

DOE Office of Scientific and Technical Information (OSTI.GOV)

Basha, Omar M.; Keller, Murphy J.; Luebke, David R.

The Ionic Liquid (IL) [hmim][Tf 2N] was used as a physical solvent in an Aspen Plus simulation, employing the Peng-Robinson Equation of State (P-R EOS) with Boston-Mathias (BM) alpha function and standard mixing rules, to develop a conceptual process for CO 2 capture from a shifted warm fuel gas stream produced from Pittsburgh # 8 coal for a 400 MWe power plant. The physical properties of the IL, including density, viscosity, surface tension, vapor pressure and heat capacity were obtained from literature and modeled as a function of temperature. Also, available experimental solubility values for CO 2, H 2, Hmore » 2S, CO, and CH 4 in this IL were compiled and their binary interaction parameters (Δ ij and l ij) were optimized and correlated as functions of temperature. The Span-Wager Equation-of-State EOS was also employed to generate CO 2 solubilities in [hmim][Tf 2N] at high pressures (up to 10 MPa) and temperatures (up to 510 K). The conceptual process developed consisted of 4 adiabatic absorbers (2.4 m ID, 30 m high) arranged in parallel and packed with Plastic Pall Rings of 0.025 m for CO 2 capture; 3 flash drums arranged in series for solvent (IL) regeneration with the pressure-swing option; and a pressure-intercooling system for separating and pumping CO 2 up to 153 bar to the sequestration sites. The compositions of all process streams, CO 2 capture efficiency, and net power were calculated using Aspen Plus simulator. The results showed that, based on the composition of the inlet gas stream to the absorbers, 95.67 mol% of CO 2 was captured and sent to sequestration sites; 99.5 mol% of H 2 was separated and sent to turbines; the solvent exhibited a minimum loss of 0.31 mol%; and the net power balance of the entire system was 30.81 MW. These results indicated that [hmim][Tf 2N] IL could be used as a physical solvent for CO 2 capture from warm shifted fuel gas streams with high efficiency.« less

Integration of CO2 Capture and Mineral Carbonation by Using Recyclable Ammonium Salts

PubMed Central

Wang, Xiaolong; Maroto-Valer, M Mercedes

2011-01-01

A new approach to capture and store CO2 by mineral carbonation using recyclable ammonium salts was studied. This process integrates CO2 capture with mineral carbonation by employing NH3, NH4HSO4, and NH4HCO3 in the capture, mineral dissolution, and carbonation steps, respectively. NH4HSO4 and NH3 can then be regenerated by thermal decomposition of (NH4)2SO4. The use of NH4HCO3 as the source of CO2 can avoid desorption and compression of CO2. The mass ratio of Mg/NH4HCO3/NH3 is the key factor controlling carbonation and the optimum ratio of 1:4:2 gives a conversion of Mg ions to hydromagnesite of 95.5 %. Thermogravimetric analysis studies indicated that the regeneration efficiency of NH4HSO4 and NH3 in this process is 95 %. The mass balance of the process shows that about 2.63 tonnes of serpentine, 0.12 tonnes of NH4HSO4, 7.48 tonnes of NH4HCO3, and 0.04 tonnes of NH3 are required to sequester 1 tonne of CO2 as hydromagnesite. PMID:21732542

Efficient solar-driven synthesis, carbon capture, and desalinization, STEP: solar thermal electrochemical production of fuels, metals, bleach.

PubMed

Licht, S

2011-12-15

STEP (solar thermal electrochemical production) theory is derived and experimentally verified for the electrosynthesis of energetic molecules at solar energy efficiency greater than any photovoltaic conversion efficiency. In STEP the efficient formation of metals, fuels, chlorine, and carbon capture is driven by solar thermal heated endothermic electrolyses of concentrated reactants occuring at a voltage below that of the room temperature energy stored in the products. One example is CO(2) , which is reduced to either fuels or storable carbon at a solar efficiency of over 50% due to a synergy of efficient solar thermal absorption and electrochemical conversion at high temperature and reactant concentration. CO(2) -free production of iron by STEP, from iron ore, occurs via Fe(III) in molten carbonate. Water is efficiently split to hydrogen by molten hydroxide electrolysis, and chlorine, sodium, and magnesium from molten chlorides. A pathway is provided for the STEP decrease of atmospheric carbon dioxide levels to pre-industial age levels in 10 years. Copyright © 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Subtask 2.18 - Advancing CO 2 Capture Technology: Partnership for CO 2 Capture (PCO 2C) Phase III

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kay, John; Azenkeng, Alexander; Fiala, Nathan

2016-03-31

Industries and utilities continue to investigate ways to decrease their carbon footprint. Carbon capture and storage (CCS) can enable existing power generation facilities to meet the current national CO 2 reduction goals. The Partnership for CO2 Capture Phase III focused on several important research areas in an effort to find ways to decrease the cost of capture across both precombustion and postcombustion platforms. Two flue gas pretreatment technologies for postcombustion capture, an SO 2 reduction scrubbing technology from Cansolv Technologies Inc. and the Tri-Mer filtration technology that combines particulate, NOx, and SO 2 control, were evaluated on the Energy &more » Environmental Research Center’s (EERC’s) pilot-scale test system. Pretreating the flue gas should enable more efficient, and therefore less expensive, CO 2 capture. Both technologies were found to be effective in pretreating flue gas prior to CO 2 capture. Two new postcombustion capture solvents were tested, one from the Korea Carbon Capture and Sequestration R&D Center (KCRC) and one from CO 2 Solutions Incorporated. Both of these solvents showed the ability to capture CO 2 while requiring less regeneration energy, which would reduce the cost of capture. Hydrogen separation membranes from Commonwealth Scientific and Industrial Research Organisation were evaluated through precombustion testing. They are composed of vanadium alloy, which is less expensive than the palladium alloys that are typically used. Their performance was comparable to that of other membranes that have been tested at the EERC. Aspen Plus® software was used to model the KCRC and CO 2 Solutions solvents and found that they would result in significantly improved overall plant performance. The modeling effort also showed that the parasitic steam load at partial capture of 45% is less than half that of 90% overall capture, indicating savings that could be accrued if 90% capture is not required. Modeling of three regional power plants using the Carnegie Mellon Integrated Environmental Control Model showed that, among other things, the use of a bypass during partial capture may minimize the size of the capture tower(s) and result in a slight reduction in the revenue required to operate the capture facility. The results reinforced that a one-size-fits-all approach cannot be taken to adding capture to a power plant. Laboratory testing indicated that Fourier transform infrared spectroscopy could be used to continuously sample stack emissions at CO 2 capture facilities to detect and quantify any residual amine or its degradation products, particularly nitrosamines. The information gathered during Phase III is important for utility stakeholders as they determine how to reduce their CO 2 emissions in a carbon-constrained world. This subtask was funded through the EERC–U.S. Department of Energy (DOE) Joint Program on Research and Development for Fossil Energy-Related Resources Cooperative Agreement No. DE-FC26-08NT43291. Nonfederal funding was provided by the North Dakota Industrial Commission, PPL Montana, Nebraska Public Power District, Tri-Mer Corporation, Montana–Dakota Utilities Co., Basin Electric Power Cooperative, KCRC/Korean Institute of Energy Research, Cansolv Technologies, and CO 2 Solutions, Inc.« less

CO2 capture by means of an enzyme-based reactor

NASA Technical Reports Server (NTRS)

Cowan, R. M.; Ge, J-J; Qin, Y-J; McGregor, M. L.; Trachtenberg, M. C.

2003-01-01

We report a means for efficient and selective extraction of carbon dioxide (CO(2)) at low to medium concentration from mixed gas streams. CO(2) capture was accomplished by use of a novel enzyme-based, facilitated transport contained liquid membrane (EBCLM) reactor. The parametric studies we report explore both structural and operational parameters of this design. The structural parameters include carbonic anhydrase (CA) concentration, buffer concentration and pH, and liquid membrane thickness. The operational parameters are temperature, humidity of the inlet gas stream, and CO(2) concentration in the feed stream. The data show that this system effectively captures CO(2) over the range 400 ppm to at least 100,000 ppm, at or around ambient temperature and pressure. In a single pass across this homogeneous catalyst design, given a feed of 0.1% CO(2), the selectivity of CO(2) versus N(2) is 1,090 : 1 and CO(2) versus O(2) is 790 :1. CO(2) permeance is 4.71 x 10(-8) molm(-2) Pa(-1) sec(-1). The CLM design results in a system that is very stable even in the presence of dry feed and sweep gases.

Near-Zero Emissions Oxy-Combustion Flue Gas Purification

DOE Office of Scientific and Technical Information (OSTI.GOV)

Minish Shah; Nich Degenstein; Monica Zanfir

2012-06-30

The objectives of this project were to carry out an experimental program to enable development and design of near zero emissions (NZE) CO{sub 2} processing unit (CPU) for oxy-combustion plants burning high and low sulfur coals and to perform commercial viability assessment. The NZE CPU was proposed to produce high purity CO{sub 2} from the oxycombustion flue gas, to achieve > 95% CO{sub 2} capture rate and to achieve near zero atmospheric emissions of criteria pollutants. Two SOx/NOx removal technologies were proposed depending on the SOx levels in the flue gas. The activated carbon process was proposed for power plantsmore » burning low sulfur coal and the sulfuric acid process was proposed for power plants burning high sulfur coal. For plants burning high sulfur coal, the sulfuric acid process would convert SOx and NOx in to commercial grade sulfuric and nitric acid by-products, thus reducing operating costs associated with SOx/NOx removal. For plants burning low sulfur coal, investment in separate FGD and SCR equipment for producing high purity CO{sub 2} would not be needed. To achieve high CO{sub 2} capture rates, a hybrid process that combines cold box and VPSA (vacuum pressure swing adsorption) was proposed. In the proposed hybrid process, up to 90% of CO{sub 2} in the cold box vent stream would be recovered by CO{sub 2} VPSA and then it would be recycled and mixed with the flue gas stream upstream of the compressor. The overall recovery from the process will be > 95%. The activated carbon process was able to achieve simultaneous SOx and NOx removal in a single step. The removal efficiencies were >99.9% for SOx and >98% for NOx, thus exceeding the performance targets of >99% and >95%, respectively. The process was also found to be suitable for power plants burning both low and high sulfur coals. Sulfuric acid process did not meet the performance expectations. Although it could achieve high SOx (>99%) and NOx (>90%) removal efficiencies, it could not produce by-product sulfuric and nitric acids that meet the commercial product specifications. The sulfuric acid will have to be disposed of by neutralization, thus lowering the value of the technology to same level as that of the activated carbon process. Therefore, it was decided to discontinue any further efforts on sulfuric acid process. Because of encouraging results on the activated carbon process, it was decided to add a new subtask on testing this process in a dual bed continuous unit. A 40 days long continuous operation test confirmed the excellent SOx/NOx removal efficiencies achieved in the batch operation. This test also indicated the need for further efforts on optimization of adsorption-regeneration cycle to maintain long term activity of activated carbon material at a higher level. The VPSA process was tested in a pilot unit. It achieved CO{sub 2} recovery of > 95% and CO{sub 2} purity of >80% (by vol.) from simulated cold box feed streams. The overall CO{sub 2} recovery from the cold box VPSA hybrid process was projected to be >99% for plants with low air ingress (2%) and >97% for plants with high air ingress (10%). Economic analysis was performed to assess value of the NZE CPU. The advantage of NZE CPU over conventional CPU is only apparent when CO{sub 2} capture and avoided costs are compared. For greenfield plants, cost of avoided CO{sub 2} and cost of captured CO{sub 2} are generally about 11-14% lower using the NZE CPU compared to using a conventional CPU. For older plants with high air intrusion, the cost of avoided CO{sub 2} and capture CO{sub 2} are about 18-24% lower using the NZE CPU. Lower capture costs for NZE CPU are due to lower capital investment in FGD/SCR and higher CO{sub 2} capture efficiency. In summary, as a result of this project, we now have developed one technology option for NZE CPU based on the activated carbon process and coldbox-VPSA hybrid process. This technology is projected to work for both low and high sulfur coal plants. The NZE CPU technology is projected to achieve near zero stack emissions, produce high purity CO{sub 2} relatively free of trace impurities and achieve ~99% CO{sub 2} capture rate while lowering the CO{sub 2} capture costs.« less

Enabling CCS via Low-temperature Geothermal Energy Integration for Fossil-fired Power Generation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Davidson, Casie L.; Heldebrant, D. J.; Bearden, M. D.

Here, among the key barriers to commercial scale deployment is the cost associated with CO 2 capture. This is particularly true for existing large, fossil-fired assets that account for a large fraction of the electricity generation fleet in developed nations, including the U.S. Fitting conventional combustion technologies with CO 2 capture systems can carry an energy penalty of thirty percent or more, resulting in an increased price of power to the grid, as well as an overall decrease in net plant output. Taken together with the positive growth in demand for electricity, this implies a need for accelerated capital build-outmore » in the power generation markets to accommodate both demand growth and decreased output at retrofitted plants. In this paper, the authors present the results of a study to assess the potential to use geothermal energy to provide boiler feedwater preheating, capturing efficiency improvements designed to offset the losses associated with CO 2 capture. Based on NETL benchmark cases and subsequent analysis of the application using site-specific data from the North Valmy power plant, several cases for CO 2 capture were evaluated. These included geothermally assisted MEA capture, CO2BOLs capture, and stand-alone hybrid power generation, compared with a baseline, no-geothermal case. Based on Case 10, and assuming 2.7 MMlb/h of geothermally sourced 150 ºC water, the parasitic power load associated with MEA capture could be offset by roughly seven percent, resulting in a small (~1 percent) overall loss to net power generation, but at levelized costs of electricity similar to the no-geothermal CCS case. For the CO 2BOLs case, the availability of 150°C geothermal fluid could allow the facility to not only offset the net power decrease associated with CO 2BOLs capture alone, but could increase nameplate capacity by two percent. The geothermally coupled CO 2BOLs case also decreases LCOE by 0.75 ¢/kWh relative to the non-hybrid CO 2BOLs case, with the improved performance over the MEA case driven by the lower regeneration temperature and associated duty for CO 2BOLs relative to MEA.« less

Enabling CCS via Low-temperature Geothermal Energy Integration for Fossil-fired Power Generation

DOE PAGES

Davidson, Casie L.; Heldebrant, D. J.; Bearden, M. D.; ...

2017-08-18

Here, among the key barriers to commercial scale deployment is the cost associated with CO 2 capture. This is particularly true for existing large, fossil-fired assets that account for a large fraction of the electricity generation fleet in developed nations, including the U.S. Fitting conventional combustion technologies with CO 2 capture systems can carry an energy penalty of thirty percent or more, resulting in an increased price of power to the grid, as well as an overall decrease in net plant output. Taken together with the positive growth in demand for electricity, this implies a need for accelerated capital build-outmore » in the power generation markets to accommodate both demand growth and decreased output at retrofitted plants. In this paper, the authors present the results of a study to assess the potential to use geothermal energy to provide boiler feedwater preheating, capturing efficiency improvements designed to offset the losses associated with CO 2 capture. Based on NETL benchmark cases and subsequent analysis of the application using site-specific data from the North Valmy power plant, several cases for CO 2 capture were evaluated. These included geothermally assisted MEA capture, CO2BOLs capture, and stand-alone hybrid power generation, compared with a baseline, no-geothermal case. Based on Case 10, and assuming 2.7 MMlb/h of geothermally sourced 150 ºC water, the parasitic power load associated with MEA capture could be offset by roughly seven percent, resulting in a small (~1 percent) overall loss to net power generation, but at levelized costs of electricity similar to the no-geothermal CCS case. For the CO 2BOLs case, the availability of 150°C geothermal fluid could allow the facility to not only offset the net power decrease associated with CO 2BOLs capture alone, but could increase nameplate capacity by two percent. The geothermally coupled CO 2BOLs case also decreases LCOE by 0.75 ¢/kWh relative to the non-hybrid CO 2BOLs case, with the improved performance over the MEA case driven by the lower regeneration temperature and associated duty for CO 2BOLs relative to MEA.« less

Two-dimensional nitrides as highly efficient potential candidates for CO2 capture and activation.

PubMed

Morales-Salvador, Raul; Morales-García, Ángel; Viñes, Francesc; Illas, Francesc

2018-06-13

The performance of novel two-dimensional nitrides in carbon capture and storage (CCS) is analyzed for a broad range of pressures and temperatures. Employing an integrated theoretical framework where CO2 adsorption/desorption rates on the M2N (M = Ti, Zr, Hf, V, Nb, Ta, Cr, Mo, and W) surfaces are derived from transition state theory and density functional theory based calculations, the present theoretical simulations consistently predict that, depending on the particular composition, CO2 can be strongly adsorbed and even activated at temperatures above 1000 K. For practical purposes, Ti2N, Zr2N, Hf2N, V2N, Nb2N, and Ta2N are predicted as the best suited materials for CO2 activation. Moreover, the estimated CO2 uptake of 2.32-7.96 mol CO2 kg-1 reinforces the potential of these materials for CO2 abatement.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Córdoba, Patricia, E-mail: pc247@hw.ac.uk; Maroto-Valer, M.; Delgado, Miguel Angel

The work presented here reports the first study in which the speciation, behaviour and fate of mercury (Hg) have been evaluated under oxy-fuel combustion at the largest oxy-Pulverised Coal Combustion (oxy-PCC) demonstration plant to date during routine operating conditions and partial exhaust flue gas re-circulation to the boiler. The effect of the CO{sub 2}-rich flue gas re-circulation on Hg has also been evaluated. Results reveal that oxy-PCC operational conditions play a significant role on Hg partitioning and fate because of the continuous CO{sub 2}-rich flue gas re-circulations to the boiler. Mercury escapes from the cyclone in a gaseous form asmore » Hg{sup 2+} (68%) and it is the prevalent form in the CO{sub 2}-rich exhaust flue gas (99%) with lower proportions of Hg{sup 0} (1.3%). The overall retention rate for gaseous Hg is around 12%; Hg{sup 0} is more prone to be retained (95%) while Hg{sup 2+} shows a negative efficiency capture for the whole installation. The negative Hg{sup 2+} capture efficiencies are due to the continuous CO{sub 2}-rich exhaust flue gas recirculation to the boiler with enhanced Hg contents. Calculations revealed that 44 mg of Hg were re-circulated to the boiler as a result of 2183 re-circulations of CO{sub 2}-rich flue gas. Especial attention must be paid to the role of the CO{sub 2}-rich exhaust flue gas re-circulation to the boiler on the Hg enrichment in Fly Ashes (FAs). - Highlights: • The fate of gaseous Hg has been evaluated under oxy-fuel combustion. • The Hg oxidation process is enhanced in CO{sub 2}-rich flue gas recirculation. • Hg{sup 2+} is the prevalent gas species in the CO{sub 2}-rich exhaust flue gas. • Hg{sup 2+}{sub (g)} shows a negative efficiency capture for the whole installation. • Especial attention must be paid to the Hg enrichment in Fly Ashes.« less

Efficient CO 2 capture by a task-specific porous organic polymer bifunctionalized with carbazole and triazine groups

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhu, Xiang; Mahurin, Shannon M.; An, Shu-Hao

2014-05-02

We synthesized a porous triazine and carbazole bifunctionalized task-specific polymer using a facile Friedel–Crafts reaction. We found that the resultant porous framework exhibited excellent CO 2 uptake (18.0 wt%, 273 K and 1 bar) and good adsorption selectivity for CO 2 over N 2.

Influence of high-temperature steam on the reactivity of CaO sorbent for CO₂ capture.

PubMed

Donat, Felix; Florin, Nicholas H; Anthony, Edward J; Fennell, Paul S

2012-01-17

Calcium looping is a high-temperature CO(2) capture technology applicable to the postcombustion capture of CO(2) from power station flue gas, or integrated with fuel conversion in precombustion CO(2) capture schemes. The capture technology uses solid CaO sorbent derived from natural limestone and takes advantage of the reversible reaction between CaO and CO(2) to form CaCO(3); that is, to achieve the separation of CO(2) from flue or fuel gas, and produce a pure stream of CO(2) suitable for geological storage. An important characteristic of the sorbent, affecting the cost-efficiency of this technology, is the decay in reactivity of the sorbent over multiple CO(2) capture-and-release cycles. This work reports on the influence of high-temperature steam, which will be present in flue (about 5-10%) and fuel (∼20%) gases, on the reactivity of CaO sorbent derived from four natural limestones. A significant increase in the reactivity of these sorbents was found for 30 cycles in the presence of steam (from 1-20%). Steam influences the sorbent reactivity in two ways. Steam present during calcination promotes sintering that produces a sorbent morphology with most of the pore volume associated with larger pores of ∼50 nm in diameter, and which appears to be relatively more stable than the pore structure that evolves when no steam is present. The presence of steam during carbonation reduces the diffusion resistance during carbonation. We observed a synergistic effect, i.e., the highest reactivity was observed when steam was present for both calcination and carbonation.

The Ca-looping process for CO2 capture and energy storage: role of nanoparticle technology

NASA Astrophysics Data System (ADS)

Valverde, Jose Manuel

2018-02-01

The calcium looping (CaL) process, based on the cyclic carbonation/calcination of CaO, has come into scene in the last years with a high potential to be used in large-scale technologies aimed at mitigating global warming. In the CaL process for CO2 capture, the CO2-loaded flue gas is used to fluidize a bed of CaO particles at temperatures around 650 °C. The carbonated particles are then circulated into a calciner reactor wherein the CaO solids are regenerated at temperatures near 950 °C under high CO2 concentration. Calcination at such harsh conditions causes a marked sintering and loss of reactivity of the regenerated CaO. This main drawback could be however compensated from the very low cost of natural CaO precursors such as limestone or dolomite. Another emerging application of the CaL process is thermochemical energy storage (TCES) in concentrated solar power (CSP) plants. Importantly, carbonation/calcination conditions to maximize the global CaL-CSP plant efficiency could differ radically from those used for CO2 capture. Thus, carbonation could be carried out at high temperatures under high CO2 partial pressure for maximum efficiency, whereas the solids could be calcined at relatively low temperatures in the absence of CO2 to promote calcination. Our work highlights the critical role of carbonation/calcination conditions on the performance of CaO derived from natural precursors. While conditions in the CaL process for CO2 capture lead to a severe CaO deactivation with the number of cycles, the same material may exhibit a high and stable conversion at optimum CaL-CSP conditions. Moreover, the type of CaL conditions influences critically the reaction kinetics, which plays a main role on the optimization of relevant operation parameters such as the residence time in the reactors. This paper is devoted to a brief review on the latest research activity in our group concerning these issues as well as the possible role of nanoparticle technology to enhance the activity of Ca-based materials at CaL conditions for CO2 capture and energy storage.

Application of halloysite nanotubes for carbon dioxide capture

NASA Astrophysics Data System (ADS)

Kim, Jinsoo; Rubino, Ilaria; Lee, Joo-Youp; Choi, Hyo-Jick

2016-04-01

Halloysite is a naturally occurring clay, with physical structure represented by halloysite nanotubes (HNTs). We investigated the potential applicability of HNTs for carbon dioxide (CO2) capture, using two amine-functionalized HNTs: (3-aminopropyl) triethoxysilane (APTES)-grafted HNTs and polyethylenimine (PEI)-impregnated HNTs. APTES-HNTs and PEI-HNTs resulted in 5.6 and 30 wt. % (in sorbent) in functionalization onto HNTs, respectively. Capture efficiency was higher in APTES-HNTs at lower temperatures, while it was maximum in PEI-HNTs at 70°C-75 °C. At 75 °C, adsorption/desorption tests showed that 95% of the two reactions occurred within 30 min, and exhibited 0.15 and 0.21 millimole of CO2 adsorption capacity per millimole of amine group for APTES-HNTs and PEI-HNTs, respectively. During 10 cycles of CO2 adsorption/desorption, there was no significant decrease in sorbent weight and adsorption capacity in both HNTs. These results show that inherent structural features of HNTs can be easily tailored for the development of operational condition-specific CO2 capture system.

The catalytic effect of H2O on the hydrolysis of CO32- in hydrated clusters and its implication in the humidity driven CO2 air capture.

PubMed

Xiao, Hang; Shi, Xiaoyang; Zhang, Yayun; Liao, Xiangbiao; Hao, Feng; Lackner, Klaus S; Chen, Xi

2017-10-18

The hydration of ions in nanoscale hydrated clusters is ubiquitous and essential in many physical and chemical processes. Here we show that the hydrolysis reaction is strongly affected by relative humidity. The hydrolysis of CO 3 2- with n = 1-8 water molecules is investigated using an ab initio method. For n = 1-5 water molecules, all the reactants follow a stepwise pathway to the transition state. For n = 6-8 water molecules, all the reactants undergo a direct proton transfer to the transition state with overall lower activation free energy. The activation free energy of the reaction is dramatically reduced from 10.4 to 2.4 kcal mol -1 as the number of water molecules increases from 1 to 6. Meanwhile, the degree of hydrolysis of CO 3 2- is significantly increased compared to the bulk water solution scenario. Incomplete hydration shells facilitate the hydrolysis of CO 3 2- with few water molecules to be not only thermodynamically favorable but also kinetically favorable. We showed that the chemical kinetics is not likely to constrain the speed of CO 2 air capture driven by the humidity-swing. Instead, the pore-diffusion of ions is expected to be the time-limiting step in the humidity driven CO 2 air capture. The effect of humidity on the speed of CO 2 air capture was studied by conducting a CO 2 absorption experiment using IER with a high ratio of CO 3 2- to H 2 O molecules. Our result is able to provide valuable insights into designing efficient CO 2 air-capture sorbents.

Climate Impact and Economic Feasibility of Solar Thermochemical Jet Fuel Production.

PubMed

Falter, Christoph; Batteiger, Valentin; Sizmann, Andreas

2016-01-05

Solar thermochemistry presents a promising option for the efficient conversion of H2O and CO2 into liquid hydrocarbon fuels using concentrated solar energy. To explore the potential of this fuel production pathway, the climate impact and economic performance are analyzed. Key drivers for the economic and ecological performance are thermochemical energy conversion efficiency, the level of solar irradiation, operation and maintenance, and the initial investment in the fuel production plant. For the baseline case of a solar tower concentrator with CO2 capture from air, jet fuel production costs of 2.23 €/L and life cycle greenhouse gas (LC GHG) emissions of 0.49 kgCO2-equiv/L are estimated. Capturing CO2 from a natural gas combined cycle power plant instead of the air reduces the production costs by 15% but leads to LC GHG emissions higher than that of conventional jet fuel. Favorable assumptions for all involved process steps (30% thermochemical energy conversion efficiency, 3000 kWh/(m(2) a) solar irradiation, low CO2 and heliostat costs) result in jet fuel production costs of 1.28 €/L at LC GHG emissions close to zero. Even lower production costs may be achieved if the commercial value of oxygen as a byproduct is considered.

An Integrated, Low Temperature Process to Capture and Sequester Carbon Dioxide from Industrial Emissions

NASA Astrophysics Data System (ADS)

Wendlandt, R. F.; Foremski, J. J.

2013-12-01

Laboratory experiments show that it is possible to integrate (1) the chemistry of serpentine dissolution, (2) capture of CO2 gas from the combustion of natural gas and coal-fired power plants using aqueous amine-based solvents, (3) long-term CO2 sequestration via solid phase carbonate precipitation, and (4) capture solvent regeneration with acid recycling in a single, continuous process. In our process, magnesium is released from serpentine at 300°C via heat treatment with ammonium sulfate salts or at temperatures as low as 50°C via reaction with sulfuric acid. We have also demonstrated that various solid carbonate phases can be precipitated directly from aqueous amine-based (NH3, MEA, DMEA) CO2 capture solvent solutions at room temperature. Direct precipitation from the capture solvent enables regenerating CO2 capture solvent without the need for heat and without the need to compress the CO2 off gas. We propose that known low-temperature electrochemical methods can be integrated with this process to regenerate the aqueous amine capture solvent and recycle acid for dissolution of magnesium-bearing mineral feedstocks and magnesium release. Although the direct precipitation of magnesite at ambient conditions remains elusive, experimental results demonstrate that at temperatures ranging from 20°C to 60°C, either nesquehonite Mg(HCO3)(OH)●2H2O or a double salt with the formula [NH4]2Mg(CO3)2●4H2O or an amorphous magnesium carbonate precipitate directly from the capture solvent. These phases are less desirable for CO2 sequestration than magnesite because they potentially remove constituents (water, ammonia) from the reaction system, reducing the overall efficiency of the sequestration process. Accordingly, the integrated process can be accomplished with minimal energy consumption and loss of CO2 capture and acid solvents, and a net generation of 1 to 4 moles of H2O/6 moles of CO2 sequestered (depending on the solid carbonate precipitate and amount of produced H2 and O2 gas reacted to produce heat and water). Features of the integrated process include the following: 1) the four separate processes have compatible chemistry, enabling design of an integrated, continuous process scheme for CO2 capture and sequestration; 2) all 4 stages of the process can be conducted at ambient or slightly elevated temperatures; 3) precipitating carbonate directly from the capture solvent eliminates the need for costly CO2 gas compression; and 4) recycling the acid used for serpentine dissolution and the solvent used for CO2 capture reduces feed stock costs.

Role of amine structure on carbon dioxide adsorption from ultradilute gas streams such as ambient air.

PubMed

Didas, Stephanie A; Kulkarni, Ambarish R; Sholl, David S; Jones, Christopher W

2012-10-01

A fundamental study on the adsorption properties of primary, secondary, and tertiary amine materials is used to evaluate what amine type(s) are best suited for ultradilute CO(2) capture applications. A series of comparable materials comprised of primary, secondary, or tertiary amines ligated to a mesoporous silica support via a propyl linker are used to systematically assess the role of amine type. Both CO(2) and water adsorption isotherms are presented for these materials in the range relevant to CO(2) capture from ambient air and it is demonstrated that primary amines are the best candidates for CO(2) capture from air. Primary amines possess both the highest amine efficiency for CO(2) adsorption as well as enhanced water affinity compared to other amine types or the bare silica support. The results suggest that the rational design of amine adsorbents for the extraction of CO(2) from ambient air should focus on adsorbents rich in primary amines. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Membrane Process to Capture CO{sub 2} from Coal-Fired Power Plant Flue Gas

DOE Office of Scientific and Technical Information (OSTI.GOV)

Merkel, Tim; Wei, Xiaotong; Firat, Bilgen

2012-03-31

This final report describes work conducted for the U.S. Department of Energy National Energy Technology Laboratory (DOE NETL) on development of an efficient membrane process to capture carbon dioxide (CO{sub 2}) from power plant flue gas (award number DE-NT0005312). The primary goal of this research program was to demonstrate, in a field test, the ability of a membrane process to capture up to 90% of CO{sub 2} in coal-fired flue gas, and to evaluate the potential of a full-scale version of the process to perform this separation with less than a 35% increase in the levelized cost of electricity (LCOE).more » Membrane Technology and Research (MTR) conducted this project in collaboration with Arizona Public Services (APS), who hosted a membrane field test at their Cholla coal-fired power plant, and the Electric Power Research Institute (EPRI) and WorleyParsons (WP), who performed a comparative cost analysis of the proposed membrane CO{sub 2} capture process. The work conducted for this project included membrane and module development, slipstream testing of commercial-sized modules with natural gas and coal-fired flue gas, process design optimization, and a detailed systems and cost analysis of a membrane retrofit to a commercial power plant. The Polaris? membrane developed over a number of years by MTR represents a step-change improvement in CO{sub 2} permeance compared to previous commercial CO{sub 2}-selective membranes. During this project, membrane optimization work resulted in a further doubling of the CO{sub 2} permeance of Polaris membrane while maintaining the CO{sub 2}/N{sub 2} selectivity. This is an important accomplishment because increased CO{sub 2} permeance directly impacts the membrane skid cost and footprint: a doubling of CO{sub 2} permeance halves the skid cost and footprint. In addition to providing high CO{sub 2} permeance, flue gas CO{sub 2} capture membranes must be stable in the presence of contaminants including SO{sub 2}. Laboratory tests showed no degradation in Polaris membrane performance during two months of continuous operation in a simulated flue gas environment containing up to 1,000 ppm SO{sub 2}. A successful slipstream field test at the APS Cholla power plant was conducted with commercialsize Polaris modules during this project. This field test is the first demonstration of stable performance by commercial-sized membrane modules treating actual coal-fired power plant flue gas. Process design studies show that selective recycle of CO{sub 2} using a countercurrent membrane module with air as a sweep stream can double the concentration of CO{sub 2} in coal flue gas with little energy input. This pre-concentration of CO{sub 2} by the sweep membrane reduces the minimum energy of CO{sub 2} separation in the capture unit by up to 40% for coal flue gas. Variations of this design may be even more promising for CO{sub 2} capture from NGCC flue gas, in which the CO{sub 2} concentration can be increased from 4% to 20% by selective sweep recycle. EPRI and WP conducted a systems and cost analysis of a base case MTR membrane CO{sub 2} capture system retrofitted to the AEP Conesville Unit 5 boiler. Some of the key findings from this study and a sensitivity analysis performed by MTR include: The MTR membrane process can capture 90% of the CO{sub 2} in coal flue gas and produce high-purity CO{sub 2} (>99%) ready for sequestration. CO{sub 2} recycle to the boiler appears feasible with minimal impact on boiler performance; however, further study by a boiler OEM is recommended. For a membrane process built today using a combination of slight feed compression, permeate vacuum, and current compression equipment costs, the membrane capture process can be competitive with the base case MEA process at 90% CO{sub 2} capture from a coal-fired power plant. The incremental LCOE for the base case membrane process is about equal to that of a base case MEA process, within the uncertainty in the analysis. With advanced membranes (5,000 gpu for CO{sub 2} and 50 for CO{sub 2}/N{sub 2}), operating with no feed compression and low-cost CO{sub 2} compression equipment, an incremental LCOE of $33/MWh at 90% capture can be achieved (40% lower than the advanced MEA case). Even with lower cost compression, it appears unlikely that a membrane process using high feed compression (>5 bar) can be competitive with amine absorption, due to the capital cost and energy consumption of this equipment. Similarly, low vacuum pressure (<0.2 bar) cannot be used due to poor efficiency and high cost of this equipment. High membrane permeance is important to reduce the capital cost and footprint of the membrane unit. CO{sub 2}/N{sub 2} selectivity is less important because it is too costly to generate a pressure ratio where high selectivity can be useful. A potential cost ?sweet spot? exists for use of membrane-based technology, if 50-70% CO{sub 2} capture is acceptable. There is a minimum in the cost of CO{sub 2} avoided/ton that membranes can deliver at 60% CO{sub 2} capture, which is 20% lower than the cost at 90% capture. Membranes operating with no feed compression are best suited for lower capture rates. Currently, it appears that the biggest hurdle to use of membranes for post-combustion CO{sub 2} capture is compression equipment cost. An alternative approach is to use sweep membranes in parallel with another CO{sub 2} capture technology that does not require feed compression or vacuum equipment. Hybrid designs that utilize sweep membranes for selective CO{sub 2} recycle show potential to significantly reduce the minimum energy of CO{sub 2} separation.« less

Efficient capture of CO2 over ordered micro-mesoporous hybrid carbon nanosphere

NASA Astrophysics Data System (ADS)

Chen, Changwei; Yu, Yanke; He, Chi; Wang, Li; Huang, Huang; Albilali, Reem; Cheng, Jie; Hao, Zhengping

2018-05-01

Four kinds of carbon-based adsorbents (micro-mesoporous hybrid carbon nanosphere and N-doped hollow carbon sphere with single-, double- or ruga-shell morphology) with different structural and textural properties were prepared and systematically studied in CO2 capture. All synthesized samples possess high specific surface area (828-910 m2 g-1), large pore volume (0.71-1.81 cm3 g-1), and different micropore contents varied from 2.1% to 46.4%. Amongst, the ordered micro-mesoporous carbon nanosphere (OM-CNS) exhibits the best adsorption performance with CO2 uptake as high as 3.01 mmol g-1 under conditions of 298 K and 1.0 bar, better than most of the reported CO2 adsorbents. The excellent CO2 adsorption capacity of OM-CNS can be reasonably attributed to the synergistic effect of ordered mesopore channels and abundant structural micropores which are beneficial for the diffusion and trapping of CO2 adsorbate. Moreover, the OM-CNS shows excellent CO2 trapping selectivity and superior stability and recyclability, which endow the OM-CNS as a promising and environmental-friendly adsorbent for CO2 capture and separation under practical conditions.

Solar Reforming of Carbon Dioxide to Produce Diesel Fuel

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dennis Schuetzle; Robert Schuetzle

2010-12-31

This project focused on the demonstration of an innovative technology, referred to as the Sunexus CO2 Solar Reformer, which utilizes waste CO2 as a feedstock for the efficient and economical production of synthetic diesel fuel using solar thermal energy as the primary energy input. The Sunexus technology employs a two stage process for the conversion of CO2 to diesel fuel. A solar reforming system, including a specially designed reactor and proprietary CO2 reforming catalyst, was developed and used to convert captured CO2 rich gas streams into syngas (primarily hydrogen and carbon monoxide) using concentrated solar energy at high conversion efficiencies.more » The second stage of the system (which has been demonstrated under other funding) involves the direct conversion of the syngas into synthetic diesel fuel using a proprietary catalyst (Terra) previously developed and validated by Pacific Renewable Fuels and Chemicals (PRFC). The overall system energy efficiency for conversion of CO2 to diesel fuel is 74%, due to the use of solar energy. The results herein describe modeling, design, construction, and testing of the Sunexus CO2 Solar Reformer. Extensive parametric testing of the solar reformer and candidate catalysts was conducted and chemical kinetic models were developed. Laboratory testing of the Solar Reformer was successfully completed using various gas mixtures, temperatures, and gas flow rates/space velocities to establish performance metrics which can be employed for the design of commercial plants. A variety of laboratory tests were conducted including dry reforming (CO2 and CH{sub 4}), combination dry/steam reforming (CO2, CH{sub 4} & H{sub 2}O), and tri-reforming (CO2, CH{sub 4}, H{sub 2}O & O{sub 2}). CH{sub 4} and CO2 conversions averaged 95-100% and 50-90% per reformer cycle, respectively, depending upon the temperatures and gas space velocities. No formation of carbon deposits (coking) on the catalyst was observed in any of these tests. A 16 ft. diameter, concentrating solar dish was modified to accommodate the Sunexus CO2 Solar Reformer and the integrated system was installed at the Pacific Renewable Fuels and Chemicals test site at McClellan, CA. Several test runs were conducted without catalyst during which the ceramic heat exchanger in the Sunexus Solar Reformer reached temperatures between 1,050 F (566 C) and 2,200 F (1,204 C) during the test period. A dry reforming mixture of CO2/CH{sub 4} (2.0/1.0 molar ratio) was chosen for all of the tests on the integrated solar dish/catalytic reformer during December 2010. Initial tests were carried out to determine heat transfer from the collimated solar beam to the catalytic reactor. The catalyst was operated successfully at a steady-state temperature of 1,125 F (607 C), which was sufficient to convert 35% of the 2/1 CO2/CH{sub 4} mixture to syngas. This conversion efficiency confirmed the results from laboratory testing of this catalyst which provided comparable syngas production efficiencies (40% at 1,200 F [650 C]) with a resulting syngas composition of 20% CO, 16% H{sub 2}, 39% CO2 and 25% CH{sub 4}. As based upon the laboratory results, it is predicted that 90% of the CO2 will be converted to syngas in the solar reformer at 1,440 F (782 C) resulting in a syngas composition of 50% CO: 43% H{sub 2}: 7% CO2: 0% CH{sub 4}. Laboratory tests show that the higher catalyst operating temperature of 1,440 F (782 C) for efficient conversion of CO2 can certainly be achieved by optimizing solar reactor heat transfer, which would result in the projected 90% CO2-to-syngas conversion efficiencies. Further testing will be carried out during 2011, through other funding support, to further optimize the solar dish CO2 reformer. Additional studies carried out in support of this project and described in this report include: (1) An Assessment of Potential Contaminants in Captured CO2 from Various Industrial Processes and Their Possible Effect on Sunexus CO2 Reforming Catalysts; (2) Recommended Measurement Methods for Assessing Contaminant Levels in Captured CO2 Streams; (3) An Assessment of Current Commercial Scale Fisher-Tropsch (F-T) Technologies for the Conversion of Syngas to Fuels; (4) An Overview of CO2 Capture Technologies from Various Industrial Sources; and (5) Lifecycle Analysis for the Capture and Conversion of CO2 to Synthetic Diesel Fuel. Commercial scale Sunexus CO2 Solar Reformer plant designs, proposed in this report, should be able to utilize waste CO2 from a wide variety of industrial sources to produce a directly usable synthetic diesel fuel that replaces petroleum derived fuel, thus improving the United States energy security while also sequestering CO2. Our material balance model shows that every 5.0 lbs of CO2 is transformed using solar energy into 6.26 lbs (1.0 U.S. gallon) of diesel fuel and into by-products, which includes water. Details are provided in the mass and energy model in this report.« less

Easily regenerable solid adsorbents based on polyamines for carbon dioxide capture from the air.

PubMed

Goeppert, Alain; Zhang, Hang; Czaun, Miklos; May, Robert B; Prakash, G K Surya; Olah, George A; Narayanan, S R

2014-05-01

Adsorbents prepared easily by impregnation of fumed silica with polyethylenimine (PEI) are promising candidates for the capture of CO2 directly from the air. These inexpensive adsorbents have high CO2 adsorption capacity at ambient temperature and can be regenerated in repeated cycles under mild conditions. Despite the very low CO2 concentration, they are able to scrub efficiently all CO2 out of the air in the initial hours of the experiments. The influence of parameters such as PEI loading, adsorption and desorption temperature, particle size, and PEI molecular weight on the adsorption behavior were investigated. The mild regeneration temperatures required could allow the use of waste heat available in many industrial processes as well as solar heat. CO2 adsorption from the air has a number of applications. Removal of CO2 from a closed environment, such as a submarine or space vehicles, is essential for life support. The supply of CO2-free air is also critical for alkaline fuel cells and batteries. Direct air capture of CO2 could also help mitigate the rising concerns about atmospheric CO2 concentration and associated climatic changes, while, at the same time, provide the first step for an anthropogenic carbon cycle. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Chemical Looping Gasification for Hydrogen Enhanced Syngas Production with In-Situ CO 2 Capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kathe, Mandar; Xu, Dikai; Hsieh, Tien-Lin

2014-12-31

This document is the final report for the project titled “Chemical Looping Gasification for Hydrogen Enhanced Syngas Production with In-Situ CO 2 Capture” under award number FE0012136 for the performance period 10/01/2013 to 12/31/2014.This project investigates the novel Ohio State chemical looping gasification technology for high efficiency, cost efficiency coal gasification for IGCC and methanol production application. The project developed an optimized oxygen carrier composition, demonstrated the feasibility of the concept and completed cold-flow model studies. WorleyParsons completed a techno-economic analysis which showed that for a coal only feed with carbon capture, the OSU CLG technology reduced the methanol requiredmore » selling price by 21%, lowered the capital costs by 28%, increased coal consumption efficiency by 14%. Further, using the Ohio State Chemical Looping Gasification technology resulted in a methanol required selling price which was lower than the reference non-capture case.« less

A Model of Carbon Capture and Storage with Demonstration of Global Warming Potential and Fossil Fuel Resource Use Efficiency

NASA Astrophysics Data System (ADS)

Suebsiri, Jitsopa

Increasing greenhouse gas concentration in the atmosphere influences global climate change even though the level of impact is still unclear. Carbon dioxide capture and storage (CCS) is increasingly seen as an important component of broadly based greenhouse gas reduction measures. Although the other greenhouse gases are more potent, the sheer volume of CO 2 makes it dominant in term of its effect in the atmosphere. To understand the implications, CCS activities should be studied from a full life cycle perspective. This thesis outlines the successful achievement of the objectives of this study in conducting life cycle assessment (LCA), reviewing the carbon dioxide implications only, combining two energy systems, coal-fired electrical generations and CO2 used for enhanced oil recovery (EOR). LCA is the primary approach used in this study to create a tool for CCS environmental evaluation. The Boundary Dam Power Station (BDPS) and the Weyburn-Midale CO 2 EOR Project in Saskatchewan, Canada, are studied and adopted as case scenarios to find the potential for effective application of CCS in both energy systems. This study demonstrates two levels of retrofitting of the BDPS, retrofit of unit 3 or retrofit of all units, combined with three options for CO 2 geological storage: deep saline aquifer, CO2 EOR, and a combination of deep saline aquifer storage and CO2 EOR. Energy output is considered the product of combining these two energy resources (coal and oil). Gigajoules (GJ) are used as the fundamental unit of measurement in comparing the combined energy types. The application of this tool effectively demonstrates the results of application of a CCS system concerning global warming potential (GWP) and fossil fuel resource use efficiency. Other environmental impacts could be analyzed with this tool as well. In addition, the results demonstrate that the GWP reduction is directly related to resource use efficiency. This means the lower the GWP of CCS, the lower resource use efficiency as well. Three processes, coal mining, power production including CO2 capture unit operation, and crude oil usage, must be included when the GWP of CCS is calculated. Moreover, the results from the sensitivity analysis of power generation efficiency present not only a significant reduction of GWP, but also a competitive solution for improving or at least preventing the decrease of fossil fuel resource use efficiency when CCS is applied.

Primary, secondary, and tertiary amines for CO2 capture: designing for mesoporous CO2 adsorbents.

PubMed

Ko, Young Gun; Shin, Seung Su; Choi, Ung Su

2011-09-15

CO(2) emissions, from fossil-fuel-burning power plants, the breathing, etc., influence the global worming on large scale and the man's work efficiency on small scale. The reversible capture of CO(2) is a prominent feature of CO(2) organic-inorganic hybrid adsorbent to sequester CO(2). Herein, (3-aminopropyl) trimethoxysilane (APTMS), [3-(methylamino)propyl] trimethoxysilane (MAPTMS), and [3-(diethylamino) propyl] trimethoxysilane (DEAPTMS) are immobilized on highly ordered mesoporous silicas (SBA-15) to catch CO(2) as primary, secondary, and tertiary aminosilica adsorbents. X-ray photoelectron spectroscopy was used to analyze the immobilized APTMS, MAPTMS, and DEAPTMS on the SBA-15. We report an interesting discovery that the CO(2) adsorption and desorption on the adsorbent depend on the amine type of the aminosilica adsorbent. The adsorbed CO(2) was easily desorbed from the adsorbent with the low energy consumption in the order of tertiary, secondary, and primary amino-adsorbents while the adsorption amount and the bonding-affinity increased in the reverse order. The effectiveness of amino-functionalized (1(o), 2(o), and 3(o) amines) SBA-15s as a CO(2) capturing agent was investigated in terms of adsorption capacity, adsorption-desorption kinetics, and thermodynamics. This work demonstrates apt amine types to catch CO(2) and regenerate the adsorbent, which may open new avenues to designing "CO(2) basket". Copyright © 2011. Published by Elsevier Inc.

Compact, Lightweight Adsorber and Sabatier Reactor for CO2 Capture and Reduction for Consumable and Propellant Production

NASA Technical Reports Server (NTRS)

Junaedi, Christian; Hawley, Kyle; Walsh, Dennis; Roychoudhury, Subir; Busby, Stacy A.; Abney, Morgan B.; Perry, Jay L.; Knox, James C.

2012-01-01

The utilization of CO2 to produce (or recycle) life support consumables, such as O2 and H2O, and to generate propellant fuels is an important aspect of NASA's concept for future, long duration planetary exploration. One potential approach is to capture and use CO2 from the Martian atmosphere to generate the consumables and propellant fuels. Precision Combustion, Inc. (PCI), with support from NASA, continues to develop its regenerable adsorber technology for capturing CO2 from gaseous atmospheres (for cabin atmosphere revitalization and in-situ resource utilization applications) and its Sabatier reactor for converting CO2 to methane and water. Both technologies are based on PCI's Microlith(R) substrates and have been demonstrated to reduce size, weight, and power consumption during CO2 capture and methanation process. For adsorber applications, the Microlith substrates offer a unique resistive heating capability that shows potential for short regeneration time and reduced power requirements compared to conventional systems. For the Sabatier applications, the combination of the Microlith substrates and durable catalyst coating permits efficient CO2 methanation that favors high reactant conversion, high selectivity, and durability. Results from performance testing at various operating conditions will be presented. An effort to optimize the Sabatier reactor and to develop a bench-top Sabatier Development Unit (SDU) will be discussed.

Synthesis and characterization of low viscosity carbon dioxide binding organic liquids for flue gas clean up

DOE Office of Scientific and Technical Information (OSTI.GOV)

Koech, Phillip K.; Malhotra, Deepika; Heldebrant, David J.

2015-01-01

Climate change is partly attributed to global anthropogenic carbon dioxide (CO2) emission to the atmosphere. These environmental effects can be mitigated by CO2 capture, utilization and storage. Alkanolamine solvents, such as monoethanolamine (MEA), which bind CO2 as carbamates or bicarbonate salts are used for CO2 capture in niche applications. These solvents consist of approximately 30 wt% of MEA in water, exhibiting a low, CO2-rich viscosity, fast kinetics and favorable thermodynamics. However, these solvents have low CO2 capacity and high heat capacity of water, resulting in prohibitively high costs of thermal solvent regeneration. Effective capture of the enormous amounts of CO2more » produced by coal-fired plants requires a material with high CO2 capacity and low regeneration energy requirements. To this end, several water-lean transformational solvents systems have been developed in order to reduce these energy penalties. These technologies include nano-material organic hybrids (NOHMs), task-specific, protic and conventional ionic liquids, phase change solvents. As part of an ongoing program in our group, we have developed new water lean transformational solvents known as CO2 binding organic liquids (CO2BOLs) which have the potential to be energy efficient CO2 capture solvents. These solvents, also known as switchable ionic liquids meaning, are organic solvents that can reversibly transform from non- ionic to ionic form and back. The zwitterionic state in these liquids is formed when low polarity non-ionic alkanolguanidines or alkanolamidines react with CO2 or SO2 to form ionic liquids with high polarity. These polar ionic liquids can be thermally converted to the less polar non-ionic solvent by releasing CO2.« less

Holey graphene frameworks for highly selective post-combustion carbon capture

PubMed Central

Chowdhury, Shamik; Balasubramanian, Rajasekhar

2016-01-01

Atmospheric CO2 concentrations continue to rise rapidly in response to increased combustion of fossil fuels, contributing to global climate change. In order to mitigate the effects of global warming, development of new materials for cost-effective and energy-efficient CO2 capture is critically important. Graphene-based porous materials are an emerging class of solid adsorbents for selectively removing CO2 from flue gases. Herein, we report a simple and scalable approach to produce three-dimensional holey graphene frameworks with tunable porosity and pore geometry, and demonstrate their application as high-performance CO2 adsorbents. These holey graphene macrostructures exhibit a significantly improved specific surface area and pore volume compared to their pristine counterparts, and can be effectively used in post-combustion CO2 adsorption systems because of their intrinsic hydrophobicity together with good gravimetric storage capacities, rapid removal capabilities, superior cycling stabilities, and moderate initial isosteric heats. In addition, an exceptionally high CO2 over N2 selectivity can be achieved under conditions relevant to capture from the dry exhaust gas stream of a coal burning power plant, suggesting the possibility of recovering highly pure CO2 for long-term sequestration and/or utilization for downstream applications. PMID:26879393

Holey graphene frameworks for highly selective post-combustion carbon capture.

PubMed

Chowdhury, Shamik; Balasubramanian, Rajasekhar

2016-02-16

Atmospheric CO2 concentrations continue to rise rapidly in response to increased combustion of fossil fuels, contributing to global climate change. In order to mitigate the effects of global warming, development of new materials for cost-effective and energy-efficient CO2 capture is critically important. Graphene-based porous materials are an emerging class of solid adsorbents for selectively removing CO2 from flue gases. Herein, we report a simple and scalable approach to produce three-dimensional holey graphene frameworks with tunable porosity and pore geometry, and demonstrate their application as high-performance CO2 adsorbents. These holey graphene macrostructures exhibit a significantly improved specific surface area and pore volume compared to their pristine counterparts, and can be effectively used in post-combustion CO2 adsorption systems because of their intrinsic hydrophobicity together with good gravimetric storage capacities, rapid removal capabilities, superior cycling stabilities, and moderate initial isosteric heats. In addition, an exceptionally high CO2 over N2 selectivity can be achieved under conditions relevant to capture from the dry exhaust gas stream of a coal burning power plant, suggesting the possibility of recovering highly pure CO2 for long-term sequestration and/or utilization for downstream applications.

Holey graphene frameworks for highly selective post-combustion carbon capture

NASA Astrophysics Data System (ADS)

Chowdhury, Shamik; Balasubramanian, Rajasekhar

2016-02-01

Atmospheric CO2 concentrations continue to rise rapidly in response to increased combustion of fossil fuels, contributing to global climate change. In order to mitigate the effects of global warming, development of new materials for cost-effective and energy-efficient CO2 capture is critically important. Graphene-based porous materials are an emerging class of solid adsorbents for selectively removing CO2 from flue gases. Herein, we report a simple and scalable approach to produce three-dimensional holey graphene frameworks with tunable porosity and pore geometry, and demonstrate their application as high-performance CO2 adsorbents. These holey graphene macrostructures exhibit a significantly improved specific surface area and pore volume compared to their pristine counterparts, and can be effectively used in post-combustion CO2 adsorption systems because of their intrinsic hydrophobicity together with good gravimetric storage capacities, rapid removal capabilities, superior cycling stabilities, and moderate initial isosteric heats. In addition, an exceptionally high CO2 over N2 selectivity can be achieved under conditions relevant to capture from the dry exhaust gas stream of a coal burning power plant, suggesting the possibility of recovering highly pure CO2 for long-term sequestration and/or utilization for downstream applications.

Hybrid photosynthesis-powering biocatalysts with solar energy captured by inorganic devices.

PubMed

Zhang, Tian; Tremblay, Pier-Luc

2017-01-01

The biological reduction of CO 2 driven by sunlight via photosynthesis is a crucial process for life on earth. However, the conversion efficiency of solar energy to biomass by natural photosynthesis is low. This translates in bioproduction processes relying on natural photosynthesis that are inefficient energetically. Recently, hybrid photosynthetic technologies with the potential of significantly increasing the efficiency of solar energy conversion to products have been developed. In these systems, the reduction of CO 2 into biofuels or other chemicals of interest by biocatalysts is driven by solar energy captured with inorganic devices such as photovoltaic cells or photoelectrodes. Here, we explore hybrid photosynthesis and examine the strategies being deployed to improve this biotechnology.

Response surface method for modeling the removal of carbon dioxide from a simulated gas using water absorption enhanced with a liquid-film-forming device.

PubMed

Nguyen, Diem-Mai Kim; Imai, Tsuyoshi; Dang, Thanh-Loc Thi; Kanno, Ariyo; Higuchi, Takaya; Yamamoto, Koichi; Sekine, Masahiko

2018-03-01

This paper presents the results from using a physical absorption process to absorb gaseous CO 2 mixed with N 2 using water by producing tiny bubbles via a liquid-film-forming device (LFFD) that improves the solubility of CO 2 in water. The influence of various parameters-pressure, initial CO 2 concentration, gas-to-liquid ratios, and temperature-on the CO 2 removal efficiency and its absorption rate in water were investigated and estimated thoroughly by statistical polynomial models obtained by the utilization of the response surface method (RSM) with a central composite design (CCD). Based on the analysis, a high efficiency of CO 2 capture can be reached in conditions such as low pressure, high CO 2 concentration at the inlet, low gas/liquid ratio, and low temperature. For instance, the highest removal efficiency in the RSM-CCD experimental matrix of nearly 80% occurred for run number 20, which was conducted at 0.30MPa, CO 2 concentration of 35%, gas/liquid ratio of 0.71, and temperature of 15°C. Furthermore, the coefficients of determination, R 2 , were 0.996 for the removal rate and 0.982 for the absorption rate, implying that the predicted values computed by the constructed models correlate strongly and fit well with the experimental values. The results obtained provide essential information for implementing this method properly and effectively and contribute a promising approach to the problem of CO 2 capture in air pollution treatment. Copyright © 2017. Published by Elsevier B.V.

Atmospheric CO2 capture for the artificial photosynthetic system.

PubMed

Nogalska, Adrianna; Zukowska, Adrianna; Garcia-Valls, Ricard

2018-04-15

The aim of these studies is to evaluate the ambient CO 2 capture abilities of the membrane contactor system in the same conditions as leafs, such as ambient temperature, pressure and low CO 2 concentration, where the only driving force is the concentration gradient. The polysulfone membrane employed was made by a phase inversion process and characterized by ESEM micrographs which were used to determine the thickness, asymmetry and pore size. Besides, the porosity of the membrane was measured from the membrane and polysulfone density correlation and the hydrophobicity was analyzed by contact angle measurements. Moreover, the compatibility of membrane and absorbent was evaluated, in order to exclude wetting issues by meaning of swelling, dynamic contact angle and AFM analysis. The prepared membranes were introduced into a cross flow module and used as contactors between CO 2 and the absorbing media, a potassium hydroxide solution. The influence of the membrane thickness, absorbent stirring rate, solution pH and absorption time on CO 2 capture were evaluated. Absorbent solution stirring rate showed no statistically significant influence on absorption. We observed a non-linear correlation between the capture rate and the increase of absorbent solution pH as well as absorption time. The results showed that the efficiency of our CO 2 capture system is similar to stomatal carbon dioxide assimilation rate, achieving stable value of 20μmol/m 2 ·s after 1h of experiment. Copyright © 2017 Elsevier B.V. All rights reserved.

Economics of carbon dioxide capture and utilization-a supply and demand perspective.

PubMed

Naims, Henriette

2016-11-01

Lately, the technical research on carbon dioxide capture and utilization (CCU) has achieved important breakthroughs. While single CO 2 -based innovations are entering the markets, the possible economic effects of a large-scale CO 2 utilization still remain unclear to policy makers and the public. Hence, this paper reviews the literature on CCU and provides insights on the motivations and potential of making use of recovered CO 2 emissions as a commodity in the industrial production of materials and fuels. By analyzing data on current global CO 2 supply from industrial sources, best practice benchmark capture costs and the demand potential of CO 2 utilization and storage scenarios with comparative statics, conclusions can be drawn on the role of different CO 2 sources. For near-term scenarios the demand for the commodity CO 2 can be covered from industrial processes, that emit CO 2 at a high purity and low benchmark capture cost of approximately 33 €/t. In the long-term, with synthetic fuel production and large-scale CO 2 utilization, CO 2 is likely to be available from a variety of processes at benchmark costs of approx. 65 €/t. Even if fossil-fired power generation is phased out, the CO 2 emissions of current industrial processes would suffice for ambitious CCU demand scenarios. At current economic conditions, the business case for CO 2 utilization is technology specific and depends on whether efficiency gains or substitution of volatile priced raw materials can be achieved. Overall, it is argued that CCU should be advanced complementary to mitigation technologies and can unfold its potential in creating local circular economy solutions.

Role of Additives in Composite PEI/Oxide CO 2 Adsorbents: Enhancement in the Amine Efficiency of Supported PEI by PEG in CO 2 Capture from Simulated Ambient Air

DOE PAGES

Sakwa-Novak, Miles A.; Tan, Shuai; Jones, Christopher W.

2015-10-20

Supported amines are promising candidate adsorbents for the removal of CO 2 from flue gases and directly from ambient air. The incorporation of additives into polymeric amines such as poly(ethylenimine) (PEI) supported on mesoporous oxides is an effective strategy to improve the performance of the materials. Here, several practical aspects of this strategy are addressed with regards to direct air capture. The influence of three additives (CTAB, PEG200, PEG1000) was systematically explored under dry simulated air capture conditions (400 ppm of CO 2, 30 °C). With SBA-15 as a model support for poly(ethylenimine) (PEI), the nature of the additive inducedmore » heterogeneities in the deposition of organic on the interior and exterior of the particles, an important consideration for future scale up to practical systems. The PEG200 additive increased the observed thermodynamic performance (~60% increase in amine efficiency) of the adsorbents regardless of the PEI content, while the other molecules had less positive effects. A threshold PEG200/PEI value was identified at which the diffusional limitations of CO 2 within the materials were nearly eliminated. The threshold PEG/PEI ratio may have physical origin in the interactions between PEI and PEG, as the optimal ratio corresponded to nearly equimolar OH/reactive (1°, 2°) amine ratios. As a result, the strategy is shown to be robust to the characteristics of the host support, as PEG200 improved the amine efficiency of PEI when supported on two varieties of mesoporous γ-alumina with PEI.« less

Role of Additives in Composite PEI/Oxide CO 2 Adsorbents: Enhancement in the Amine Efficiency of Supported PEI by PEG in CO 2 Capture from Simulated Ambient Air

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sakwa-Novak, Miles A.; Tan, Shuai; Jones, Christopher W.

Supported amines are promising candidate adsorbents for the removal of CO 2 from flue gases and directly from ambient air. The incorporation of additives into polymeric amines such as poly(ethylenimine) (PEI) supported on mesoporous oxides is an effective strategy to improve the performance of the materials. Here, several practical aspects of this strategy are addressed with regards to direct air capture. The influence of three additives (CTAB, PEG200, PEG1000) was systematically explored under dry simulated air capture conditions (400 ppm of CO 2, 30 °C). With SBA-15 as a model support for poly(ethylenimine) (PEI), the nature of the additive inducedmore » heterogeneities in the deposition of organic on the interior and exterior of the particles, an important consideration for future scale up to practical systems. The PEG200 additive increased the observed thermodynamic performance (~60% increase in amine efficiency) of the adsorbents regardless of the PEI content, while the other molecules had less positive effects. A threshold PEG200/PEI value was identified at which the diffusional limitations of CO 2 within the materials were nearly eliminated. The threshold PEG/PEI ratio may have physical origin in the interactions between PEI and PEG, as the optimal ratio corresponded to nearly equimolar OH/reactive (1°, 2°) amine ratios. As a result, the strategy is shown to be robust to the characteristics of the host support, as PEG200 improved the amine efficiency of PEI when supported on two varieties of mesoporous γ-alumina with PEI.« less

CO2 Fixation, Lipid Production, and Power Generation by a Novel Air-Lift-Type Microbial Carbon Capture Cell System.

PubMed

Hu, Xia; Liu, Baojun; Zhou, Jiti; Jin, Ruofei; Qiao, Sen; Liu, Guangfei

2015-09-01

An air-lift-type microbial carbon capture cell (ALMCC) was constructed for the first time by using an air-lift-type photobioreactor as the cathode chamber. The performance of ALMCC in fixing high concentration of CO2, producing energy (power and biodiesel), and removing COD together with nutrients was investigated and compared with the traditional microbial carbon capture cell (MCC) and air-lift-type photobioreactor (ALP). The ALMCC system produced a maximum power density of 972.5 mW·m(-3) and removed 86.69% of COD, 70.52% of ammonium nitrogen, and 69.24% of phosphorus, which indicate that ALMCC performed better than MCC in terms of power generation and wastewater treatment efficiency. Besides, ALMCC demonstrated 9.98- and 1.88-fold increases over ALP and MCC in the CO2 fixation rate, respectively. Similarly, the ALMCC significantly presented a higher lipid productivity compared to those control reactors. More importantly, the preliminary analysis of energy balance suggested that the net energy of the ALMCC system was significantly superior to other systems and could theoretically produce enough energy to cover its consumption. In this work, the established ALMCC system simultaneously achieved the high level of CO2 fixation, energy recycle, and municipal wastewater treatment effectively and efficiently.

Large Pilot Scale Testing of Linde/BASF Post-Combustion CO 2 Capture Technology at the Abbott Coal-Fired Power Plant

DOE Office of Scientific and Technical Information (OSTI.GOV)

O'Brien, Kevin C.

The work summarized in this report is the first step towards a project that will re-train and create jobs for personnel in the coal industry and continue regional economic development to benefit regions impacted by previous downturns. The larger project is aimed at capturing ~300 tons/day (272 metric tonnes/day) CO 2 at a 90% capture rate from existing coal- fired boilers at the Abbott Power Plant on the campus of University of Illinois (UI). It will employ the Linde-BASF novel amine-based advanced CO 2 capture technology, which has already shown the potential to be cost-effective, energy efficient and compact atmore » the 0.5-1.5 MWe pilot scales. The overall objective of the project is to design and install a scaled-up system of nominal 15 MWe size, integrate it with the Abbott Power Plant flue gas, steam and other utility systems, and demonstrate the viability of continuous operation under realistic conditions with high efficiency and capacity. The project will also begin to build a workforce that understands how to operate and maintain the capture plants by including students from regional community colleges and universities in the operation and evaluation of the capture system. This project will also lay the groundwork for follow-on projects that pilot utilization of the captured CO 2 from coal-fired power plants. The net impact will be to demonstrate a replicable means to (1) use a standardized procedure to evaluate power plants for their ability to be retrofitted with a pilot capture unit; (2) design and construct reliable capture systems based on the Linde-BASF technology; (3) operate and maintain these systems; (4) implement training programs with local community colleges and universities to establish a workforce to operate and maintain the systems; and (5) prepare to evaluate at the large pilot scale level various methods to utilize the resulting captured CO 2. Towards the larger project goal, the UI-led team, together with Linde, has completed a preliminary design for the carbon capture pilot plant with basic engineering and cost estimates, established permitting needs, identified approaches to address Environmental, Health, and Safety concerns related to pilot plant installation and operation, developed approaches for long-term use of the captured carbon, and established strategies for workforce development and job creation that will re-train coal operators to operate carbon capture plants. This report describes Phase I accomplishments and demonstrates that the project team is well-prepared for full implementation of Phase 2, to design, build, and operate the carbon capture pilot plant.« less

Efficient CO2 capture by tertiary amine-functionalized ionic liquids through Li+-stabilized zwitterionic adduct formation

PubMed Central

Yang, Zhen-Zhen

2014-01-01

Summary Highly efficient CO2 absorption was realized through formation of zwitterionic adducts, combining synthetic strategies to ionic liquids (ILs) and coordination. The essence of our strategy is to make use of multidentate cation coordination between Li+ and an organic base. Also PEG-functionalized organic bases were employed to enhance the CO2-philicity. The ILs were reacted with CO2 to form the zwitterionic adduct. Coordination effects between various lithium salts and neutral ligands, as well as the CO2 capacity of the chelated ILs obtained were investigated. For example, the CO2 capacity of PEG150MeBu2N increased steadily from 0.10 to 0.66 (mol CO2 absorbed per mol of base) through the formation of zwitterionic adducts being stabilized by Li+. PMID:25246955

Tuning anion-functionalized ionic liquids for improved SO2 capture.

PubMed

Cui, Guokai; Zheng, Junjie; Luo, Xiaoyan; Lin, Wenjun; Ding, Fang; Li, Haoran; Wang, Congmin

2013-09-27

You can have your cake and eat it too: A "dual-tuning" strategy for improving the capture of SO2 was developed by introducing electron-withdrawing sites on the anions to produce several kinds of functionalized ionic liquids. Those functionalized with a halogen group exhibited improved performance over their non-halogenated counterparts, leading to highly efficient and reversible capture. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Formation of Carbamate Anions by the Gas-phase Reaction of Anilide Ions with CO2

NASA Astrophysics Data System (ADS)

Liu, Chongming; Nishshanka, Upul; Attygalle, Athula B.

2016-05-01

The anilide anion ( m/z 92) generated directly from aniline, or indirectly as a fragmentation product of deprotonated acetanilide, captures CO2 readily to form the carbamate anion ( m/z 136) in the collision cell, when CO2 is used as the collision gas in a tandem-quadrupole mass spectrometer. The gas-phase affinity of the anilide ion to CO2 is significantly higher than that of the phenoxide anion ( m/z 93), which adds to CO2 only very sluggishly. Our results suggest that the efficacy of CO2 capture depends on the natural charge density on the nitrogen atom, and relative nucleophilicity of the anilide anion. Generally, conjugate bases generated from aniline derivatives with proton affinities (PA) less than 350 kcal/mol do not tend to add CO2 to form gaseous carbamate ions. For example, the anion generated from p-methoxyaniline (PA = 367 kcal/mol) reacts significantly faster than that obtained from p-nitroaniline (PA = 343 kcal/mol). Although deprotonated p-aminobenzoic acid adds very poorly because the negative charge is now located primarily on the carboxylate group, it reacts more efficiently with CO2 if the carboxyl group is esterified. Moreover, mixture of CO2 and He as the collision gas was found to afford more efficient adduct formation than CO2 alone, or as mixtures made with nitrogen or argon, because helium acts as an effective "cooling" gas and reduces the internal energy of reactant ions.

Global carbon management using air capture and geosequestration at remote locations

NASA Astrophysics Data System (ADS)

Lackner, K. S.; Goldberg, D.

2014-12-01

CO2 emissions need not only stop; according the IPCC, emissions need to turn negative. This requires means to remove CO2 from air and store it safely and permanently. We outline a combination of secure geosequestration and direct capture of CO2 from ambient air to create negative emissions at remote locations. Operation at remote sites avoids many difficulties associated with capture at the source, where space for added equipment is limited, good storage sites are in short supply, and proximity to private property engenders resistance. Large Igneous Provinces have been tested as secure CO2 reservoirs. CO2 and water react with reservoir rock to form stable carbonates, permanently sequestering the carbon. Outfitting reservoirs in large igneous provinces far from human habitation with ambient air capture systems creates large CO2 sequestration sites. Their remoteness offers advantages in environmental security and public acceptance and, thus, can smooth the path toward CO2 stabilization. Direct capture of CO2 from ambient air appears energetically and economically viable and could be scaled up quickly. Thermodynamic energy requirements are very small and a number of approaches have shown to be energy efficient in practice. Sorbent technologies include supported organoamines, alkaline brines, and quaternary ammonium based ion-exchange resins. To demonstrate that the stated goals of low cost and low energy consumption can be reached at scale, public research and demonstration projects are essential. We suggest co-locating air capture and geosequestration at sites where renewable energy resources can power both activities. Ready renewable energy would also allow for the co-production of synthetic fuels. Possible locations with large wind and basalt resources include Iceland and Greenland, the north-western United States, the Kerguelen plateau, Siberia and Morocco. Capture and sequestration in these reservoirs could recover all of the emissions of the 20th century and still contribute to a carbon neutral economy throughout the 21st century. Mobilizing industrial infrastructure to these areas poses a challenge. However, the urgency of the climate problem requires immediate action, with economic incentives and commitments to site evaluation and engineering development.

Energy-efficient stirred-tank photobioreactors for simultaneous carbon capture and municipal wastewater treatment.

PubMed

Mohammed, K; Ahammad, S Z; Sallis, P J; Mota, C R

2014-01-01

Algal based wastewater treatment (WWT) technologies are attracting renewed attention because they couple energy-efficient sustainable treatment with carbon capture, and reduce the carbon footprint of the process. A low-cost energy-efficient mixed microalgal culture-based pilot WWT system, coupled with carbon dioxide (CO2) sequestration, was investigated. The 21 L stirred-tank photobioreactors (STPBR) used light-emitting diodes as the light source, resulting in substantially reduced operational costs. The STPBR were operated at average optimal light intensity of 582.7 μmol.s(-1).m(-2), treating synthetic municipal wastewater containing approximately 250, 90 and 10 mg.L(-1) of soluble chemical oxygen demand (SCOD), ammonium (NH4-N), and phosphate, respectively. The STPBR were maintained for 64 days without oxygen supplementation, but had a supply of CO2 (25 mL.min(-1), 25% v/v in N2). Relatively high SCOD removal efficiency (>70%) was achieved in all STPBR. Low operational cost was achieved by eliminating the need for mechanical aeration, with microalgal photosynthesis providing all oxygenation. The STPBR achieved an energy saving of up to 95%, compared to the conventional AS system. This study demonstrates that microalgal photobioreactors can provide effective WWT and carbon capture, simultaneously, in a system with potential for scaling-up to municipal WWT plants.

Updated (BP3) Technical and Economic Feasibility Study - Electrochemical Membrane for Carbon Dioxide Capture and Power Generation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ghezel-Ayagh, Hossein

This topical report summarizes the results of an updated Technical & Economic Feasibility Study (T&EFS) which was conducted in Budget Period 3 of the project to evaluate the performance and cost of the Electrochemical Membrane (ECM)-based CO 2 capture system. The ECM technology is derived from commercially available inorganic membranes; the same used in FuelCell Energy’s commercial fuel cell power plants and sold under the trade name Direct FuelCell® (DFC®). The ECM stacks are utilized in the Combined Electric Power (generation) And Carbon dioxide Separation (CEPACS) systems which can be deployed as add-ons to conventional power plants (Pulverized Coal, Combinedmore » Cycle, etc.) or industrial facilities to simultaneously produce power while capturing >90% of the CO 2 from the flue gas. In this study, an ECM-based CEPACS plant was designed to capture and compress >90% of the CO 2 (for sequestration or beneficial use) from the flue gas of a reference 550 MW (nominal, net AC) Pulverized Coal (PC) Rankine Cycle (Subcritical steam) power plant. ECM performance was updated based on bench scale ECM stack test results. The system process simulations were performed to generate the CEPACS plant performance estimates. The performance assessment included estimation of the parasitic power consumption for CO 2 capture and compression, and the efficiency impact on the PC plant. While the ECM-based CEPACS system for the 550 MW PC plant captures 90% of CO 2 from the flue gas, it generates additional (net AC) power after compensating for the auxiliary power requirements of CO 2 capture and compression. An equipment list, ECM stacks packaging design, and CEPACS plant layout were developed to facilitate the economic analysis. Vendor quotes were also solicited. The economic feasibility study included estimation of CEPACS plant capital cost, cost of electricity (COE) analyses and estimation of cost per ton of CO 2 captured. The incremental COE for the ECM-based CO 2 capture is expected to meet U.S. DOE’s target of 35%. This study has indicated that CEPACS systems offer significant benefits with respect to cost, performance, water consumption and emissions to environment. The realization of these benefits will provide a single solution to carbon dioxide capture in addition to meeting the increasing demand for electricity.« less

Updated (BP3) Technical and Economic Feasibility Study - Electrochemical Membrane for Carbon Dioxide Capture and Power Generation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ghezel-Ayagh, Hossein

This topical report summarizes the results of an updated Technical & Economic Feasibility Study (T&EFS) which was conducted in Budget Period 3 of the project to evaluate the performance and cost of the Electrochemical Membrane (ECM)-based CO2 capture system. The ECM technology is derived from commercially available inorganic membranes; the same used in FuelCell Energy’s commercial fuel cell power plants and sold under the trade name Direct FuelCell® (DFC®). The ECM stacks are utilized in the Combined Electric Power (generation) And Carbon dioxide Separation (CEPACS) systems which can be deployed as add-ons to conventional power plants (Pulverized Coal, Combined Cycle,more » etc.) or industrial facilities to simultaneously produce power while capturing >90% of the CO2 from the flue gas. In this study, an ECM-based CEPACS plant was designed to capture and compress >90% of the CO2 (for sequestration or beneficial use) from the flue gas of a reference 550 MW (nominal, net AC) Pulverized Coal (PC) Rankine Cycle (Subcritical steam) power plant. ECM performance was updated based on bench scale ECM stack test results. The system process simulations were performed to generate the CEPACS plant performance estimates. The performance assessment included estimation of the parasitic power consumption for CO2 capture and compression, and the efficiency impact on the PC plant. While the ECM-based CEPACS system for the 550 MW PC plant captures 90% of CO2 from the flue gas, it generates additional (net AC) power after compensating for the auxiliary power requirements of CO2 capture and compression. An equipment list, ECM stacks packaging design, and CEPACS plant layout were developed to facilitate the economic analysis. Vendor quotes were also solicited. The economic feasibility study included estimation of CEPACS plant capital cost, cost of electricity (COE) analyses and estimation of cost per ton of CO2 captured. The incremental COE for the ECM-based CO2 capture is expected to meet U.S. DOE’s target of 35%. This study has indicated that CEPACS systems offer significant benefits with respect to cost, performance, water consumption and emissions to environment. The realization of these benefits will provide a single solution to carbon dioxide capture in addition to meeting the increasing demand for electricity.« less

About how to capture and exploit the CO2 surplus that nature, per se, is not capable of fixing.

PubMed

Godoy, Manuel S; Mongili, Beatrice; Fino, Debora; Prieto, M Auxiliadora

2017-09-01

Human activity has been altering many ecological cycles for decades, disturbing the natural mechanisms which are responsible for re-establishing the normal environmental balances. Probably, the most disrupted of these cycles is the cycle of carbon. In this context, many technologies have been developed for an efficient CO 2 removal from the atmosphere. Once captured, it could be stored in large geological formations and other reservoirs like oceans. This strategy could present some environmental and economic problems. Alternately, CO 2 can be transformed into carbonates or different added-value products, such as biofuels and bioplastics, recycling CO 2 from fossil fuel. Currently different methods are being studied in this field. We classified them into biological, inorganic and hybrid systems for CO 2 transformation. To be environmentally compatible, they should be powered by renewable energy sources. Although hybrid systems are still incipient technologies, they have made great advances in the recent years. In this scenario, biotechnology is the spearhead of ambitious strategies to capture CO 2 and reduce global warming. © 2017 The Authors. Microbial Biotechnology published by John Wiley & Sons Ltd and Society for Applied Microbiology.

Efficient light hydrocarbon separation and CO2 capture and conversion in a stable MOF with oxalamide-decorated polar tubes.

PubMed

Li, Xiu-Yuan; Li, Yong-Zhi; Yang, Yun; Hou, Lei; Wang, Yao-Yu; Zhu, Zhonghua

2017-11-30

The first strontium-based MOF possessing polar tubular channels embedded with a high density of open Lewis acidic metal sites and basic oxalamide groups was constructed, which shows not only a high CO 2 and C 2 H 6 adsorption capability and significant selectivity for CO 2 over both CH 4 and CO, and for C 2 H 6 over CH 4 , but also size-selective chemical conversion of CO 2 with epoxides producing cyclic carbonates under ambient conditions.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tande, Brian; Seames, Wayne; Benson, Steve

The objective of this project was to evaluate the use of composite polymer membranes and porous membrane contactors to regenerate physical and chemical solvents for capture of carbon dioxide (CO 2) from synthesis gas or flue gas, with the goal of improving the energy efficiency of carbon capture. Both a chemical solvent (typical for a post-combustion capture of CO 2 from flue gas) and a physical solvent (typical for pre- combustion capture of CO 2 from syngas) were evaluated using two bench-scale test systems constructed for this project. For chemical solvents, polytetrafluoroethylene and polypropylene membranes were found to be ablemore » to strip CO 2 from a monoethanolamine (MEA) solution with high selectivity without significant degradation of the material. As expected, the regeneration temperature was the most significant parameter affecting the CO 2 flux through the membrane. Pore size was also found to be important, as pores larger than 5 microns lead to excessive pore wetting. For physical solvents, polydimethyl-siloxane (PDMS)-based membranes were found to have a higher CO 2 permeability than polyvinylalcohol (PVOH) based membranes, while also minimizing solvent loss. Overall, however, the recovery of CO 2 in these systems is low – less than 2% for both chemical and physical solvents – primarily due to the small surface area of the membrane test apparatus. To obtain the higher regeneration rates needed for this application, a much larger surface area would be needed. Further experiments using, for example, a hollow fiber membrane module could determine if this process could be commercially viable.« less

Ambient Carbon Dioxide Capture Using Boron-Rich Porous Boron Nitride: A Theoretical Study.

PubMed

Li, Lanlan; Liu, Yan; Yang, Xiaojing; Yu, Xiaofei; Fang, Yi; Li, Qiaoling; Jin, Peng; Tang, Chengchun

2017-05-10

The development of highly efficient sorbent materials for CO 2 capture under ambient conditions is of great importance for reducing the impact of CO 2 on the environment and climate change. In this account, strong CO 2 adsorption on a boron antisite (B N ) in boron-rich porous boron nitrides (p-BN) was developed and studied. The results indicated that the material achieved larger adsorption energies of 2.09 eV (201.66 kJ/mol, PBE-D). The electronic structure calculations suggested that the introduction of B N in p-BN induced defect electronic states in the energy gap region, which strongly impacted the adsorption properties of the material. The bonding between the B N defect and the CO 2 molecule was clarified, and it was found that the electron donation first occurred from CO 2 to the B N double-acceptor state then, followed by electron back-donation from B N to CO 2 accompanied by the formation of a B N -C bond. The thermodynamic properties indicated that the adsorption of CO 2 on the B N defect to form anionic CO 2 δ- species was spontaneous at temperatures below 350 K. Both the large adsorption energies and the thermodynamic properties ensured that p-BN with a B N defect could effectively capture CO 2 under ambient conditions. Finally, to evaluate the energetic stability, the defect formation energies were estimated. The formation energy of the B N defects was found to strongly depend on the chemical environment, and the selection of different reactants (B or N sources) would achieve the goal of reducing the formation energy. These findings provided a useful guidance for the design and fabrication of a porous BN sorbent for CO 2 capture.

Micro-Encapsulation of non-aqueous solvents for energy-efficient carbon capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Stolaroff, Joshua K; Ye, Congwang; Oakdale, James

Here, we demonstrate micro-encapsulation of several promising designer solvents: an IL, PCIL, and CO2BOL. We develop custom polymers that cure by UV light in the presence of each solvent while maintaining high CO2 permeability. We use several new process strategies to accommodate the viscosity and phase changes. We then measure and compare the CO2 absorption rate and capacity as well as the multi-cycle performance of the encapsulated solvents. These results are compared with previous work on encapsulated sodium carbonate solution. The prospects for designer solvents to reduce the cost of post-combustion capture and the implications for process design with encapsulatedmore » solvents are discussed.« less

Hyper-crosslinked cyclodextrin porous polymer: An efficient CO 2 capturing material with tunable porosity

DOE Office of Scientific and Technical Information (OSTI.GOV)

Meng, Bo; Li, Haiyang; East China Univ. of Science and Technology, Shanghai

We designed and synthesized the cyclodextrin (CD)-based hyper-crosslinked porous polymers (HCPPs) for selective CO 2 adsorption and storage. We also explored the effect of monomer size on micropore formation, and determined a feasible way to tailor the porosity of the materials during the hyper-crosslinking process.

Hyper-crosslinked cyclodextrin porous polymer: An efficient CO 2 capturing material with tunable porosity

DOE PAGES

Meng, Bo; Li, Haiyang; East China Univ. of Science and Technology, Shanghai; ...

2016-11-11

We designed and synthesized the cyclodextrin (CD)-based hyper-crosslinked porous polymers (HCPPs) for selective CO 2 adsorption and storage. We also explored the effect of monomer size on micropore formation, and determined a feasible way to tailor the porosity of the materials during the hyper-crosslinking process.

Novel ZIF-300 Mixed-Matrix Membranes for Efficient CO2 Capture.

PubMed

Yuan, Jianwei; Zhu, Haipeng; Sun, Jiajia; Mao, Yangyang; Liu, Gongping; Jin, Wanqin

2017-11-08

Because of the high separation performance and easy preparation, mixed-matrix membranes (MMMs) consisting of metal-organic frameworks have received much attention. In this article, we report a novel ZIF-300/PEBA MMM consisting of zeolite imidazolate framework (ZIF-300) crystals and polyether block amide (PEBA) matrix. The ZIF-300 crystal size was effectively reduced by optimizing the hydrothermal reaction condition from ∼15 to ∼1 μm. The morphology and physicochemical and sorption properties of the synthesized ZIF-300 crystals and as-prepared ZIF-300/PEBA MMMs were systematically studied. The results showed that ZIF-300 crystals with a size of ∼1 μm maintained excellent preferential CO 2 sorption over N 2 without degradation of the crystal structure in the MMMs. As a result, uniformly incorporated ZIF-300 crystals highly enhanced both the CO 2 permeability and the CO 2 /N 2 selectivity of pure PEBA membrane. The optimized ZIF-300-PEBA MMMs with a ZIF-300 loading of 30 wt % exhibited a high and stable CO 2 permeability of 83 Barrer and CO 2 /N 2 selectivity of 84, which are 59.2% and 53.5% higher than pure PEBA membrane, respectively. The obtained performance surpassed the upper bound of state-of-the-art membranes for CO 2 /N 2 separation. This work demonstrated that the proposed ZIF-300/PEBA MMM could be a potential candidate for an efficient CO 2 capture process.

Charged Covalent Triazine Frameworks for CO2 Capture and Conversion.

PubMed

Buyukcakir, Onur; Je, Sang Hyun; Talapaneni, Siddulu Naidu; Kim, Daeok; Coskun, Ali

2017-03-01

The quest for the development of new porous materials addressing both CO 2 capture from various sources and its conversion into useful products is a very active research area and also critical in order to develop a more sustainable and environmentally-friendly society. Here, we present the first charged covalent triazine framework (cCTF) prepared by simply heating nitrile functionalized dicationic viologen derivatives under ionothermal reaction conditions using ZnCl 2 as both solvent and trimerization catalyst. It has been demonstrated that the surface area, pore volume/size of cCTFs can be simply controlled by varying the synthesis temperature and the ZnCl 2 content. Specifically, increasing the reaction temperature led to controlled increase in the mesopore content and facilitated the formation of hierarchical porosity, which is critical to ensure efficient mass transport within porous materials. The resulting cCTFs showed high specific surface areas up to 1247 m 2 g -1 , and high physicochemical stability. The incorporation of ionic functional moieties to porous organic polymers improved substantially their CO 2 affinity (up to 133 mg g -1 , at 1 bar and 273 K) and transformed them into hierarchically porous organocatalysts for CO 2 conversion. More importantly, the ionic nature of cCTFs, homogeneous charge distribution together with hierarchical porosity offered a perfect platform for the catalytic conversion of CO 2 into cyclic carbonates in the presence of epoxides through an atom economy reaction in high yields and exclusive product selectivity. These results clearly demonstrate the promising aspect of incorporation of charged units into the porous organic polymers for the development of highly efficient porous organocatalysts for CO 2 capture and fixation.

Carbon Dioxide (CO2) Adsorption by Activated Carbon Functionalized with Deep Eutectic Solvent (DES)

NASA Astrophysics Data System (ADS)

Zulkurnai, N. Z.; Ali, U. F. Md.; Ibrahim, N.; Manan, N. S. Abdul

2017-06-01

In recent years, carbon dioxide (CO2) emission has become a major concern as the amount of the emitted gas significantly increases annually. Consequently, this phenomenon contributes to global warming. Several CO2 capture methods, including chemical adsorption by activated carbon, have been proposed. In this study, activated carbon was prepared from sea mango (Cerbera odollam), which was functionalized with deep eutectic solvent (DES) composed of choline chloride and glycerol to increase the efficiency of CO2 capture. The samples underwent pre-carbonization and carbonization processes at 200 °C and 500 °C, respectively, with nitrogen gas and flowing several gases, namely, CO2 and steam, and then followed by impregnation with 50 phosphoric acid (H3PO4) at 1:2 precursor-to-activant ratio. The prepared activated carbon was impregnated with DES at 1:2 precursor-to-activant ratio. The optimum CO2 adsorption capacity of the activated carbon was obtained by using CO2 gas treatment method (9.851 mgCO2/gsol), followed by the absence of gases (9.685 mgCO2/gsol), steam (9.636 mgCO2/gsol), and N2 (9.536 mgCO2/gsol).

Porous Ionic Polymers as a Robust and Efficient Platform for Capture and Chemical Fixation of Atmospheric CO2.

PubMed

Sun, Qi; Jin, Yingyin; Aguila, Briana; Meng, Xiangju; Ma, Shengqian; Xiao, Feng-Shou

2017-03-22

Direct use of atmospheric CO 2 as a C 1 source to synthesize high-value chemicals through environmentally benign processes is of great interest, yet challenging. Porous heterogeneous catalysts that are capable of simultaneously capturing and converting CO 2 are promising candidates for such applications. Herein, a family of organic ionic polymers with nanoporous structure, large surface area, strong affinity for CO 2 , and very high density of catalytic active sites (halide ions) was synthesized through the free-radical polymerization of vinylfunctionalized quaternary phosphonium salts. The resultant porous ionic polymers (PIPs) exhibit excellent activities in the cycloaddition of epoxides with atmospheric CO 2 , outperforming the corresponding soluble phosphonium salt analogues and ranking among the highest of known metal-free catalytic systems. The high CO 2 uptake capacity of the PIPs facilitates the enrichment of CO 2 molecules around the catalytic centers, thereby benefiting its conversion. We have demonstrated for the first time that atmospheric CO 2 can be directly converted to cyclic carbonates at room temperature using a heterogeneous catalytic system under metal-solvent free conditions. Moreover, the catalysts proved to be robust and fully recyclable, demonstrating promising potential for practical utilization for the chemical fixation of CO 2 . Our work thereby paves a way to the advance of PIPs as a new type of platform for capture and conversion of CO 2 . © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Final Techno-Economic Analysis of 550 MWe Supercritical PC Power Plant CO 2 Capture with Linde-BASF Advanced PCC Technology

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bostick, Devin; Stoffregen, Torsten; Rigby, Sean

This topical report presents the techno-economic evaluation of a 550 MWe supercritical pulverized coal (PC) power plant utilizing Illinois No. 6 coal as fuel, integrated with 1) a previously presented (for a subcritical PC plant) Linde-BASF post-combustion CO 2 capture (PCC) plant incorporating BASF’s OASE® blue aqueous amine-based solvent (LB1) [Ref. 6] and 2) a new Linde-BASF PCC plant incorporating the same BASF OASE® blue solvent that features an advanced stripper interstage heater design (SIH) to optimize heat recovery in the PCC process. The process simulation and modeling for this report is performed using Aspen Plus V8.8. Technical information frommore » the PCC plant is determined using BASF’s proprietary thermodynamic and process simulation models. The simulations developed and resulting cost estimates are first validated by reproducing the results of DOE/NETL Case 12 representing a 550 MWe supercritical PC-fired power plant with PCC incorporating a monoethanolamine (MEA) solvent as used in the DOE/NETL Case 12 reference [Ref. 2]. The results of the techno-economic assessment are shown comparing two specific options utilizing the BASF OASE® blue solvent technology (LB1 and SIH) to the DOE/NETL Case 12 reference. The results are shown comparing the energy demand for PCC, the incremental fuel requirement, and the net higher heating value (HHV) efficiency of the PC power plant integrated with the PCC plant. A comparison of the capital costs for each PCC plant configuration corresponding to a net 550 MWe power generation is also presented. Lastly, a cost of electricity (COE) and cost of CO 2 captured assessment is shown illustrating the substantial cost reductions achieved with the Linde-BASF PCC plant utilizing the advanced SIH configuration in combination with BASF’s OASE® blue solvent technology as compared to the DOE/NETL Case 12 reference. The key factors contributing to the reduction of COE and the cost of CO 2 captured, along with quantification of the magnitude of the reductions achieved by each of these factors, are also discussed. Additionally, a high-level techno-economic analysis of one more highly advanced Linde-BASF PCC configuration case (LB1-CREB) is also presented to demonstrate the significant impact of innovative PCC plant process design improvements on further reducing COE and cost of CO 2 captured for overall plant cost and performance comparison purposes. Overall, the net efficiency of the integrated 550 MWe supercritical PC power plant with CO 2 capture is increased from 28.4% with the DOE/NETL Case 12 reference to 30.9% with the Linde-BASF PCC plant previously presented utilizing the BASF OASE® blue solvent [Ref. 6], and is further increased to 31.4% using Linde-BASF PCC plant with BASF OASE® blue solvent and an advanced SIH configuration. The Linde-BASF PCC plant incorporating the BASF OASE® blue solvent also results in significantly lower overall capital costs, thereby reducing the COE and cost of CO 2 captured from $147.25/MWh and $56.49/MT CO 2, respectively, for the reference DOE/NETL Case 12 plant, to $128.49/MWh and $41.85/MT CO 2 for process case LB1, respectively, and $126.65/MWh and $40.66/MT CO 2 for process case SIH, respectively. With additional innovative Linde-BASF PCC process configuration improvements, the COE and cost of CO2 captured can be further reduced to $125.51/MWh and $39.90/MT CO 2 for LB1-CREB. Most notably, the Linde-BASF process options presented here have already demonstrated the potential to lower the cost of CO2 captured below the DOE target of $40/MT CO 2 at the 550 MWe scale for second generation PCC technologies.« less

Co-location of air capture, sub-ocean CO2 storage and energy production on the Kerguelen plateau

NASA Astrophysics Data System (ADS)

Goldberg, D.; Han, P.; Lackner, K.; Wang, T.

2011-12-01

How can carbon capture and storage activities be sustained from an energy perspective while keeping the entire activity out of sight and away from material risk and social refrain near populated areas? In light of reducing the atmospheric CO2 level to mitigate its effect on climate change, the combination of new air-capture technologies and large offshore storage reservoirs, supplemented by carbon neutral renewable energy, could address both of these engineering and public policy concerns. Because CO2 mixes rapidly in the atmosphere, air capture scrubbers could be located anywhere in the world. Although the power requirements for this technology may reduce net efficiencies, the local availability of carbon-neutral renewable energy for this purpose would eliminate some net energy loss. Certain locations where wind speeds are high and steady, such as those observed at high latitude and across the open ocean, appeal as carbon-neutral energy sources in close proximity to immense and secure reservoirs for geological sequestration of captured CO2. In particular, sub-ocean basalt flows are vast and carry minimal risks of leakage and damages compared to on-land sites. Such implementation of a localized renewable energy source coupled with carbon capture and storage infrastructure could result in a global impact of lowered CO2 levels. We consider an extreme location on the Kerguelen plateau in the southern Indian Ocean, where high wind speeds and basalt storage reservoirs are both plentiful. Though endowed with these advantages, this mid-ocean location incurs clear material and economic challenges due to its remoteness and technological challenges for CO2 capture due to constant high humidity. We study the wind energy-air capture power balance and consider related factors in the feasibility of this location for carbon capture and storage. Other remote oceanic sites where steady winds blow and near large geological reservoirs may be viable as well, although all would require extensive research. Using these mitigation technologies in combination may offer a pivotal option for reducing atmospheric carbon to pre-industrial levels with minimal human risk or inconvenience.

Asphalt-derived high surface area activated porous carbons for carbon dioxide capture.

PubMed

Jalilov, Almaz S; Ruan, Gedeng; Hwang, Chih-Chau; Schipper, Desmond E; Tour, Josiah J; Li, Yilun; Fei, Huilong; Samuel, Errol L G; Tour, James M

2015-01-21

Research activity toward the development of new sorbents for carbon dioxide (CO2) capture have been increasing quickly. Despite the variety of existing materials with high surface areas and high CO2 uptake performances, the cost of the materials remains a dominant factor in slowing their industrial applications. Here we report preparation and CO2 uptake performance of microporous carbon materials synthesized from asphalt, a very inexpensive carbon source. Carbonization of asphalt with potassium hydroxide (KOH) at high temperatures (>600 °C) yields porous carbon materials (A-PC) with high surface areas of up to 2780 m(2) g(-1) and high CO2 uptake performance of 21 mmol g(-1) or 93 wt % at 30 bar and 25 °C. Furthermore, nitrogen doping and reduction with hydrogen yields active N-doped materials (A-NPC and A-rNPC) containing up to 9.3% nitrogen, making them nucleophilic porous carbons with further increase in the Brunauer-Emmett-Teller (BET) surface areas up to 2860 m(2) g(-1) for A-NPC and CO2 uptake to 26 mmol g(-1) or 114 wt % at 30 bar and 25 °C for A-rNPC. This is the highest reported CO2 uptake among the family of the activated porous carbonaceous materials. Thus, the porous carbon materials from asphalt have excellent properties for reversibly capturing CO2 at the well-head during the extraction of natural gas, a naturally occurring high pressure source of CO2. Through a pressure swing sorption process, when the asphalt-derived material is returned to 1 bar, the CO2 is released, thereby rendering a reversible capture medium that is highly efficient yet very inexpensive.

Metal–organic framework based mixed matrix membranes: a solution for highly efficient CO2 capture?† †Electronic supplementary information (ESI) available. See DOI: 10.1039/c4cs00437j Click here for additional data file.

PubMed Central

Seoane, Beatriz; Coronas, Joaquin; Gascon, Ignacio; Benavides, Miren Etxeberria; Karvan, Oğuz; Caro, Jürgen; Kapteijn, Freek

2015-01-01

The field of metal–organic framework based mixed matrix membranes (M4s) is critically reviewed, with special emphasis on their application in CO2 capture during energy generation. After introducing the most relevant parameters affecting membrane performance, we define targets in terms of selectivity and productivity based on existing literature on process design for pre- and post-combustion CO2 capture. Subsequently, the state of the art in M4s is reviewed against these targets. Because final application of these membranes will only be possible if thin separation layers can be produced, the latest advances in the manufacture of M4 hollow fibers are discussed. Finally, the recent efforts in understanding the separation performance of these complex composite materials and future research directions are outlined. PMID:25692487

Graphene Oxide Membranes with Heterogeneous Nanodomains for Efficient CO2 Separations.

PubMed

Wang, Shaofei; Xie, Yu; He, Guangwei; Xin, Qingping; Zhang, Jinhui; Yang, Leixin; Li, Yifan; Wu, Hong; Zhang, Yuzhong; Guiver, Michael D; Jiang, Zhongyi

2017-11-06

Achieving high membrane performance in terms of gas permeance and carbon dioxide selectivity is an important target in carbon capture. Aiming to manipulate the channel affinity towards CO 2 to implement efficient separations, gas separation membranes containing CO 2 -philic and non-CO 2 -philic nanodomains in the interlayer channels of graphene oxide (GO) were formed by intercalating poly(ethylene glycol) diamines (PEGDA). PEGDA reacts with epoxy groups on the GO surface, constructing CO 2 -philic nanodomains and rendering a high sorption capacity, whereas unreacted GO surfaces give non-CO 2 -philic nanodomains, rendering low-friction diffusion. Owing to the orderly stacking of nanochannels through cross-linking and the heterogeneous nanodomains with moderate CO 2 affinity, a GO-PEGDA500 membrane exhibits a high CO 2 permeance of 175.5 GPU and a CO 2 /CH 4 selectivity of 69.5, which is the highest performance reported for dry-state GO-stacking membranes. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

The Role of Natural Gas Power Plants with Carbon Capture and Storage in a Low-Carbon Future

EPA Science Inventory

Natural gas combined-cycle (NGCC) turbines with carbon capture and storage (CCS) are a promising technology for reducing carbon dioxide (CO2) emissions in the electric sector. However, the high cost and efficiency penalties associated with CCS, as well as methane leakage from nat...

[Fluorine removal efficiency of organic-calcium during coal combustion].

PubMed

Liu, Jing; Liu, Jian-Zhong; Zhou, Jun-Hu; Xiao, Hai-Ping; Cen, Ke-Fa

2006-08-01

Effectiveness of calcium magnesium acetate (CMA) and calcium acetate(CA) as feasible HF capture were studied by means of fixed bed tube furnaces. The effects of temperature, particle diameter and Ca/S molar ratio on the fluorine removal efficiency were studied. By contract with CaCO3 at the same condition, we find that the HF capture effectiveness of those sorbents is superior to CaCO3, especially at high temperature. At 1 000 - 1 100 degrees C, the efficiency of fluorine removal during coal combustion of CMA is 1.68 - 1.74 times as that of CaCO3; the efficiency of fluorine removal during coal combustion of CA is 1.28 - 1.37 times as that of CaCO3.

Efficient Purification and Release of Circulating Tumor Cells by Synergistic Effect of Biomarker and SiO2 @Gel-Microbead-Based Size Difference Amplification.

PubMed

Huang, Qinqin; Cai, Bo; Chen, Bolei; Rao, Lang; He, Zhaobo; He, Rongxiang; Guo, Feng; Zhao, Libo; Kondamareddy, Kiran Kumar; Liu, Wei; Guo, Shishang; Zhao, Xing-Zhong

2016-07-01

Microfluidics-based circulating tumor cell (CTC) isolation is achieved by using gelatin-coated silica microbeads conjugated to CTC-specific antibodies. Bead-binding selectively enlarges target cell size, providing efficient high-purity capture. CTCs captured can be further released non-invasively. This stratagem enables high-performance CTC isolation for subsequent studies. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Balsam-Pear-Skin-Like Porous Polyacrylonitrile Nanofibrous Membranes Grafted with Polyethyleneimine for Postcombustion CO2 Capture.

PubMed

Zhang, Yufei; Guan, Jiming; Wang, Xianfeng; Yu, Jianyong; Ding, Bin

2017-11-22

Amine-containing sorbents have been extensively studied for postcombustion carbon dioxide (CO 2 ) capture because of their ability to chemisorb CO 2 from the flue gas. However, most sorbents are in the form of powders currently, which is not the ideal configuration for the flue gas separation because of the fragile nature and poor mechanical properties, resulting in blocking of the flow pipes and difficult recycling. Herein, we present a novel approach for the facile fabrication of flexible, robust, and polyethyleneimine-grafted (PEI-grafted) hydrolyzed porous PAN nanofibrous membranes (HPPAN-PEI NFMs) through the combination of electrospinning, pore-forming process, hydrolysis reaction, and the subsequent grafting technique. Excitingly, we find that all the resultant porous PAN (PPAN) fibers exhibit a balsam-pear-skin-like porous structure due to the selective removal of poly(vinylpyrrolidone) (PVP) from PAN/PVP fibers by water extraction. Significantly, the HPPAN-PEI NFMs retain their mesoporosity, as well as exhibit good thermal stability and prominent tensile strength (11.1 MPa) after grafting, guaranteeing their application in CO 2 trapping from the flue gas. When exposed to CO 2 at 40 °C, the HPPAN-PEI NFMs show an enhanced CO 2 adsorption capacity of 1.23 mmol g -1 (based on the overall quantity of the sample) or 6.15 mmol g -1 (based on the quantity of grafted PEI). Moreover, the developed HPPAN-PEI NFMs display significantly selective capture for CO 2 over N 2 and excellent recyclability. The CO 2 capacity retains 92% of the initial value after 20 adsorption-desorption cycle tests, indicating that the resultant HPPAN-PEI NFMs have good long-term stability. This work paves the way for fabricating NFM-based solid adsorption materials endowed with a porous structure applied to efficient postcombustion CO 2 capture.

Assessing Atmospheric CO2 Entrapped in Clay Nanotubes using Residual Gas Analyzer.

PubMed

Das, Sankar; Maity, Abhijit; Pradhan, Manik; Jana, Subhra

2016-02-16

A residual gas analyzer (RGA) coupled with a high-vacuum chamber has been explored to measure atmospheric CO2 entrapped in aminosilane-modified clay nanotubes. Ambient CO2 uptake efficacy together with stability of these novel adsorbents composed of both primary and/or secondary amine sites has been demonstrated at standard ambient temperature and pressure. The unprecedented sensitivity and accuracy of the RGA-based mass spectrometry technique toward atmospheric CO2 measurement has been substantiated with a laser-based optical cavity-enhanced integrated cavity output spectroscopy. The adsorption kinetics of atmospheric CO2 on amine-functionalized clay nanotubes followed the fractional-order kinetic model compared to that of the pseudo-first-order or pseudo-second-order rate equations. The efficiency along with stability of these novel adsorbents has also been demonstrated by their repetitive use for CO2 capture in the oxidative environment. Our findings thus point to a fundamental study on the atmospheric CO2 adsorption by amine-loaded adsorbents using an easy handling and low-cost benchtop RGA-based mass spectrometer, opening a new strategy for CO2 capture and sequestering study.

Sourcing of Steam and Electricity for Carbon Capture Retrofits.

PubMed

Supekar, Sarang D; Skerlos, Steven J

2017-11-07

This paper compares different steam and electricity sources for carbon capture and sequestration (CCS) retrofits of pulverized coal (PC) and natural gas combined cycle (NGCC) power plants. Analytical expressions for the thermal efficiency of these power plants are derived under 16 different CCS retrofit scenarios for the purpose of illustrating their environmental and economic characteristics. The scenarios emerge from combinations of steam and electricity sources, fuel used in each source, steam generation equipment and process details, and the extent of CO 2 capture. Comparing these scenarios reveals distinct trade-offs between thermal efficiency, net power output, levelized cost, profit, and net CO 2 reduction. Despite causing the highest loss in useful power output, bleeding steam and extracting electric power from the main power plant to meet the CCS plant's electricity and steam demand maximizes plant efficiency and profit while minimizing emissions and levelized cost when wholesale electricity prices are below 4.5 and 5.2 US¢/kWh for PC-CCS and NGCC-CCS plants, respectively. At prices higher than these higher profits for operating CCS retrofits can be obtained by meeting 100% of the CCS plant's electric power demand using an auxiliary natural gas turbine-based combined heat and power plant.

Effective Approach for Increasing the Heteroatom Doping Levels of Porous Carbons for Superior CO2 Capture and Separation Performance.

PubMed

Abdelmoaty, Yomna H; Tessema, Tsemre-Dingel; Norouzi, Nazgol; El-Kadri, Oussama M; Turner, Joseph B McGee; El-Kaderi, Hani M

2017-10-18

Development of efficient sorbents for carbon dioxide (CO 2 ) capture from flue gas or its removal from natural gas and landfill gas is very important for environmental protection. A new series of heteroatom-doped porous carbon was synthesized directly from pyrazole/KOH by thermolysis. The resulting pyrazole-derived carbons (PYDCs) are highly doped with nitrogen (14.9-15.5 wt %) as a result of the high nitrogen-to-carbon ratio in pyrazole (43 wt %) and also have a high oxygen content (16.4-18.4 wt %). PYDCs have a high surface area (SA BET = 1266-2013 m 2 g -1 ), high CO 2 Q st (33.2-37.1 kJ mol -1 ), and a combination of mesoporous and microporous pores. PYDCs exhibit significantly high CO 2 uptakes that reach 2.15 and 6.06 mmol g -1 at 0.15 and 1 bar, respectively, at 298 K. At 273 K, the CO 2 uptake improves to 3.7 and 8.59 mmol g -1 at 0.15 and 1 bar, respectively. The reported porous carbons also show significantly high adsorption selectivity for CO 2 /N 2 (128) and CO 2 /CH 4 (13.4) according to ideal adsorbed solution theory calculations at 298 K. Gas breakthrough studies of CO 2 /N 2 (10:90) at 298 K showed that PYDCs display excellent separation properties. The ability to tailor the physical properties of PYDCs as well as their chemical composition provides an effective strategy for designing efficient CO 2 sorbents.

Doping of alkali, alkaline-earth, and transition metals in covalent-organic frameworks for enhancing CO2 capture by first-principles calculations and molecular simulations.

PubMed

Lan, Jianhui; Cao, Dapeng; Wang, Wenchuan; Smit, Berend

2010-07-27

We use the multiscale simulation approach, which combines the first-principles calculations and grand canonical Monte Carlo simulations, to comprehensively study the doping of a series of alkali (Li, Na, and K), alkaline-earth (Be, Mg, and Ca), and transition (Sc and Ti) metals in nanoporous covalent organic frameworks (COFs), and the effects of the doped metals on CO2 capture. The results indicate that, among all the metals studied, Li, Sc, and Ti can bind with COFs stably, while Be, Mg, and Ca cannot, because the binding of Be, Mg, and Ca with COFs is very weak. Furthermore, Li, Sc, and Ti can improve the uptakes of CO2 in COFs significantly. However, the binding energy of a CO2 molecule with Sc and Ti exceeds the lower limit of chemisorptions and, thus, suffers from the difficulty of desorption. By the comparative studies above, it is found that Li is the best surface modifier of COFs for CO2 capture among all the metals studied. Therefore, we further investigate the uptakes of CO2 in the Li-doped COFs. Our simulation results show that at 298 K and 1 bar, the excess CO2 uptakes of the Li-doped COF-102 and COF-105 reach 409 and 344 mg/g, which are about eight and four times those in the nondoped ones, respectively. As the pressure increases to 40 bar, the CO2 uptakes of the Li-doped COF-102 and COF-105 reach 1349 and 2266 mg/g at 298 K, respectively, which are among the reported highest scores to date. In summary, doping of metals in porous COFs provides an efficient approach for enhancing CO2 capture.

Optimizing and Quantifying CO 2 Storage Resource in Saline Formations and Hydrocarbon Reservoirs

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bosshart, Nicholas W.; Ayash, Scott C.; Azzolina, Nicholas A.

In an effort to reduce carbon dioxide (CO 2) emissions from large stationary sources, carbon capture and storage (CCS) is being investigated as one approach. This work assesses CO 2 storage resource estimation methods for deep saline formations (DSFs) and hydrocarbon reservoirs undergoing CO 2 enhanced oil recovery (EOR). Project activities were conducted using geologic modeling and simulation to investigate CO 2 storage efficiency. CO 2 storage rates and efficiencies in DSFs classified by interpreted depositional environment were evaluated at the regional scale over a 100-year time frame. A focus was placed on developing results applicable to future widespread commercial-scalemore » CO 2 storage operations in which an array of injection wells may be used to optimize storage in saline formations. The results of this work suggest future investigations of prospective storage resource in closed or semiclosed formations need not have a detailed understanding of the depositional environment of the reservoir to generate meaningful estimates. However, the results of this work also illustrate the relative importance of depositional environment, formation depth, structural geometry, and boundary conditions on the rate of CO 2 storage in these types of systems. CO 2 EOR occupies an important place in the realm of geologic storage of CO 2, as it is likely to be the primary means of geologic CO 2 storage during the early stages of commercial implementation, given the lack of a national policy and the viability of the current business case. This work estimates CO 2 storage efficiency factors using a unique industry database of CO 2 EOR sites and 18 different reservoir simulation models capturing fluvial clastic and shallow shelf carbonate depositional environments for reservoir depths of 1219 and 2438 meters (4000 and 8000 feet) and 7.6-, 20-, and 64-meter (25-, 66,- and 209-foot) pay zones. The results of this work provide practical information that can be used to quantify CO 2 storage resource estimates in oil reservoirs during CO 2 EOR operations (as opposed to storage following depletion) and the uncertainty associated with those estimates.« less

Reducing cement's CO2 footprint

USGS Publications Warehouse

van Oss, Hendrik G.

2011-01-01

The manufacturing process for Portland cement causes high levels of greenhouse gas emissions. However, environmental impacts can be reduced by using more energy-efficient kilns and replacing fossil energy with alternative fuels. Although carbon capture and new cements with less CO2 emission are still in the experimental phase, all these innovations can help develop a cleaner cement industry.

Environmental Benefit Assessment for the Carbonation Process of Petroleum Coke Fly Ash in a Rotating Packed Bed.

PubMed

Pei, Si-Lu; Pan, Shu-Yuan; Li, Ye-Mei; Chiang, Pen-Chi

2017-09-19

A high-gravity carbonation process was deployed at a petrochemical plant using petroleum coke fly ash and blowdown wastewater to simultaneously mineralized CO 2 and remove nitrogen oxides and particulate matters from the flue gas. With a high-gravity carbonation process, the CO 2 removal efficiency was found to be 95.6%, corresponding to a capture capacity of 600 kg CO 2 per day, at a gas flow rate of 1.47 m 3 /min under ambient temperature and pressure. Moreover, the removal efficiency of nitrogen oxides and particulate matters was 99.1% and 83.2%, respectively. After carbonation, the reacted fly ash was further utilized as supplementary cementitious materials in the blended cement mortar. The results indicated that cement with carbonated fly ash exhibited superior compressive strength (38.1 ± 2.5 MPa at 28 days in 5% substitution ratio) compared to the cement with fresh fly ash. Furthermore, the environmental benefits for the high-gravity carbonation process using fly ash were critically assessed. The energy consumption of the entire high-gravity carbonation ranged from 80 to 169 kWh/t-CO 2 (0.29-0.61 GJ/t-CO 2 ). Compared with the scenarios of business-as-usual and conventional carbon capture and storage plant, the economic benefit from the high-gravity carbonation process was approximately 90 and 74 USD per ton of CO 2 fixation, respectively.

The Quest CCS Project - MMV Technology Deployment Through Two Years of Operation

NASA Astrophysics Data System (ADS)

O'Brien, S.

2017-12-01

In September 2012, Shell, on behalf of the Athabasca Oil Sands Project venture (Shell Canada Energy, Chevron Canada Limited, Marathon Oil Canada Corporation), announced that it was proceeding to construct the Quest Carbon Capture and Storage (CCS) project near Fort Saskatchewan. Quest is the world's first large-scale commercial application of CCS at an oil sands operation, and it is now capturing more than one million tonnes of CO2 per year from the Scotford Upgrader. It is a fully integrated project, involving CO2 capture at the bitumen upgrader, transportation along a 65 km pipeline, and CO2 storage in a deep saline aquifer (the Basal Cambrian Sands). Construction was completed in August 2015, and the Quest project was certified for commercial operation in September 2015. The Measurement, Monitoring and Verification (MMV) program for Quest is comprehensive, with a variety of technologies being used to monitor the atmosphere, hydrosphere, biosphere and geosphere. These include a Lightsource system for atmospheric monitoring, extensive groundwater sampling, DAS VSPs to assess the development of the CO2 plume, a microseismic array to measure any induced seismic activity, and temperature and pressure gauges for reservoir monitoring. Over two years of operations, this program has been optimized to address key risks while improving operational efficiency. Quest has now successfully captured and stored more than 2 million tonnes of CO2 with no MMV indications of any storage issues.

Reinventing Design Principles for Developing Low-Viscosity Carbon Dioxide-Binding Organic Liquids for Flue Gas Clean Up

DOE Office of Scientific and Technical Information (OSTI.GOV)

None, None

2017-01-11

Anthropogenic carbon dioxide (CO 2) emission from point sources, such as coal fired-power plants, account for the majority of the green houses gasses in the atmosphere. Capture, storage and utilization are required to mitigate adverse environmental effects. Aqueous amine-based CO 2 capture solvents are currently considered the industry standard, but deployment to market is limited by their high regeneration energy demand. In that context, energy efficient and less-viscous water-lean transformational solvent systems known as CO 2 Binding Organic Liquids (CO 2BOLs) are being developed in our group to advance this technology to commercialization. Herein, we present a logical design approachmore » based on fundamental concepts of organic chemistry and computer simulations aimed at lowering solvent viscosity. Conceptually, viscosity reduction would be achieved by systemmatic methods such as introduction of steric hindrance on the anion to minimize the intermolecular cation-anion interactions, fine tuning the electronics, hydrogen bonding orientation and strength, and charge solvation. Conventional standard trial-and-error approaches while effective, are time consuming and economically expensive. Herein, we rethink the metrics and design principles of low-viscosity CO 2 capture solvents using a combined synthesis and computational modeling approach. We critically study the impacts of modyfying factors such as as orientation of hydrogen bonding, introduction of higher degrees of freedom and cation or anion charge solvation and assess if or how each factor impacts viscosity of CO 2BOL CO 2 capture solvents. Ultimately, we found that hydrogen bond orientation and strength is predominantly influencing the viscosity in CO 2BOL solvents. With this knowledge, a new 1-MEIPADM-2-BOL CO 2BOL variant was synthesized and tested, resulting in a solvent that is approximately 60% less viscous at 25 mol% CO 2 loading with respect to our base compound 1-IPADM-2-BOL. The insights gained from the current study redefines the fundamental concepts and understanding of what influences viscosity in concentrated organic CO 2 capture solvents.« less

Biomimetic CO2 capture using a highly thermostable bacterial α-carbonic anhydrase immobilized on a polyurethane foam.

PubMed

Migliardini, Fortunato; De Luca, Viviana; Carginale, Vincenzo; Rossi, Mosè; Corbo, Pasquale; Supuran, Claudiu T; Capasso, Clemente

2014-02-01

The biomimetic approach represents an interesting strategy for carbon dioxide (CO2) capture, offering advantages over other methods, due to its specificity for CO2 and its eco-compatibility, as it allows concentration of CO2 from other gases, and its conversion to water soluble ions. This approach uses microorganisms capable of fixing CO2 through metabolic pathways or via the use of an enzyme, such as carbonic anhydrase (CA, EC 4.2.1.1). Recently, our group cloned and purified a novel bacterial α-CA, named SspCA, from the thermophilic bacteria, Sulfurihydrogenibium yellowstonense YO3AOP1 living in hot springs at temperatures of up to 110 °C. This enzyme showed an exceptional thermal stability, retaining its high catalytic activity for the CO2 hydration reaction even after being heated at 70 °C for several hours. In the present paper, the SspCA was immobilized within a polyurethane (PU) foam. The immobilized enzyme was found to be catalytically active and showed a long-term stability. A bioreactor containing the "PU-immobilized enzyme" (PU-SspCA) as shredded foam was used for experimental tests aimed to verify the CO2 capture capability in conditions close to those of a power plant application. In this bioreactor, a gas phase, containing CO2, was put into contact with a liquid phase under conditions, where CO2 contained in the gas phase was absorbed and efficiently converted into bicarbonate by the extremo-α-CA.

CO2 capture from air by Chlorella vulgaris microalgae in an airlift photobioreactor.

PubMed

Sadeghizadeh, Aziz; Farhad Dad, Farid; Moghaddasi, Leila; Rahimi, Rahbar

2017-11-01

In this work, hydrodynamics and CO 2 biofixation study was conducted in an airlift bioreactor at the temperature of 30±2°C. The main objective of this work was to investigate the effect of high gas superficial velocity on CO 2 biofixation using Chlorella vulgaris microalgae and its growth. The study showed that Chlorella vulgaris in high input gas superficial velocity also had the ability to grow and remove the CO 2 by less than 80% efficiency. Copyright © 2017 Elsevier Ltd. All rights reserved.

Catalysis of CO₂ absorption in aqueous solution by inorganic oxoanions and their application to post combustion capture.

PubMed

Phan, Duong T; Maeder, Marcel; Burns, Robert C; Puxty, Graeme

2014-04-15

To reduce CO2 emission into the atmosphere, particularly from coal-fired power stations, post combustion capture (PCC) using amine-based solvents to chemically absorb CO2 has been extensively developed. From an infrastructure viewpoint, the faster the absorption of CO2, the smaller the absorber required. The use of catalysts for this process has been broadly studied. In this manuscript, a study of the catalytic efficiencies of inorganic oxoanions such as arsenite, arsenate, phosphite, phosphate, and borate is described. The kinetics of the accelerated CO2 absorption at 25 °C was investigated using stopped-flow spectrophotometry. The catalytic rate constants of these anions for the reaction of CO2 with H2O were determined to be 137.7(3), 30.3(7), 69(2), 32.7(9), and 13.66(7) M(-1)s(-1), respectively. A new mechanism for the catalytic reaction of oxoanions with CO2 has also been proposed. The applicability of these catalysts to PCC was further studied by simulation of the absorption process under PCC conditions using their experimental catalytic rate constants. Arsenite and phosphite were confirmed to be the best catalysts for CO2 capture. However, considering the toxicological effect of arsenic and the oxidative instability of phosphite, phosphate would be the most promising inorganic catalyst for PCC process from the series of inorganic oxoanions studied.

A CO2-Free Synthetic Host-Odor Mixture That Attracts and Captures Triatomines: Effect of Emitted Odorant Ratios.

PubMed

Guidobaldi, F; Guerenstein, P G

2016-07-01

Triatomines, vectors of Chagas Disease, are hematophagous insects. Efforts have been made to develop synthetic attractants based on vertebrate odor-to lure them into traps. However, because those lures are not practical or have low capture efficiency, they are not in use in control programs. Therefore, more work is needed to reach a practical and efficient odor lure. Recently, a three-component, CO 2 -free, synthetic blend of vertebrate odor (consisting of ammonia, l-(+)-lactic acid, and hexanoic acid), known as Sweetscent (Biogents AG, Regensburg, Germany), was shown to attract and capture triatomines in the laboratory. In this study, using a trap olfactometer and an odor blend with constituents similar to those of Sweetscent (delivered from low-density polyethylene sachets) we found that the odorant ratios of the mixtures have a strong effect in the capture of triatomines. The blend with the most efficient combination of odorant ratios evoked ca. 81% capture in two relevant triatomine species. In the case of the most effective odor mixtures, we measured the odor mass emission for the three components of the mixture and therefore were able to estimate the odorant ratios emitted that were responsible for such a high capture performance. Thus, in those mixtures, pentanoic acid was the main component (ca. 65 %) followed by ammonia (ca. 28%) and, l(+)-lactic acid (ca. 7 %). Our results are encouraging as efficient, practical, and cheap odor baits to trap triatomines in the field would be within reach. The odor-delivery system used should be improved to increase stability of odor emission. © The Authors 2016. Published by Oxford University Press on behalf of Entomological Society of America. All rights reserved. For Permissions, please email: journals.permissions@oup.com.

Electrochemical separation of hydrogen from reformate using PEM fuel cell technology

NASA Astrophysics Data System (ADS)

Gardner, C. L.; Ternan, M.

This article is an examination of the feasibility of electrochemically separating hydrogen obtained by steam reforming a hydrocarbon or alcohol source. A potential advantage of this process is that the carbon dioxide rich exhaust stream should be able to be captured and stored thereby reducing greenhouse gas emissions. Results are presented for the performance of the anode of proton exchange membrane (PEM) electrochemical cell for the separation of hydrogen from a H 2-CO 2 gas mixture and from a H 2-CO 2-CO gas mixture. Experiments were carried out using a single cell state-of-the-art PEM fuel cell. The anode was fed with either a H 2-CO 2 gas mixture or a H 2-CO 2-CO gas mixture and hydrogen was evolved at the cathode. All experiments were performed at room temperature and atmospheric pressure. With the H 2-CO 2 gas mixture the hydrogen extraction efficiency is quite high. When the gas mixture included CO, however, the hydrogen extraction efficiency is relatively poor. To improve the efficiency for the separation of the gas mixture containing CO, the effect of periodic pulsing on the anode potential was examined. Results show that pulsing can substantially reduce the anode potential thereby improving the overall efficiency of the separation process although the anode potential of the CO poisoned and pulsed cell still lies above that of an unpoisoned cell.

The cost of meeting increased cooling-water demands for CO2 capture and storage utilizing non-traditional waters from geologic saline formations

NASA Astrophysics Data System (ADS)

Klise, Geoffrey T.; Roach, Jesse D.; Kobos, Peter H.; Heath, Jason E.; Gutierrez, Karen A.

2013-05-01

Deep (> ˜800 m) saline water-bearing formations in the United States have substantial pore volume that is targeted for storage of carbon dioxide (CO2) and the associated saline water can be extracted to increase CO2 storage efficiency, manage pressure build up, and create a new water source that, once treated, can be used for power-plant cooling or other purposes. Extraction, treatment and disposal costs of saline formation water to meet added water demands from CO2 capture and storage (CCS) are discussed. This underutilized water source may be important in meeting new water demand associated with CCS. For a representative natural gas combined-cycle (NGCC) power plant, simultaneous extraction of brine from the storage formation could provide enough water to meet all CCS-related cooling demands for 177 out of the 185 (96 %) saline formations analyzed in this study. Calculated total cost of water extraction, treatment and disposal is less than 4.00 US Dollars (USD) m-3 for 93 % of the 185 formations considered. In 90 % of 185 formations, treated water costs are less than 10.00 USD tonne-1 of CO2 injected. On average, this represents approximately 6 % of the total CO2 capture and injection costs for the NGCC scenario.

CO2 Capture by Absorption with Potassium Carbonate

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gary T. Rochelle; Eric Chen; Babatunde Oyenekan

The objective of this work is to improve the process for CO{sub 2} capture by alkanolamine absorption/stripping by developing an alternative solvent, aqueous K{sub 2}CO{sub 3} promoted by piperazine. Ethylenediamine was detected in a degraded solution of MEA/PZ solution, suggesting that piperazine is subject to oxidation. Stripper modeling has demonstrated that vacuum strippers will be more energy efficient if constructed short and fat rather than tall and skinny. The matrix stripper has been identified as a configuration that will significantly reduce energy use. Extensive measurements of CO{sub 2} solubility in 7 m MEA at 40 and 60 C have confirmedmore » the work by Jou and Mather. Corrosion of carbon steel without inhibitors increases from 19 to 181 mpy in lean solutions of 6.2 m MEA/PZ as piperazine increases from 0 to 3.1 m.« less

The Potential Role of Natural Gas Power Plants with Carbon Capture and Storage as a Bridge to a Low-Carbon Future

EPA Science Inventory

Natural gas combined-cycle (NGCC) turbines with carbon capture and storage (CCS) are a promising technology for reducing carbon dioxide (CO2) emissions in the electric sector. However, the high cost and efficiency penalties associated with CCS, as well as methane leakage from nat...

PNNL Report on the Development of Bench-scale CFD Simulations for Gas Absorption across a Wetted Wall Column

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Chao; Xu, Zhijie; Lai, Canhai

This report is prepared for the demonstration of hierarchical prediction of carbon capture efficiency of a solvent-based absorption column. A computational fluid dynamics (CFD) model is first developed to simulate the core phenomena of solvent-based carbon capture, i.e., the CO2 physical absorption and chemical reaction, on a simplified geometry of wetted wall column (WWC) at bench scale. Aqueous solutions of ethanolamine (MEA) are commonly selected as a CO2 stream scrubbing liquid. CO2 is captured by both physical and chemical absorption using highly CO2 soluble and reactive solvent, MEA, during the scrubbing process. In order to provide confidence bound on themore » computational predictions of this complex engineering system, a hierarchical calibration and validation framework is proposed. The overall goal of this effort is to provide a mechanism-based predictive framework with confidence bound for overall mass transfer coefficient of the wetted wall column (WWC) with statistical analyses of the corresponding WWC experiments with increasing physical complexity.« less

Linking CO 2 Sorption Performance to Polymer Morphology in Aminopolymer/Silica Composites through Neutron Scattering

DOE PAGES

Holewinski, Adam; Sakwa-Novak, Miles A.; Jones, Christopher W.

2015-08-26

Composites of poly(ethylenimine) (PEI) and mesoporous silica are effective, reversible adsorbents for CO 2, both from flue gas and in direct air-capture applications. The morphology of the PEI within the silica can strongly impact the overall carbon capture efficiency and rate of saturation. Here, we directly probe the spatial distribution of the supported polymer through small-angle neutron scattering (SANS). Combined with textural characterization from physisorption analysis, the data indicate that PEI first forms a thin conformal coating on the pore walls, but all additional polymer aggregates into plug(s) that grow along the pore axis. This model is consistent with observedmore » trends in amine-efficiency (CO 2/N binding ratio) and pore size distributions, and points to a trade-off between achieving high chemical accessibility of the amine binding sites, which are inaccessible when they strongly interact with the silica, and high accessibility for mass transport, which can be hampered by diffusion through PEI plugs. In conclusion, we illustrate this design principle by demonstrating higher CO 2 capacity and uptake rate for PEI supported in a hydrophobically modified silica, which exhibits repulsive interactions with the PEI, freeing up binding sites.« less

CO2 Removal from Biogas by Cyanobacterium Leptolyngbya sp. CChF1 Isolated from the Lake Chapala, Mexico: Optimization of the Temperature and Light Intensity.

PubMed

Choix, Francisco J; Snell-Castro, Raúl; Arreola-Vargas, Jorge; Carbajal-López, Alberto; Méndez-Acosta, Hugo O

2017-12-01

In the present study, the capacity of the cyanobacterium Leptolyngbya sp. CChF1 to remove CO 2 from real and synthetic biogas was evaluated. The identification of the cyanobacterium, isolated from the lake Chapala, was carried out by means of morphological and molecular analyses, while its potential for CO 2 removal from biogas streams was evaluated by kinetic experiments and optimized by a central composite design coupled to a response surface methodology. Results demonstrated that Leptolyngbya sp. CChF1 is able to remove CO 2 and grow indistinctly in real or synthetic biogas streams, showing tolerance to high concentrations of CO 2 and CH 4 , 25 and 75%, respectively. The characterization of the biomass composition at the end of the kinetic assays revealed that the main accumulated by-products under both biogas streams were lipids, followed by proteins and carbohydrates. Regarding the optimization experiments, light intensity and temperature were the studied variables, while synthetic biogas was the carbon source. Results showed that light intensity was significant for CO 2 capture efficiency (p = 0.0290), while temperature was significant for biomass production (p = 0.0024). The predicted CO 2 capture efficiency under optimal conditions (27.1 °C and 920 lx) was 93.48%. Overall, the results of the present study suggest that Leptolyngbya sp. CChF1 is a suitable candidate for biogas upgrading.

A Diaminopropane-Appended Metal–Organic Framework Enabling Efficient CO 2 Capture from Coal Flue Gas via a Mixed Adsorption Mechanism

DOE Office of Scientific and Technical Information (OSTI.GOV)

Milner, Phillip J.; Siegelman, Rebecca L.; Forse, Alexander C.

A new diamine-functionalized metal–organic framework comprised of 2,2-dimethyl-1,3-diaminopropane (dmpn) appended to the Mg 2+ sites lining the channels of Mg 2(dobpdc) (dobpdc4– = 4,4'-dioxidobiphenyl-3,3'-dicarboxylate) is characterized for the removal of CO 2 from the flue gas emissions of coal-fired power plants. Unique to members of this promising class of adsorbents, dmpn–Mg2(dobpdc) displays facile step-shaped adsorption of CO 2 from coal flue gas at 40 °C and near complete CO 2 desorption upon heating to 100 °C, enabling a high CO 2 working capacity (2.42 mmol/g, 9.1 wt %) with a modest 60 °C temperature swing. Evaluation of the thermodynamic parametersmore » of adsorption for dmpn–Mg 2(dobpdc) suggests that the narrow temperature swing of its CO 2 adsorption steps is due to the high magnitude of its differential enthalpy of adsorption (Δhads = -73 ± 1 kJ/mol), with a larger than expected entropic penalty for CO 2 adsorption (Δsads = -204 ± 4 J/mol·K) positioning the step in the optimal range for carbon capture from coal flue gas. In addition, thermogravimetric analysis and breakthrough experiments indicate that, in contrast to many adsorbents, dmpn–Mg 2(dobpdc) captures CO 2 effectively in the presence of water and can be subjected to 1000 humid adsorption/desorption cycles with minimal degradation. Solid-state 13C NMR spectra and single-crystal X-ray diffraction structures of the Zn analogue reveal that this material adsorbs CO 2 via formation of both ammonium carbamates and carbamic acid pairs, the latter of which are crystallographically verified for the first time in a porous material. Taken together, these properties render dmpn–Mg 2(dobpdc) one of the most promising adsorbents for carbon capture applications.« less

A Diaminopropane-Appended Metal-Organic Framework Enabling Efficient CO2 Capture from Coal Flue Gas via a Mixed Adsorption Mechanism.

PubMed

Milner, Phillip J; Siegelman, Rebecca L; Forse, Alexander C; Gonzalez, Miguel I; Runčevski, Tomče; Martell, Jeffrey D; Reimer, Jeffrey A; Long, Jeffrey R

2017-09-27

A new diamine-functionalized metal-organic framework comprised of 2,2-dimethyl-1,3-diaminopropane (dmpn) appended to the Mg 2+ sites lining the channels of Mg 2 (dobpdc) (dobpdc 4- = 4,4'-dioxidobiphenyl-3,3'-dicarboxylate) is characterized for the removal of CO 2 from the flue gas emissions of coal-fired power plants. Unique to members of this promising class of adsorbents, dmpn-Mg 2 (dobpdc) displays facile step-shaped adsorption of CO 2 from coal flue gas at 40 °C and near complete CO 2 desorption upon heating to 100 °C, enabling a high CO 2 working capacity (2.42 mmol/g, 9.1 wt %) with a modest 60 °C temperature swing. Evaluation of the thermodynamic parameters of adsorption for dmpn-Mg 2 (dobpdc) suggests that the narrow temperature swing of its CO 2 adsorption steps is due to the high magnitude of its differential enthalpy of adsorption (Δh ads = -73 ± 1 kJ/mol), with a larger than expected entropic penalty for CO 2 adsorption (Δs ads = -204 ± 4 J/mol·K) positioning the step in the optimal range for carbon capture from coal flue gas. In addition, thermogravimetric analysis and breakthrough experiments indicate that, in contrast to many adsorbents, dmpn-Mg 2 (dobpdc) captures CO 2 effectively in the presence of water and can be subjected to 1000 humid adsorption/desorption cycles with minimal degradation. Solid-state 13 C NMR spectra and single-crystal X-ray diffraction structures of the Zn analogue reveal that this material adsorbs CO 2 via formation of both ammonium carbamates and carbamic acid pairs, the latter of which are crystallographically verified for the first time in a porous material. Taken together, these properties render dmpn-Mg 2 (dobpdc) one of the most promising adsorbents for carbon capture applications.

Cu-BTC/aminated graphite oxide composites as high-efficiency CO2 capture media.

PubMed

Policicchio, Alfonso; Zhao, Yunxia; Zhong, Qin; Agostino, Raffaele G; Bandosz, Teresa J

2014-01-08

CO2 adsorption isotherms on Cu-BTC/aminated graphite oxide composites were measured in the pressure range up to 1.5 MPa at three different temperatures close to ambient. Adsorption capacity, isosteric heat of adsorption, and regenerability were investigated. They are considered as significant factors determining the practical application of materials for CO2 capture. The results indicate a significant improvement in the performance of the composites as CO2 adsorbents in comparison with the parent Cu-BTC MOF. Among all samples analyzed, the composite of Cu-BTC and modified graphite oxide with the highest N content (MOF/GO-U3) is the best performing sample. On its surface 13.41 mmol/g CO2 was adsorbed at room temperature and 1.5 MPa. A high selectivity for CO2 adsorption over that of CH4 was found. The selectivities for CO2 adsorption over N2 are governed by the properties of the MOF phase. A relatively low heat of CO2 adsorption and the high degree of surface homogeneity cause that the composites can be fully regenerated and used in multicycle adsorption with the minimum energy demand.

Imine-Linked Polymer Based Nitrogen-Doped Porous Activated Carbon for Efficient and Selective CO2 Capture.

PubMed

Alabadi, Akram; Abbood, Hayder A; Li, Qingyin; Jing, Ni; Tan, Bien

2016-12-13

The preparation of nitrogen-doped activated carbon (NACs) has received significant attention because of their applications in CO 2 capture and sequestration (CCS) owing to abundant nitrogen atoms on their surface and controllable pore structures by carefully controlled carbonization. We report high-surface-area porous N-doped activated carbons (NAC) by using soft-template-assisted self-assembly followed by thermal decomposition and KOH activation. The activation process was carried out under different temperature conditions (600-800 °C) using polyimine as precursor. The NAC-800 was found to have a high specific surface area (1900 m 2  g -1 ), a desirable micropore size below 1 nm and, more importantly, a large micropore volume (0.98 cm 3  g -1 ). NAC-800 also exhibits a significant capacity of CO 2 capture i.e., over 6. 25 and 4.87 mmol g -1 at 273 K and 298 K respectively at 1.13 bar, which is one of among the highest values reported for porous carbons so far. Moreover, NAC also shows an excellent separation selectivity for CO 2 over N 2 .

Imine-Linked Polymer Based Nitrogen-Doped Porous Activated Carbon for Efficient and Selective CO2 Capture

PubMed Central

Alabadi, Akram; Abbood, Hayder A.; Li, Qingyin; Jing, Ni; Tan, Bien

2016-01-01

The preparation of nitrogen-doped activated carbon (NACs) has received significant attention because of their applications in CO2 capture and sequestration (CCS) owing to abundant nitrogen atoms on their surface and controllable pore structures by carefully controlled carbonization. We report high-surface-area porous N-doped activated carbons (NAC) by using soft-template-assisted self-assembly followed by thermal decomposition and KOH activation. The activation process was carried out under different temperature conditions (600–800 °C) using polyimine as precursor. The NAC-800 was found to have a high specific surface area (1900 m2 g−1), a desirable micropore size below 1 nm and, more importantly, a large micropore volume (0.98 cm3 g−1). NAC-800 also exhibits a significant capacity of CO2 capture i.e., over 6. 25 and 4.87 mmol g−1 at 273 K and 298 K respectively at 1.13 bar, which is one of among the highest values reported for porous carbons so far. Moreover, NAC also shows an excellent separation selectivity for CO2 over N2. PMID:27958305

Process and Material Design for Micro-Encapsulated Ionic Liquids in Post-Combustion CO 2 Capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hong, Bo; Brennecke, Joan F; McCready, Mark

Aprotic Heterocyclic Anion (AHA) Ionic Liquids (ILs) have been identified as promising new solvents for post-combustion carbon capture due to their high CO 2 uptake and the high tenability 1,2 of their binding energy with CO 2. Some of these compounds change phase (solid to liquid) on absorption of CO 2; these Phase Change ILs (PCILs)3 offer the additional advantage that part of the heat needed to desorb the CO2 from the absorbent is provided by the heat of fusion as the PCIL solidifies upon release of CO 2. However, the relatively high viscosity of AHA ILs and the occurrencemore » of a phase change in PCILs present challenges for conventional absorption equipment. To overcome these challenges we are pursuing the use of new technology to micro-encapsulate the AHA ILs and PCILs. Our partners at Lawrence Livermore National Laboratory have successfully demonstrated this technology in the application of post-combustion carbon capture with sodium and potassium carbonate solutions,4 and have recently shown the feasibility of micro-encapsulation of an AHA IL for carbon capture.5 The large effective surface area and high CO 2 permeability of the micro-capsules is expected to offset the drawback of the high IL viscosity and to provide for a more efficient and cost-effective mass transfer operation involving AHA ILs and PCILs. These opportunities, however, present us with both process and materials design questions. For example, what is the target CO 2 absorption strength (enthalpy of chemical absorption) for the tunable AHA IL? What is the target for micro-capsule diameter in order to obtain a high mass transfer rate and good fluidization performance? What are the appropriate temperatures and pressures for the absorber and stripper? In order to address these and other questions, we have developed a rate-based model of a post-combustion CO 2 capture process using micro-encapsulated ILs. As a performance baseline, we have also developed a rate-based model of a standard packed bed absorber using an un-encapsulated AHA IL absorbent. Using such models we can determine optimal CO 2 capture performance and investigate the sensitivity of the optimum with respect to the key thermo-physical and transport properties of the IL (e.g., CO 2 binding energy, viscosity, etc.) and the micro-capsules (e.g. diameter, CO 2 permeability, etc.). Results of these process and material design studies will be presented, and the performance of this novel micro-encapsulation technology will be assessed.« less

The O2-assisted Al/CO2 electrochemical cell: A system for CO2 capture/conversion and electric power generation.

PubMed

Al Sadat, Wajdi I; Archer, Lynden A

2016-07-01

Economical and efficient carbon capture, utilization, and sequestration technologies are a requirement for successful implementation of global action plans to reduce carbon emissions and to mitigate climate change. These technologies are also essential for longer-term use of fossil fuels while reducing the associated carbon footprint. We demonstrate an O2-assisted Al/CO2 electrochemical cell as a new approach to sequester CO2 emissions and, at the same time, to generate substantial amounts of electrical energy. We report on the fundamental principles that guide operations of these cells using multiple intrusive electrochemical and physical analytical methods, including chronopotentiometry, cyclic voltammetry, direct analysis in real-time mass spectrometry, energy-dispersive x-ray spectroscopy, x-ray photoelectron spectroscopy, and coupled thermogravimetric analysis-Fourier transform infrared spectroscopy. On this basis, we demonstrate that an electrochemical cell that uses metallic aluminum as anode and a carbon dioxide/oxygen gas mixture as the active material in the cathode provides a path toward electrochemical generation of a valuable (C2) species and electrical energy. Specifically, we show that the cell first reduces O2 at the cathode to form superoxide intermediates. Chemical reaction of the superoxide with CO2 sequesters the CO2 in the form of aluminum oxalate, Al2(C2O4)3, as the dominant product. On the basis of an analysis of the overall CO2 footprint, which considers emissions associated with the production of the aluminum anode and the CO2 captured/abated by the Al/CO2-O2 electrochemical cell, we conclude that the proposed process offers an important strategy for net reduction of CO2 emissions.

The O2-assisted Al/CO2 electrochemical cell: A system for CO2 capture/conversion and electric power generation

PubMed Central

Al Sadat, Wajdi I.; Archer, Lynden A.

2016-01-01

Economical and efficient carbon capture, utilization, and sequestration technologies are a requirement for successful implementation of global action plans to reduce carbon emissions and to mitigate climate change. These technologies are also essential for longer-term use of fossil fuels while reducing the associated carbon footprint. We demonstrate an O2-assisted Al/CO2 electrochemical cell as a new approach to sequester CO2 emissions and, at the same time, to generate substantial amounts of electrical energy. We report on the fundamental principles that guide operations of these cells using multiple intrusive electrochemical and physical analytical methods, including chronopotentiometry, cyclic voltammetry, direct analysis in real-time mass spectrometry, energy-dispersive x-ray spectroscopy, x-ray photoelectron spectroscopy, and coupled thermogravimetric analysis–Fourier transform infrared spectroscopy. On this basis, we demonstrate that an electrochemical cell that uses metallic aluminum as anode and a carbon dioxide/oxygen gas mixture as the active material in the cathode provides a path toward electrochemical generation of a valuable (C2) species and electrical energy. Specifically, we show that the cell first reduces O2 at the cathode to form superoxide intermediates. Chemical reaction of the superoxide with CO2 sequesters the CO2 in the form of aluminum oxalate, Al2(C2O4)3, as the dominant product. On the basis of an analysis of the overall CO2 footprint, which considers emissions associated with the production of the aluminum anode and the CO2 captured/abated by the Al/CO2-O2 electrochemical cell, we conclude that the proposed process offers an important strategy for net reduction of CO2 emissions. PMID:27453949

Comparing post-combustion CO2 capture operation at retrofitted coal-fired power plants in the Texas and Great Britain electric grids

NASA Astrophysics Data System (ADS)

Cohen, Stuart M.; Chalmers, Hannah L.; Webber, Michael E.; King, Carey W.

2011-04-01

This work analyses the carbon dioxide (CO2) capture system operation within the Electric Reliability Council of Texas (ERCOT) and Great Britain (GB) electric grids using a previously developed first-order hourly electricity dispatch and pricing model. The grids are compared in their 2006 configuration with the addition of coal-based CO2 capture retrofits and emissions penalties from 0 to 100 US dollars per metric ton of CO2 (USD/tCO2). CO2 capture flexibility is investigated by comparing inflexible CO2 capture systems to flexible ones that can choose between full- and zero-load CO2 capture depending on which operating mode has lower costs or higher profits. Comparing these two grids is interesting because they have similar installed capacity and peak demand, and both are isolated electricity systems with competitive wholesale electricity markets. However, differences in capacity mix, demand patterns, and fuel markets produce diverging behaviours of CO2 capture at coal-fired power plants. Coal-fired facilities are primarily base load in ERCOT for a large range of CO2 prices but are comparably later in the dispatch order in GB and consequently often supply intermediate load. As a result, the ability to capture CO2 is more important for ensuring dispatch of coal-fired facilities in GB than in ERCOT when CO2 prices are high. In GB, higher overall coal prices mean that CO2 prices must be slightly higher than in ERCOT before the emissions savings of CO2 capture offset capture energy costs. However, once CO2 capture is economical, operating CO2 capture on half the coal fleet in each grid achieves greater emissions reductions in GB because the total coal-based capacity is 6 GW greater than in ERCOT. The market characteristics studied suggest greater opportunity for flexible CO2 capture to improve operating profits in ERCOT, but profit improvements can be offset by a flexibility cost penalty.

Assessment of Solid Sorbent Systems for Post-Combustion Carbon Dioxide Capture at Coal-Fired Power Plants

NASA Astrophysics Data System (ADS)

Glier, Justin C.

In an effort to lower future CO2 emissions, a wide range of technologies are being developed to scrub CO2 from the flue gases of fossil fuel-based electric power and industrial plants. This thesis models one of several early-stage post-combustion CO2 capture technologies, solid sorbent-based CO2 capture process, and presents performance and cost estimates of this system on pulverized coal power plants. The spreadsheet-based software package Microsoft Excel was used in conjunction with AspenPlus modelling results and the Integrated Environmental Control Model to develop performance and cost estimates for the solid sorbent-based CO2 capture technology. A reduced order model also was created to facilitate comparisons among multiple design scenarios. Assumptions about plant financing and utilization, as well as uncertainties in heat transfer and material design that affect heat exchanger and reactor design were found to produce a wide range of cost estimates for solid sorbent-based systems. With uncertainties included, costs for a supercritical power plant with solid sorbent-based CO2 capture ranged from 167 to 533 per megawatt hour for a first-of-a-kind installation (with all costs in constant 2011 US dollars) based on a 90% confidence interval. The median cost was 209/MWh. Post-combustion solid sorbent-based CO2 capture technology is then evaluated in terms of the potential cost for a mature system based on historic experience as technologies are improved with sequential iterations of the currently available system. The range costs for a supercritical power plant with solid sorbent-based CO2 capture was found to be 118 to 189 per megawatt hour with a nominal value of 163 per megawatt hour given the expected range of technological improvement in the capital and operating costs and efficiency of the power plant after 100 GW of cumulative worldwide experience. These results suggest that the solid sorbent-based system will not be competitive with currently available liquid amine-systems in the absence of significant new improvements in solid sorbent properties and process system design to reduce the heat exchange surface area in the regenerator and cross-flow heat exchanger. Finally, the importance of these estimates for policy makers is discussed.

Borophene as a Promising Material for Charge-Modulated Switchable CO2 Capture.

PubMed

Tan, Xin; Tahini, Hassan A; Smith, Sean C

2017-06-14

Ideal carbon dioxide (CO 2 ) capture materials for practical applications should bind CO 2 molecules neither too weakly to limit good loading kinetics nor too strongly to limit facile release. Although charge-modulated switchable CO 2 capture has been proposed to be a controllable, highly selective, and reversible CO 2 capture strategy, the development of a practical gas-adsorbent material remains a great challenge. In this study, by means of density functional theory (DFT) calculations, we have examined the possibility of conductive borophene nanosheets as promising sorbent materials for charge-modulated switchable CO 2 capture. Our results reveal that the binding strength of CO 2 molecules on negatively charged borophene can be significantly enhanced by injecting extra electrons into the adsorbent. At saturation CO 2 capture coverage, the negatively charged borophene achieves CO 2 capture capacities up to 6.73 × 10 14 cm -2 . In contrast to the other CO 2 capture methods, the CO 2 capture/release processes on negatively charged borophene are reversible with fast kinetics and can be easily controlled via switching on/off the charges carried by borophene nanosheets. Moreover, these negatively charged borophene nanosheets are highly selective for separating CO 2 from mixtures with CH 4 , H 2 , and/or N 2 . This theoretical exploration will provide helpful guidance for identifying experimentally feasible, controllable, highly selective, and high-capacity CO 2 capture materials with ideal thermodynamics and reversibility.

High throughput screening of CO2 solubility in aqueous monoamine solutions.

PubMed

Porcheron, Fabien; Gibert, Alexandre; Mougin, Pascal; Wender, Aurélie

2011-03-15

Post-combustion Carbon Capture and Storage technology (CCS) is viewed as an efficient solution to reduce CO(2) emissions of coal-fired power stations. In CCS, an aqueous amine solution is commonly used as a solvent to selectively capture CO(2) from the flue gas. However, this process generates additional costs, mostly from the reboiler heat duty required to release the carbon dioxide from the loaded solvent solution. In this work, we present thermodynamic results of CO(2) solubility in aqueous amine solutions from a 6-reactor High Throughput Screening (HTS) experimental device. This device is fully automated and designed to perform sequential injections of CO(2) within stirred-cell reactors containing the solvent solutions. The gas pressure within each reactor is monitored as a function of time, and the resulting transient pressure curves are transformed into CO(2) absorption isotherms. Solubility measurements are first performed on monoethanolamine, diethanolamine, and methyldiethanolamine aqueous solutions at T = 313.15 K. Experimental results are compared with existing data in the literature to validate the HTS device. In addition, a comprehensive thermodynamic model is used to represent CO(2) solubility variations in different classes of amine structures upon a wide range of thermodynamic conditions. This model is used to fit the experimental data and to calculate the cyclic capacity, which is a key parameter for CO(2) process design. Solubility measurements are then performed on a set of 50 monoamines and cyclic capacities are extracted using the thermodynamic model, to asses the potential of these molecules for CO(2) capture.

New Directions for the Photocatalytic Reduction of CO2: Supramolecular, scCO2 or Biphasic Ionic Liquid-scCO2 Systems

DOE Office of Scientific and Technical Information (OSTI.GOV)

Grills, D.C.; Fujita, E.

2010-09-02

There is an urgent need for the discovery of carbon-neutral sources of energy to avoid the consequences of global warming caused by ever-increasing atmospheric CO{sub 2} levels. An attractive possibility is to use CO{sub 2} captured from industrial emissions as a feedstock for the production of useful fuels and precursors such as carbon monoxide and methanol. An active field of research to achieve this goal is the development of catalysts capable of harnessing solar energy for use in artificial photosynthetic processes for CO{sub 2} reduction. Transition-metal complexes are excellent candidates, and it has already been shown that they can bemore » used to reduce CO{sub 2} with high quantum efficiency. However, they generally suffer from poor visible light absorption, short catalyst lifetimes, and poor reaction rates. In this Perspective, the field of photocatalytic CO{sub 2} reduction is introduced, and recent developments that seek to improve the efficiency of such catalytic processes are highlighted, especially CO{sub 2} reduction with supramolecules and molecular systems in supercritical CO{sub 2} (scCO{sub 2}) or biphasic ionic liquid-scCO{sub 2} mixtures.« less

Flow Distribution Measurement Feasibility in Supercritical CO 2

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lance, Blake

2017-12-01

Supercritical CO 2 (sCO 2) is a fluid of interest for advanced power cycles that can reach thermal to electric energy conversion efficiencies of 50% or higher. Of particular interest for fossil-fired natural gas is the Allam cycle that captures nearly all CO 2 emissions and exports it as a fluid stream where it may be of value. The combustion process conditions are unlike any before realized with 90-95% CO 2 concentration, temperatures around 1000°C, and pressures near 300 bar. This work outlines the experimental feasibility of flow measurements to acquire the first known data in pure sCO 2 atmore » similar but reduced temperature and pressure conditions.« less

A recyclable and highly active Co{sub 3}O{sub 4} nanoparticles/titanate nanowire catalyst for organic dyes degradation with peroxymonosulfate

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chen, Zhili; Chen, Shihua; Li, Yonghe

2014-09-15

Sodium ions of TNWs were exchanged with hydrogen ions, and this protocol was very suitable for capturing high density of cobalt ions. Meanwhile, the fabricated Co{sub 3}O{sub 4}/TNWs nano-material presented a highly catalytic and stable activity for dye degradation. - Highlights: • Co{sub 3}O{sub 4} nanoparticles were deposited on the pretreated TNWs surface. • The TNWs treated by hydrogen ions captures higher density of cobalt ions. • The Co{sub 3}O{sub 4}/TNWs catalyst possesses highly efficiency for dyes degradation with oxone. - Abstract: In this paper, we reported a recyclable and highly active porous catalyst of titanate nanowires (TNWs) coated withmore » well-distributed Co{sub 3}O{sub 4} nanoparticles (NPs) (Co{sub 3}O{sub 4}/TNWs). Sodium ions of TNWs were exchanged with hydrogen ions in the dilute nitric acid, and this protocol was very suitable for capturing cobalt ions. X-ray diffraction (XRD) demonstrated the existence of Co{sub 3}O{sub 4} phase with unique lattice planes, such as (2 2 0), (3 1 1) and (5 1 1). Electron microscopes (FE-SEM and TEM) indicated that the Co{sub 3}O{sub 4} NPs with an average diameter of 22 ± 3 nm were coated uniformly on TNWs surface (average diameter: 37 ± 5.5 nm), and the Co{sub 3}O{sub 4} NPs mainly exposed their (2 2 0) and (2 2 2) active planes. XPS analysis confirms the formation of Co{sub 3}O{sub 4} phase by the presence of Co 2p peaks at 780.1 eV (2p 3/2) and 795.5 eV (2p 1/2). Methylene blue (MB) and other organic dyes (rhodamine B (RhB) and methyl orange (MO)) were chosen as target compounds for catalytic degradation under indoor scattering light. Compared to the original Co{sub 3}O{sub 4}/TNWs catalyst, the catalytic efficiency of nanoscaled catalyst with oxone for MB was about 15 times higher, and the MB solution (10 mg L{sup −1}) was completely degraded within 8 min. The catalytic activity of recycled catalyst used in the sixth run still remained very active, and the degradation time for MB was only 16 min. The nanosized catalyst also had a high activity for dyes of RhB (10 mg L{sup −1}) and MO (10 mg L{sup −1}), as the degradation efficiencies of RhB and MO after 10 min of contact time were about 90.2% and 92.6%, respectively.« less

Thermal degradation of aqueous 2-aminoethylethanolamine in CO2 capture; identification of degradation products, reaction mechanisms and computational studies.

PubMed

Saeed, Idris Mohamed; Lee, Vannajan Sanghiran; Mazari, Shaukat Ali; Si Ali, B; Basirun, Wan Jeffrey; Asghar, Anam; Ghalib, Lubna; Jan, Badrul Mohamed

2017-01-01

Amine degradation is the main significant problems in amine-based post-combustion CO 2 capture, causes foaming, increase in viscosity, corrosion, fouling as well as environmental issues. Therefore it is very important to develop the most efficient solvent with high thermal and chemical stability. This study investigated thermal degradation of aqueous 30% 2-aminoethylethanolamine (AEEA) using 316 stainless steel cylinders in the presence and absence of CO 2 for 4 weeks. The degradation products were identified by gas chromatography mass spectrometry (GC/MS) and liquid chromatography-time-of-flight-mass spectrometry (LC-QTOF/MS). The results showed AEEA is stable in the absence of CO 2 , while in the presence of CO 2 AEEA showed to be very unstable and numbers of degradation products were identified. 1-(2-Hydroxyethyl)-2-imidazolidinone (HEIA) was the most abundance degradation product. A possible mechanism for the thermal degradation of AEEA has been developed to explain the formation of degradation products. In addition, the reaction energy of formation of the most abundance degradation product HEIA was calculated using quantum mechanical calculation.

Research on structural integration of thermodynamic system for double reheat coal-fired unit with CO2 capture

NASA Astrophysics Data System (ADS)

Wang, Lanjing; Shao, Wenjing; Wang, Zhiyue; Fu, Wenfeng; Zhao, Wensheng

2018-02-01

Taking the MEA chemical absorption carbon capture system with 85% of the carbon capture rate of a 660MW ultra-super critical unit as an example,this paper puts forward a new type of turbine which dedicated to supply steam to carbon capture system. The comparison of the thermal systems of the power plant under different steam supply schemes by using the EBSILON indicated optimal extraction scheme for Steam Extraction System in Carbon Capture System. The results show that the cycle heat efficiency of the unit introduced carbon capture turbine system is higher than that of the usual scheme without it. With the introduction of the carbon capture turbine, the scheme which extracted steam from high pressure cylinder’ s steam input point shows the highest cycle thermal efficiency. Its indexes are superior to other scheme, and more suitable for existing coal-fired power plant integrated post combustion carbon dioxide capture system.

Flying MOFs: polyamine-containing fluidized MOF/SiO2 hybrid materials for CO2 capture from post-combustion flue gas.

PubMed

Luz, Ignacio; Soukri, Mustapha; Lail, Marty

2018-05-28

Solid-state synthesis ensures a high loading and well-dispersed growth of a large collection of metal-organic framework (MOF) nanostructures within a series of commercially available mesoporous silica. This approach provides a general, highly efficient, scalable, environmentally friendly, and inexpensive strategy for shaping MOFs into a fluidized form, thereby allowing their application in fluidized-bed reactors for diverse applications, such as CO 2 capture from post-combustion flue gas. A collection of polyamine-impregnated MOF/SiO 2 hybrid sorbents were evaluated for CO 2 capture under simulated flue gas conditions in a packed-bed reactor. Hybrid sorbents containing a moderate loading of (Zn)ZIF-8 are the most promising sorbents in terms of CO 2 adsorption capacity and long-term stability (up to 250 cycles in the presence of contaminants: SO 2 , NO x and H 2 S) and were successfully prepared at the kilogram scale. These hybrid sorbents demonstrated excellent fluidizability and performance under the relevant process conditions in a visual fluidized-bed reactor. Moreover, a biochemically inspired strategy for covalently linking polyamines to MOF/SiO 2 through strong phosphine bonds has been first introduced in this work as a powerful and highly versatile post-synthesis modification for MOF chemistry, thus providing a novel alternative towards more stable CO 2 solid sorbents.

Molten salt CO2 capture and electro-transformation (MSCC-ET) into capacitive carbon at medium temperature: effect of the electrolyte composition.

PubMed

Deng, Bowen; Chen, Zhigang; Gao, Muxing; Song, Yuqiao; Zheng, Kaiyuan; Tang, Juanjuan; Xiao, Wei; Mao, Xuhui; Wang, Dihua

2016-08-15

Electrochemical transformation of CO2 into functional materials or fuels (i.e., carbon, CO) in high temperature molten salts has been demonstrated as a promising way of carbon capture, utilisation and storage (CCUS) in recent years. In a view of continuous operation, the electrolysis process should match very well with the CO2 absorption kinetics. At the same time, in consideration of the energy efficiency, a molten salt electrochemical cell running at lower temperature is more beneficial to a process powered by the fluctuating renewable electricity from solar/wind farms. Ternary carbonates (Li : Na : K = 43.5 : 31.5 : 25.0) and binary chlorides (Li : K = 58.5 : 41.5), two typical kinds of eutectic melt with low melting points and a wide electrochemical potential window, could be the ideal supporting electrolyte for the molten salt CO2 capture and electro-transformation (MSCC-ET) process. In this work, the CO2 absorption behaviour in Li2O/CaO containing carbonates and chlorides were investigated on a home-made gas absorption testing system. The electrode processes as well as the morphology and properties of carbon obtained in different salts are compared to each other. It was found that the composition of molten salts significantly affects the absorption of CO2, electrode processes and performance of the product. Furthermore, the relationship between the absorption and electro-transformation kinetics are discussed based on the findings.

Nitrogen-Rich Porous Polymers for Carbon Dioxide and Iodine Sequestration for Environmental Remediation.

PubMed

Abdelmoaty, Yomna H; Tessema, Tsemre-Dingel; Choudhury, Fatema Akthar; El-Kadri, Oussama M; El-Kaderi, Hani M

2018-05-09

The use of fossil fuels for energy production is accompanied by carbon dioxide release into the environment causing catastrophic climate changes. Meanwhile, replacing fossil fuels with carbon-free nuclear energy has the potential to release radioactive iodine during nuclear waste processing and in case of a nuclear accident. Therefore, developing efficient adsorbents for carbon dioxide and iodine capture is of great importance. Two nitrogen-rich porous polymers (NRPPs) derived from 4-bis-(2,4-diamino-1,3,5-triazine)-benzene building block were prepared and tested for use in CO 2 and I 2 capture. Copolymerization of 1,4-bis-(2,4-diamino-1,3,5-triazine)-benzene with terephthalaldehyde and 1,3,5-tris(4-formylphenyl)benzene in dimethyl sulfoxide at 180 °C afforded highly porous NRPP-1 (SA BET = 1579 m 2 g -1 ) and NRPP-2 (SA BET = 1028 m 2 g -1 ), respectively. The combination of high nitrogen content, π-electron conjugated structure, and microporosity makes NRPPs very effective in CO 2 uptake and I 2 capture. NRPPs exhibit high CO 2 uptakes (NRPP-1, 6.1 mmol g -1 and NRPP-2, 7.06 mmol g -1 ) at 273 K and 1.0 bar. The 7.06 mmol g -1 CO 2 uptake by NRPP-2 is the second highest value reported to date for porous organic polymers. According to vapor iodine uptake studies, the polymers display high capacity and rapid reversible uptake release for I 2 (NRPP-1, 192 wt % and NRPP-2, 222 wt %). Our studies show that the green nature (metal-free) of NRPPs and their effective capture of CO 2 and I 2 make this class of porous materials promising for environmental remediation.

Sustainable microalgae for the simultaneous synthesis of carbon quantum dots for cellular imaging and porous carbon for CO2 capture.

PubMed

Guo, Li-Ping; Zhang, Yan; Li, Wen-Cui

2017-05-01

Microalgae biomass is a sustainable source with the potential to produce a range of products. However, there is currently a lack of practical and functional processes to enable the high-efficiency utilization of the microalgae. We report here a hydrothermal process to maximize the utilizability of microalgae biomass. Specifically, our concept involves the simultaneous conversion of microalgae to (i) hydrophilic and stable carbon quantum dots and (ii) porous carbon. The synthesis is easily scalable and eco-friendly. The microalgae-derived carbon quantum dots possess a strong two-photon fluorescence property, have a low cytotoxicity and an efficient cellular uptake, and show potential for high contrast bioimaging. The microalgae-based porous carbons show excellent CO 2 capture capacities of 6.9 and 4.2mmolg -1 at 0 and 25°C respectively, primarily due to the high micropore volume (0.59cm 3 g -1 ) and large specific surface area (1396m 2 g -1 ). Copyright © 2017 Elsevier Inc. All rights reserved.

High-throughput screening of metal-porphyrin-like graphenes for selective capture of carbon dioxide

PubMed Central

Bae, Hyeonhu; Park, Minwoo; Jang, Byungryul; Kang, Yura; Park, Jinwoo; Lee, Hosik; Chung, Haegeun; Chung, ChiHye; Hong, Suklyun; Kwon, Yongkyung; Yakobson, Boris I.; Lee, Hoonkyung

2016-01-01

Nanostructured materials, such as zeolites and metal-organic frameworks, have been considered to capture CO2. However, their application has been limited largely because they exhibit poor selectivity for flue gases and low capture capacity under low pressures. We perform a high-throughput screening for selective CO2 capture from flue gases by using first principles thermodynamics. We find that elements with empty d orbitals selectively attract CO2 from gaseous mixtures under low CO2 pressures (~10−3 bar) at 300 K and release it at ~450 K. CO2 binding to elements involves hybridization of the metal d orbitals with the CO2 π orbitals and CO2-transition metal complexes were observed in experiments. This result allows us to perform high-throughput screening to discover novel promising CO2 capture materials with empty d orbitals (e.g., Sc– or V–porphyrin-like graphene) and predict their capture performance under various conditions. Moreover, these findings provide physical insights into selective CO2 capture and open a new path to explore CO2 capture materials. PMID:26902156

High-throughput screening of metal-porphyrin-like graphenes for selective capture of carbon dioxide.

PubMed

Bae, Hyeonhu; Park, Minwoo; Jang, Byungryul; Kang, Yura; Park, Jinwoo; Lee, Hosik; Chung, Haegeun; Chung, ChiHye; Hong, Suklyun; Kwon, Yongkyung; Yakobson, Boris I; Lee, Hoonkyung

2016-02-23

Nanostructured materials, such as zeolites and metal-organic frameworks, have been considered to capture CO2. However, their application has been limited largely because they exhibit poor selectivity for flue gases and low capture capacity under low pressures. We perform a high-throughput screening for selective CO2 capture from flue gases by using first principles thermodynamics. We find that elements with empty d orbitals selectively attract CO2 from gaseous mixtures under low CO2 pressures (~10(-3) bar) at 300 K and release it at ~450 K. CO2 binding to elements involves hybridization of the metal d orbitals with the CO2 π orbitals and CO2-transition metal complexes were observed in experiments. This result allows us to perform high-throughput screening to discover novel promising CO2 capture materials with empty d orbitals (e.g., Sc- or V-porphyrin-like graphene) and predict their capture performance under various conditions. Moreover, these findings provide physical insights into selective CO2 capture and open a new path to explore CO2 capture materials.

High-throughput screening of metal-porphyrin-like graphenes for selective capture of carbon dioxide

NASA Astrophysics Data System (ADS)

Bae, Hyeonhu; Park, Minwoo; Jang, Byungryul; Kang, Yura; Park, Jinwoo; Lee, Hosik; Chung, Haegeun; Chung, Chihye; Hong, Suklyun; Kwon, Yongkyung; Yakobson, Boris I.; Lee, Hoonkyung

2016-02-01

Nanostructured materials, such as zeolites and metal-organic frameworks, have been considered to capture CO2. However, their application has been limited largely because they exhibit poor selectivity for flue gases and low capture capacity under low pressures. We perform a high-throughput screening for selective CO2 capture from flue gases by using first principles thermodynamics. We find that elements with empty d orbitals selectively attract CO2 from gaseous mixtures under low CO2 pressures (~10-3 bar) at 300 K and release it at ~450 K. CO2 binding to elements involves hybridization of the metal d orbitals with the CO2 π orbitals and CO2-transition metal complexes were observed in experiments. This result allows us to perform high-throughput screening to discover novel promising CO2 capture materials with empty d orbitals (e.g., Sc- or V-porphyrin-like graphene) and predict their capture performance under various conditions. Moreover, these findings provide physical insights into selective CO2 capture and open a new path to explore CO2 capture materials.

Low Cost, High Capacity Regenerable Sorbent for Carbon Dioxide Capture from Existing Coal-fired Power Plants

DOE Office of Scientific and Technical Information (OSTI.GOV)

Alptekin, Gokhan; Jayaraman, Ambalavanan; Dietz, Steven

In this project TDA Research, Inc (TDA) has developed a new post combustion carbon capture technology based on a vacuum swing adsorption system that uses a steam purge and demonstrated its technical feasibility and economic viability in laboratory-scale tests and tests in actual coal derived flue gas. TDA uses an advanced physical adsorbent to selectively remove CO 2 from the flue gas. The sorbent exhibits a much higher affinity for CO 2 than N 2, H 2O or O 2, enabling effective CO 2 separation from the flue gas. We also carried out a detailed process design and analysis ofmore » the new system as part of both sub-critical and super-critical pulverized coal fired power plants. The new technology uses a low cost, high capacity adsorbent that selectively removes CO 2 in the presence of moisture at the flue gas temperature without a need for significant cooling of the flue gas or moisture removal. The sorbent is based on a TDA proprietary mesoporous carbon that consists of surface functionalized groups that remove CO 2 via physical adsorption. The high surface area and favorable porosity of the sorbent also provides a unique platform to introduce additional functionality, such as active groups to remove trace metals (e.g., Hg, As). In collaboration with the Advanced Power and Energy Program of the University of California, Irvine (UCI), TDA developed system simulation models using Aspen PlusTM simulation software to assess the economic viability of TDA’s VSA-based post-combustion carbon capture technology. The levelized cost of electricity including the TS&M costs for CO 2 is calculated as $116.71/MWh and $113.76/MWh for TDA system integrated with sub-critical and super-critical pulverized coal fired power plants; much lower than the $153.03/MWhand $147.44/MWh calculated for the corresponding amine based systems. The cost of CO 2 captured for TDA’s VSA based system is $38.90 and $39.71 per tonne compared to $65.46 and $66.56 per tonne for amine based system on 2011 $ basis, providing 40% lower cost of CO 2 captured. In this analysis we have used a sorbent life of 4 years. If a longer sorbent life can be maintained (which is not unreasonable for fixed bed commercial PSA systems), this would lower the cost of CO 2 captured by $0.05 per tonne (e.g., to $38.85 and $39.66 per tonne at 5 years sorbent replacement). These system analysis results suggest that TDA’s VSA-based post-combustion capture technology can substantially improve the power plant’s thermal performance while achieving near zero emissions, including greater than 90% carbon capture. The higher net plant efficiency and lower capital and operating costs results in a substantial reduction in the cost of carbon capture and cost of electricity for the power plant equipped with TDA’s technology.« less

Production of biodiesel from microalgae through biological carbon capture: a review.

PubMed

Mondal, Madhumanti; Goswami, Shrayanti; Ghosh, Ashmita; Oinam, Gunapati; Tiwari, O N; Das, Papita; Gayen, K; Mandal, M K; Halder, G N

2017-06-01

Gradual increase in concentration of carbon dioxide (CO 2 ) in the atmosphere due to the various anthropogenic interventions leading to significant alteration in the global carbon cycle has been a subject of worldwide attention and matter of potential research over the last few decades. In these alarming scenario microalgae seems to be an attractive medium for capturing the excess CO 2 present in the atmosphere generated from different sources such as power plants, automobiles, volcanic eruption, decomposition of organic matters and forest fires. This captured CO 2 through microalgae could be used as potential carbon source to produce lipids for the generation of biofuel for replacing petroleum-derived transport fuel without affecting the supply of food and crops. This comprehensive review strives to provide a systematic account of recent developments in the field of biological carbon capture through microalgae for its utilization towards the generation of biodiesel highlighting the significance of certain key parameters such as selection of efficient strain, microalgal metabolism, cultivation systems (open and closed) and biomass production along with the national and international biodiesel specifications and properties. The potential use of photobioreactors for biodiesel production under the influence of various factors viz., light intensity, pH, time, temperature, CO 2 concentration and flow rate has been discussed. The review also provides an economic overview and future outlook on biodiesel production from microalgae.

Pathway To Low-Carbon Lignite Utilization; U.S. Department of Energy (DOE) National Energy Technology Laboratory (NETL) Cooperative Agreement No. DE-FE0024233

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kay, John; Stanislowski, Joshua; Tolbert, Scott

Utilities continue to investigate ways to decrease their carbon footprint. Carbon capture and storage (CCS) can enable existing power generation facilities to maintain operations and address carbon reduction. Subtask 2.1 – Pathway to Low-Carbon Lignite Utilization focused on several research areas in an effort to find ways to decrease the cost of capture across both precombustion and postcombustion platforms. Two postcombustion capture solvents were tested, one from CO 2 Solutions Inc. and one from ARCTECH, Inc. The CO 2 Solutions solvent had been evaluated previously, and the company had incorporated the concept of a rotating packed bed (RPB) to replacemore » the traditional packed columns typically used. In the limited testing performed at the Energy & Environmental Research Center (EERC), no CO 2 reduction benefit was seen from the RPB; however, if the technology could be scaled up, it may introduce some savings in capital expense and overall system footprint. Rudimentary tests were conducted with the ARCTECH solvent to evaluate if it could be utilized in a spray tower configuration contactor and capture CO 2, SO 2, and NO x. This solvent after loading can be processed to make an additional product to filter wastewater, providing a second-tier usable product. Modeling of the RPB process for scaling to a 550-MW power system was also conducted. The reduced cost of RPB systems combined with a smaller footprint highlight the potential for reducing the cost of capturing CO 2; however, more extensive testing is needed to truly evaluate their potential for use at full scale. Hydrogen separation membranes from Commonwealth Scientific and Industrial Research Organisation (CSIRO) were evaluated through precombustion testing. These had also been previously tested and were improved by CSIRO for this test campaign. They are composed of vanadium alloy, which is less expensive than the palladium alloys that are typically used. Their performance was good, and they may be good candidates for medium-pressure gasifiers, but much more scale-up work is needed. Next-generation power cycles are currently being developed and show promise for high efficiency, and the utilization of supercritical CO 2 to drive a turbine could significantly increase cycle efficiency over traditional steam cycles. The EERC evaluated pressurized oxy-combustion technology from the standpoint of CO 2 purification. If impurities can be removed, the costs for CO 2 capture can be lowered significantly over postcombustion capture systems. Impurity removal consisted of a simple water scrubber referred to as the DeSNO x process. The process worked well, but corrosion management is crucial to its success. A model of this process was constructed. Finally, an integrated gasification combined-cycle (IGCC) system model, developed by the Massachusetts Institute of Technology (MIT), was modified to allow for the modeling of membrane systems in the IGCC process. This modified model was used to provide an assessment of the costs of membrane use at full scale. An economic estimation indicated a 14% reduction in cost for CO 2 separation over the SELEXOL™ process. This subtask was funded through the EERC–DOE Joint Program on Research and Development for Fossil Energy-Related Resources Cooperative Agreement No. DE-FE0024233. Nonfederal sponsors for this project were the North Dakota Industrial Commission, Basin Electric Power Cooperative, and Allete, Inc. (including BNI Coal and Minnesota Power).« less

Microstructural response of variably hydrated Ca-rich montmorillonite to supercritical CO2.

PubMed

Lee, Mal-Soon; McGrail, B Peter; Glezakou, Vassiliki-Alexandra

2014-01-01

First-principles molecular dynamics simulations were carried out to explore the mechanistic and thermodynamic ramifications of the exposure of variably hydrated Ca-rich montmorillonites to supercritical CO2 and CO2-SO2 mixtures under geologic storage conditions. In sub- to single-hydrated systems (≤ 1W), CO2 intercalation causes interlamellar expansion of 8-12%, while systems transitioning to 2W may undergo contraction (∼ 7%) or remain almost unchanged. When compared to ∼2W hydration state, structural analysis of the ≤ 1W systems, reveals more Ca-CO2 contacts and partial transition to vertically confined CO2 molecules. Infrared spectra and projected vibrational frequency analysis imply that intercalated Ca-bound CO2 are vibrationally constrained and contribute to the higher frequencies of the asymmetric stretch band. Reduced diffusion coefficients of intercalated H2O and CO2 (10(-6)-10(-7) cm(2)/s) indicate that Ca-montmorillonites in ∼ 1W hydration states can be more efficient in capturing CO2. Simulations including SO2 imply that ∼ 0.66 mmol SO2/g clay can be intercalated without other significant structural changes. SO2 is likely to divert H2O away from the cations, promoting Ca-CO2 interactions and CO2 capture by further reducing CO2 diffusion (10(-8) cm(2)/s). Vibrational bands at ∼ 1267 or 1155 cm(-1) may be used to identify the chemical state (oxidation states +4 or +6, respectively) and the fate of sulfur contaminants.

Speciation, behaviour, and fate of mercury under oxy-fuel combustion conditions.

PubMed

Córdoba, Patricia; Maroto-Valer, M; Delgado, Miguel Angel; Diego, Ruth; Font, Oriol; Querol, Xavier

2016-02-01

The work presented here reports the first study in which the speciation, behaviour and fate of mercury (Hg) have been evaluated under oxy-fuel combustion at the largest oxy-Pulverised Coal Combustion (oxy-PCC) demonstration plant to date during routine operating conditions and partial exhaust flue gas re-circulation to the boiler. The effect of the CO2-rich flue gas re-circulation on Hg has also been evaluated. Results reveal that oxy-PCC operational conditions play a significant role on Hg partitioning and fate because of the continuous CO2-rich flue gas re-circulations to the boiler. Mercury escapes from the cyclone in a gaseous form as Hg(2+) (68%) and it is the prevalent form in the CO2-rich exhaust flue gas (99%) with lower proportions of Hg(0) (1.3%). The overall retention rate for gaseous Hg is around 12%; Hg(0) is more prone to be retained (95%) while Hg(2+) shows a negative efficiency capture for the whole installation. The negative Hg(2+) capture efficiencies are due to the continuous CO2-rich exhaust flue gas recirculation to the boiler with enhanced Hg contents. Calculations revealed that 44mg of Hg were re-circulated to the boiler as a result of 2183 re-circulations of CO2-rich flue gas. Especial attention must be paid to the role of the CO2-rich exhaust flue gas re-circulation to the boiler on the Hg enrichment in Fly Ashes (FAs). Copyright © 2015 Elsevier Inc. All rights reserved.

CO Oxidation and Subsequent CO 2 Chemisorption on Alkaline Zirconates: Li 2 ZrO 3 and Na 2 ZrO 3

DOE Office of Scientific and Technical Information (OSTI.GOV)

Alcántar-Vázquez, Brenda; Duan, Yuhua; Pfeiffer, Heriberto

Here, two different alkaline zirconates (Li 2ZrO 3 and Na 2ZrO 3) were studied as possible bifunctional catalytic-captor materials for CO oxidation and the subsequent CO 2 chemisorption process. Initially, CO oxidation reactions were analyzed in a catalytic reactor coupled to a gas chromatograph, using Li 2ZrO 3 and Na 2ZrO 3, under different O 2 partial flows. We found results clearly showed that Na 2ZrO 3 possesses much better catalytic properties than Li 2ZrO 3. After the CO-O 2 oxidation catalytic analysis, CO2 chemisorption process was analyzed by thermogravimetric analysis, only for the Na 2ZrO 3 ceramic. The resultsmore » confirmed that Na 2ZrO 3 is able to work as a bifunctional material (CO oxidation and subsequent CO 2 chemisorption), although the kinetic CO 2 capture process was not the best one under the physicochemical condition used in this case. For Na 2ZrO 3, the best CO conversions were found between 445 and 580 °C (100%), while Li 2ZrO 3 only showed a 35% of efficiency between 460 and 503 °C. However, in the Na 2ZrO 3 case, at temperatures higher than 580 °C its catalytic activity gradually decreases as a result of CO 2 capture process. Finally, all these experiments were compared and supported with theoretical thermodynamic data.« less

CO Oxidation and Subsequent CO 2 Chemisorption on Alkaline Zirconates: Li 2 ZrO 3 and Na 2 ZrO 3

DOE PAGES

Alcántar-Vázquez, Brenda; Duan, Yuhua; Pfeiffer, Heriberto

2016-08-26

Here, two different alkaline zirconates (Li 2ZrO 3 and Na 2ZrO 3) were studied as possible bifunctional catalytic-captor materials for CO oxidation and the subsequent CO 2 chemisorption process. Initially, CO oxidation reactions were analyzed in a catalytic reactor coupled to a gas chromatograph, using Li 2ZrO 3 and Na 2ZrO 3, under different O 2 partial flows. We found results clearly showed that Na 2ZrO 3 possesses much better catalytic properties than Li 2ZrO 3. After the CO-O 2 oxidation catalytic analysis, CO2 chemisorption process was analyzed by thermogravimetric analysis, only for the Na 2ZrO 3 ceramic. The resultsmore » confirmed that Na 2ZrO 3 is able to work as a bifunctional material (CO oxidation and subsequent CO 2 chemisorption), although the kinetic CO 2 capture process was not the best one under the physicochemical condition used in this case. For Na 2ZrO 3, the best CO conversions were found between 445 and 580 °C (100%), while Li 2ZrO 3 only showed a 35% of efficiency between 460 and 503 °C. However, in the Na 2ZrO 3 case, at temperatures higher than 580 °C its catalytic activity gradually decreases as a result of CO 2 capture process. Finally, all these experiments were compared and supported with theoretical thermodynamic data.« less

Large size biogas-fed Solid Oxide Fuel Cell power plants with carbon dioxide management: Technical and economic optimization

NASA Astrophysics Data System (ADS)

Curletti, F.; Gandiglio, M.; Lanzini, A.; Santarelli, M.; Maréchal, F.

2015-10-01

This article investigates the techno-economic performance of large integrated biogas Solid Oxide Fuel Cell (SOFC) power plants. Both atmospheric and pressurized operation is analysed with CO2 vented or captured. The SOFC module produces a constant electrical power of 1 MWe. Sensitivity analysis and multi-objective optimization are the mathematical tools used to investigate the effects of Fuel Utilization (FU), SOFC operating temperature and pressure on the plant energy and economic performances. FU is the design variable that most affects the plant performance. Pressurized SOFC with hybridization with a gas turbine provides a notable boost in electrical efficiency. For most of the proposed plant configurations, the electrical efficiency ranges in the interval 50-62% (LHV biogas) when a trade-off of between energy and economic performances is applied based on Pareto charts obtained from multi-objective plant optimization. The hybrid SOFC is potentially able to reach an efficiency above 70% when FU is 90%. Carbon capture entails a penalty of more 10 percentage points in pressurized configurations mainly due to the extra energy burdens of captured CO2 pressurization and oxygen production and for the separate and different handling of the anode and cathode exhausts and power recovery from them.

Response of Integrated CO 2 Capture and Storage Systems in Saline Aquifers and Fractured Shale Formations to Changes in CO 2 Capture Costs

DOE Office of Scientific and Technical Information (OSTI.GOV)

Langenfeld, Julie K.; Bielicki, Jeffrey M.; Tao, Zhiyuan

Fractured shale formations are new potential target reservoirs for CO 2 capture and storage (CCS) and provide several potential advantages over storage in saline aquifers in terms of storage capacity, leakage risk, and cost savings from brownfield development. Here, we used a geospatial-optimization, engineering-economic model to investigate the sensitivity of integrated CCS networks in Ohio, Pennsylvania, and West Virginia to reductions in CO 2 capture costs. The resulting reductions in CO 2 capture costs were based on hypothetical cases where technological innovation reduced CO 2 capture costs. There were also small differences in the spatial organization of the CCS deploymentmore » when the capture costs were reduced. We also found that the percent reduction in average cost of CCS systems became smaller as the CO 2 capture costs were decreased.« less

Response of Integrated CO 2 Capture and Storage Systems in Saline Aquifers and Fractured Shale Formations to Changes in CO 2 Capture Costs

DOE PAGES

Langenfeld, Julie K.; Bielicki, Jeffrey M.; Tao, Zhiyuan; ...

2017-08-18

Fractured shale formations are new potential target reservoirs for CO 2 capture and storage (CCS) and provide several potential advantages over storage in saline aquifers in terms of storage capacity, leakage risk, and cost savings from brownfield development. Here, we used a geospatial-optimization, engineering-economic model to investigate the sensitivity of integrated CCS networks in Ohio, Pennsylvania, and West Virginia to reductions in CO 2 capture costs. The resulting reductions in CO 2 capture costs were based on hypothetical cases where technological innovation reduced CO 2 capture costs. There were also small differences in the spatial organization of the CCS deploymentmore » when the capture costs were reduced. We also found that the percent reduction in average cost of CCS systems became smaller as the CO 2 capture costs were decreased.« less

Electrochemical capture and release of carbon dioxide

DOE PAGES

Rheinhardt, Joseph H.; Singh, Poonam; Tarakeshwar, Pilarisetty; ...

2017-01-18

Understanding the chemistry of carbon dioxide is key to affecting changes in atmospheric concentrations. One area of intense interest is CO 2 capture in chemically reversible cycles relevant to carbon capture technologies. Most CO 2 capture methods involve thermal cycles in which a nucleophilic agent captures CO 2 from impure gas streams (e.g., flue gas), followed by a thermal process in which pure CO 2 is released. Several reviews have detailed progress in these approaches. A less explored strategy uses electrochemical cycles to capture CO 2 and release it in pure form. These cycles typically rely on electrochemical generation ofmore » nucleophiles that attack CO 2 at the electrophilic carbon atom, forming a CO 2 adduct. Then, CO 2 is released in pure form via a subsequent electrochemical step. In this Perspective, we describe electrochemical cycles for CO 2 capture and release, emphasizing electrogenerated nucleophiles. As a result, we also discuss some advantages and disadvantages inherent in this general approach.« less

Mercury Adsorption and Oxidation over Cobalt Oxide Loaded Magnetospheres Catalyst from Fly Ash in Oxyfuel Combustion Flue Gas.

PubMed

Yang, Jianping; Zhao, Yongchun; Chang, Lin; Zhang, Junying; Zheng, Chuguang

2015-07-07

Cobalt oxide loaded magnetospheres catalyst from fly ash (Co-MF catalyst) showed good mercury removal capacity and recyclability under air combustion flue gas in our previous study. In this work, the Hg(0) removal behaviors as well as the involved reactions mechanism were investigated in oxyfuel combustion conditions. Further, the recyclability of Co-MF catalyst in oxyfuel combustion atmosphere was also evaluated. The results showed that the Hg(0) removal efficiency in oxyfuel combustion conditions was relative high compared to that in air combustion conditions. The presence of enriched CO2 (70%) in oxyfuel combustion atmosphere assisted the mercury oxidation due to the oxidation of function group of C-O formed from CO2. Under both atmospheres, the mercury removal efficiency decreased with the addition of SO2, NO, and H2O. However, the enriched CO2 in oxyfuel combustion atmosphere could somewhat weaken the inhibition of SO2, NO, and H2O. The multiple capture-regeneration cycles demonstrated that the Co-MF catalyst also present good regeneration performance in oxyfuel combustion atmosphere.

Throwing new light on the reduction of CO2.

PubMed

Ozin, Geoffrey A

2015-03-18

While the chemical energy in fossil fuels has enabled the rapid rise of modern civilization, their utilization and accompanying anthropogenic CO2 emissions is occurring at a rate that is outpacing nature's carbon cycle. Its effect is now considered to be irreversible and this could lead to the demise of human society. This is a complex issue without a single solution, yet from the burgeoning global research activity and development in the field of CO2 capture and utilization, there is light at the end of the tunnel. In this article a couple of recent advances are illuminated. Attention is focused on the discovery of gas-phase, light-assisted heterogeneous catalytic materials and processes for CO2 photoreduction that operate at sufficiently high rates and conversion efficiencies, and under mild conditions, to open a new pathway for an energy transition from today's "fossil fuel economy" to a new and sustainable "CO2 economy". Whichever of the competing CO2 capture and utilization approaches proves to be the best way forward for the development of a future CO2-based solar fuels economy, hopefully this can occur in a period short enough to circumvent the predicted adverse consequences of greenhouse gas climate change. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Electroreduction of carbon monoxide to liquid fuel on oxide-derived nanocrystalline copper.

PubMed

Li, Christina W; Ciston, Jim; Kanan, Matthew W

2014-04-24

The electrochemical conversion of CO2 and H2O into liquid fuel is ideal for high-density renewable energy storage and could provide an incentive for CO2 capture. However, efficient electrocatalysts for reducing CO2 and its derivatives into a desirable fuel are not available at present. Although many catalysts can reduce CO2 to carbon monoxide (CO), liquid fuel synthesis requires that CO is reduced further, using H2O as a H(+) source. Copper (Cu) is the only known material with an appreciable CO electroreduction activity, but in bulk form its efficiency and selectivity for liquid fuel are far too low for practical use. In particular, H2O reduction to H2 outcompetes CO reduction on Cu electrodes unless extreme overpotentials are applied, at which point gaseous hydrocarbons are the major CO reduction products. Here we show that nanocrystalline Cu prepared from Cu2O ('oxide-derived Cu') produces multi-carbon oxygenates (ethanol, acetate and n-propanol) with up to 57% Faraday efficiency at modest potentials (-0.25 volts to -0.5 volts versus the reversible hydrogen electrode) in CO-saturated alkaline H2O. By comparison, when prepared by traditional vapour condensation, Cu nanoparticles with an average crystallite size similar to that of oxide-derived copper produce nearly exclusive H2 (96% Faraday efficiency) under identical conditions. Our results demonstrate the ability to change the intrinsic catalytic properties of Cu for this notoriously difficult reaction by growing interconnected nanocrystallites from the constrained environment of an oxide lattice. The selectivity for oxygenates, with ethanol as the major product, demonstrates the feasibility of a two-step conversion of CO2 to liquid fuel that could be powered by renewable electricity.

Efficient MgO-based mesoporous CO2 trapper and its performance at high temperature.

PubMed

Han, Kun Kun; Zhou, Yu; Chun, Yuan; Zhu, Jian Hua

2012-02-15

A novel MgO-based porous adsorbent has been synthesized in a facile co-precipitation method for the first time, in order to provide a candidate for trapping CO(2) in flue gas at high temperature. The resulting composite exhibits a mesoporous structure with a wide pore size distribution, due to the even dispersion and distribution of microcrystalline MgO in the framework of alumina to form a concrete-like structure. These sorbents can capture CO(2) at high temperature (150-400°C), possessing high reactivity and stability in cyclic adsorption-desorption processes, providing competitive candidates to control CO(2) emission. Copyright © 2011 Elsevier B.V. All rights reserved.

CO2 Dissociation using the Versatile Atmospheric Dielectric Barrier Discharge Experiment (VADER)

NASA Astrophysics Data System (ADS)

Lindon, Michael Allen

As of 2013, the Carbon Dioxide Information Analysis Center (CDIAC) estimates that the world emits approximately 36 trillion metric tons of Carbon Dioxide (CO2) into the atmosphere every year. These large emissions have been correlated to global warming trends that have many consequences across the globe, including glacial retraction, ocean acidification and increased severity of weather events. With green technologies still in the infancy stage, it can be expected that CO2 emissions will stay this way for along time to come. Approximately 41% of the emissions are due to electricity production, which pump out condensed forms of CO2. This danger to our world is why research towards new and innovative ways of controlling CO2 emissions from these large sources is necessary. As of now, research is focused on two primary methods of CO2 reduction from condensed CO2 emission sources (like fossil fuel power plants): Carbon Capture and Sequestration (CCS) and Carbon Capture and Utilization (CCU). CCS is the process of collecting CO2 using absorbers or chemicals, extracting the gas from those absorbers and finally pumping the gas into reservoirs. CCU on the other hand, is the process of reacting CO2 to form value added chemicals, which can then be recycled or stored chemically. A Dielectric Barrier discharge (DBD) is a pulsed, low temperature, non-thermal, atmospheric pressure plasma which creates high energy electrons suitable for dissociating CO2 into its components (CO and O) as one step in the CCU process. Here I discuss the viability of using a DBD for CO2 dissociation on an industrial scale as well as the fundamental physics and chemistry of a DBD for CO2 dissociation. This work involved modeling the DBD discharge and chemistry, which showed that there are specific chemical pathways and plasma parameters that can be adjusted to improve the CO2 reaction efficiencies and rates. Experimental studies using the Versatile Atmospheric dielectric barrier Discharge ExpeRiment (VADER) demonstrated how different factors, like voltage, frequency and the addition of a photocatalyst, change the efficiency of CO2 dissociation in VADER and the plasma chemistry involved.

Liquid Hydrocarbon Production from CO2 : Recent Development in Metal-Based Electrocatalysis.

PubMed

Daiyan, Rahman; Lu, Xunyu; Ng, Yun Hau; Amal, Rose

2017-11-23

Rising levels of CO 2 accumulation in the atmosphere have attracted considerable interest in technologies capable of CO 2 capture, storage and conversion. The electrochemical reduction of CO 2 into high-value liquid organic products could be of vital importance to mitigate this issue. The conversion of CO 2 into liquid fuels by using photovoltaic cells, which can readily be integrated in the current infrastructure, will help realize the creation of a sustainable cycle of carbon-based fuel that will promote zero net CO 2 emissions. Despite promising findings, significant challenges still persist that must be circumvented to make the technology profitable for large-scale utilization. With such possibilities, this Minireview presents the current high-performing catalysts for the electrochemical reduction of CO 2 to liquid hydrocarbons, address the limitations and unify the current understanding of the different reaction mechanisms. The Minireview also explores current research directions to improve process efficiencies and production rate and discusses the scope of using photo-assisted electrochemical reduction systems to find stable, highly efficient catalysts that can harvest solar energy directly to convert CO 2 into liquid hydrocarbons. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

The Biological Deep Sea Hydrothermal Vent as a Model to Study Carbon Dioxide Capturing Enzymes

PubMed Central

Minic, Zoran; Thongbam, Premila D.

2011-01-01

Deep sea hydrothermal vents are located along the mid-ocean ridge system, near volcanically active areas, where tectonic plates are moving away from each other. Sea water penetrates the fissures of the volcanic bed and is heated by magma. This heated sea water rises to the surface dissolving large amounts of minerals which provide a source of energy and nutrients to chemoautotrophic organisms. Although this environment is characterized by extreme conditions (high temperature, high pressure, chemical toxicity, acidic pH and absence of photosynthesis) a diversity of microorganisms and many animal species are specially adapted to this hostile environment. These organisms have developed a very efficient metabolism for the assimilation of inorganic CO2 from the external environment. In order to develop technology for the capture of carbon dioxide to reduce greenhouse gases in the atmosphere, enzymes involved in CO2 fixation and assimilation might be very useful. This review describes some current research concerning CO2 fixation and assimilation in the deep sea environment and possible biotechnological application of enzymes for carbon dioxide capture. PMID:21673885

Reversible capture of SO2 through functionalized ionic liquids.

PubMed

Yang, Dezhong; Hou, Minqiang; Ning, Hui; Ma, Jun; Kang, Xinchen; Zhang, Jianling; Han, Buxing

2013-07-01

Emission of SO2 in flue gas from the combustion of fossil fuels leads to severe environmental problems. Exploration of green and efficient methods to capture SO2 is an interesting topic, especially at lower SO2 partial pressures. In this work, ionic liquids (ILs) 1-(2-diethylaminoethyl)-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([Et2 NEMim][Tf2 N]) and 1-(2-diethylaminoethyl)-3-methylimidazolium tetrazolate ([Et2 NEMim][Tetz]) were synthesized. The performances of the two ILs to capture SO2 were studied under different conditions. It was demonstrated that the ILs were very efficient for SO2 absorption. The [Et2 NEMim][Tetz] IL designed in this work could absorb 0.47 g(SO2)g(IL)(-1) at 0.0101 MPa SO2 partial pressure, which is the highest capacity reported to date under the same conditions. The main reason for the large capacity was that both the cation and the anion could capture SO2 chemically. In addition, the IL could easily be regenerated, and the very high absorption capacity and rapid absorption/desorption rates were not changed over five repeated cycles. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Development of robust fluorinated TiO2/PVDF composite hollow fiber membrane for CO2 capture in gas-liquid membrane contactor

NASA Astrophysics Data System (ADS)

Lin, Yuqing; Xu, Yilin; Loh, Chun Heng; Wang, Rong

2018-04-01

Gas-liquid membrane contactor (GLMC) is a promising method to attain high efficiency for CO2 capture from flue gas, biogas and natural gas. However, membranes used in GLMC are prone to pore wetting due to insufficient hydrophobicity and low chemical resistance, resulting in significant increase in mass transfer resistance. To mitigate this issue, inorganic-organic fluorinated titania/polyvinylidene fluoride (fTiO2/PVDF) composite hollow fiber (HF) membranes was prepared via facile in-situ vapor induced hydrolyzation method, followed by hydrophobic modification. The proposed composite membranes were expected to couple the superb chemical stability of inorganic and high permeability/low cost of organic materials. The continuous fTiO2 layer deposited on top of PVDF substrate was found to possess a tighter microstructure and better hydrophobicity, which effectively prevented the membrane from wetting and lead to a high CO2 absorption flux (12.7 × 10-3 mol m-2 s-1). In a stability test with 21-day operation of GLMC using 1M monoethanolamine (MEA) as the absorbent, the fTiO2/PVDF membrane remained to be intact with a CO2 absorption flux decline of ∼16%, while the pristine PVDF membrane suffered from a flux decline of ∼80% due to membrane damage. Overall, this work provides an insight into the preparation of high-quality inorganic/organic composite HF membranes for CO2 capture in GLMC application.

Immobilized carbonic anhydrase on mesoporous cruciate flower-like metal organic framework for promoting CO2 sequestration.

PubMed

Ren, Sizhu; Feng, Yuxiao; Wen, Huan; Li, Conghai; Sun, Baoting; Cui, Jiandong; Jia, Shiru

2018-05-25

CO 2 capture by immobilized carbonic anhydrase (CA) has become an alternative and environmental friendly approach in CO 2 sequestration technology. However, the immobilized CA usually exhibits low CO 2 sequestration efficiency due to no gas adsorption function for the conventional CA supports. Metal organic frameworks (MOFs) are an excellent material for gas adsorption and enzyme immobilization. Herein, a combined immobilization system of CA and ZIF-8 with cruciate flower-like morphology for CO 2 adsorption was prepared for the first time by adsorbing CA onto ZIF-8. The immobilization efficiency was greater than 95%, and the maximum activity recovery reached 75%, indicating the highly efficient immobilization process. The resultant CA@ZIF-8 composites exhibited outstanding thermostability, the tolerance against denaturants, and reusability compared with free CA. Furthermore, we demonstrated for the first time that the shape of ZIF-8 could be controlled by adjusting concentrations of Zn 2+ ions at the high concentration of 2-methylimidazole (1 M). More importantly, we also demonstrated the applicability of the CA@ZIF-8 composites to the sequestration of CO 2 in carbonate minerals. The yields of the CaCO 3 obtained by using CA@ZIF-8 composites were 22-folds compared to free CA. Thus, this CA@ZIF-8 composite can be successfully used as a robust biocatalyst for sequestration of CO 2 . Copyright © 2018 Elsevier B.V. All rights reserved.

Geological Sequestration Training and Research Program in Capture and Transport: Development of the Most Economical Separation Method for CO2 Capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Vahdat, Nader

2013-09-30

The project provided hands-on training and networking opportunities to undergraduate students in the area of carbon dioxide (CO2) capture and transport, through fundamental research study focused on advanced separation methods that can be applied to the capture of CO2 resulting from the combustion of fossil-fuels for power generation . The project team’s approach to achieve its objectives was to leverage existing Carbon Capture and Storage (CCS) course materials and teaching methods to create and implement an annual CCS short course for the Tuskegee University community; conduct a survey of CO2 separation and capture methods; utilize data to verify and developmore » computer models for CO2 capture and build CCS networks and hands-on training experiences. The objectives accomplished as a result of this project were: (1) A comprehensive survey of CO2 capture methods was conducted and mathematical models were developed to compare the potential economics of the different methods based on the total cost per year per unit of CO2 avoidance; and (2) Training was provided to introduce the latest CO2 capture technologies and deployment issues to the university community.« less

Fingerprinting captured CO2 using natural tracers: Determining CO2 fate and proving ownership

NASA Astrophysics Data System (ADS)

Flude, Stephanie; Gilfillan, Stuart; Johnston, Gareth; Stuart, Finlay; Haszeldine, Stuart

2016-04-01

In the long term, captured CO2 will most likely be stored in large saline formations and it is highly likely that CO2 from multiple operators will be injected into a single saline formation. Understanding CO2 behavior within the reservoir is vital for making operational decisions and often uses geochemical techniques. Furthermore, in the event of a CO2 leak, being able to identify the owner of the CO2 is of vital importance in terms of liability and remediation. Addition of geochemical tracers to the CO2 stream is an effective way of tagging the CO2 from different power stations, but may become prohibitively expensive at large scale storage sites. Here we present results from a project assessing whether the natural isotopic composition (C, O and noble gas isotopes) of captured CO2 is sufficient to distinguish CO2 captured using different technologies and from different fuel sources, from likely baseline conditions. Results include analytical measurements of CO2 captured from a number of different CO2 capture plants and a comprehensive literature review of the known and hypothetical isotopic compositions of captured CO2 and baseline conditions. Key findings from the literature review suggest that the carbon isotope composition will be most strongly controlled by that of the feedstock, but significant fractionation is possible during the capture process; oxygen isotopes are likely to be controlled by the isotopic composition of any water used in either the industrial process or the capture technology; and noble gases concentrations will likely be controlled by the capture technique employed. Preliminary analytical results are in agreement with these predictions. Comparison with summaries of likely storage reservoir baseline and shallow or surface leakage reservoir baseline data suggests that C-isotopes are likely to be valuable tracers of CO2 in the storage reservoir, while noble gases may be particularly valuable as tracers of potential leakage.

Recent enlightening strategies for co2 capture: a review

NASA Astrophysics Data System (ADS)

Yuan, Peng; Qiu, Ziyang; Liu, Jia

2017-05-01

The global climate change has seriously affected the survival and prosperity of mankind, where greenhouse effect owing to atmospheric carbon dioxide (CO2) enrichment is a great cause. Accordingly, a series of down-to-earth measures need to be implemented urgently to control the output of CO2. As CO2 capture appears as a core issue in developing low-carbon economy, this review provides a comprehensive introduction of recent CO2 capture technologies used in power plants or other industries. Strategies for CO2 capture, e.g. pre-combustion, post-combustion and oxyfuel combustion, are covered in this article. Another enlightening technology for CO2 capture based on fluidized beds is intensively discussed.

Ship-in-a-bottle synthesis of amine-functionalized ionic liquids in NaY zeolite for CO2 capture

PubMed Central

Yu, Yinghao; Mai, Jingzhang; Wang, Lefu; Li, Xuehui; Jiang, Zheng; Wang, Furong

2014-01-01

CO2 capture on solid materials possesses significant advantages on the operation cost, process for large-scale CO2 capture and storage (CCS) that stimulates great interest in exploring high-performance solid CO2 adsorbents. A ship-in-a-bottle strategy was successfully developed to prepare the [APMIM]Br@NaY host–guest system in which an amine-functionalized ionic liquid (IL), 1-aminopropyl-3-methylimidazolium bromide ([APMIM]Br), was in-situ encapsulated in the NaY supercages. The genuine host-guest systems were thoroughly characterized and tested in CO2 capture from simulated flue gas. It was evidenced the encapsulated ILs are more stable than the bulk ILs. These host–guest systems exhibited superb overall CO2 capture capacity up to 4.94 mmol g−1 and the chemically adsorbed CO2 achieved 1.85 mmol g−1 depending on the [APMIM]Br loading amount. The chemisorbed CO2 can be desorbed rapidly by flushing with N2 gas at 50°C. The optimized [APMIM]Br@NaY system remains its original CO2 capture capacity in multiple cycling tests under prolonged harsh adsorption-desorption conditions. The excellent physicochemical properties and the CO2 capture performance of the host-guest systems offer them great promise for the future practice in the industrial CO2 capture. PMID:25104324

Inefficient power generation as an optimal route to negative emissions via BECCS?

NASA Astrophysics Data System (ADS)

Mac Dowell, Niall; Fajardy, Mathilde

2017-04-01

Current ambitions to limit climate change to no more than 1.5 °C-2 °C by the end of the 21st century rely heavily on the availability of negative emissions technologies (NETs)—bioenergy with CO2 capture and storage (BECCS) and direct air capture in particular. In this context, these NETs are providing a specific service by removing CO2 from the atmosphere, and therefore investors would expect an appropriate risk-adjusted rate of return, varying as a function of the quantity of public money involved. Uniquely, BECCS facilities have the possibility to generate both low carbon power and remove CO2 from the atmosphere, but in an energy system characterised by high penetration of intermittent renewable energy such as wind and solar power plants, the dispatch load factor of such BECCS facilities may be small relative to their capacity. This has the potential to significantly under utilise these assets for their primary purpose of removing CO2 from the atmosphere. In this study, we present a techno-economic environmental evaluation of BECCS plants with a range of operating efficiencies, considering their full- and part-load operation relative to a national-scale annual CO2 removal target. We find that in all cases, a lower capital cost, lower efficiency BECCS plant is superior to a higher cost, higher efficiency facility from both environmental and economic perspectives. We show that it may be preferable to operate the BECCS facility in base-load fashion, constantly removing CO2 from the atmosphere and dispatching electricity on an as-needed basis. We show that the use of this ‘spare capacity’ to produce hydrogen for, e.g. injection to a natural gas system for the provision of low carbon heating can add to the overall environmental and economic benefit of such a system. The only point where this hypothesis appears to break down is where the CO2 emissions associated with the biomass supply chain are sufficiently large so as to eliminate the service of CO2 removal.

Separation and capture of CO2 from large stationary sources and sequestration in geological formations--coalbeds and deep saline aquifers.

PubMed

White, Curt M; Strazisar, Brian R; Granite, Evan J; Hoffman, James S; Pennline, Henry W

2003-06-01

The topic of global warming as a result of increased atmospheric CO2 concentration is arguably the most important environmental issue that the world faces today. It is a global problem that will need to be solved on a global level. The link between anthropogenic emissions of CO2 with increased atmospheric CO2 levels and, in turn, with increased global temperatures has been well established and accepted by the world. International organizations such as the United Nations Framework Convention on Climate Change (UNFCCC) and the Intergovernmental Panel on Climate Change (IPCC) have been formed to address this issue. Three options are being explored to stabilize atmospheric levels of greenhouse gases (GHGs) and global temperatures without severely and negatively impacting standard of living: (1) increasing energy efficiency, (2) switching to less carbon-intensive sources of energy, and (3) carbon sequestration. To be successful, all three options must be used in concert. The third option is the subject of this review. Specifically, this review will cover the capture and geologic sequestration of CO2 generated from large point sources, namely fossil-fuel-fired power gasification plants. Sequestration of CO2 in geological formations is necessary to meet the President's Global Climate Change Initiative target of an 18% reduction in GHG intensity by 2012. Further, the best strategy to stabilize the atmospheric concentration of CO2 results from a multifaceted approach where sequestration of CO2 into geological formations is combined with increased efficiency in electric power generation and utilization, increased conservation, increased use of lower carbon-intensity fuels, and increased use of nuclear energy and renewables. This review covers the separation and capture of CO2 from both flue gas and fuel gas using wet scrubbing technologies, dry regenerable sorbents, membranes, cryogenics, pressure and temperature swing adsorption, and other advanced concepts. Existing commercial CO2 capture facilities at electric power-generating stations based on the use of monoethanolamine are described, as is the Rectisol process used by Dakota Gasification to separate and capture CO2 from a coal gasifier. Two technologies for storage of the captured CO2 are reviewed--sequestration in deep unmineable coalbeds with concomitant recovery of CH4 and sequestration in deep saline aquifers. Key issues for both of these techniques include estimating the potential storage capacity, the storage integrity, and the physical and chemical processes that are initiated by injecting CO2 underground. Recent studies using computer modeling as well as laboratory and field experimentation are presented here. In addition, several projects have been initiated in which CO2 is injected into a deep coal seam or saline aquifer. The current status of several such projects is discussed. Included is a commercial-scale project in which a million tons of CO2 are injected annually into an aquifer under the North Sea in Norway. The review makes the case that this can all be accomplished safely with off-the-shelf technologies. However, substantial research and development must be performed to reduce the cost, decrease the risks, and increase the safety of sequestration technologies. This review also includes discussion of possible problems related to deep injection of CO2. There are safety concerns that need to be addressed because of the possibilities of leakage to the surface and induced seismic activity. These issues are presented along with a case study of a similar incident in the past. It is clear that monitoring and verification of storage will be a crucial part of all geological sequestration practices so that such problems may be avoided. Available techniques include direct measurement of CO2 and CH4 surface soil fluxes, the use of chemical tracers, and underground 4-D seismic monitoring. Ten new hypotheses were formulated to describe what happens when CO2 is pumped into a coal seam. These hypotheses provide significant insight into the fundamental chemical, physical, and thermodynamic phenomena that occur during coal seam sequestration of CO2.

Alkali Metal CO2 Sorbents and the Resulting Metal Carbonates: Potential for Process Intensification of Sorption-Enhanced Steam Reforming.

PubMed

Memon, Muhammad Zaki; Zhao, Xiao; Sikarwar, Vineet Singh; Vuppaladadiyam, Arun K; Milne, Steven J; Brown, Andy P; Li, Jinhui; Zhao, Ming

2017-01-03

Sorption-enhanced steam reforming (SESR) is an energy and cost efficient approach to produce hydrogen with high purity. SESR makes it economically feasible to use a wide range of feedstocks for hydrogen production such as methane, ethanol, and biomass. Selection of catalysts and sorbents plays a vital role in SESR. This article reviews the recent research aimed at process intensification by the integration of catalysis and chemisorption functions into a single material. Alkali metal ceramic powders, including Li 2 ZrO 3 , Li 4 SiO 4 and Na 2 ZrO 3 display characteristics suitable for capturing CO 2 at low concentrations (<15% CO 2 ) and high temperatures (>500 °C), and thus are applicable to precombustion technologies such as SESR, as well as postcombustion capture of CO 2 from flue gases. This paper reviews the progress made in improving the operational performance of alkali metal ceramics under conditions that simulate power plant and SESR operation, by adopting new methods of sorbent synthesis and doping with additional elements. The paper also discusses the role of carbonates formed after in situ CO 2 chemisorption during a steam reforming process in respect of catalysts for tar cracking.

Conductive Graphitic Carbon Nitride as an Ideal Material for Electrocatalytically Switchable CO2 Capture

PubMed Central

Tan, Xin; Kou, Liangzhi; Tahini, Hassan A.; Smith, Sean C.

2015-01-01

Good electrical conductivity and high electron mobility of the sorbent materials are prerequisite for electrocatalytically switchable CO2 capture. However, no conductive and easily synthetic sorbent materials are available until now. Here, we examined the possibility of conductive graphitic carbon nitride (g-C4N3) nanosheets as sorbent materials for electrocatalytically switchable CO2 capture. Using first-principle calculations, we found that the adsorption energy of CO2 molecules on g-C4N3 nanosheets can be dramatically enhanced by injecting extra electrons into the adsorbent. At saturation CO2 capture coverage, the negatively charged g-C4N3 nanosheets achieve CO2 capture capacities up to 73.9 × 1013 cm−2 or 42.3 wt%. In contrast to other CO2 capture approaches, the process of CO2 capture/release occurs spontaneously without any energy barriers once extra electrons are introduced or removed, and these processes can be simply controlled and reversed by switching on/off the charging voltage. In addition, these negatively charged g-C4N3 nanosheets are highly selective for separating CO2 from mixtures with CH4, H2 and/or N2. These predictions may prove to be instrumental in searching for a new class of experimentally feasible high-capacity CO2 capture materials with ideal thermodynamics and reversibility. PMID:26621618

Innovative nano-layered solid sorbents for CO2 capture.

PubMed

Li, Bingyun; Jiang, Bingbing; Fauth, Daniel J; Gray, McMahan L; Pennline, Henry W; Richards, George A

2011-02-14

Nano-layered sorbents for CO(2) capture, for the first time, were developed using layer-by-layer nanoassembly. A CO(2)-adsorbing polymer and a strong polyelectrolyte were alternately immobilized within porous particles. The developed sorbents had fast CO(2) adsorption and desorption properties and their CO(2) capture capacity increased with increasing nano-layers of the CO(2)-adsorbing polymer.

Highly Efficient Oxygen-Storage Material with Intrinsic Coke Resistance for Chemical Looping Combustion-Based CO2 Capture.

PubMed

Imtiaz, Qasim; Kurlov, Alexey; Rupp, Jennifer Lilia Marguerite; Müller, Christoph Rüdiger

2015-06-22

Chemical looping combustion (CLC) and chemical looping with oxygen uncoupling (CLOU) are emerging thermochemical CO2 capture cycles that allow the capture of CO2 with a small energy penalty. Here, the development of suitable oxygen carrier materials is a key aspect to transfer these promising concepts to practical installations. CuO is an attractive material for CLC and CLOU because of its high oxygen-storage capacity (20 wt %), fast reaction kinetics, and high equilibrium partial pressure of oxygen at typical operating temperatures (850-1000 °C). However, despite its promising characteristics, its low Tammann temperature requires the development of new strategies to phase-stabilize CuO-based oxygen carriers. In this work, we report a strategy based on stabilization by co-precipitated ceria (CeO2-x ), which allowed us to increase the oxygen capacity, coke resistance, and redox stability of CuO-based oxygen carriers substantially. The performance of the new oxygen carriers was evaluated in detail and compared to the current state-of-the-art materials, that is, Al2 O3 -stabilized CuO with similar CuO loadings. We also demonstrate that the higher intrinsic oxygen uptake, release, and mobility in CeO2-x -stabilized CuO leads to a three times higher carbon deposition resistance compared to that of Al2 O3 -stabilized CuO. Moreover, we report a high cyclic stability without phase intermixing for CeO2-x -supported CuO. This was accompanied by a lower reduction temperature compared to state-of-the-art Al2 O3 -supported CuO. As a result of its high resistance towards carbon deposition and fast oxygen uncoupling kinetics, CeO2-x -stabilized CuO is identified as a very promising material for CLC- and CLOU-based CO2 capture architectures. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Surface modification of a low cost bentonite for post-combustion CO2 capture

NASA Astrophysics Data System (ADS)

Chen, Chao; Park, Dong-Wha; Ahn, Wha-Seung

2013-10-01

A low cost bentonite was modified with PEI (polyethylenimine) through a physical impregnation method. Bentonite in its natural state and after amine modification were characterized by scanning electron microscopy-energy dispersive X-ray spectroscopy, X-ray diffraction, N2 adsorption-desorption isotherms, and investigated for CO2 capture using a thermogravimetric analysis unit connected to a flow panel. The effect of adsorption temperature, PEI loading and CO2 partial pressure on the CO2 capture performance of the PEI-modified bentonite was examined. A cyclic CO2 adsorption-desorption test was also carried out to assess the stability of PEI-modified bentonite as a CO2 adsorbent. Bentonite in its natural state showed negligible CO2 uptake. After amine modification, the CO2 uptake increased significantly due to CO2 capture by amine species introduced via chemisorption. The PEI-modified bentonites showed high CO2 capture selectivity over N2, and exhibited excellent stability in cyclic CO2 adsorption-desorption runs.

Predicting long-term performance of engineered geologic carbon dioxide storage systems to inform decisions amidst uncertainty

NASA Astrophysics Data System (ADS)

Pawar, R.

2016-12-01

Risk assessment and risk management of engineered geologic CO2 storage systems is an area of active investigation. The potential geologic CO2 storage systems currently under consideration are inherently heterogeneous and have limited to no characterization data. Effective risk management decisions to ensure safe, long-term CO2 storage requires assessing and quantifying risks while taking into account the uncertainties in a storage site's characteristics. The key decisions are typically related to definition of area of review, effective monitoring strategy and monitoring duration, potential of leakage and associated impacts, etc. A quantitative methodology for predicting a sequestration site's long-term performance is critical for making key decisions necessary for successful deployment of commercial scale geologic storage projects where projects will require quantitative assessments of potential long-term liabilities. An integrated assessment modeling (IAM) paradigm which treats a geologic CO2 storage site as a system made up of various linked subsystems can be used to predict long-term performance. The subsystems include storage reservoir, seals, potential leakage pathways (such as wellbores, natural fractures/faults) and receptors (such as shallow groundwater aquifers). CO2 movement within each of the subsystems and resulting interactions are captured through reduced order models (ROMs). The ROMs capture the complex physical/chemical interactions resulting due to CO2 movement and interactions but are computationally extremely efficient. The computational efficiency allows for performing Monte Carlo simulations necessary for quantitative probabilistic risk assessment. We have used the IAM to predict long-term performance of geologic CO2 sequestration systems and to answer questions related to probability of leakage of CO2 through wellbores, impact of CO2/brine leakage into shallow aquifer, etc. Answers to such questions are critical in making key risk management decisions. A systematic uncertainty quantification approach can been used to understand how uncertain parameters associated with different subsystems (e.g., reservoir permeability, wellbore cement permeability, wellbore density, etc.) impact the overall site performance predictions.

Multishelled CaO Microspheres Stabilized by Atomic Layer Deposition of Al2 O3 for Enhanced CO2 Capture Performance.

PubMed

Armutlulu, Andac; Naeem, Muhammad Awais; Liu, Hsueh-Ju; Kim, Sung Min; Kierzkowska, Agnieszka; Fedorov, Alexey; Müller, Christoph R

2017-11-01

CO 2 capture and storage is a promising concept to reduce anthropogenic CO 2 emissions. The most established technology for capturing CO 2 relies on amine scrubbing that is, however, associated with high costs. Technoeconomic studies show that using CaO as a high-temperature CO 2 sorbent can significantly reduce the costs of CO 2 capture. A serious disadvantage of CaO derived from earth-abundant precursors, e.g., limestone, is the rapid, sintering-induced decay of its cyclic CO 2 uptake. Here, a template-assisted hydrothermal approach to develop CaO-based sorbents exhibiting a very high and cyclically stable CO 2 uptake is exploited. The morphological characteristics of these sorbents, i.e., a porous shell comprised of CaO nanoparticles coated by a thin layer of Al 2 O 3 (<3 nm) containing a central void, ensure (i) minimal diffusion limitations, (ii) space to accompany the substantial volumetric changes during CO 2 capture and release, and (iii) a minimal quantity of Al 2 O 3 for structural stabilization, thus maximizing the fraction of CO 2 -capture-active CaO. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Direct Air Capture of CO2 with an Amine Resin: A Molecular Modeling Study of the CO2 Capturing Process

PubMed Central

2017-01-01

Several reactions, known from other amine systems for CO2 capture, have been proposed for Lewatit R VP OC 1065. The aim of this molecular modeling study is to elucidate the CO2 capture process: the physisorption process prior to the CO2-capture and the reactions. Molecular modeling yields that the resin has a structure with benzyl amine groups on alternating positions in close vicinity of each other. Based on this structure, the preferred adsorption mode of CO2 and H2O was established. Next, using standard Density Functional Theory two catalytic reactions responsible for the actual CO2 capture were identified: direct amine and amine-H2O catalyzed formation of carbamic acid. The latter is a new type of catalysis. Other reactions are unlikely. Quantitative verification of the molecular modeling results with known experimental CO2 adsorption isotherms, applying a dual site Langmuir adsorption isotherm model, further supports all results of this molecular modeling study. PMID:29142339

Modeling of sonochemistry in water in the presence of dissolved carbon dioxide.

PubMed

Authier, Olivier; Ouhabaz, Hind; Bedogni, Stefano

2018-07-01

CO 2 capture and utilization (CCU) is a process that captures CO 2 emissions from sources such as fossil fuel power plants and reuses them so that they will not enter the atmosphere. Among the various ways of recycling CO 2 , reduction reactions are extensively studied at lab-scale. However, CO 2 reduction by standard methods is difficult. Sonochemistry may be used in CO 2 gas mixtures bubbled through water subjected to ultrasound waves. Indeed, the sonochemical reduction of CO 2 in water has been already investigated by some authors, showing that fuel species (CO and H 2 ) are obtained in the final products. The aim of this work is to model, for a single bubble, the close coupling of the mechanisms of bubble dynamics with the kinetics of gas phase reactions in the bubble that can lead to CO 2 reduction. An estimation of time-scales is used to define the controlling steps and consequently to solve a reduced model. The calculation of the concentration of free radicals and gases formed in the bubble is undertaken over many cycles to look at the effects of ultrasound frequency, pressure amplitude, initial bubble radius and bubble composition in CO 2 . The strong effect of bubble composition on the CO 2 reduction rate is confirmed in accordance with experimental data from the literature. When the initial fraction of CO 2 in the bubble is low, bubble growth and collapse are slightly modified with respect to simulation without CO 2 , and chemical reactions leading to CO 2 reduction are promoted. However, the peak collapse temperature depends on the thermal properties of the CO 2 and greatly decreases as the CO 2 increases in the bubble. The model shows that initial bubble radius, ultrasound frequency and pressure amplitude play a critical role in CO 2 reduction. Hence, in the case of a bubble with an initial radius of around 5 μm, CO 2 reduction appears to be more favorable at a frequency around 300 kHz than at a low frequency of around 20 kHz. Finally, the industrial application of ultrasound to CO 2 reduction in water would be largely dependent on sonochemical efficiency. Under the conditions tested, this process does not seem to be sufficiently efficient. Copyright © 2018 Elsevier B.V. All rights reserved.

Biotechnological storage and utilization of entrapped solar energy.

PubMed

Bhattacharya, Sumana; Schiavone, Marc; Nayak, Amiya; Bhattacharya, Sanjoy K

2005-03-01

Our laboratory has recently developed a device employing immobilized F0F1 adenosine triphosphatase (ATPase) that allows synthesis of adenosine triphosphate (ATP) from adenosine 5'-diphosphate and inorganic phosphate using solar energy. We present estimates of total solar energy received by Earth's land area and demonstrate that its efficient capture may allow conversion of solar energy and storage into bonds of biochemicals using devices harboring either immobilized ATPase or NADH dehydrogenase. Capture and storage of solar energy into biochemicals may also enable fixation of CO2 emanating from polluting units. The cofactors ATP and NADH synthesized using solar energy could be used for regeneration of acceptor D-ribulose-1,5-bisphosphate from 3-phosphoglycerate formed during CO2 fixation.

Increased light-use efficiency in northern terrestrial ecosystems indicated by CO 2 and greening observations: INCREASE IN NH LIGHT USE EFFICIENCY

DOE Office of Scientific and Technical Information (OSTI.GOV)

Thomas, Rebecca T.; Prentice, Iain Colin; Graven, Heather

2016-11-04

Observations show an increasing amplitude in the seasonal cycle of CO2 (ASC) north of 45°N of 56 ± 9.8% over the last 50 years and an increase in vegetation greenness of 7.5–15% in high northern latitudes since the 1980s. However, the causes of these changes remain uncertain. Historical simulations from terrestrial biosphere models in the Multiscale Synthesis and Terrestrial Model Intercomparison Project are compared to the ASC and greenness observations, using the TM3 atmospheric transport model to translate surface fluxes into CO2 concentrations. We find that the modeled change in ASC is too small but the mean greening trend ismore » generally captured. Modeled increases in greenness are primarily driven by warming, whereas ASC changes are primarily driven by increasing CO2. We suggest that increases in ecosystem-scale light use efficiency (LUE) have contributed to the observed ASC increase but are underestimated by current models. We highlight potential mechanisms that could increase modeled LUE.« less

Porous MOF with Highly Efficient Selectivity and Chemical Conversion for CO2.

PubMed

Wang, Hai-Hua; Hou, Lei; Li, Yong-Zhi; Jiang, Chen-Yu; Wang, Yao-Yu; Zhu, Zhonghua

2017-05-31

A new Co(II)-based MOF, {[Co 2 (tzpa)(OH)(H 2 O) 2 ]·DMF} n (1) (H 3 tzpa = 5-(4-(tetrazol-5-yl)phenyl)isophthalic acid), was constructed by employing a tetrazolyl-carboxyl ligand H 3 tzpa. 1 possesses 1D tubular channels that are decorated by μ 3 -OH groups, uncoordinated carboxylate O atoms, and open metal centers generated by the removal of coordinated water molecules, leading to high CO 2 adsorption capacity and significantly selective capture for CO 2 over CH 4 and CO in the temperature range of 298-333 K. Moreover, 1 shows the chemical stability in acidic and basic aqueous solutions. Grand canonical Monte Carlo simulations identified multiple CO 2 -philic sites in 1. In addition, the activated 1 as the heterogeneous Lewis and Brønsted acid bifunctional catalyst facilitates the chemical fixation of CO 2 coupling with epoxides into cyclic carbonates under ambient conditions.

Synergistic Carbon Dioxide Capture and Conversion in Porous Materials.

PubMed

Zhang, Yugen; Lim, Diane S W

2015-08-24

Global climate change and excessive CO2 emissions have caused widespread public concern in recent years. Tremendous efforts have been made towards CO2 capture and conversion. This has led to the development of numerous porous materials as CO2 capture sorbents. Concurrently, the conversion of CO2 into value-added products by chemical methods has also been well-documented recently. However, realizing the attractive prospect of direct, in situ chemical conversion of captured CO2 into other chemicals remains a challenge. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Mineral Carbonation Potential of CO2 from Natural and Industrial-based Alkalinity Sources

NASA Astrophysics Data System (ADS)

Wilcox, J.; Kirchofer, A.

2014-12-01

Mineral carbonation is a Carbon Capture and Storage (CSS) technology where gaseous CO2 is reacted with alkaline materials (such as silicate minerals and alkaline industrial wastes) and converted into stable and environmentally benign carbonate minerals (Metz et al., 2005). Here, we present a holistic, transparent life cycle assessment model of aqueous mineral carbonation built using a hybrid process model and economic input-output life cycle assessment approach. We compared the energy efficiency and the net CO2 storage potential of various mineral carbonation processes based on different feedstock material and process schemes on a consistent basis by determining the energy and material balance of each implementation (Kirchofer et al., 2011). In particular, we evaluated the net CO2 storage potential of aqueous mineral carbonation for serpentine, olivine, cement kiln dust, fly ash, and steel slag across a range of reaction conditions and process parameters. A preliminary systematic investigation of the tradeoffs inherent in mineral carbonation processes was conducted and guidelines for the optimization of the life-cycle energy efficiency are provided. The life-cycle assessment of aqueous mineral carbonation suggests that a variety of alkalinity sources and process configurations are capable of net CO2 reductions. The maximum carbonation efficiency, defined as mass percent of CO2 mitigated per CO2 input, was 83% for CKD at ambient temperature and pressure conditions. In order of decreasing efficiency, the maximum carbonation efficiencies for the other alkalinity sources investigated were: olivine, 66%; SS, 64%; FA, 36%; and serpentine, 13%. For natural alkalinity sources, availability is estimated based on U.S. production rates of a) lime (18 Mt/yr) or b) sand and gravel (760 Mt/yr) (USGS, 2011). The low estimate assumes the maximum sequestration efficiency of the alkalinity source obtained in the current work and the high estimate assumes a sequestration efficiency of 85%. The total CO2 storage potential for the alkalinity sources considered in the U.S. ranges from 1.3% to 23.7% of U.S. CO2 emissions, depending on the assumed availability of natural alkalinity sources and efficiency of the mineral carbonation processes.

Sensor placement algorithm development to maximize the efficiency of acid gas removal unit for integrated gasifiction combined sycle (IGCC) power plant with CO2 capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Paul, P.; Bhattacharyya, D.; Turton, R.

2012-01-01

Future integrated gasification combined cycle (IGCC) power plants with CO{sub 2} capture will face stricter operational and environmental constraints. Accurate values of relevant states/outputs/disturbances are needed to satisfy these constraints and to maximize the operational efficiency. Unfortunately, a number of these process variables cannot be measured while a number of them can be measured, but have low precision, reliability, or signal-to-noise ratio. In this work, a sensor placement (SP) algorithm is developed for optimal selection of sensor location, number, and type that can maximize the plant efficiency and result in a desired precision of the relevant measured/unmeasured states. In thismore » work, an SP algorithm is developed for an selective, dual-stage Selexol-based acid gas removal (AGR) unit for an IGCC plant with pre-combustion CO{sub 2} capture. A comprehensive nonlinear dynamic model of the AGR unit is developed in Aspen Plus Dynamics® (APD) and used to generate a linear state-space model that is used in the SP algorithm. The SP algorithm is developed with the assumption that an optimal Kalman filter will be implemented in the plant for state and disturbance estimation. The algorithm is developed assuming steady-state Kalman filtering and steady-state operation of the plant. The control system is considered to operate based on the estimated states and thereby, captures the effects of the SP algorithm on the overall plant efficiency. The optimization problem is solved by Genetic Algorithm (GA) considering both linear and nonlinear equality and inequality constraints. Due to the very large number of candidate sets available for sensor placement and because of the long time that it takes to solve the constrained optimization problem that includes more than 1000 states, solution of this problem is computationally expensive. For reducing the computation time, parallel computing is performed using the Distributed Computing Server (DCS®) and the Parallel Computing® toolbox from Mathworks®. In this presentation, we will share our experience in setting up parallel computing using GA in the MATLAB® environment and present the overall approach for achieving higher computational efficiency in this framework.« less

Sensor placement algorithm development to maximize the efficiency of acid gas removal unit for integrated gasification combined cycle (IGCC) power plant with CO{sub 2} capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Paul, P.; Bhattacharyya, D.; Turton, R.

2012-01-01

Future integrated gasification combined cycle (IGCC) power plants with CO{sub 2} capture will face stricter operational and environmental constraints. Accurate values of relevant states/outputs/disturbances are needed to satisfy these constraints and to maximize the operational efficiency. Unfortunately, a number of these process variables cannot be measured while a number of them can be measured, but have low precision, reliability, or signal-to-noise ratio. In this work, a sensor placement (SP) algorithm is developed for optimal selection of sensor location, number, and type that can maximize the plant efficiency and result in a desired precision of the relevant measured/unmeasured states. In thismore » work, an SP algorithm is developed for an selective, dual-stage Selexol-based acid gas removal (AGR) unit for an IGCC plant with pre-combustion CO{sub 2} capture. A comprehensive nonlinear dynamic model of the AGR unit is developed in Aspen Plus Dynamics® (APD) and used to generate a linear state-space model that is used in the SP algorithm. The SP algorithm is developed with the assumption that an optimal Kalman filter will be implemented in the plant for state and disturbance estimation. The algorithm is developed assuming steady-state Kalman filtering and steady-state operation of the plant. The control system is considered to operate based on the estimated states and thereby, captures the effects of the SP algorithm on the overall plant efficiency. The optimization problem is solved by Genetic Algorithm (GA) considering both linear and nonlinear equality and inequality constraints. Due to the very large number of candidate sets available for sensor placement and because of the long time that it takes to solve the constrained optimization problem that includes more than 1000 states, solution of this problem is computationally expensive. For reducing the computation time, parallel computing is performed using the Distributed Computing Server (DCS®) and the Parallel Computing® toolbox from Mathworks®. In this presentation, we will share our experience in setting up parallel computing using GA in the MATLAB® environment and present the overall approach for achieving higher computational efficiency in this framework.« less

Bench-Scale Development of a Hot Carbonate Absorption Process with Crystallization-Enabled High-Pressure Stripping for Post-Combustion CO{sub 2} Capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lu, Yongqi; DeVries, Nicholas; Ruhter, David

A novel Hot Carbonate Absorption Process with Crystallization-Enabled High-Pressure Stripping (Hot-CAP) has been developed by the University of Illinois at Urbana-Champaign and Carbon Capture Scientific, LLC in this three-year, bench-scale project. The Hot-CAP features a concentrated carbonate solution (e.g., K{sub 2}CO{sub 3}) for CO{sub 2} absorption and a bicarbonate slurry (e.g., KHCO{sub 3}) for high-pressure CO{sub 2} stripping to overcome the energy use and other disadvantages associated with the benchmark monoethanolamine (MEA) process. The project was aimed at performing laboratory- and bench-scale experiments to prove its technical feasibility and generate process engineering and scale-up data, and conducting a techno-economic analysismore » (TEA) to demonstrate its energy use and cost competitiveness over MEA. To meet project goals and objectives, a combination of experimental, modeling, process simulation, and economic analysis studies were applied. Carefully designed and intensive experiments were conducted to measure thermodynamic and reaction engineering data relevant to four major unit operations in the Hot-CAP (i.e., CO{sub 2} absorption, CO{sub 2} stripping, bicarbonate crystallization, and sulfate reclamation). The rate promoters that could accelerate the CO{sub 2} absorption rate into the potassium carbonate/bicarbonate (PCB) solution to a level greater than that into the 5 M MEA solution were identified, and the superior performance of CO{sub 2} absorption into PCB was demonstrated in a bench-scale packed-bed column. Kinetic data on bicarbonate crystallization were developed and applied for crystallizer design and sizing. Parametric testing of high-pressure CO{sub 2} stripping with concentrated bicarbonate-dominant slurries at high temperatures ({>=}140{degrees}C) in a bench-scale stripping column demonstrated lower heat use than with MEA. The feasibility of a modified process for combining SO{sub 2} removal with CO{sub 2} capture was preliminarily demonstrated. In addition to the experimental studies, the technical challenges pertinent to fouling of slurry-handling equipment and the design of the crystallizer and stripper were addressed through consultation with vendors and engineering analyses. A process flow diagram of the Hot-CAP was then developed and a TEA was performed to compare the energy use and cost performance of a nominal 550-MWe subcritical pulverized coal (PC)-fired power plant without CO{sub 2} capture (DOE/NETL Case 9) with the benchmark MEA-based post-combustion CO{sub 2} capture (PCC; DOE/NETL Case 10) and the Hot-CAP-based PCC. The results revealed that the net power produced in the PC + Hot-CAP is 609 MWe, greater than the PC + MEA (550 MWe). The 20-year levelized cost of electricity (LCOE) for the PC + Hot-CAP, including CO{sub 2} transportation and storage, is 120.3 mills/kWh, a 60% increase over the base PC plant without CO{sub 2} capture. The LCOE increase for the Hot-CAP is 29% lower than that for MEA. TEA results demonstrated that the Hot-CAP is energy-efficient and cost-effective compared with the benchmark MEA process.« less

Electropolymerized carbonic anhydrase immobilization for carbon dioxide capture.

PubMed

Merle, Geraldine; Fradette, Sylvie; Madore, Eric; Barralet, Jake E

2014-06-17

Biomimetic carbonation carried out with carbonic anhydrase (CA) in CO2-absorbing solutions, such as methyldiethanolamine (MDEA), is one approach that has been developed to accelerate the capture of CO2. However, there are several practical issues, such as high cost and limited enzyme stability, that need to be overcome. In this study, the capacity of CA immobilization on a porous solid support was studied to improve the instability in the tertiary amine solvent. We have shown that a 63% porosity macroporous carbon foam support makes separation and reuse facile and allows for an efficient supply and presentation of CO2 to an aqueous solvent and the enzyme catalytic center. These enzymatic supports conserved 40% of their initial activity after 42 days at 70 °C in an amine solvent, whereas the free enzyme shows no activity after 1 h in the same conditions. In this work, we have overcome the technical barrier associated with the recovery of the biocatalyst after operation, and most of all, these electropolymerized enzymatic supports have shown a remarkable increase of thermal stability in an amine-based CO2 sequestration solvent.

Enhancing Catalyzed Decomposition of Na2CO3 with Co2MnO x Nanowire-Decorated Carbon Fibers for Advanced Na-CO2 Batteries.

PubMed

Fang, Cong; Luo, Jianmin; Jin, Chengbin; Yuan, Huadong; Sheng, Ouwei; Huang, Hui; Gan, Yongping; Xia, Yang; Liang, Chu; Zhang, Jun; Zhang, Wenkui; Tao, Xinyong

2018-05-23

The metal-CO 2 batteries, especially Na-CO 2 , batteries come into sight owing to their high energy density, ability for CO 2 capture, and the abundance of sodium resource. Besides the sluggish electrochemical reactions at the gas cathodes and the instability of the electrolyte at a high voltage, the final discharge product Na 2 CO 3 is a solid and poor conductor of electricity, which may cause the high overpotential and poor cycle performance for the Na-CO 2 batteries. The promotion of decomposition of Na 2 CO 3 should be an efficient strategy to enhance the electrochemical performance. Here, we design a facile Na 2 CO 3 activation experiment to screen the efficient cathode catalyst for the Na-CO 2 batteries. It is found that the Co 2 MnO x nanowire-decorated carbon fibers (CMO@CF) can promote the Na 2 CO 3 decomposition at the lowest voltage among all these metal oxide-decorated carbon fiber structures. After assembling the Na-CO 2 batteries, the electrodes based on CMO@CF show lower overpotential and better cycling performance compared with the electrodes based on pristine carbon fibers and other metal oxide-modified carbon fibers. We believe this catalyst screening method and the freestanding structure of the CMO@CF electrode may provide an important reference for the development of advanced Na-CO 2 batteries.

Flexibility of CCS Power Plants and Transport Systems

NASA Astrophysics Data System (ADS)

Nimtz, Michael; Krautz, Hans-Joachim

2013-04-01

Growing shares of renewable energy in the German power grid urge fossil fuelled power plants to reduce load or to shut down completely with increasing frequency and amplitude. Shut down, load changes and the following restart or ramp-up often have to be carried out as fast as possible. To realize such fast transitions is already complicated and expensive for conventional power plants - if further measures for CO2 reduction are applied, the task is even harder. Capture equipment and transport systems will add further process steps as well as additional masses of fluids and construction material. This will result in a change of time constants and a generally slower system reaction on changes in parameters like load, temperature and pressure in the power plant components and capture units. On the other hand there is only limited time to earn money by selling electricity - if there is a chance to sell more electricity in a short term, efficiencies should be as high as possible. Any capture unit that would reduce the efficiency causes economic conflicts. Therefore measures are analysed to offset the power generation from the capture process in time or to reduce the capture load temporarily. The poster will present a case study for different CCS power plant configurations and load scenarios representing typical grid load from renewable energies. Approaches to balance the load and/or the CO2 output of these power plants will be presented. These approaches comprise: bypassing of flue gas, intermediate storage of heat and/or fluids. Amounts of additional steam, electrical energy and other process fluids (e.g. scrubbing fluids like MEA) and size of auxiliary equipment will be shown .Finally, effects on the transport system (e.g. cooling down of CO2 in the pipeline and changes in mass and volume flow) will be presented and discussed.

Computational evaluation of metal-organic frameworks for carbon dioxide capture

NASA Astrophysics Data System (ADS)

Yu, Jiamei

Metal-organic frameworks (MOFs), a new class of porous solids comprised of metal-containing nodes linked by organic ligands, have become promising materials for gas separations. In particular, their flexible chemistry makes them attractive for CO2 capture from flue gas streams in post-combustion plants. Although numerous efforts have been exerted on the investigation of MOFs for CO2 capture, the exploration of the effects from coexisting components present in very dilute proportions in flue gases is limited because of the experimental difficulty to determine the coadsorption of CO2 with trace components. In this regard, molecular simulations show superiority. In this study, molecular simulations are used to estimate the influence of impurities: water, O2, and SO2 on post-combustion CO2 capture in MOFs. Firstly, two MOFs with coordinatively unsaturated metal sites (CUMs), HKUST-1 and Mg-MOF-74 are explored. Increase of CO 2 adsorption is observed for hydrated HKUST-1; on the contrary, the opposite water adsorption behavior is observed in hydrated Mg-MOF-74, leading to decrease of CO2 adsorption. Further, water effects on CO 2 capture in M-HKUST1 (M = Mg, Zn, Co, Ni) are evaluated to test whether comparing the binding energy could be a general method to evaluate water effects in MOFs with CUMs. It is found that the method works well for Zn-, Co-, and Ni-HKUST1 but partially for Mg-HKUST1. In addition, the effects of O2 and SO2 on CO2 capture in MOFs are also investigated for the first time, showing that the effects of O2 may be negligible but SO2 has negative effects in the CO 2 capture process in HKUST-1 systems. Secondly, the influences of water on CO2 capture in three UiO-66 MOFs with functional groups, --NH2, --OH and --Br are explored, respectively. For UiO-66-NH2 and -OH, the presence of water lowers CO2 adsorption significantly; in contrast, water shows much smaller effects in UiO-66-Br. Moreover, the presence of SO 2 decreases water adsorption but enhances CO2 uptakes slightly in both UiO-66-NH2 and -Br. Finally, the effects of impurities on CO2 capture in a MOF with suitable pore size (PCN-200) are analyzed. The adsorption of both CO 2 and N2 decrease substantially even with 1% water present in the mixture. In addition, the presence of low SO2 does not show obvious effect in PCN-200. However, a lower CO2 adsorption is observed for a mixture with a high SO2 content. In collaboration with experimental groups, the performances of three new MOFs in CO2 capture are evaluated using molecular simulations. The computational results demonstrate the feasibility of precisely designing single-molecule traps (SMT) for CO2 capture. Also, a multi-functional MOF with micro-porosity, open Cu2+ sites and amine groups has also proved computationally the selective adsorption of CO2 over CH4 and N2. Last, we demonstrate that charge separation is an effective strategy for improving CO2 capture in MOFs.

Capturing CO2 from Coal-Fired Power Plants: Challenges for a Comprehensive Strategy

DTIC Science & Technology

2008-08-15

efficient flue gas desulfurization (FGD) or selective catalytic reduction (SCR) devices (or none), requiring either upgrading of existing FGD and SCR...saturated flue Figure 6. CO2 Price Projections CRS-16 42 Donald Shattuck, et al., A History of Flue Gas Desulfurization (FGD) — The Early Years, UE Technical...available in both the eastern and western parts of the United States, or by the use of emerging flue gas desulfurization (FGD) devices.46 At the time

Geophysical monitoring technology for CO2 sequestration

NASA Astrophysics Data System (ADS)

Ma, Jin-Feng; Li, Lin; Wang, Hao-Fan; Tan, Ming-You; Cui, Shi-Ling; Zhang, Yun-Yin; Qu, Zhi-Peng; Jia, Ling-Yun; Zhang, Shu-Hai

2016-06-01

Geophysical techniques play key roles in the measuring, monitoring, and verifying the safety of CO2 sequestration and in identifying the efficiency of CO2-enhanced oil recovery. Although geophysical monitoring techniques for CO2 sequestration have grown out of conventional oil and gas geophysical exploration techniques, it takes a long time to conduct geophysical monitoring, and there are many barriers and challenges. In this paper, with the initial objective of performing CO2 sequestration, we studied the geophysical tasks associated with evaluating geological storage sites and monitoring CO2 sequestration. Based on our review of the scope of geophysical monitoring techniques and our experience in domestic and international carbon capture and sequestration projects, we analyzed the inherent difficulties and our experiences in geophysical monitoring techniques, especially, with respect to 4D seismic acquisition, processing, and interpretation.

Cost Implications of Uncertainty in CO{sub 2} Storage Resource Estimates: A Review

DOE Office of Scientific and Technical Information (OSTI.GOV)

Anderson, Steven T., E-mail: sanderson@usgs.gov

Carbon capture from stationary sources and geologic storage of carbon dioxide (CO{sub 2}) is an important option to include in strategies to mitigate greenhouse gas emissions. However, the potential costs of commercial-scale CO{sub 2} storage are not well constrained, stemming from the inherent uncertainty in storage resource estimates coupled with a lack of detailed estimates of the infrastructure needed to access those resources. Storage resource estimates are highly dependent on storage efficiency values or storage coefficients, which are calculated based on ranges of uncertain geological and physical reservoir parameters. If dynamic factors (such as variability in storage efficiencies, pressure interference,more » and acceptable injection rates over time), reservoir pressure limitations, boundaries on migration of CO{sub 2}, consideration of closed or semi-closed saline reservoir systems, and other possible constraints on the technically accessible CO{sub 2} storage resource (TASR) are accounted for, it is likely that only a fraction of the TASR could be available without incurring significant additional costs. Although storage resource estimates typically assume that any issues with pressure buildup due to CO{sub 2} injection will be mitigated by reservoir pressure management, estimates of the costs of CO{sub 2} storage generally do not include the costs of active pressure management. Production of saline waters (brines) could be essential to increasing the dynamic storage capacity of most reservoirs, but including the costs of this critical method of reservoir pressure management could increase current estimates of the costs of CO{sub 2} storage by two times, or more. Even without considering the implications for reservoir pressure management, geologic uncertainty can significantly impact CO{sub 2} storage capacities and costs, and contribute to uncertainty in carbon capture and storage (CCS) systems. Given the current state of available information and the scarcity of (data from) long-term commercial-scale CO{sub 2} storage projects, decision makers may experience considerable difficulty in ascertaining the realistic potential, the likely costs, and the most beneficial pattern of deployment of CCS as an option to reduce CO{sub 2} concentrations in the atmosphere.« less

Cost implications of uncertainty in CO2 storage resource estimates: A review

USGS Publications Warehouse

Anderson, Steven T.

2017-01-01

Carbon capture from stationary sources and geologic storage of carbon dioxide (CO2) is an important option to include in strategies to mitigate greenhouse gas emissions. However, the potential costs of commercial-scale CO2 storage are not well constrained, stemming from the inherent uncertainty in storage resource estimates coupled with a lack of detailed estimates of the infrastructure needed to access those resources. Storage resource estimates are highly dependent on storage efficiency values or storage coefficients, which are calculated based on ranges of uncertain geological and physical reservoir parameters. If dynamic factors (such as variability in storage efficiencies, pressure interference, and acceptable injection rates over time), reservoir pressure limitations, boundaries on migration of CO2, consideration of closed or semi-closed saline reservoir systems, and other possible constraints on the technically accessible CO2 storage resource (TASR) are accounted for, it is likely that only a fraction of the TASR could be available without incurring significant additional costs. Although storage resource estimates typically assume that any issues with pressure buildup due to CO2 injection will be mitigated by reservoir pressure management, estimates of the costs of CO2 storage generally do not include the costs of active pressure management. Production of saline waters (brines) could be essential to increasing the dynamic storage capacity of most reservoirs, but including the costs of this critical method of reservoir pressure management could increase current estimates of the costs of CO2 storage by two times, or more. Even without considering the implications for reservoir pressure management, geologic uncertainty can significantly impact CO2 storage capacities and costs, and contribute to uncertainty in carbon capture and storage (CCS) systems. Given the current state of available information and the scarcity of (data from) long-term commercial-scale CO2 storage projects, decision makers may experience considerable difficulty in ascertaining the realistic potential, the likely costs, and the most beneficial pattern of deployment of CCS as an option to reduce CO2 concentrations in the atmosphere.

Probing the Role of Zr Addition versus Textural Properties in Enhancement of CO 2 Adsorption Performance in Silica/PEI Composite Sorbents

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sakwa-Novak, Miles A.; Holewinski, Adam; Hoyt, Caroline B.

2015-08-08

Polymeric amines such as poly(ethylenimine) (PEI) supported on mesoporous oxides are promising candidate adsorbents for CO 2 capture processes. One important aspect to the design and optimization of these materials is a fundamental understanding of how the properties of the oxide support such as pore structure, particle morphology, and surface properties affect the efficiency of the guest polymer in its interactions with CO 2. Previously, the efficiency of impregnated PEI to adsorb CO 2 was shown to increase upon the addition of Zr as a surface modifier in SBA-15. But, the efficacy of this method to tune the adsorption performancemore » has not been explored in materials of differing textural and morphological nature. These issues are directly addressed via the preparation of an array of SBA-15 support materials with varying textural and morphological properties, as well as varying content of zirconium doped into the material. Zirconium is incorporated into the SBA-15 either during the synthesis of the SBA-15, or postsynthetically via deposition of Zr species onto pure-silica SBA-15. The method of Zr incorporation alters the textural and morphological properties of the parent SBA-15 in different ways. Importantly, the CO 2 capacity of SBA-15 impregnated with PEI increases by a maximum of ~60% with the quantity of doped Zr for a “standard” SBA-15 containing significant microporosity, while no increase in the CO 2 capacity is observed upon Zr incorporation for an SBA-15 with reduced microporosity and a larger pore size, pore volume, and particle size. Finally, adsorbents supported on SBA-15 with controlled particle morphology show only modest increases in CO 2 capacity upon inclusion of Zr to the silica framework. The data demonstrate that the textural and morphological properties of the support have a more significant impact on the ability of PEI to capture CO 2 than the support surface composition.« less

A preliminary investigation of cryogenic CO2 capture utilizing a reverse Brayton Cycle

NASA Astrophysics Data System (ADS)

Yuan, L. C.; Pfotenhauer, J. M.; Qiu, L. M.

2014-01-01

Utilizing CO2 capture and storage (CCS) technologies is a significant way to reduce carbon emissions from coal fired power plants. Cryogenic CO2 capture (CCC) is an innovative and promising CO2 capture technology, which has an apparent energy and environmental advantage compared to alternatives. A process of capturing CO2 from the flue gas of a coal-fired electrical power plant by cryogenically desublimating CO2 has been discussed and demonstrated theoretically. However, pressurizing the inlet flue gas to reduce the energy penalty for the cryogenic process will lead to a more complex system. In this paper, a modified CCC system utilizing a reverse Brayton Cycle is proposed, and the energy penalty of these two systems are compared theoretically.

The Description and Validation of a Computationally-Efficient CH4-CO-OH (ECCOHv1.01) Chemistry Module for 3D Model Applications

NASA Technical Reports Server (NTRS)

Elshorbany, Yasin F.; Duncan, Bryan N.; Strode, Sarah A.; Wang, James S.; Kouatchou, Jules

2016-01-01

We present the Efficient CH4-CO-OH (ECCOH) chemistry module that allows for the simulation of the methane, carbon monoxide, and hydroxyl radical (CH4-CO- OH) system, within a chemistry climate model, carbon cycle model, or Earth system model. The computational efficiency of the module allows many multi-decadal sensitivity simulations of the CH4-CO-OH system, which primarily determines the global atmospheric oxidizing capacity. This capability is important for capturing the nonlinear feedbacks of the CH4-CO-OH system and understanding the perturbations to methane, CO, and OH, and the concomitant impacts on climate. We implemented the ECCOH chemistry module in the NASA GEOS-5 atmospheric global circulation model (AGCM), performed multiple sensitivity simulations of the CH4-CO-OH system over 2 decades, and evaluated the model output with surface and satellite data sets of methane and CO. The favorable comparison of output from the ECCOH chemistry module (as configured in the GEOS- 5 AGCM) with observations demonstrates the fidelity of the module for use in scientific research.

Potential of two-stage membrane system with recycle stream for CO{sub 2} capture from postcombustion gas

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dongxiao Yang; Zhi Wang; Jixiao Wang

2009-09-15

In order to restrict greenhouse gases emissions, CO{sub 2} should be captured from the postcombustion gas for further treatment, for example, geosequestration. In this work, the separation performance of the two-stage membrane system with a recycle stream was investigated using the cross-flow model. For larger CO{sub 2}/N{sub 2} selectivities that can be achieved in the lab, for example, selectivity of 52, the separation target of CO{sub 2} purity >95% and CO{sub 2} recovery >90% can be fulfilled by the two-stage system. The process cost of the two-stage membrane process was investigated. There is an optimum pressure ratio with which themore » capital cost and the energy cost can be balanced to minimize the total cost. Using the optimum pressure ratios and efficient membranes, the total cost of the two-stage system can be reduced to a range that is competitive with the process cost of the traditional chemical absorption method. For example, with feed compression applied, the total cost of the two-stage membrane system using the membrane with CO{sub 2}/N{sub 2} selectivity of 52 and CO{sub 2} permeance of 3.12 x 10{sup -3} m{sup 3} (STP) m{sup -2} s{sup -1} MPa{sup -1} is estimated to be $47.9/(ton CO{sub 2} recovered). 22 refs., 11 figs., 3 tabs.« less

Capture efficiency of cooking-related fine and ultrafine particles by residential exhaust hoods.

PubMed

Lunden, M M; Delp, W W; Singer, B C

2015-02-01

Effective exhaust hoods can mitigate the indoor air quality impacts of pollutant emissions from residential cooking. This study reports capture efficiencies (CE) measured for cooking-generated particles for scripted cooking procedures in a 121-m3 chamber with kitchenette. CEs also were measured for burner produced CO2 during cooking and separately for pots and pans containing water. The study used four exhaust hoods previously tested by Delp and Singer (Environ. Sci. Technol., 2012, 46, 6167-6173). For pan-frying a hamburger over medium heat on the back burner, CEs for particles were similar to those for burner produced CO2 and mostly above 80%. For stir-frying green beans in a wok (high heat, front burner), CEs for burner CO2 during cooking varied by hood and airflow: CEs were 34-38% for low (51-68 l/s) and 54-72% for high (109-138 l/s) settings. CEs for 0.3-2.0 μm particles during front burner stir-frying were 3-11% on low and 16-70% on high settings. Results indicate that CEs measured for burner CO2 are not predictive of CEs of cooking-generated particles under all conditions, but they may be suitable to identify devices with CEs above 80% both for burner combustion products and for cooking-related particles. Published 2014. This article is a U.S. Government work and is in the public domain in the USA.

Pilot plant studies of the CO{sub 2} capture performance of aqueous MEA and mixed MEA/MDEA solvents at the University of Regina CO{sub 2} capture technology development plant and the Boundary Dam CO{sub 2} capture demonstration

DOE Office of Scientific and Technical Information (OSTI.GOV)

Idem, R.; Wilson, M.; Tontiwachwuthikul, P.

2006-04-12

Evaluations of the benefits of using a mixed MEA/MDEA solvent for CO{sub 2} capture in terms of the heat requirement for solvent regeneration, lean and rich loadings, CO{sub 2} production, and solvent stability were performed by comparing the performance of aqueous 5 kmol/m{sup 3} MEA with that of an aqueous 4:1 molar ratio MEA/MDEA blend of 5 kmol/ml total amine concentration as a function of the operating time. The tests were performed using two pilot CO{sub 2} capture plants of the International Test Centre for CO{sub 2} Capture (ITC), which provided two different sources and compositions of flue gas. Themore » University of Regina CO{sub 2} plant (UR unit) processes flue gas from the combustion of natural gas while the Boundary Dam CO{sub 2} plant (BD unit) processes flue gas from a coal-fired electric power station. The results show that a huge heat-duty reduction can be achieved by using a mixed MEA/MDEA solution instead of a single MEA solution in an industrial environment of a CO{sub 2} capture plant. However, this benefit is dependent on whether the chemical stability of the solvent can be maintained.« less

Bench-scale Development of an Advanced Solid Sorbent-based CO 2 Capture Process for Coal-fired Power Plants

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nelson, Thomas; Kataria, Atish; Soukri, Mustapha

It is increasingly clear that CO 2 capture and sequestration (CCS) must play a critical role in curbing worldwide CO 2 emissions to the atmosphere. Development of these technologies to cost-effectively remove CO 2 from coal-fired power plants is very important to mitigating the impact these power plants have within the world’s power generation portfolio. Currently, conventional CO 2 capture technologies, such as aqueous-monoethanolamine based solvent systems, are prohibitively expensive and if implemented could result in a 75 to 100% increase in the cost of electricity for consumers worldwide. Solid sorbent CO 2 capture processes – such as RTI’s Advancedmore » Solid Sorbent CO 2, Capture Process – are promising alternatives to conventional, liquid solvents. Supported amine sorbents – of the nature RTI has developed – are particularly attractive due to their high CO 2 loadings, low heat capacities, reduced corrosivity/volatility and the potential to reduce the regeneration energy needed to carry out CO 2 capture. Previous work in this area has failed to adequately address various technology challenges such as sorbent stability and regenerability, sorbent scale-up, improved physical strength and attrition-resistance, proper heat management and temperature control, proper solids handling and circulation control, as well as the proper coupling of process engineering advancements that are tailored for a promising sorbent technology. The remaining challenges for these sorbent processes have provided the framework for the project team’s research and development and target for advancing the technology beyond lab- and bench-scale testing. Under a cooperative agreement with the US Department of Energy, and part of NETL’s CO 2 Capture Program, RTI has led an effort to address and mitigate the challenges associated with solid sorbent CO 2 capture. The overall objective of this project was to mitigate the technical and economic risks associated with the scale-up of solid sorbent-based CO 2 capture processes, enabling subsequent larger pilot demonstrations and ultimately commercial deployment. An integrated development approach has been a key focus of this project in which process development, sorbent development, and economic analyses have informed each of the other development processes. Development efforts have focused on improving the performance stability of sorbent candidates, refining process engineering and design, and evaluating the viability of the technology through detailed economic analyses. Sorbent advancements have led to a next generation, commercially-viable CO 2 capture sorbent exhibiting performance stability in various gas environments and a physically strong fluidizable form. The team has reduced sorbent production costs and optimized the production process and scale-up of PEI-impregnated, fluidizable sorbents. Refinement of the process engineering and design, as well as the construction and operation of a bench-scale research unit has demonstrated promising CO 2 capture performance under simulated coal-fired flue gas conditions. Parametric testing has shown how CO 2 capture performance is impacted by changing process variables, such as Adsorber temperature, Regenerator temperature, superficial flue gas velocity, solids circulation rate, CO 2 partial pressure in the Regenerator, and many others. Long-term testing has generated data for the project team to set the process conditions needed to operate a solids-based system for optimal performance, with continuous 90% CO 2 capture, and no operational interruptions. Data collected from all phases of testing has been used to develop a detailed techno-economic assessment of RTI’s technology. These detailed analyses show that RTI’s technology has significant economic advantages over current amine scrubbing and potential to achieve the DOE’s Carbon Capture Program’s goal of >90% CO 2 capture rate at a cost of < $40/T-CO 2 captured by 2025. Through this integrated technology development approach, the project team has advanced RTI’s CO 2 capture technology to TRL-4 (nearly TRL-5, with the missing variable being testing on actual, coal-fired flue gas), according to the DOE/FE definitions for Technology Readiness Levels. At a broader level, this project has advanced the whole of the solid sorbent CO 2 capture field, with advancements in process engineering and design, technical risk mitigation, sorbent scale-up optimization, and an understanding of the commercial viability and applicability of solid sorbent CO 2 capture technologies for the U.S. existing fleet of coal-fired power plants.« less

Increased light-use efficiency in northern terrestrial ecosystems indicated by CO 2 and greening observations

DOE PAGES

Ricciuto, Daniel M.; Mao, Jiafu; Shi, Xiaoying

2016-11-04

Observations show an increasing amplitude in the seasonal cycle of CO 2 (ASC) north of 45°N of 56 ± 9.8% over the last 50 years and an increase in vegetation greenness of 7.5 - 15% in high northern latitudes since the 1980s. However, the causes of these changes remain uncertain. Historical simulations from terrestrial biosphere models in the Multiscale Synthesis and Terrestrial Model Intercomparison Project are compared to the ASC and greenness observations, using the TM3 atmospheric transport model to translate surface fluxes into CO 2 concentrations. We find that the modeled change in ASC is too small but themore » mean greening trend is generally captured. Modeled increases in greenness are primarily driven by warming, whereas ASC changes are primarily driven by increasing CO 2. We suggest that increases in ecosystem-scale light use efficiency (LUE) have contributed to the observed ASC increase but are underestimated by current models. We highlight potential mechanisms that could increase modeled LUE.« less

Macroalgae for CO 2 Capture and Renewable Energy - A Pilot Project

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wiley, Kristine

2011-01-31

The objective of this project was to demonstrate, at a pilot scale, the beneficial use of carbon dioxide (CO 2) through a technology designed to capture CO 2 from fossil-fuel fired power plant stack gas, generating macroalgae and converting the macroalgae at high efficiency to renewable methane that can be utilized in the power plant or introduced into a natural gas pipeline. The proposed pilot plant would demonstrate the cost-effectiveness and CO 2/ NO x flue-gas removal efficiency of an innovative algal scrubber technology where seaweeds are grown out of water on specially-designed supporting structures contained within greenhouses where themore » plants are constantly bathed by recycled nutrient sprays enriched by flue gas constituents. The work described in this document addresses Phase 1 of the project only. The scope of work for Phase 1 includes the completion of a preliminary design package; the collection of additional experimental data to support the preliminary and detailed design for a pilot scale utilization of CO 2 to cultivate macroalage and to process that algae to produce methane; and a technological and economic analysis to evaluate the potential of the system. Selection criteria for macroalgae that could survive the elevated temperatures and potential periodic desiccation of near desert project sites were identified. Samples of the selected macroalgae species were obtained and then subjected to anaerobic digestion to determine conversions and potential methane yields. A Process Design Package (PDP) was assembled that included process design, process flow diagram, material balance, instrumentation, and equipment list, sizes, and cost for the Phase 2 pilot plant. Preliminary economic assessments were performed under the various assumptions made, which are purposely conservative. Based on the results, additional development work should be conducted to delineate the areas for improving efficiency, reducing contingencies, and reducing overall costs.« less

SYSTEM LEVEL IMPLICATIONS OF FLEXIBLE CO2 CAPTURE OPERATION

EPA Science Inventory

In ERCOT, turning flexible CO₂ capture systems off during infrequent periods of peak electricity demand can avoid hundreds of millions to billions of dollars in capital costs to replace the power output lost to CO₂ capture energy requirements.  When CO...

Plant growth responses to elevated atmospheric CO2 are increased by phosphorus sufficiency but not by arbuscular mycorrhizas.

PubMed

Jakobsen, Iver; Smith, Sally E; Smith, F Andrew; Watts-Williams, Stephanie J; Clausen, Signe S; Grønlund, Mette

2016-11-01

Capturing the full growth potential in crops under future elevated CO 2 (eCO 2 ) concentrations would be facilitated by improved understanding of eCO 2 effects on uptake and use of mineral nutrients. This study investigates interactions of eCO 2 , soil phosphorus (P), and arbuscular mycorrhizal (AM) symbiosis in Medicago truncatula and Brachypodium distachyon grown under the same conditions. The focus was on eCO 2 effects on vegetative growth, efficiency in acquisition and use of P, and expression of phosphate transporter (PT) genes. Growth responses to eCO 2 were positive at P sufficiency, but under low-P conditions they ranged from non-significant in M. truncatula to highly significant in B. distachyon Growth of M. truncatula was increased by AM at low P conditions at both CO 2 levels and eCO 2 ×AM interactions were sparse. Elevated CO 2 had small effects on P acquisition, but enhanced conversion of tissue P into biomass. Expression of PT genes was influenced by eCO 2 , but effects were inconsistent across genes and species. The ability of eCO 2 to partly mitigate P limitation-induced growth reductions in B. distachyon was associated with enhanced P use efficiency, and requirements for P fertilizers may not increase in such species in future CO 2 -rich climates. © The Author 2016. Published by Oxford University Press on behalf of the Society for Experimental Biology.

Systems Analysis of Physical Absorption of CO2 in Ionic Liquids for Pre-Combustion Carbon Capture.

PubMed

Zhai, Haibo; Rubin, Edward S

2018-04-17

This study develops an integrated technical and economic modeling framework to investigate the feasibility of ionic liquids (ILs) for precombustion carbon capture. The IL 1-hexyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide is modeled as a potential physical solvent for CO 2 capture at integrated gasification combined cycle (IGCC) power plants. The analysis reveals that the energy penalty of the IL-based capture system comes mainly from the process and product streams compression and solvent pumping, while the major capital cost components are the compressors and absorbers. On the basis of the plant-level analysis, the cost of CO 2 avoided by the IL-based capture and storage system is estimated to be $63 per tonne of CO 2 . Technical and economic comparisons between IL- and Selexol-based capture systems at the plant level show that an IL-based system could be a feasible option for CO 2 capture. Improving the CO 2 solubility of ILs can simplify the capture process configuration and lower the process energy and cost penalties to further enhance the viability of this technology.

Effects of heat exchanger tubes on hydrodynamics and CO 2 capture of a sorbent-based fluidized bed reactor

DOE PAGES

Lai, Canhai; Xu, Zhijie; Li, Tingwen; ...

2017-08-05

In virtual design and scale up of pilot-scale carbon capture systems, the coupled reactive multiphase flow problem must be solved to predict the adsorber's performance and capture efficiency under various operation conditions. This paper focuses on the detailed computational fluid dynamics (CFD) modeling of a pilot-scale fluidized bed adsorber equipped with vertical cooling tubes. Multiphase Flow with Interphase eXchanges (MFiX), an open-source multiphase flow CFD solver, is used for the simulations with custom code to simulate the chemical reactions and filtered sub-grid models to capture the effect of the unresolved details in the coarser mesh for simulations with reasonable accuracymore » and manageable computational effort. Previously developed filtered models for horizontal cylinder drag, heat transfer, and reaction kinetics have been modified to derive the 2D filtered models representing vertical cylinders in the coarse-grid CFD simulations. The effects of the heat exchanger configurations (i.e., horizontal or vertical tubes) on the adsorber's hydrodynamics and CO 2 capture performance are then examined. A one-dimensional three-region process model is briefly introduced for comparison purpose. The CFD model matches reasonably well with the process model while provides additional information about the flow field that is not available with the process model.« less

DEVELOPMENT OF A NOVEL GAS PRESSURIZED STRIPPING (GPS)-BASED TECHNOLOGY FOR CO 2 CAPTURE FROM POST-COMBUSTION FLUE GASES Topical Report: Techno-Economic Analysis of GPS-based Technology for CO 2 Capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chen, Shiaoguo

This topical report presents the techno-economic analysis, conducted by Carbon Capture Scientific, LLC (CCS) and Nexant, for a nominal 550 MWe supercritical pulverized coal (PC) power plant utilizing CCS patented Gas Pressurized Stripping (GPS) technology for post-combustion carbon capture (PCC). Illinois No. 6 coal is used as fuel. Because of the difference in performance between the GPS-based PCC and the MEA-based CO2 absorption technology, the net power output of this plant is not exactly 550 MWe. DOE/NETL Case 11 supercritical PC plant without CO2 capture and Case 12 supercritical PC plant with benchmark MEA-based CO2 capture are chosen as references.more » In order to include CO2 compression process for the baseline case, CCS independently evaluated the generic 30 wt% MEA-based PCC process together with the CO2 compression section. The net power produced in the supercritical PC plant with GPS-based PCC is 647 MW, greater than the MEA-based design. The levelized cost of electricity (LCOE) over a 20-year period is adopted to assess techno-economic performance. The LCOE for the supercritical PC plant with GPS-based PCC, not considering CO2 transport, storage and monitoring (TS&M), is 97.4 mills/kWh, or 152% of the Case 11 supercritical PC plant without CO2 capture, equivalent to $39.6/tonne for the cost of CO2 capture. GPS-based PCC is also significantly superior to the generic MEA-based PCC with CO2 compression section, whose LCOE is as high as 109.6 mills/kWh.« less

Reducing the cost of Ca-based direct air capture of CO2.

PubMed

Zeman, Frank

2014-10-07

Direct air capture, the chemical removal of CO2 directly from the atmosphere, may play a role in mitigating future climate risk or form the basis of a sustainable transportation infrastructure. The current discussion is centered on the estimated cost of the technology and its link to "overshoot" trajectories, where atmospheric CO2 levels are actively reduced later in the century. The American Physical Society (APS) published a report, later updated, estimating the cost of a one million tonne CO2 per year air capture facility constructed today that highlights several fundamental concepts of chemical air capture. These fundamentals are viewed through the lens of a chemical process that cycles between removing CO2 from the air and releasing the absorbed CO2 in concentrated form. This work builds on the APS report to investigate the effect of modifications to the air capture system based on suggestions in the report and subsequent publications. The work shows that reduced carbon electricity and plastic packing materials (for the contactor) may have significant effects on the overall price, reducing the APS estimate from $610 to $309/tCO2 avoided. Such a reduction does not challenge postcombustion capture from point sources, estimated at $80/tCO2, but does make air capture a feasible alternative for the transportation sector and a potential negative emissions technology. Furthermore, air capture represents atmospheric reductions rather than simply avoided emissions.

Hollow fiber-supported designer ionic liquid sponges for post-combustion CO2 scrubbing

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lee, JS; Hillesheim, PC; Huang, DK

A proof of concept study for a new type of carbon capture system is considered for post-combustion CO2 capture based on porous hollow fiber sorbents with ionic liquids sorbed in the cell walls of the fiber. This study proves that delicate morphological features in the open-celled porous wall can be maintained during the infusion process. Mixtures of task specific ionic liquid (i.e. [BMIM][Tf2N]) and superbase (i.e. DBU) were loaded into polyamide-imide (PAI) fibers by a so-called two-step non-solvent infusion protocol. In the protocol, methanol carries ionic liquids into the pore cell walls of hollow fibers and then hexane carries superbasemore » to create an efficient CO2 sorbent. Our ionic liquid/superbase impregnation technique overcomes a serious increase in mass transfer resistance upon reaction with CO2, thereby allowing its large scale utilization for post-combustion CO2 capture. The investigation on the effect of different pore former additives (different molecular weights of polyvinylpyrrolidone, lithium nitrate, and their mixtures) suggested that a large molecular weight of PVP (M-w; 1300k) including dope composition produces highly interconnected open cell pore structures of PAI hollow fibers. Lastly, a lumen side barrier layer was successfully formed on the bore side of neat PAI fibers by using a mixture of Neoprene (R) with crosslinking agents (TSR-633) via a post-treatment process. The lumen layer will enable heat removal from the fiber sorbents during their application in rapid thermal swing cycling processes. (C) 2012 Elsevier Ltd. All rights reserved.« less

Jumpstarting commercial-scale CO 2 capture and storage with ethylene production and enhanced oil recovery in the US Gulf

DOE PAGES

Middleton, Richard S.; Levine, Jonathan S.; Bielicki, Jeffrey M.; ...

2015-04-27

CO 2 capture, utilization, and storage (CCUS) technology has yet to be widely deployed at a commercial scale despite multiple high-profile demonstration projects. We suggest that developing a large-scale, visible, and financially viable CCUS network could potentially overcome many barriers to deployment and jumpstart commercial-scale CCUS. To date, substantial effort has focused on technology development to reduce the costs of CO 2 capture from coal-fired power plants. Here, we propose that near-term investment could focus on implementing CO 2 capture on facilities that produce high-value chemicals/products. These facilities can absorb the expected impact of the marginal increase in the costmore » of production on the price of their product, due to the addition of CO 2 capture, more than coal-fired power plants. A financially viable demonstration of a large-scale CCUS network requires offsetting the costs of CO 2 capture by using the CO 2 as an input to the production of market-viable products. As a result, we demonstrate this alternative development path with the example of an integrated CCUS system where CO 2 is captured from ethylene producers and used for enhanced oil recovery in the U.S. Gulf Coast region.« less

Light-Triggered CO2 Breathing Foam via Nonsurfactant High Internal Phase Emulsion.

PubMed

Zhang, Shiming; Wang, Dingguan; Pan, Qianhao; Gui, Qinyuan; Liao, Shenglong; Wang, Yapei

2017-10-04

Solid materials for CO 2 capture and storage have attracted enormous attention for gaseous separation, environmental protection, and climate governance. However, their preparation and recovery meet the problems of high energy and financial cost. Herein, a controllable CO 2 capture and storage process is accomplished in an emulsion-templated polymer foam, in which CO 2 is breathed-in under dark and breathed-out under light illumination. Such a process is likely to become a relay of natural CO 2 capture by plants that on the contrary breathe out CO 2 at night. Recyclable CO 2 capture at room temperature and release under light irradiation guarantee its convenient and cost-effective regeneration in industry. Furthermore, CO 2 mixed with CH 4 is successfully separated through this reversible breathing in and out system, which offers great promise for CO 2 enrichment and practical methane purification.

Framing and bias in CO2 capture and storage communication films: Reflections from a CO2 capture and storage research group.

PubMed

Maynard, Carly M; Shackley, Simon

2017-03-01

There has been a growing trend towards incorporating short, educational films as part of research funding and project proposals. Researchers and developers in CO 2 capture and storage are using films to communicate outcomes, but such films can be influenced by experiences and values of the producers. We document the content and presentation of seven online CO 2 capture and storage films to determine how framing occurs and its influence on the tone of films. The core frame presents CO 2 capture and storage as a potential solution to an imminent crisis in climatic warming and lack of a sustainable energy supply. Three subsidiary frames represent CO 2 capture and storage as (1) the only option, (2) a partial option or (3) a scientific curiosity. The results demonstrate that an understanding of the nuanced explicit and implicit messages portrayed by films is essential both for effective framing according to one's intention and for wider public understanding of a field.

MEMBRANE PROCESS TO SEQUESTER CO2 FROM POWER PLANT FLUE GAS

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tim Merkel; Karl Amo; Richard Baker

2009-03-31

The objective of this project was to assess the feasibility of using a membrane process to capture CO2 from coal-fired power plant flue gas. During this program, MTR developed a novel membrane (Polaris™) with a CO2 permeance tenfold higher than commercial CO2-selective membranes used in natural gas treatment. The Polaris™ membrane, combined with a process design that uses a portion of combustion air as a sweep stream to generate driving force for CO2 permeation, meets DOE post-combustion CO2 capture targets. Initial studies indicate a CO2 separation and liquefaction cost of $20 - $30/ton CO2 using about 15% of the plantmore » energy at 90% CO2 capture from a coal-fired power plant. Production of the Polaris™ CO2 capture membrane was scaled up with MTR’s commercial casting and coating equipment. Parametric tests of cross-flow and countercurrent/sweep modules prepared from this membrane confirm their near-ideal performance under expected flue gas operating conditions. Commercial-scale, 8-inch diameter modules also show stable performance in field tests treating raw natural gas. These findings suggest that membranes are a viable option for flue gas CO2 capture. The next step will be to conduct a field demonstration treating a realworld power plant flue gas stream. The first such MTR field test will capture 1 ton CO2/day at Arizona Public Service’s Cholla coal-fired power plant, as part of a new DOE NETL funded program.« less

Life cycle assessment of carbon capture and utilization from ammonia process in Mexico.

PubMed

Morales Mora, M A; Vergara, C Pretelín; Leiva, M A; Martínez Delgadillo, S A; Rosa-Domínguez, E R

2016-12-01

Post-combustion CO 2 capture (PCC) of flue gas from an ammonia plant (AP) and the environmental performance of the carbon capture utilization (CCU) technology for greenhouse gas (GHG) emissions to an enhanced oil recovery (EOR) system in Mexico was performed as case study. The process simulations (PS) and life cycle assessment (LCA) were used as supporting tools to quantify the CO 2 capture and their environmental impacts, respectively. Two scenarios were considered: 1) the AP with its shift and CO 2 removal unit and 2) Scenario 1 plus PCC of the flue gas from the AP primary reformer (AP-2CO 2 ) and the global warming (GW) impact. Also, the GW of the whole of a CO 2 -EOR project, from these two streams of captured CO 2 , was evaluated. Results show that 372,426 tCO 2 /year can be PCC from the flue gas of the primary reformer and 480,000 tons/y of capacity from the AP. The energy requirement for solvent regeneration is estimated to be 2.8 MJ/kgCO 2 or a GW impact of 0.22 kgCO 2e /kgCO 2 captured. GW performances are 297.6 kgCO 2e emitted/barrel (bbl) for scenario one, and 106.5 kgCO 2e emitted/bbl for the second. The net emissions, in scenario one, were 0.52 tCO 2e /bbl and 0.33 tCO 2e /bbl in scenario two. Based on PS, this study could be used to evaluate the potential of CO 2 capture of 4080 t/d of 4 ammonia plants. The integration of PS-LCA to a PCC study allows the applicability as methodological framework for the development of a cluster of projects in which of CO 2 could be recycled back to fuel, chemical, petrochemical products or for enhanced oil recovery (EOR). With AP-2CO 2, "CO 2 emission free" ammonia production could be achieved. Copyright © 2016 Elsevier Ltd. All rights reserved.

Pilot plant test of the advanced flash stripper for CO2 capture.

PubMed

Lin, Yu-Jeng; Chen, Eric; Rochelle, Gary T

2016-10-20

Alternative stripping processes have been proposed to reduce energy use for CO 2 capture, but only a few have been applied to pilot-scale experiments. This paper presents the first pilot plant test results of one of the most promising stripper configurations, the advanced flash stripper with cold and warm rich solvent bypass. The campaign using aqueous piperazine was carried out at UT Austin in 2015. The advanced flash stripper improves the heat duty by over 25% compared to previous campaigns using the two-stage flash, achieving 2.1 GJ per tonne CO 2 of heat duty and 32 kJ mol -1 CO 2 of total equivalent work. The bypass control strategy proposed minimized the heat duty. The test successfully demonstrated the remarkable energy performance and the operability of this advanced system. An Aspen Plus® model was validated using the pilot plant data and used to explore optimum operating and design conditions. The irreversibility analysis showed that the pilot plant performance has attained 50% thermodynamic efficiency and further energy improvement should focus on the absorber and the cross exchanger by increasing absorption rate and solvent capacity.

A Reversed Photosynthesis-like Process for Light-Triggered CO2 Capture, Release, and Conversion.

PubMed

Wang, Dingguan; Liao, Shenglong; Zhang, Shiming; Wang, Yapei

2017-06-22

Materials for CO 2 capture have been extensively exploited for climate governance and gas separation. However, their regeneration is facing the problems of high energy cost and secondary CO 2 contamination. Herein, a reversed photosynthesis-like process is proposed, in which CO 2 is absorbed in darkness while being released under light illumination. The process is likely supplementary to natural photosynthesis of plants, in which, on the contrary, CO 2 is released during the night. Remarkably, the material used here is able to capture 9.6 wt.% CO 2 according to its active component. Repeatable CO 2 capture at room temperature and release under light irradiation ensures its convenient and cost-effective regeneration. Furthermore, CO 2 released from the system is successfully converted into a stable compound in tandem with specific catalysts. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Structures for capturing CO.sub.2, methods of making the structures, and methods of capturing CO.sub.2

DOEpatents

Jones, Christopher W; Hicks, Jason C; Fauth, Daniel J; McMahan, Gray

2012-10-30

Briefly described, embodiments of this disclosure, among others, include carbon dioxide (CO.sub.2) sorption structures, methods of making CO.sub.2 sorption structures, and methods of using CO.sub.2 sorption structures.

The system-wide economics of a carbon dioxide capture, utilization, and storage network: Texas Gulf Coast with pure CO2-EOR flood

NASA Astrophysics Data System (ADS)

King, Carey W.; Gülen, Gürcan; Cohen, Stuart M.; Nuñez-Lopez, Vanessa

2013-09-01

This letter compares several bounding cases for understanding the economic viability of capturing large quantities of anthropogenic CO2 from coal-fired power generators within the Electric Reliability Council of Texas electric grid and using it for pure CO2 enhanced oil recovery (EOR) in the onshore coastal region of Texas along the Gulf of Mexico. All captured CO2 in excess of that needed for EOR is sequestered in saline formations at the same geographic locations as the oil reservoirs but at a different depth. We analyze the extraction of oil from the same set of ten reservoirs within 20- and five-year time frames to describe how the scale of the carbon dioxide capture, utilization, and storage (CCUS) network changes to meet the rate of CO2 demand for oil recovery. Our analysis shows that there is a negative system-wide net present value (NPV) for all modeled scenarios. The system comes close to breakeven economics when capturing CO2 from three coal-fired power plants to produce oil via CO2-EOR over 20 years and assuming no CO2 emissions penalty. The NPV drops when we consider a larger network to produce oil more quickly (21 coal-fired generators with CO2 capture to produce 80% of the oil within five years). Upon applying a CO2 emissions penalty of 602009/tCO2 to fossil fuel emissions to ensure that coal-fired power plants with CO2 capture remain in baseload operation, the system economics drop significantly. We show near profitability for the cash flow of the EOR operations only; however, this situation requires relatively cheap electricity prices during operation.

Probing the Role of Zr Addition versus Textural Properties in Enhancement of CO₂ Adsorption Performance in Silica/PEI Composite Sorbents.

PubMed

Sakwa-Novak, Miles A; Holewinski, Adam; Hoyt, Caroline B; Yoo, Chun-Jae; Chai, Song-Hai; Dai, Sheng; Jones, Christopher W

2015-09-01

Polymeric amines such as poly(ethylenimine) (PEI) supported on mesoporous oxides are promising candidate adsorbents for CO2 capture processes. An important aspect to the design and optimization of these materials is a fundamental understanding of how the properties of the oxide support such as pore structure, particle morphology, and surface properties affect the efficiency of the guest polymer in its interactions with CO2. Previously, the efficiency of impregnated PEI to adsorb CO2 was shown to increase upon the addition of Zr as a surface modifier in SBA-15. However, the efficacy of this method to tune the adsorption performance has not been explored in materials of differing textural and morphological nature. Here, these issues are directly addressed via the preparation of an array of SBA-15 support materials with varying textural and morphological properties, as well as varying content of zirconium doped into the material. Zirconium is incorporated into the SBA-15 either during the synthesis of the SBA-15, or postsynthetically via deposition of Zr species onto pure-silica SBA-15. The method of Zr incorporation alters the textural and morphological properties of the parent SBA-15 in different ways. Importantly, the CO2 capacity of SBA-15 impregnated with PEI increases by a maximum of ∼60% with the quantity of doped Zr for a "standard" SBA-15 containing significant microporosity, while no increase in the CO2 capacity is observed upon Zr incorporation for an SBA-15 with reduced microporosity and a larger pore size, pore volume, and particle size. Finally, adsorbents supported on SBA-15 with controlled particle morphology show only modest increases in CO2 capacity upon inclusion of Zr to the silica framework. The data demonstrate that the textural and morphological properties of the support have a more significant impact on the ability of PEI to capture CO2 than the support surface composition.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sakwa-Novak, Miles A.; Holewinski, Adam; Hoyt, Caroline B.

Polymeric amines such as poly(ethylenimine) (PEI) supported on mesoporous oxides are promising candidate adsorbents for CO2 capture processes. An important aspect to the design and optimization of these materials is a fundamental understanding of how the properties of the oxide support such as pore structure, particle morphology, and surface properties affect the efficiency of the guest polymer in its interactions with CO2. Previously, the efficiency of impregnated PEI to adsorb CO2 was shown to increase upon the addition of Zr as a surface modifier in SBA-15. However, the efficacy of this method to tune the adsorption performance has not beenmore » explored in materials of differing textural and morphological nature. Here, these issues are directly addressed via the preparation of an array of SBA-15 support materials with varying textural and morphological properties, as well as varying content of zirconium doped into the material. Zirconium is incorporated into the SBA-15 either during the synthesis of the SBA-15, or postsynthetically via deposition of Zr species onto pure-silica SBA-15. The method of Zr incorporation alters the textural and morphological properties of the parent SBA-15 in different ways. Importantly, the CO2 capacity of SBA-15 impregnated with PEI increases by a maximum of ~60% with the quantity of doped Zr for a “standard” SBA-15 containing significant microporosity, while no increase in the CO2 capacity is observed upon Zr incorporation for an SBA-15 with reduced microporosity and a larger pore size, pore volume, and particle size. Finally, adsorbents supported on SBA-15 with controlled particle morphology show only modest increases in CO2 capacity upon inclusion of Zr to the silica framework. The data demonstrate that the textural and morphological properties of the support have a more significant impact on the ability of PEI to capture CO2 than the support surface composition.« less

Opportunities for Decarbonizing Existing U.S. Coal-Fired Power Plants via CO2 Capture, Utilization and Storage.

PubMed

Zhai, Haibo; Ou, Yang; Rubin, Edward S

2015-07-07

This study employs a power plant modeling tool to explore the feasibility of reducing unit-level emission rates of CO2 by 30% by retrofitting carbon capture, utilization, and storage (CCUS) to existing U.S. coal-fired electric generating units (EGUs). Our goal is to identify feasible EGUs and their key attributes. The results indicate that for about 60 gigawatts of the existing coal-fired capacity, the implementation of partial CO2 capture appears feasible, though its cost is highly dependent on the unit characteristics and fuel prices. Auxiliary gas-fired boilers can be employed to power a carbon capture process without significant increases in the cost of electricity generation. A complementary CO2 emission trading program can provide additional economic incentives for the deployment of CCS with 90% CO2 capture. Selling and utilizing the captured CO2 product for enhanced oil recovery can further accelerate CCUS deployment and also help reinforce a CO2 emission trading market. These efforts would allow existing coal-fired EGUs to continue to provide a significant share of the U.S. electricity demand.

Imidazolium salt-modified porous hypercrosslinked polymers for synergistic CO2 capture and conversion.

PubMed

Wang, Jinquan; Sng, Waihong; Yi, Guangshun; Zhang, Yugen

2015-08-04

A new type of imidazolium salt-modified porous hypercrosslinked polymer (BET surface area up to 926 m(2) g(-1)) was reported. These porous materials exhibited good CO2 capture capacities (14.5 wt%) and catalytic activities for the conversion of CO2 into various cyclic carbonates under metal-free conditions. The synergistic effect of CO2 capture and conversion was observed.

Photocatalytic conversion of CO2 into value-added and renewable fuels

NASA Astrophysics Data System (ADS)

Yuan, Lan; Xu, Yi-Jun

2015-07-01

The increasing energy crisis and the worsening global climate caused by the excessive utilization of fossil fuel have boosted tremendous research activities about CO2 capture, storage and utilization. Artificial photosynthesis that uses solar light energy to convert CO2 to form value-added and renewable fuels such as methane or methanol has been consistently drawing increasing attention. It is like killing two birds with one stone since it can not only reduce the greenhouse effects caused by CO2 emission but also produce value added chemicals for alternative energy supplying. This review provides a brief introduction about the basic principles of artificial photosynthesis of CO2 and the progress made in exploring more efficient photocatalysts from the viewpoint of light harvesting and photogenerated charge carriers boosting. Moreover, the undergoing mechanisms of CO2 photoreduction are discussed with selected examples, in terms of adsorption of reactants, CO2 activation as well as the possible reaction pathways. Finally, perspectives on future research directions and open issues in CO2 photoreduction are outlined.

Conversion of CO2 from Air into Methanol Using a Polyamine and a Homogeneous Ruthenium Catalyst.

PubMed

Kothandaraman, Jotheeswari; Goeppert, Alain; Czaun, Miklos; Olah, George A; Prakash, G K Surya

2016-01-27

A highly efficient homogeneous catalyst system for the production of CH3OH from CO2 using pentaethylenehexamine and Ru-Macho-BH (1) at 125-165 °C in an ethereal solvent has been developed (initial turnover frequency = 70 h(-1) at 145 °C). Ease of separation of CH3OH is demonstrated by simple distillation from the reaction mixture. The robustness of the catalytic system was shown by recycling the catalyst over five runs without significant loss of activity (turnover number > 2000). Various sources of CO2 can be used for this reaction including air, despite its low CO2 concentration (400 ppm). For the first time, we have demonstrated that CO2 captured from air can be directly converted to CH3OH in 79% yield using a homogeneous catalytic system.

Computational Modeling of Mixed Solids for CO2 CaptureSorbents

DOE Office of Scientific and Technical Information (OSTI.GOV)

Duan, Yuhua

2015-01-01

Since current technologies for capturing CO2 to fight global climate change are still too energy intensive, there is a critical need for development of new materials that can capture CO2 reversibly with acceptable energy costs. Accordingly, solid sorbents have been proposed to be used for CO2 capture applications through a reversible chemical transformation. By combining thermodynamic database mining with first principles density functional theory and phonon lattice dynamics calculations, a theoretical screening methodology to identify the most promising CO2 sorbent candidates from the vast array of possible solid materials has been proposed and validated. The calculated thermodynamic properties of differentmore » classes of solid materials versus temperature and pressure changes were further used to evaluate the equilibrium properties for the CO2 adsorption/desorption cycles. According to the requirements imposed by the pre- and post- combustion technologies and based on our calculated thermodynamic properties for the CO2 capture reactions by the solids of interest, we were able to screen only those solid materials for which lower capture energy costs are expected at the desired pressure and temperature conditions. Only those selected CO2 sorbent candidates were further considered for experimental validations. The ab initio thermodynamic technique has the advantage of identifying thermodynamic properties of CO2 capture reactions without any experimental input beyond crystallographic structural information of the solid phases involved. Such methodology not only can be used to search for good candidates from existing database of solid materials, but also can provide some guidelines for synthesis new materials. In this presentation, we apply our screening methodology to mixing solid systems to adjust the turnover temperature to help on developing CO2 capture Technologies.« less

How green can black be? Assessing the potential for equipping USA's existing coal fleet with carbon capture and storage

NASA Astrophysics Data System (ADS)

Patrizio, Piera; Leduc, Sylvain; Mesfun, Sennai; Yowargana, Ping; Kraxner, Florian

2017-04-01

The mitigation of adverse environmental impacts due to climate change requires the reduction of carbon dioxide emissions - also from the U.S. energy sector, a dominant source of greenhouse-gas emissions. This is especially true for the existing fleet of coal-fired power plants, accounting for roughly two-thirds of the U.S. energy sectors' total CO2 emissions. With this aim, different carbon mitigation options have been proposed in literature, such as increasing the energy efficiency, co-firing of biomass and/or the adoption of carbon capturing technologies (BECCS). However, the extent to which these solutions can be adopted depends on a suite of site specific factors and therefore needs to be evaluated on a site-specific basis. We propose a spatially explicit approach to identify candidate coal plants for which carbon capture technologies are economically feasible, according to different economic and policy frameworks. The methodology implies the adoption of IIASA's techno economic model BeWhere, which optimizes the cost of the entire BECCS supply chain, from the biomass resources to the storage of the CO2 in the nearest geological sink. The results shows that biomass co-firing appears to be the most appealing economic solution for a larger part of the existing U.S. coal fleet, while the adoption of CCS technologies is highly dependent on the level of CO2 prices as well as on local factors such as the type of coal firing technology and proximity of storage sites.

Dual phase high-temperature membranes for CO2 separation - performance assessment in post- and pre-combustion processes.

PubMed

Anantharaman, Rahul; Peters, Thijs; Xing, Wen; Fontaine, Marie-Laure; Bredesen, Rune

2016-10-20

Dual phase membranes are highly CO 2 -selective membranes with an operating temperature above 400 °C. The focus of this work is to quantify the potential of dual phase membranes in pre- and post-combustion CO 2 capture processes. The process evaluations show that the dual phase membranes integrated with an NGCC power plant for CO 2 capture are not competitive with the MEA process for post-combustion capture. However, dual phase membrane concepts outperform the reference Selexol technology for pre-combustion CO 2 capture in an IGCC process. The two processes evaluated in this work, post-combustion NGCC and pre-combustion IGCC, represent extremes in CO 2 partial pressure fed to the separation unit. Based on the evaluations it is expected that dual phase membranes could be competitive for post-combustion capture from a pulverized coal fired power plant (PCC) and pre-combustion capture from an Integrated Reforming Cycle (IRCC).

Hybrid Encapsulated Ionic Liquids for Post-Combustion Carbon Dioxide (CO 2) Capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Brennecke, Joan; Degnan, Thomas; McCready, Mark

Ionic liquids (ILs) and Phase Change Ionic Liquids (PCILs) are excellent materials for selective removal of carbon dioxide from dilute post-combustion streams. However, they are typically characterized as having high viscosities, which impairs their effectiveness due to mass transfer limitations, caused by the high viscosities. In this project, we are examining the benefits of encapsulating ILs and PCILs in thin polymeric shells to produce particles of approximately 100 to 600 μm in diameter that can be used in a fluidized bed absorber. The particles are produced by microencapsulation of the ILs and PCILs in CO 2-permeable polymer shells. Here wemore » report on the synthesis of the IL and PCIL materials, measurements of thermophysical properties including CO 2 capacity and reprotonation equilibrium and kinetics, encapsulation of the ILs and PCILs, mechanical and thermodynamic testing of the encapsulated materials, development of a rate based model of the absorber, and the design of a laboratory scale unit to test the encapsulated particles for CO 2 capture ability and efficiency. We show that the IL/PCIL materials can be successfully encapsulated, that they retain CO 2 uptake capacity, and that the uptake rates are increased relative to a stagnant sample of IL liquid or PCIL powder.« less

Ocean sequestration of crop residue carbon: recycling fossil fuel carbon back to deep sediments.

PubMed

Strand, Stuart E; Benford, Gregory

2009-02-15

For significant impact any method to remove CO2 from the atmosphere must process large amounts of carbon efficiently, be repeatable, sequester carbon for thousands of years, be practical, economical and be implemented soon. The only method that meets these criteria is removal of crop residues and burial in the deep ocean. We show here that this method is 92% efficient in sequestration of crop residue carbon while cellulosic ethanol production is only 32% and soil sequestration is about 14% efficient. Deep ocean sequestration can potentially capture 15% of the current global CO2 annual increase, returning that carbon backto deep sediments, confining the carbon for millennia, while using existing capital infrastructure and technology. Because of these clear advantages, we recommend enhanced research into permanent sequestration of crop residues in the deep ocean.

Capture-ready power plants - options, technologies and economics

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bohm, M.C.

2006-06-15

A plant can be considered to be capture-ready if at some point in the future it can be retrofitted for carbon capture and sequestration and still be economical to operate. The first part of the thesis outlines the two major designs that are being considered for construction in the near-term - pulverized coal (PC) and integrated gasification/combined cycle (IGCC). It details the steps that are necessary to retrofit each of these plants for CO{sub 2} capture and sequestration and assesses the steps that can be taken to reduce the costs and output de-rating of the plant after a retrofit. The second part of the thesis evaluates the lifetime (40 year) net present value (NPV) costs of plants with differing levels of pre-investment for CO{sub 2} capture. Three scenarios are evaluated - a baseline supercritical PC plant, a baseline IGCC plant and an IGCC plant with pre-investment for capture. The results of this thesis show that a baseline PC plant is the most economical choice under low CO{sub 2} tax rates, and IGCC plants are preferable at higher tax rates. The third part of this thesis evaluates the concept of CO{sub 2} 'lock-in'. CO{sub 2} lock-in occurs when a newly built plant is so prohibitively expensive to retrofit for CO{sub 2} capture that it will never be retrofitted for capture, and offers no economic opportunity to reduce the CO{sub 2} emissions from the plant, besides shutting down or rebuilding. The results show that IGCC plants are expected to have lower lifetime CO{sub 2} emissions than a PC plant, given moderate (10-35more » $$/ton CO{sub 2}) initial tax rates. Higher 4 (above $$40) or lower (below $7) initial tax rates do not result in significant differences in lifetime CO{sub 2} emissions from these plants. Little difference is seen in the lifetime CO{sub 2} emissions between the IGCC plants with and without pre-investment for CO{sub 2} capture. 32 refs., 22 figs., 20 tabs., 1 app.« less

A process for capturing CO 2 from the atmosphere

DOE PAGES

Keith, David W.; Holmes, Geoffrey; St. Angelo, David; ...

2018-06-07

Here, we describe a process for capturing CO 2 from the atmosphere in an industrial plant. The design captures ~1 Mt-CO 2/year in a continuous process using an aqueous KOH sorbent coupled to a calcium caustic recovery loop. We describe the design rationale, summarize performance of the major unit operations, and provide a capital cost breakdown developed with an independent consulting engineering firm. We report results from a pilot plant which provides data on performance of the major unit operations. We summarize the energy and material balance computed using an Aspen process simulation. When CO 2 is delivered at 15more » MPa the design requires either 8.81 GJ of natural gas, or 5.25 GJ of gas and 366 kWhr of electricity, per ton of CO 2 captured. Depending on financial assumptions, energy costs, and the specific choice of inputs and outputs, the levelized cost per ton CO 2 captured from the atmosphere ranges from 94 to 232 $/t-CO 2.« less

CO 2 Capture from Ambient Air by Crystallization with a Guanidine Sorbent

DOE PAGES

Seipp, Charles A.; Univ. of Texas, Austin, TX; Williams, Neil J.; ...

2016-12-21

Carbon capture and storage is an important strategy for stabilizing the increasing concentration of atmospheric CO 2 and the global temperature. A possible approach toward reversing this trend and decreasing the atmospheric CO 2 concentration is to remove the CO 2 directly from air (direct air capture). In this paper, we report a simple aqueous guanidine sorbent that captures CO 2 from ambient air and binds it as a crystalline carbonate salt by guanidinium hydrogen bonding. The resulting solid has very low aqueous solubility (K sp=1.0(4)×10 -8), which facilitates its separation from solution by filtration. The bound CO 2 canmore » be released by relatively mild heating of the crystals at 80–120 °C, which regenerates the guanidine sorbent quantitatively. Finally and thus, this crystallization-based approach to CO 2 separation from air requires minimal energy and chemical input, and offers the prospect for low-cost direct air capture technologies.« less

A process for capturing CO 2 from the atmosphere

DOE Office of Scientific and Technical Information (OSTI.GOV)

Keith, David W.; Holmes, Geoffrey; St. Angelo, David

Here, we describe a process for capturing CO 2 from the atmosphere in an industrial plant. The design captures ~1 Mt-CO 2/year in a continuous process using an aqueous KOH sorbent coupled to a calcium caustic recovery loop. We describe the design rationale, summarize performance of the major unit operations, and provide a capital cost breakdown developed with an independent consulting engineering firm. We report results from a pilot plant which provides data on performance of the major unit operations. We summarize the energy and material balance computed using an Aspen process simulation. When CO 2 is delivered at 15more » MPa the design requires either 8.81 GJ of natural gas, or 5.25 GJ of gas and 366 kWhr of electricity, per ton of CO 2 captured. Depending on financial assumptions, energy costs, and the specific choice of inputs and outputs, the levelized cost per ton CO 2 captured from the atmosphere ranges from 94 to 232 $/t-CO 2.« less

Computational designing and screening of solid materials for CO2capture

NASA Astrophysics Data System (ADS)

Duan, Yuhua

In this presentation, we will update our progress on computational designing and screening of solid materials for CO2 capture. By combining thermodynamic database mining with first principles density functional theory and phonon lattice dynamics calculations, a theoretical screening methodology to identify the most promising CO2 sorbent candidates from the vast array of possible solid materials have been proposed and validated at NETL. The advantage of this method is that it identifies the thermodynamic properties of the CO2 capture reaction as a function of temperature and pressure without any experimental input beyond crystallographic structural information of the solid phases involved. The calculated thermodynamic properties of different classes of solid materials versus temperature and pressure changes were further used to evaluate the equilibrium properties for the CO2 adsorption/desorption cycles. According to the requirements imposed by the pre- and post- combustion technologies and based on our calculated thermodynamic properties for the CO2 capture reactions by the solids of interest, we were able to identify only those solid materials for which lower capture energy costs are expected at the desired working conditions. In addition, we present a simulation scheme to increase and decrease the turnover temperature (Tt) of solid capturing CO2 reaction by mixing other solids. Our results also show that some solid sorbents can serve as bi-functional materials: CO2 sorbent and CO oxidation catalyst. Such dual functionality could be used for removing both CO and CO2 after water-gas-shift to obtain pure H2.

Hydrogen sulfide capture by limestone and dolomite at elevated pressure. 2: Sorbent particle conversion modeling

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zevenhoven, C.A.P.; Yrjas, K.P.; Hupa, M.M.

1996-03-01

The physical structure of a limestone or dolomite to be used in in-bed sulfur capture in fluidized bed gasifiers has a great impact on the efficiency of sulfur capture and sorbent use. In this study an unreacted shrinking core model with variable effective diffusivity is applied to sulfidation test data from a pressurized thermogravimetric apparatus (P-TGA) for a set of physically and chemically different limestone and dolomite samples. The particle size was 250--300 {micro}m for all sorbents, which were characterized by chemical composition analysis, particle density measurement, mercury porosimetry, and BET internal surface measurement. Tests were done under typical conditionsmore » for a pressurized fluidized-bed gasifier, i.e., 20% CO{sub 2}, 950 C, 20 bar. At these conditions the limestone remains uncalcined, while the dolomite is half-calcined. Additional tests were done at low CO{sub 2} partial pressures, yielding calcined limestone and fully calcined dolomite. The generalized model allows for determination of values for the initial reaction rate and product layer diffusivity.« less

CO 2 capture from IGCC gas streams using the AC-ABC process

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nagar, Anoop; McLaughlin, Elisabeth; Hornbostel, Marc

The objective of this project was to develop a novel, low-cost CO 2 capture process from pre-combustion gas streams. The bench-scale work was conducted at the SRI International. A 0.15-MWe integrated pilot plant was constructed and operated for over 700 hours at the National Carbon Capture Center, Wilsonville, AL. The AC-ABC (ammonium carbonate-ammonium bicarbonate) process for capture of CO 2 and H 2S from the pre-combustion gas stream offers many advantages over Selexol-based technology. The process relies on the simple chemistry of the NH 3-CO 2-H 2O-H 2S system and on the ability of the aqueous ammoniated solution to absorbmore » CO 2 at near ambient temperatures and to release it as a high-purity, high-pressure gas at a moderately elevated regeneration temperature. It is estimated the increase in cost of electricity (COE) with the AC-ABC process will be ~ 30%, and the cost of CO 2 captured is projected to be less than $27/metric ton of CO 2 while meeting 90% CO 2 capture goal. The Bechtel Pressure Swing Claus (BPSC) is a complementary technology offered by Bechtel Hydrocarbon Technology Solutions, Inc. BPSC is a high-pressure, sub-dew-point Claus process that allows for nearly complete removal of H 2S from a gas stream. It operates at gasifier pressures and moderate temperatures and does not affect CO 2 content. When coupled with AC-ABC, the combined technologies allow a nearly pure CO 2 stream to be captured at high pressure, something which Selexol and other solvent-based technologies cannot achieve.« less

Device-scale CFD modeling of gas-liquid multiphase flow and amine absorption for CO 2 capture: Original Research Article: Device-scale CFD modeling of gas-liquid multiphase flow and amine absorption for CO 2 capture

DOE PAGES

Pan, Wenxiao; Galvin, Janine; Huang, Wei Ling; ...

2018-03-25

In this paper we aim to develop a validated device-scale CFD model that can predict quantitatively both hydrodynamics and CO 2 capture efficiency for an amine-based solvent absorber column with random Pall ring packing. A Eulerian porous-media approach and a two-fluid model were employed, in which the momentum and mass transfer equations were closed by literature-based empirical closure models. We proposed a hierarchical approach for calibrating the parameters in the closure models to make them accurate for the packed column. Specifically, a parameter for momentum transfer in the closure was first calibrated based on data from a single experiment. Withmore » this calibrated parameter, a parameter in the closure for mass transfer was next calibrated under a single operating condition. Last, the closure of the wetting area was calibrated for each gas velocity at three different liquid flow rates. For each calibration, cross validations were pursued using the experimental data under operating conditions different from those used for calibrations. This hierarchical approach can be generally applied to develop validated device-scale CFD models for different absorption columns.« less

The mechanism of vapor phase hydration of calcium oxide: implications for CO2 capture.

PubMed

Kudłacz, Krzysztof; Rodriguez-Navarro, Carlos

2014-10-21

Lime-based sorbents are used for fuel- and flue-gas capture, thereby representing an economic and effective way to reduce CO2 emissions. Their use involves cyclic carbonation/calcination which results in a significant conversion reduction with increasing number of cycles. To reactivate spent CaO, vapor phase hydration is typically performed. However, little is known about the ultimate mechanism of such a hydration process. Here, we show that the vapor phase hydration of CaO formed after calcination of calcite (CaCO3) single crystals is a pseudomorphic, topotactic process, which progresses via an intermediate disordered phase prior to the final formation of oriented Ca(OH)2 nanocrystals. The strong structural control during this solid-state phase transition implies that the microstructural features of the CaO parent phase predetermine the final structural and physicochemical (reactivity and attrition) features of the product hydroxide. The higher molar volume of the product can create an impervious shell around unreacted CaO, thereby limiting the efficiency of the reactivation process. However, in the case of compact, sintered CaO structures, volume expansion cannot be accommodated in the reduced pore volume, and stress generation leads to pervasive cracking. This favors complete hydration but also detrimental attrition. Implications of these results in carbon capture and storage (CCS) are discussed.

Device-scale CFD modeling of gas-liquid multiphase flow and amine absorption for CO 2 capture: Original Research Article: Device-scale CFD modeling of gas-liquid multiphase flow and amine absorption for CO 2 capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pan, Wenxiao; Galvin, Janine; Huang, Wei Ling

In this paper we aim to develop a validated device-scale CFD model that can predict quantitatively both hydrodynamics and CO 2 capture efficiency for an amine-based solvent absorber column with random Pall ring packing. A Eulerian porous-media approach and a two-fluid model were employed, in which the momentum and mass transfer equations were closed by literature-based empirical closure models. We proposed a hierarchical approach for calibrating the parameters in the closure models to make them accurate for the packed column. Specifically, a parameter for momentum transfer in the closure was first calibrated based on data from a single experiment. Withmore » this calibrated parameter, a parameter in the closure for mass transfer was next calibrated under a single operating condition. Last, the closure of the wetting area was calibrated for each gas velocity at three different liquid flow rates. For each calibration, cross validations were pursued using the experimental data under operating conditions different from those used for calibrations. This hierarchical approach can be generally applied to develop validated device-scale CFD models for different absorption columns.« less

Hydroquinone and Quinone-Grafted Porous Carbons for Highly Selective CO2 Capture from Flue Gases and Natural Gas Upgrading.

PubMed

Wang, Jun; Krishna, Rajamani; Yang, Jiangfeng; Deng, Shuguang

2015-08-04

Hydroquinone and quinone functional groups were grafted onto a hierarchical porous carbon framework via the Friedel-Crafts reaction to develop more efficient adsorbents for the selective capture and removal of carbon dioxide from flue gases and natural gas. The oxygen-doped porous carbons were characterized with scanning electron microscopy, transmission electron microscopy, X-ray powder diffraction, Fourier transform infrared spectroscopy, and Raman spectroscopy. CO2, CH4, and N2 adsorption isotherms were measured and correlated with the Langmuir model. An ideal adsorbed solution theory (IAST) selectivity for the CO2/N2 separation of 26.5 (298 K, 1 atm) was obtained on the hydroquinone-grafted carbon, which is 58.7% higher than that of the pristine porous carbon, and a CO2/CH4 selectivity value of 4.6 (298 K, 1 atm) was obtained on the quinone-grafted carbon (OAC-2), which represents a 28.4% improvement over the pristine porous carbon. The highest CO2 adsorption capacity on the oxygen-doped carbon adsorbents is 3.46 mmol g(-1) at 298 K and 1 atm. In addition, transient breakthrough simulations for CO2/CH4/N2 mixture separation were conducted to demonstrate the good separation performance of the oxygen-doped carbons in fixed bed adsorbers. Combining excellent adsorption separation properties and low heats of adsorption, the oxygen-doped carbons developed in this work appear to be very promising for flue gas treatment and natural gas upgrading.

Potential evaluation of CO2 storage and enhanced oil recovery of tight oil reservoir in the Ordos Basin, China.

PubMed

Tian, Xiaofeng; Cheng, Linsong; Cao, Renyi; Zhang, Miaoyi; Guo, Qiang; Wang, Yimin; Zhang, Jian; Cui, Yu

2015-07-01

Carbon -di-oxide (CO2) is regarded as the most important greenhouse gas to accelerate climate change and ocean acidification. The Chinese government is seeking methods to reduce anthropogenic CO2 gas emission. CO2 capture and geological storage is one of the main methods. In addition, injecting CO2 is also an effective method to replenish formation energy in developing tight oil reservoirs. However, exiting methods to estimate CO2 storage capacity are all based on the material balance theory. This was absolutely correct for normal reservoirs. However, as natural fractures widely exist in tight oil reservoirs and majority of them are vertical ones, tight oil reservoirs are not close. Therefore, material balance theory is not adaptive. In the present study, a new method to calculate CO2 storage capacity is presented. The CO2 effective storage capacity, in this new method, consisted of free CO2, CO2 dissolved in oil and CO2 dissolved in water. Case studies of tight oil reservoir from Ordos Basin was conducted and it was found that due to far lower viscosity of CO2 and larger solubility in oil, CO2 could flow in tight oil reservoirs more easily. As a result, injecting CO2 in tight oil reservoirs could obviously enhance sweep efficiency by 24.5% and oil recovery efficiency by 7.5%. CO2 effective storage capacity of Chang 7 tight oil reservoir in Longdong area was 1.88 x 10(7) t. The Chang 7 tight oil reservoir in Ordos Basin was estimated to be 6.38 x 10(11) t. As tight oil reservoirs were widely distributed in Songliao Basin, Sichuan Basin and so on, geological storage capacity of CO2 in China is potential.

Microbial Electrolytic Capture, Separation and Regeneration of CO2 for Biogas Upgrading.

PubMed

Jin, Xiangdan; Zhang, Yifeng; Li, Xiaohu; Zhao, Nannan; Angelidaki, Irini

2017-08-15

Biogas upgrading to natural gas quality is essential for the efficient use of biogas in various applications. Carbon dioxide (CO 2 ) which constitutes a major part of the biogas is generally removed by physicochemical methods. However, most of the methods are expensive and often present environmental challenges. In this study, an innovative microbial electrolytic system was developed to capture, separate and regenerate CO 2 for biogas upgrading without external supply of chemicals, and potentially to treat wastewater. The new system was operated at varied biogas flow rates and external applied voltages. CO 2 was effectively separated from the raw biogas and the CH 4 content in the outlet reached as high as 97.0 ± 0.2% at the external voltage of 1.2 V and gas flow rate of 19.6 mL/h. Regeneration of CO 2 was also achieved in the regeneration chamber with low pH (1.34 ± 0.04). The relatively low electric energy consumption (≤0.15 kWh/m 3 biogas) along with the H 2 production which can contribute to the energy input makes the overall energy need of the system low, and thereby makes the technology promising. This work provides the first attempt for development of a sustainable biogas upgrading technology and potentially expands the application of microbial electrochemical technologies.

Phase-Change Aminopyridines as Carbon Dioxide Capture Solvents

DOE Office of Scientific and Technical Information (OSTI.GOV)

Malhotra, Deepika; Page, Jordan P.; Bowden, Mark E.

Carbon dioxide is the main atmospheric greenhouse gas released from industrial point sources. In order to mitigate adverse environmental effects of these emissions, carbon capture, storage and utilization is required. To this end, several CO2 capture technologies are being developed for application in carbon capture, which include aqueous amines and water-lean solvents. Herein we report new aminopyridine solvents with the potential for CO2 capture from coal-fired power plants. These four solvents 2-picolylamine, 3-picolylamine, 4-picolylamine and N’-(pyridin-4-ylmethyl)ethane-1,2-diamine are liquids that rapidly bind CO2 to form crystalline solids at standard room temperature and pressure. These solvents have displayed high CO2 capture capacitymore » (11 - 20 wt%) and can be regenerated at temperatures in the range of 120 - 150 C. The advantage of these primary aminopyridine solvents is that crystalline salt product can be separated, making it possible to regenerate only the CO2-rich solid ultimately resulting in reduced energy penalty.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Middleton, Richard S.; Levine, Jonathan S.; Bielicki, Jeffrey M.

CO 2 capture, utilization, and storage (CCUS) technology has yet to be widely deployed at a commercial scale despite multiple high-profile demonstration projects. We suggest that developing a large-scale, visible, and financially viable CCUS network could potentially overcome many barriers to deployment and jumpstart commercial-scale CCUS. To date, substantial effort has focused on technology development to reduce the costs of CO 2 capture from coal-fired power plants. Here, we propose that near-term investment could focus on implementing CO 2 capture on facilities that produce high-value chemicals/products. These facilities can absorb the expected impact of the marginal increase in the costmore » of production on the price of their product, due to the addition of CO 2 capture, more than coal-fired power plants. A financially viable demonstration of a large-scale CCUS network requires offsetting the costs of CO 2 capture by using the CO 2 as an input to the production of market-viable products. As a result, we demonstrate this alternative development path with the example of an integrated CCUS system where CO 2 is captured from ethylene producers and used for enhanced oil recovery in the U.S. Gulf Coast region.« less

Investigation of CO2 capture mechanisms of liquid-like nanoparticle organic hybrid materials via structural characterization.

PubMed

Park, Youngjune; Decatur, John; Lin, Kun-Yi Andrew; Park, Ah-Hyung Alissa

2011-10-28

Nanoparticle organic hybrid materials (NOHMs) have been recently developed that comprise an oligomeric or polymeric canopy tethered to surface-modified nanoparticles via ionic or covalent bonds. It has already been shown that the tunable nature of the grafted polymeric canopy allows for enhanced CO(2) capture capacity and selectivity via the enthalpic intermolecular interactions between CO(2) and the task-specific functional groups, such as amines. Interestingly, for the same amount of CO(2) loading NOHMs have also exhibited significantly different swelling behavior compared to that of the corresponding polymers, indicating a potential structural effect during CO(2) capture. If the frustrated canopy species favor spontaneous ordering due to steric and/or entropic effects, the inorganic cores of NOHMs could be organized into unusual structural arrangements. Likewise, the introduction of small gaseous molecules such as CO(2) could reduce the free energy of the frustrated canopy. This entropic effect, the result of unique structural nature, could allow NOHMs to capture CO(2) more effectively. In order to isolate the entropic effect, NOHMs were synthesized without the task-specific functional groups. The relationship between their structural conformation and the underlying mechanisms for the CO(2) absorption behavior were investigated by employing NMR and ATR FT-IR spectroscopies. The results provide fundamental information needed for evaluating and developing novel liquid-like CO(2) capture materials and give useful insights for designing and synthesizing NOHMs for more effective CO(2) capture. This journal is © the Owner Societies 2011

Scoping Alternatives for Negative Emission Technologies. FRACCC - Possible Routes to Biomass-Derived Carbon Injection in Shallow Aquifers?

NASA Astrophysics Data System (ADS)

Correa Silva, R.; Larter, S.

2016-12-01

Atmospheric CO2 capture into biomass is one of the capture options for negative emission technologies, although proposed sequestration systems such as the permanent burial of total fresh biomass, algal lipids or soil amendment with biochar are yet to be successfully demonstrated as effective at scale. In the context of carbon sequestration, shallow geological reservoirs have not been exhaustively explored, even though they pose, away from groundwater protection zones, potentially low implementation cost, and geographically abundant potential carbon storage reservoirs. Typical carbon storage vectors considered, such as CO2 and biochar, are not suitable for shallow aquifer disposal, due either to cap rock containment requirements, or shallow aquifer CO2 densities, or issues related to formation damage from solid particles. Thus, a cost-effective technology, aimed at converting biomass into a large-scale carbon vector fit-for-disposal in shallow formations could be significant, linking promising carbon capture and containment strategies. In this work, we discuss the development of unconventional carbon vectors for subsurface storage in the form of Functionalized, Refractory and Aqueous Compatible Carbon Compounds (FRACCC), as a potential alternative negative emission technology (Larter et al., 2010). The concept is based on CO2 capture into microbial and algal biomass, followed by the modification of biomass constituents through facile chemical reactions aimed at rendering the biomass efficiently into a stable, biologically refractory but water soluble form, similar in some regards, to dissolved organic matter in the oceans, then sequestering the material in geological settings. As the injected material is not buoyant, containment specifications are more modest than for CO2 injection and potentially, more reservoirs could be accessible! This work analyses the technological, economic and societal implications of such potential FRACCC technologies, and make an assessment of whether such routes are likely to be technically, economically and politically viable.

The urgency of the development of CO2 capture from ambient air

PubMed Central

Lackner, Klaus S.; Brennan, Sarah; Matter, Jürg M.; Park, A.-H. Alissa; Wright, Allen; van der Zwaan, Bob

2012-01-01

CO2 capture and storage (CCS) has the potential to develop into an important tool to address climate change. Given society’s present reliance on fossil fuels, widespread adoption of CCS appears indispensable for meeting stringent climate targets. We argue that for conventional CCS to become a successful climate mitigation technology—which by necessity has to operate on a large scale—it may need to be complemented with air capture, removing CO2 directly from the atmosphere. Air capture of CO2 could act as insurance against CO2 leaking from storage and furthermore may provide an option for dealing with emissions from mobile dispersed sources such as automobiles and airplanes. PMID:22843674

Carbon dioxide capture from a cement manufacturing process

DOEpatents

Blount, Gerald C [North Augusta, SC; Falta, Ronald W [Seneca, SC; Siddall, Alvin A [Aiken, SC

2011-07-12

A process of manufacturing cement clinker is provided in which a clean supply of CO.sub.2 gas may be captured. The process also involves using an open loop conversion of CaO/MgO from a calciner to capture CO.sub.2 from combustion flue gases thereby forming CaCO.sub.3/CaMg(CO.sub.3).sub.2. The CaCO.sub.3/CaMg(CO.sub.3).sub.2 is then returned to the calciner where CO.sub.2 gas is evolved. The evolved CO.sub.2 gas, along with other evolved CO.sub.2 gases from the calciner are removed from the calciner. The reactants (CaO/MgO) are feed to a high temperature calciner for control of the clinker production composition.

Efficient CO2 capture by functionalized graphene oxide nanosheets as fillers to fabricate multi-permselective mixed matrix membranes.

PubMed

Li, Xueqin; Cheng, Youdong; Zhang, Haiyang; Wang, Shaofei; Jiang, Zhongyi; Guo, Ruili; Wu, Hong

2015-03-11

A novel multi-permselective mixed matrix membrane (MP-MMM) is developed by incorporating versatile fillers functionalized with ethylene oxide (EO) groups and an amine carrier into a polymer matrix. The as-prepared MP-MMMs can separate CO2 efficiently because of the simultaneous enhancement of diffusivity selectivity, solubility selectivity, and reactivity selectivity. To be specific, MP-MMMs were fabricated by incorporating polyethylene glycol- and polyethylenimine-functionalized graphene oxide nanosheets (PEG-PEI-GO) into a commercial low-cost Pebax matrix. The PEG-PEI-GO plays multiple roles in enhancing membrane performance. First, the high-aspect ratio GO nanosheets in a polymer matrix increase the length of the tortuous path of gas diffusion and generate a rigidified interface between the polymer matrix and fillers, enhancing the diffusivity selectivity. Second, PEG consisting of EO groups has excellent affinity for CO2 to enhance the solubility selectivity. Third, PEI with abundant primary, secondary, and tertiary amine groups reacts reversibly with CO2 to enhance reactivity selectivity. Thus, the as-prepared MP-MMMs exhibit excellent CO2 permeability and CO2/gas selectivity. The MP-MMM doped with 10 wt % PEG-PEI-GO displays optimal gas separation performance with a CO2 permeability of 1330 Barrer, a CO2/CH4 selectivity of 45, and a CO2/N2 selectivity of 120, surpassing the upper bound lines of the Robeson study of 2008 (1 Barrer = 10(-10) cm(3) (STP) cm(-2) s(-1) cm(-1) Hg).

Near-term deployment of carbon capture and sequestration from biorefineries in the United States.

PubMed

Sanchez, Daniel L; Johnson, Nils; McCoy, Sean T; Turner, Peter A; Mach, Katharine J

2018-05-08

Capture and permanent geologic sequestration of biogenic CO 2 emissions may provide critical flexibility in ambitious climate change mitigation. However, most bioenergy with carbon capture and sequestration (BECCS) technologies are technically immature or commercially unavailable. Here, we evaluate low-cost, commercially ready CO 2 capture opportunities for existing ethanol biorefineries in the United States. The analysis combines process engineering, spatial optimization, and lifecycle assessment to consider the technical, economic, and institutional feasibility of near-term carbon capture and sequestration (CCS). Our modeling framework evaluates least cost source-sink relationships and aggregation opportunities for pipeline transport, which can cost-effectively transport small CO 2 volumes to suitable sequestration sites; 216 existing US biorefineries emit 45 Mt CO 2 annually from fermentation, of which 60% could be captured and compressed for pipeline transport for under $25/tCO 2 A sequestration credit, analogous to existing CCS tax credits, of $60/tCO 2 could incent 30 Mt of sequestration and 6,900 km of pipeline infrastructure across the United States. Similarly, a carbon abatement credit, analogous to existing tradeable CO 2 credits, of $90/tCO 2 can incent 38 Mt of abatement. Aggregation of CO 2 sources enables cost-effective long-distance pipeline transport to distant sequestration sites. Financial incentives under the low-carbon fuel standard in California and recent revisions to existing federal tax credits suggest a substantial near-term opportunity to permanently sequester biogenic CO 2 This financial opportunity could catalyze the growth of carbon capture, transport, and sequestration; improve the lifecycle impacts of conventional biofuels; support development of carbon-negative fuels; and help fulfill the mandates of low-carbon fuel policies across the United States. Copyright © 2018 the Author(s). Published by PNAS.

Near-term deployment of carbon capture and sequestration from biorefineries in the United States

PubMed Central

Johnson, Nils; McCoy, Sean T.; Turner, Peter A.; Mach, Katharine J.

2018-01-01

Capture and permanent geologic sequestration of biogenic CO2 emissions may provide critical flexibility in ambitious climate change mitigation. However, most bioenergy with carbon capture and sequestration (BECCS) technologies are technically immature or commercially unavailable. Here, we evaluate low-cost, commercially ready CO2 capture opportunities for existing ethanol biorefineries in the United States. The analysis combines process engineering, spatial optimization, and lifecycle assessment to consider the technical, economic, and institutional feasibility of near-term carbon capture and sequestration (CCS). Our modeling framework evaluates least cost source–sink relationships and aggregation opportunities for pipeline transport, which can cost-effectively transport small CO2 volumes to suitable sequestration sites; 216 existing US biorefineries emit 45 Mt CO2 annually from fermentation, of which 60% could be captured and compressed for pipeline transport for under $25/tCO2. A sequestration credit, analogous to existing CCS tax credits, of $60/tCO2 could incent 30 Mt of sequestration and 6,900 km of pipeline infrastructure across the United States. Similarly, a carbon abatement credit, analogous to existing tradeable CO2 credits, of $90/tCO2 can incent 38 Mt of abatement. Aggregation of CO2 sources enables cost-effective long-distance pipeline transport to distant sequestration sites. Financial incentives under the low-carbon fuel standard in California and recent revisions to existing federal tax credits suggest a substantial near-term opportunity to permanently sequester biogenic CO2. This financial opportunity could catalyze the growth of carbon capture, transport, and sequestration; improve the lifecycle impacts of conventional biofuels; support development of carbon-negative fuels; and help fulfill the mandates of low-carbon fuel policies across the United States. PMID:29686063

Kinetics of CO2 diffusion in human carbonic anhydrase: a study using molecular dynamics simulations and the Markov-state model.

PubMed

Chen, Gong; Kong, Xian; Lu, Diannan; Wu, Jianzhong; Liu, Zheng

2017-05-10

Molecular dynamics (MD) simulations, in combination with the Markov-state model (MSM), were applied to probe CO 2 diffusion from an aqueous solution into the active site of human carbonic anhydrase II (hCA-II), an enzyme useful for enhanced CO 2 capture and utilization. The diffusion process in the hydrophobic pocket of hCA-II was illustrated in terms of a two-dimensional free-energy landscape. We found that CO 2 diffusion in hCA-II is a rate-limiting step in the CO 2 diffusion-binding-reaction process. The equilibrium distribution of CO 2 shows its preferential accumulation within a hydrophobic domain in the protein core region. An analysis of the committors and reactive fluxes indicates that the main pathway for CO 2 diffusion into the active site of hCA-II is through a binding pocket where residue Gln 136 contributes to the maximal flux. The simulation results offer a new perspective on the CO 2 hydration kinetics and useful insights toward the development of novel biochemical processes for more efficient CO 2 sequestration and utilization.

Multifluid geo-energy systems: Using geologic CO 2 storage for geothermal energy production and grid-scale energy storage in sedimentary basins

DOE PAGES

Buscheck, Thomas A.; Bielicki, Jeffrey M.; Edmunds, Thomas A.; ...

2016-05-05

We present an approach that uses the huge fluid and thermal storage capacity of the subsurface, together with geologic carbon dioxide (CO 2) storage, to harvest, store, and dispatch energy from subsurface (geothermal) and surface (solar, nuclear, fossil) thermal resources, as well as excess energy on electric grids. Captured CO 2 is injected into saline aquifers to store pressure, generate artesian flow of brine, and provide a supplemental working fluid for efficient heat extraction and power conversion. Concentric rings of injection and production wells create a hydraulic mound to store pressure, CO 2, and thermal energy. This energy storage canmore » take excess power from the grid and excess/waste thermal energy, and dispatch that energy when it is demanded and thus enable higher penetration of variable renewable energy technologies (e.g., wind, solar). CO 2 stored in the subsurface functions as a cushion gas to provide enormous pressure-storage capacity and displace large quantities of brine, some of which can be treated for a variety of beneficial uses. Geothermal power and energy-storage applications may generate enough revenues to compensate for CO 2 capture costs. While our approach can use nitrogen (N 2), in addition to CO 2, as a supplemental fluid, and store thermal energy, this study focuses using CO 2 for geothermal energy production and grid-scale energy storage. We conduct a techno-economic assessment to determine the levelized cost of electricity of using this approach to generate geothermal power. We present a reservoir pressure-management strategy that diverts a small portion of the produced brine for beneficial consumptive use to reduce the pumping cost of fluid recirculation, while reducing the risk of seismicity, caprock fracture, and CO 2 leakage.« less

Method and system for capturing carbon dioxide and/or sulfur dioxide from gas stream

DOEpatents

Chang, Shih-Ger; Li, Yang; Zhao, Xinglei

2014-07-08

The present invention provides a system for capturing CO.sub.2 and/or SO.sub.2, comprising: (a) a CO.sub.2 and/or SO.sub.2 absorber comprising an amine and/or amino acid salt capable of absorbing the CO.sub.2 and/or SO.sub.2 to produce a CO.sub.2- and/or SO.sub.2-containing solution; (b) an amine regenerator to regenerate the amine and/or amino acid salt; and, when the system captures CO.sub.2, (c) an alkali metal carbonate regenerator comprising an ammonium catalyst capable catalyzing the aqueous alkali metal bicarbonate into the alkali metal carbonate and CO.sub.2 gas. The present invention also provides for a system for capturing SO.sub.2, comprising: (a) a SO.sub.2 absorber comprising aqueous alkali metal carbonate, wherein the alkali metal carbonate is capable of absorbing the SO.sub.2 to produce an alkali metal sulfite/sulfate precipitate and CO.sub.2.

Theoretical calculating the thermodynamic properties of solid sorbents for CO{sub 2} capture applications

DOE Office of Scientific and Technical Information (OSTI.GOV)

Duan, Yuhua

2012-11-02

Since current technologies for capturing CO{sub 2} to fight global climate change are still too energy intensive, there is a critical need for development of new materials that can capture CO{sub 2} reversibly with acceptable energy costs. Accordingly, solid sorbents have been proposed to be used for CO{sub 2} capture applications through a reversible chemical transformation. By combining thermodynamic database mining with first principles density functional theory and phonon lattice dynamics calculations, a theoretical screening methodology to identify the most promising CO{sub 2} sorbent candidates from the vast array of possible solid materials has been proposed and validated. The calculatedmore » thermodynamic properties of different classes of solid materials versus temperature and pressure changes were further used to evaluate the equilibrium properties for the CO{sub 2} adsorption/desorption cycles. According to the requirements imposed by the pre- and post- combustion technologies and based on our calculated thermodynamic properties for the CO{sub 2} capture reactions by the solids of interest, we were able to screen only those solid materials for which lower capture energy costs are expected at the desired pressure and temperature conditions. Only those selected CO{sub 2} sorbent candidates were further considered for experimental validations. The ab initio thermodynamic technique has the advantage of identifying thermodynamic properties of CO{sub 2} capture reactions without any experimental input beyond crystallographic structural information of the solid phases involved. Such methodology not only can be used to search for good candidates from existing database of solid materials, but also can provide some guidelines for synthesis new materials. In this presentation, we first introduce our screening methodology and the results on a testing set of solids with known thermodynamic properties to validate our methodology. Then, by applying our computational method to several different kinds of solid systems, we demonstrate that our methodology can predict the useful information to help developing CO{sub 2} capture Technologies.« less

Emerging materials for lowering atmospheric carbon

DOE PAGES

Barkakaty, Balaka; Sumpter, Bobby G.; Ivanov, Ilia N.; ...

2016-12-08

CO 2 emissions from anthropogenic sources and the rate at which they increase could have deep global ramifications such as irreversible climate change and increased natural disasters. Because greater than 50% of anthropogenic CO 2 emissions come from small, distributed sectors such as homes, offices, and transportation sources, most renewable energy systems and on-site carbon capture technologies for reducing future CO 2 emissions cannot be effectively utilized. This problem might be mediated by considering novel materials and technologies for directly capturing/removing CO 2 from air. But, compared to materials for capturing CO 2 at on-site emission sources, materials for capturingmore » CO 2 directly from air must be more selective to CO 2, and should operate and be stable at near ambient conditions. Here, we briefly summarize the recent developments in materials for capturing carbon dioxide directly from air. Furthermore, we discuss the challenges in this field and offer a perspective for developing the current state-of-art and also highlight the potential of a few recent discoveries in materials science that show potential for advanced application of air capture technology.« less

Convenient and large-scale synthesis of nitrogen-rich hierarchical porous carbon spheres for supercapacitors and CO2 capture

NASA Astrophysics Data System (ADS)

Chang, Binbin; Zhang, Shouren; Yin, Hang; Yang, Baocheng

2017-08-01

Herein, considering the great potential of nitrogen-doped hierarchical porous carbons in energy storage and CO2 capture, we designed a convenient and easily large-scale production strategy for preparing nitrogen-doped hierarchical porous carbon sphere (NHPCS) materials. In this synthesis route, spherical resorcinol-formaldehyde (RF) resins were selected as carbon precursor, and then the ZnCl2-impregnated RF resin spheres were carbonized in a NH3 atmosphere at a temperature range of 600-800 °C. During the one-step heat-treatment process, nitrogen atom could be efficiently incorporated into the carbon skeleton, and the interconnected and hierarchical pore structure with different micro/mesopore proportion could be generated and tuned by adjusting the activating agent ZnCl2 dosage and carbonization temperature. The resultant nitrogen-doped hierarchical porous carbon sphere materials exhibited a satisfactory charge storage capacity, and the optimal sample of NHPCS-2-8 with a high mesopore proportion obtained at 800 °C with a ZnCl2/RF mass ratio of 2:1 presented a specific capacitance of 273.8 F g-1 at a current density of 0.5 A g-1. More importantly, the assembled NHPCS-2-8-based symmetric capacitor displayed a high energy density of 17.2 Wh kg-1 at a power density of 178.9 W kg-1 within a voltage window of 0 ∼ 1.8 V in 0.5 M Na2SO4 aqueous electrolyte. In addition, the CO2 capture application of these NHPCS materials was also explored, and the optimal sample of NHPCS-0-8 with a large micropore proportion prepared at 800 °C exhibited an exceptional CO2 uptake capacity at ambient pressures of up to 4.23 mmol g-1 at 0 °C.

Electrochemical Membrane for Carbon Dioxide Capture and Power Generation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ghezel-Ayagh, Hossein

FuelCell Energy, Inc. (FCE), in collaboration with AECOM Corporation (formerly URS Corporation) and Pacific Northwest National Laboratory, has been developing a novel Combined Electric Power and Carbon-dioxide Separation (CEPACS) system. The CEPACS system is based on electrochemical membrane (ECM) technology derived from FCE’s carbonate fuel cell products featuring internal (methane steam) reforming and carrying the trade name of Direct FuelCell®. The unique chemistry of carbonate fuel cells offers an innovative approach for separation of CO 2 from existing fossil-fuel power plant exhaust streams (flue gases). The ECM-based CEPACS system has the potential to become a transformational CO 2-separation technology bymore » working as two devices in one: it separates the CO 2 from the exhaust of other plants such as an existing coal-fired plant and simultaneously produces clean electric power at high efficiency using a supplementary fuel. The development effort was carried out under the U.S. Department of Energy (DOE) cooperative agreement DE-FE0007634. The overall objective of this project was to successfully demonstrate the ability of FCE’s ECM-based CEPACS system technology to separate ≥90% of the CO 2 from a simulated Pulverized Coal (PC) power plant flue gas stream and to compress the captured CO2 to a state that can be easily transported for sequestration or beneficial use. In addition, a key objective was to show, through the technical and economic feasibility study and bench scale testing, that the ECM-based CEPACS system is an economical alternative for CO 2 capture in PC power plants, and that it meets DOE’s objective related to the incremental cost of electricity (COE) for post-combustion CO 2 capture (no more than 35% increase in COE). The project was performed in three budget periods (BP). The specific objective for BP1 was to complete the Preliminary Technical and Economic Feasibility Study. The T&EF study was based on the carbon capture system size suitable for a reference 550 MW PC power plant. The specific objectives for BP2 were to perform (flue gas) contaminant effect evaluation tests, small area membrane tests using clean simulated flue gas, design a flue gas pretreatment system for processing of the gas feed to ECM, update the Technical & Economic Feasibility Study (T&EFS) incorporating results of contaminant effect tests and small area membrane tests, and to prepare a test facility for bench scale testing. The specific objectives for BP3 were to perform bench scale testing (parametric and long-duration testing) of a 11.7 m 2 ECM-based CO 2 capture, purification and compression system, and update (as final) the Technical and Economic Feasibility Study. In addition, an Environmental Health and Safety evaluation (assessment) of the ECM technology was included. This final technical report presents the progress made under the project.« less

Direct electrolytic dissolution of silicate minerals for air CO2 mitigation and carbon-negative H2 production

PubMed Central

Rau, Greg H.; Carroll, Susan A.; Bourcier, William L.; Singleton, Michael J.; Smith, Megan M.; Aines, Roger D.

2013-01-01

We experimentally demonstrate the direct coupling of silicate mineral dissolution with saline water electrolysis and H2 production to effect significant air CO2 absorption, chemical conversion, and storage in solution. In particular, we observed as much as a 105-fold increase in OH− concentration (pH increase of up to 5.3 units) relative to experimental controls following the electrolysis of 0.25 M Na2SO4 solutions when the anode was encased in powdered silicate mineral, either wollastonite or an ultramafic mineral. After electrolysis, full equilibration of the alkalized solution with air led to a significant pH reduction and as much as a 45-fold increase in dissolved inorganic carbon concentration. This demonstrated significant spontaneous air CO2 capture, chemical conversion, and storage as a bicarbonate, predominantly as NaHCO3. The excess OH− initially formed in these experiments apparently resulted via neutralization of the anolyte acid, H2SO4, by reaction with the base mineral silicate at the anode, producing mineral sulfate and silica. This allowed the NaOH, normally generated at the cathode, to go unneutralized and to accumulate in the bulk electrolyte, ultimately reacting with atmospheric CO2 to form dissolved bicarbonate. Using nongrid or nonpeak renewable electricity, optimized systems at large scale might allow relatively high-capacity, energy-efficient (<300 kJ/mol of CO2 captured), and inexpensive (<$100 per tonne of CO2 mitigated) removal of excess air CO2 with production of carbon-negative H2. Furthermore, when added to the ocean, the produced hydroxide and/or (bi)carbonate could be useful in reducing sea-to-air CO2 emissions and in neutralizing or offsetting the effects of ongoing ocean acidification. PMID:23729814

Sequential Design of Experiments to Maximize Learning from Carbon Capture Pilot Plant Testing

DOE Office of Scientific and Technical Information (OSTI.GOV)

Soepyan, Frits B.; Morgan, Joshua C.; Omell, Benjamin P.

Pilot plant test campaigns can be expensive and time-consuming. Therefore, it is of interest to maximize the amount of learning and the efficiency of the test campaign given the limited number of experiments that can be conducted. This work investigates the use of sequential design of experiments (SDOE) to overcome these challenges by demonstrating its usefulness for a recent solvent-based CO2 capture plant test campaign. Unlike traditional design of experiments methods, SDOE regularly uses information from ongoing experiments to determine the optimum locations in the design space for subsequent runs within the same experiment. However, there are challenges that needmore » to be addressed, including reducing the high computational burden to efficiently update the model, and the need to incorporate the methodology into a computational tool. We address these challenges by applying SDOE in combination with a software tool, the Framework for Optimization, Quantification of Uncertainty and Surrogates (FOQUS) (Miller et al., 2014a, 2016, 2017). The results of applying SDOE on a pilot plant test campaign for CO2 capture suggests that relative to traditional design of experiments methods, SDOE can more effectively reduce the uncertainty of the model, thus decreasing technical risk. Future work includes integrating SDOE into FOQUS and using SDOE to support additional large-scale pilot plant test campaigns.« less

Photoinduced Cobalt(III)-Trifluoromethyl Bond Activation Enables Arene C-H Trifluoromethylation.

PubMed

Harris, Caleb F; Kuehner, Christopher S; Bacsa, John; Soper, Jake D

2018-01-26

Visible-light capture activates a thermodynamically inert Co III -CF 3 bond for direct C-H trifluoromethylation of arenes and heteroarenes. New trifluoromethylcobalt(III) complexes supported by a redox-active [OCO] pincer ligand were prepared. Coordinating solvents, such as MeCN, afford green, quasi-octahedral [( S OCO)Co III (CF 3 )(MeCN) 2 ] (2), but in non-coordinating solvents the complex is red, square pyramidal [( S OCO)Co III (CF 3 )(MeCN)] (3). Both are thermally stable, and 2 is stable in light. But exposure of 3 to low-energy light results in facile homolysis of the Co III -CF 3 bond, releasing . CF 3 radical, which is efficiently trapped by TEMPO . or (hetero)arenes. The homolytic aromatic substitution reactions do not require a sacrificial or substrate-derived oxidant because the Co II by-product of Co III -CF 3 homolysis produces H 2 . The photophysical properties of 2 and 3 provide a rationale for the disparate light stability. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Carbon dioxide adsorption on micro-mesoporous composite materials of ZSM-12/MCM-48 type: The role of the contents of zeolite and functionalized amine

DOE Office of Scientific and Technical Information (OSTI.GOV)

Santos, S.C.G.; Pedrosa, A.M.Garrido; Souza, M.J.B., E-mail: mjbsufs@gmail.com

2015-10-15

Highlights: • Synthesis of the micro-mesoporous composite materials of ZSM-12/MCM-48 type. • Application of these adsorbents in the carbon dioxide adsorption. • Effects of the contents of zeolite and amino group in the material surface on the CO{sub 2} capture efficiency. - Abstract: In this study ZSM-12/MCM-48 adsorbents have been synthesized at three ZSM-12 content, and also were functionalizated with amine groups by grafting. All the adsorbents synthesized were evaluated for CO{sub 2} capture. The X-ray diffraction analysis of the ZSM-12/MCM-48 composite showed the main characteristic peaks of ZSM-12 and MCM-48, and after the functionalization, the structure of MCM-48 onmore » the composite impregnated was affected due amine presence. For the composites without amine, the ZSM-12 content was the factor determining in the adsorption capacity of CO{sub 2} and for the composites with amine the amount of amine was that influenced in the adsorption capacity.« less

The role of CO2 capture and utilization in mitigating climate change

NASA Astrophysics Data System (ADS)

Mac Dowell, Niall; Fennell, Paul S.; Shah, Nilay; Maitland, Geoffrey C.

2017-04-01

To offset the cost associated with CO2 capture and storage (CCS), there is growing interest in finding commercially viable end-use opportunities for the captured CO2. In this Perspective, we discuss the potential contribution of carbon capture and utilization (CCU). Owing to the scale and rate of CO2 production compared to that of utilization allowing long-term sequestration, it is highly improbable the chemical conversion of CO2 will account for more than 1% of the mitigation challenge, and even a scaled-up enhanced oil recovery (EOR)-CCS industry will likely only account for 4-8%. Therefore, whilst CO2-EOR may be an important economic incentive for some early CCS projects, CCU may prove to be a costly distraction, financially and politically, from the real task of mitigation.

CO2 Capture Using Electric Fields: Low-Cost Electrochromic Film on Plastic for Net-Zero Energy Building

DOE Office of Scientific and Technical Information (OSTI.GOV)

None

2010-01-01

Broad Funding Opportunity Announcement Project: Two faculty members at Lehigh University created a new technique called supercapacitive swing adsorption (SSA) that uses electrical charges to encourage materials to capture and release CO2. Current CO2 capture methods include expensive processes that involve changes in temperature or pressure. Lehigh University’s approach uses electric fields to improve the ability of inexpensive carbon sorbents to trap CO2. Because this process uses electric fields and not electric current, the overall energy consumption is projected to be much lower than conventional methods. Lehigh University is now optimizing the materials to maximize CO2 capture and minimize themore » energy needed for the process.« less

Binding CO2 from Air by a Bulky Organometallic Cation Containing Primary Amines.

PubMed

Luo, Yang-Hui; Chen, Chen; Hong, Dan-Li; He, Xiao-Tong; Wang, Jing-Wen; Ding, Ting; Wang, Bo-Jun; Sun, Bai-Wang

2018-03-21

The organometallic cation 1 (Fe(bipy-NH 2 ) 3 2+ , bipy-NH 2 = 4,4'-diamino-2,2'-bipyridine), which was constructed in situ in solution, can bind CO 2 from air effectively with a stoichiometric ratio of 1:4 (1/CO 2 ), through the formation of "H-bonded CO 2 " species: [CO 2 -OH-CO 2 ] - and [CO 2 -CO 2 -OH] - . These two species, along with the captured individual CO 2 molecules, connected 1 into a novel 3D (three-dimensional) architecture, that was crystal 1·2(OH - )·4(CO 2 ). The adsorption isotherms, recycling investigations, and the heat capacity of 1 have been investigated; the results revealed that the organometallic cation 1 can be recycled at least 10 times for the real-world CO 2 capture applications. The strategies presented here may provide new hints for the development of new alkanolamine-related absorbents or technologies for CO 2 capture and sequestration.

Operation of a 25 KWth Calcium Looping Pilot-plant with High Oxygen Concentrations in the Calciner.

PubMed

Erans, María; Jeremias, Michal; Manovic, Vasilije; Anthony, Edward J

2017-10-25

Calcium looping (CaL) is a post-combustion CO2 capture technology that is suitable for retrofitting existing power plants. The CaL process uses limestone as a cheap and readily available CO2 sorbent. While the technology has been widely studied, there are a few available options that could be applied to make it more economically viable. One of these is to increase the oxygen concentration in the calciner to reduce or eliminate the amount of recycled gas (CO2, H2O and impurities); therefore, decreasing or removing the energy necessary to heat the recycled gas stream. Moreover, there is a resulting increase in the energy input due to the change in the combustion intensity; this energy is used to enable the endothermic calcination reaction to occur in the absence of recycled flue gases. This paper presents the operation and first results of a CaL pilot plant with 100% oxygen combustion of natural gas in the calciner. The gas coming into the carbonator was a simulated flue gas from a coal-fired power plant or cement industry. Several limestone particle size distributions are also tested to further explore the effect of this parameter on the overall performance of this operating mode. The configuration of the reactor system, the operating procedures, and the results are described in detail in this paper. The reactor showed good hydrodynamic stability and stable CO2 capture, with capture efficiencies of up to 70% with a gas mixture simulating the flue gas of a coal-fired power plant.

Ab initio thermodynamic approach to identify mixed solid sorbents for CO 2 capture technology

DOE PAGES

Duan, Yuhua

2015-10-15

Because the current technologies for capturing CO 2 are still too energy intensive, new materials must be developed that can capture CO 2 reversibly with acceptable energy costs. At a given CO 2 pressure, the turnover temperature (T t) of the reaction of an individual solid that can capture CO 2 is fixed. Such T t may be outside the operating temperature range (ΔT o) for a practical capture technology. To adjust T t to fit the practical ΔT o, in this study, three scenarios of mixing schemes are explored by combining thermodynamic database mining with first principles density functionalmore » theory and phonon lattice dynamics calculations. Our calculated results demonstrate that by mixing different types of solids, it’s possible to shift T t to the range of practical operating temperature conditions. According to the requirements imposed by the pre- and post- combustion technologies and based on our calculated thermodynamic properties for the CO 2 capture reactions by the mixed solids of interest, we were able to identify the mixing ratios of two or more solids to form new sorbent materials for which lower capture energy costs are expected at the desired pressure and temperature conditions.« less

Dynamics of Postcombustion CO2 Capture Plants: Modeling, Validation, and Case Study

PubMed Central

2017-01-01

The capture of CO2 from power plant flue gases provides an opportunity to mitigate emissions that are harmful to the global climate. While the process of CO2 capture using an aqueous amine solution is well-known from experience in other technical sectors (e.g., acid gas removal in the gas processing industry), its operation combined with a power plant still needs investigation because in this case, the interaction with power plants that are increasingly operated dynamically poses control challenges. This article presents the dynamic modeling of CO2 capture plants followed by a detailed validation using transient measurements recorded from the pilot plant operated at the Maasvlakte power station in the Netherlands. The model predictions are in good agreement with the experimental data related to the transient changes of the main process variables such as flow rate, CO2 concentrations, temperatures, and solvent loading. The validated model was used to study the effects of fast power plant transients on the capture plant operation. A relevant result of this work is that an integrated CO2 capture plant might enable more dynamic operation of retrofitted fossil fuel power plants because the large amount of steam needed by the capture process can be diverted rapidly to and from the power plant. PMID:28413256

Application of CFB technology for large power generating units and CO{sub 2} capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ryabov, G. A., E-mail: georgy.ryabov@gmail.com; Folomeev, O. M.; Sankin, D. A.

2010-07-15

Data on the development of the circulating fluidized bed (CFB) technology for combustion of fuels in large power generating units are examined. The problems with raising the steam parameters and unit power of boilers with a circulating fluidized bed are examined. With the boiler system at the 460 MW unit at Lagisza (Poland) as an example, the feasibility of raising the efficiency of units with CFB boilers through deep recovery of the heat of the effluent gases and reducing expenditure for in-house needs is demonstrated. Comparative estimates of the capital and operating costs of 225 and 330 MW units aremore » used to determine the conditions for optimum use of CFB boilers in the engineering renovation of thermal power plants in Russia. New areas for the application of CFB technology in CO{sub 2} capture are analyzed in connection with the problem of reducing greenhouse gas emissions.« less

A comparative study of biomass integrated gasification combined cycle power systems: Performance analysis.

PubMed

Zang, Guiyan; Tejasvi, Sharma; Ratner, Albert; Lora, Electo Silva

2018-05-01

The Biomass Integrated Gasification Combined Cycle (BIGCC) power system is believed to potentially be a highly efficient way to utilize biomass to generate power. However, there is no comparative study of BIGCC systems that examines all the latest improvements for gasification agents, gas turbine combustion methods, and CO 2 Capture and Storage options. This study examines the impact of recent advancements on BIGCC performance through exergy analysis using Aspen Plus. Results show that the exergy efficiency of these systems is ranged from 22.3% to 37.1%. Furthermore, exergy analysis indicates that the gas turbine with external combustion has relatively high exergy efficiency, and Selexol CO 2 removal method has low exergy destruction. Moreover, the sensitivity analysis shows that the system exergy efficiency is more sensitive to the initial temperature and pressure ratio of the gas turbine, whereas has a relatively weak dependence on the initial temperature and initial pressure of the steam turbine. Copyright © 2018 Elsevier Ltd. All rights reserved.

Hybrid Membrane/Absorption Process for Post-combustion CO2 Capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Li, Shiguang; Shou, S.; Pyrzynski, Travis

2013-12-31

This report summarizes scientific/technical progress made for bench-scale membrane contactor technology for post-combustion CO2 capture from DOE Contract No. DE-FE-0004787. Budget Period 1 (BP1) membrane absorber, Budget Period 2 (BP2) membrane desorber and Budget Period 3 (BP3) integrated system and field testing studies have been completed successfully and met or exceeded the technical targets (≥ 90% CO2 removal and CO2 purity of 97% in one membrane stage). Significant breakthroughs are summarized below: BP1 research: The feasibility of utilizing the poly (ether ether ketone), PEEK, based hollow fiber contractor (HFC) in combination with chemical solvents to separate and capture at leastmore » 90% of the CO2 from simulated flue gases has been successfully established. Excellent progress has been made as we have achieved the BP1 goal: ≥ 1,000 membrane intrinsic CO2 permeance, ≥ 90% CO2 removal in one stage, ≤ 2 psi gas side pressure drop, and ≥ 1 (sec)-1 mass transfer coefficient. Initial test results also show that the CO2 capture performance, using activated Methyl Diethanol Amine (aMDEA) solvent, was not affected by flue gas contaminants O2 (~3%), NO2 (66 ppmv), and SO2 (145 ppmv). BP2 research: The feasibility of utilizing the PEEK HFC for CO2-loaded solvent regeneration has been successfully established High CO2 stripping flux, one order of magnitude higher than CO2 absorption flux, have been achieved. Refined economic evaluation based on BP1 membrane absorber and BP2 membrane desorber laboratory test data indicate that the CO2 capture costs are 36% lower than DOE’s benchmark amine absorption technology. BP3 research: A bench-scale system utilizing a membrane absorber and desorber was integrated into a continuous CO2 capture process using contactors containing 10 to 20 ft2 of membrane area. The integrated process operation was stable through a 100-hour laboratory test, utilizing a simulated flue gas stream. Greater than 90% CO2 capture combined with 97% CO2 product purity was achieved throughout the test. Membrane contactor modules have been scaled from bench scale 2-inch diameter by 12-inch long (20 ft2 membrane surface area) modules to 4-inch diameter by 60-inch long pilot scale modules (165 ft2 membrane surface area). Pilot scale modules were tested in an integrated absorption/regeneration system for CO2 capture field tests at a coal-fired power plant (Midwest Generation’s Will County Station located in Romeoville, IL). Absorption and regeneration contactors were constructed utilizing high performance super-hydrophobic, nano-porous PEEK membranes with CO2 gas permeance of 2,000 GPU and a 1,000 GPU, respectively. Field tests using aMDEA solvent achieved greater than 90% CO2 removal in a single stage. The absorption mass transfer coefficient was 1.2 (sec)-1, exceeding the initial target of 1.0 (sec)-1. This mass transfer coefficient is over one order of magnitude greater than that of conventional gas/liquid contacting equipment. The economic evaluation based on field tests data indicates that the CO2 capture cost associated with membrane contactor technology is $54.69 (Yr 2011$)/tonne of CO2 captured when using aMDEA as a solvent. It is projected that the DOE’s 2025 cost goal of $40 (Yr 2011$)/tonne of CO2 captured can be met by decreasing membrane module cost and by utilizing advanced CO2 capture solvents. In the second stage of the field test, an advanced solvent, Hitachi’s H3-1 was utilized. The use of H3-1 solvent increased mass transfer coefficient by 17% as compared to aMDEA solvent. The high mass transfer coefficient of H3-1 solvent combined with much more favorable solvent regeneration requirements, indicate that the projected savings achievable with membrane contactor process can be further improved. H3-1 solvent will be used in the next pilot-scale development phase. The integrated absorption/regeneration process design and high performance membrane contactors developed in the current bench-scale program will be used as the base technology for future pilot-scale development.« less

Geological Sequestration of CO2 A Brief Overview and Potential for Application for Oklahoma

EPA Science Inventory

Geologic sequestration of CO2 is a component of C capture and storage (CCS), an emerging technology for reducing CO2 emissions to the atmosphere, and involves injection of captured CO2 into deep subsurface formations. Similar to the injection of hazardous wastes, before injection...

Direct membrane-carbonation photobioreactor producing photoautotrophic biomass via carbon dioxide transfer and nutrient removal.

PubMed

Kim, Hyun-Woo; Cheng, Jing; Rittmann, Bruce E

2016-03-01

An advanced-material photobioreactor, the direct membrane-carbonation photobioreactor (DMCPBR), was tested to investigate the impact of directly submerging a membrane carbonation (MC) module of hollow-fiber membranes inside the photobioreactor. Results demonstrate that the DMCPBR utilized over 90% of the supplied CO2 by matching the CO2 flux to the C demand of photoautotrophic biomass growth. The surface area of the submerged MC module was the key to control CO2 delivery and biomass productivity. Tracking the fate of supplied CO2 explained how the DMCPBR reduced loss of gaseous CO2 while matching the inorganic carbon (IC) demand to its supply. Accurate fate analysis required that the biomass-associated C include soluble microbial products as a sink for captured CO2. With the CO2 supply matched to the photosynthetic demand, light attenuation limited the rate microalgal photosynthesis. The DMCPBR presents an opportunity to improve CO2-deliver efficiency and make microalgae a more effective strategy for C-neutral resource recovery. Copyright © 2015 Elsevier Ltd. All rights reserved.

High-performance multilayer composite membranes with mussel-inspired polydopamine as a versatile molecular bridge for CO2 separation.

PubMed

Li, Panyuan; Wang, Zhi; Li, Wen; Liu, Yanni; Wang, Jixiao; Wang, Shichang

2015-07-22

It is desirable to develop high-performance composite membranes for efficient CO2 separation in CO2 capture process. Introduction of a highly permeable polydimethylsiloxane (PDMS) intermediate layer between a selective layer and a porous support has been considered as a simple but efficient way to enhance gas permeance while maintaining high gas selectivity, because the introduced intermediate layer could benefit the formation of an ultrathin defect-free selective layer owing to the circumvention of pore penetration phenomenon. However, the selection of selective layer materials is unfavorably restricted because of the low surface energy of PDMS. Various highly hydrophilic membrane materials such as amino group-rich polyvinylamine (PVAm), a representative facilitated transport membrane material for CO2 separation, could not be facilely coated over the surface of the hydrophobic PDMS intermediate layer uniformly. Inspired by the hydrophilic nature and strong adhesive ability of polydopamine (PDA), PDA was therefore selected as a versatile molecular bridge between hydrophobic PDMS and hydrophilic PVAm. The PDA coating endows a highly compatible interface between both components with a large surface energy difference via multiple-site cooperative interactions. The resulting multilayer composite membrane with a thin facilitated transport PVAm selective layer exhibits a notably enhanced CO2 permeance (1887 GPU) combined with a slightly improved CO2/N2 selectivity (83), as well as superior structural stability. Similarly, the multilayer composite membrane with a hydrophilic CO2-philic Pebax 1657 selective layer was also developed for enhanced CO2 separation performance.

Carbon Management in the Electric Power Industry

NASA Astrophysics Data System (ADS)

Stringer, John

2002-03-01

Approximately 53States in 2000 came from the combustion of coal in Rankine cycle plant; 16principally in Brayton cycle or combined cycle units. Electricity generation is responsible for 36amthropogenic CO2. This compares with 32transportation sector, but since the electric utility generators are large fixed sources it is likely that any legislation designed to reduce CO2 production will adress the utility generators first. Over the last 100 years there has been a continuous decrease in the carbon fraction of the fuels used for energy production world wide, and it is expected that this will continue, principally as a result of the increasing fraction of natural gas. It appears probable that the retirement of the existing nuclear fleet will be delayed by relicensing, and it seems more possible that new nuclear plant will be built than seemed likely even a couple of years ago. The impact of renewables should be increasing, but currently only about 2way currently, and without some considerable incentives, the rate of increase in this component over the next twenty years will probably be small. Currently, hydroelectric plants account for 7indication that this will increase appreciably. At the moment, a significant change would appear to require the capture of CO2 from the exhaust of the combustion plants, and particularly the large existing fleet of coal-fired Rankine units. Following the capture, the CO2 must then be sequestered in secure long-term locations. In addition, increases in the efficiency of power generation, and increases in the efficiency of end use leading to reductions in the energy intensity of the Gross Domestic Product, will be necessary. This paper will review the current state of art in these various approaches to the problem.

Pre-Combustion Carbon Dioxide Capture by a New Dual Phase Ceramic-Carbonate Membrane Reactor

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lin, Jerry Y. S.

2015-01-31

This report documents synthesis, characterization and carbon dioxide permeation and separation properties of a new group of ceramic-carbonate dual-phase membranes and results of a laboratory study on their application for water gas shift reaction with carbon dioxide separation. A series of ceramic-carbonate dual phase membranes with various oxygen ionic or mixed ionic and electronic conducting metal oxide materials in disk, tube, symmetric, and asymmetric geometric configurations was developed. These membranes, with the thickness of 10 μm to 1.5 mm, show CO 2 permeance in the range of 0.5-5×10 -7 mol·m -2·s -1·Pa -1 in 500-900°C and measured CO 2/N 2more » selectivity of up to 3000. CO 2 permeation mechanism and factors that affect CO 2 permeation through the dual-phase membranes have been identified. A reliable CO 2 permeation model was developed. A robust method was established for the optimization of the microstructures of ceramic-carbonate membranes. The ceramic-carbonate membranes exhibit high stability for high temperature CO 2 separations and water gas shift reaction. Water gas shift reaction in the dual-phase membrane reactors was studied by both modeling and experiments. It is found that high temperature syngas water gas shift reaction in tubular ceramic-carbonate dual phase membrane reactor is feasible even without catalyst. The membrane reactor exhibits good CO 2 permeation flux, high thermal and chemical stability and high thermal shock resistance. Reaction and separation conditions in the membrane reactor to produce hydrogen of 93% purity and CO 2 stream of >95% purity, with 90% CO 2 capture have been identified. Integration of the ceramic-carbonate dual-phase membrane reactor with IGCC process for carbon dioxide capture was analyzed. A methodology was developed to identify optimum operation conditions for a membrane tube of given dimensions that would treat coal syngas with targeted performance. The calculation results show that the dual-phase membrane reactor could improve IGCC process efficiency but the cost of the membrane reactor with membranes having current CO 2 permeance is high. Further research should be directed towards improving the performance of the membranes and developing cost-effective, scalable methods for fabrication of dual-phase membranes and membrane reactors.« less

Efficient Removal of Cationic and Anionic Radioactive Pollutants from Water Using Hydrotalcite-Based Getters.

PubMed

Bo, Arixin; Sarina, Sarina; Liu, Hongwei; Zheng, Zhanfeng; Xiao, Qi; Gu, Yuantong; Ayoko, Godwin A; Zhu, Huaiyong

2016-06-29

Hydrotalcite (HT)-based materials are usually applied to capture anionic pollutants in aqueous solutions. Generally considered anion exchangers, their ability to capture radioactive cations is rarely exploited. In the present work, we explored the ability of pristine and calcined HT getters to effectively capture radioactive cations (Sr(2+) and Ba(2+)) which can be securely stabilized at the getter surface. It is found that calcined HT outperforms its pristine counterpart in cation removal ability. Meanwhile, a novel anion removal mechanism targeting radioactive I(-) is demonstrated. This approach involves HT surface modification with silver species, namely, Ag2CO3 nanoparticles, which can attach firmly on HT surface by forming coherent interface. This HT-based anion getter can be further used to capture I(-) in aqueous solution. The observed I(-) uptake mechanism is distinctly different from the widely reported ion exchange mechanism of HT and much more efficient. As a result of the high local concentrations of precipitants on the getters, radioactive ions in water can be readily immobilized onto the getter surface by forming precipitates. The secured ionic pollutants can be subsequently removed from water by filtration or sedimentation for safe disposal. Overall, these stable, inexpensive getters are the materials of choice for removal of trace ionic pollutants from bulk radioactive liquids, especially during episodic environmental crisis.

Thermodynamic Properties of CO{sub 2} Capture Reaction by Solid Sorbents: Theoretical Predictions and Experimental Validations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Duan, Yuhua; Luebke, David; Pennline, Henry

2012-01-01

It is generally accepted that current technologies for capturing CO{sub 2} are still too energy intensive. Hence, there is a critical need for development of new materials that can capture CO{sub 2} reversibly with acceptable energy costs. Accordingly, solid sorbents have been proposed to be used for CO{sub 2} capture applications through a reversible chemical transformation. By combining thermodynamic database mining with first principles density functional theory and phonon lattice dynamics calculations, a theoretical screening methodology to identify the most promising CO{sub 2} sorbent candidates from the vast array of possible solid materials has been proposed and validated. The calculatedmore » thermodynamic properties of different classes of solid materials versus temperature and pressure changes were further used to evaluate the equilibrium properties for the CO{sub 2} adsorption/desorption cycles. According to the requirements imposed by the pre- and post- combustion technologies and based on our calculated thermodynamic properties for the CO{sub 2} capture reactions by the solids of interest, we were able to screen only those solid materials for which lower capture energy costs are expected at the desired pressure and temperature conditions. These CO{sub 2} sorbent candidates were further considered for experimental validations. In this presentation, we first introduce our screening methodology with validating by solid dataset of alkali and alkaline metal oxides, hydroxides and bicarbonates which thermodynamic properties are available. Then, by studying a series of lithium silicates, we found that by increasing the Li{sub 2}O/SiO{sub 2} ratio in the lithium silicates their corresponding turnover temperatures for CO{sub 2} capture reactions can be increased. Compared to anhydrous K{sub 2}CO{sub 3}, the dehydrated K{sub 2}CO{sub 3}1.5H{sub 2}O can only be applied for post-combustion CO{sub 2} capture technology at temperatures lower than its phase transition (to anhydrous phase) temperature, which depends on the CO{sub 2} pressure and the steam pressure with the best range being PH{sub 2}O≤1.0 bar. Above the phase-transition temperature, the sorbent will be regenerated into anhydrous K{sub 2}CO{sub 3}. Our theoretical investigations on Na-promoted MgO sorbents revealed that the sorption process takes place through formation of the Na{sub 2}Mg(CO{sub 3}){sub 2} double carbonate with better reaction kinetics over porous MgO, that of pure MgO sorbent. The experimental sorption tests also indicated that the Na-promoted MgO sorbent has high reactivity and capacity towards CO{sub 2} sorption and can be easily regenerated either through pressure or temperature swing processes.« less

Diurnal activity of four species of thrips (Thysanoptera: Thripidae) and efficiencies of three nondestructive sampling techniques for thrips in mango inflorescences.

PubMed

Aliakbarpour, H; Rawi, Che Salmah Md

2010-06-01

Thrips cause considerable economic loss to mango, Mangifera indica L., in Penang, Malaysia. Three nondestructive sampling techniques--shaking mango panicles over a moist plastic tray, washing the panicles with ethanol, and immobilization of thrips by using CO2--were evaluated for their precision to determine the most effective technique to capture mango flower thrips (Thysanoptera: Thripidae) in an orchard located at Balik Pulau, Penang, Malaysia, during two flowering seasons from December 2008 to February 2009 and from August to September 2009. The efficiency of each of the three sampling techniques was compared with absolute population counts on whole panicles as a reference. Diurnal flight activity of thrips species was assessed using yellow sticky traps. All three sampling methods and sticky traps were used at two hourly intervals from 0800 to 1800 hours to get insight into diurnal periodicity of thrips abundance in the orchard. Based on pooled data for the two seasons, the CO2 method was the most efficient procedure extracting 80.7% adults and 74.5% larvae. The CO2 method had the lowest relative variation and was the most accurate procedure compared with the absolute method as shown by regression analysis. All collection techniques showed that the numbers of all thrips species in mango panicles increased after 0800 hours, reaching a peak between 1200 and 1400 hours. Adults thrips captured on the sticky traps were the most abundant between 0800-1000 and 1400-1600 hours. According to results of this study, the CO2 method is recommended for sampling of thrips in the field. It is a nondestructive sampling procedure that neither damages flowers nor diminishes fruit production. Management of thrips populations in mango orchards with insecticides would be more effectively carried out during their peak population abundance on the flower panicles at midday to 1400 hours.

Preliminary Modelling of the Effect of Impurity in CO2 Streams on the Storage Capacity and the Plume Migration in Pohang Basin, Korea

NASA Astrophysics Data System (ADS)

Park, Yongchan; Choi, Byoungyoung; Shinn, Youngjae

2015-04-01

Captured CO2 streams contain various levels of impurities which vary depending on the combustion technology and CO2 sources such as a power plant and iron and steel production processes. Common impurities or contaminants are non-condensable gases like nitrogen, oxygen and hydrogen, and are also air pollutants like sulphur and nitrogen oxides. Specifically for geological storage, the non-condensable gases in CO2 streams are not favourable because they can decrease density of the injected CO2 stream and can affect buoyancy of the plume. However, separation of these impurities to obtain the CO2 purity higher than 99% would greatly increase the cost of capture. In 2010, the Korean Government announced a national framework to develop CCS, with the aim of developing two large scale integrated CCS projects by 2020. In order to achieve this goal, a small scale injection project into Pohang basin near shoreline has begun which is seeking the connection with a capture project, especially at a steel company. Any onshore sites that are suitable for the geological storage are not identified by this time so we turned to the shallow offshore Pohang basin where is close to a large-scale CO2 source. Currently, detailed site surveys are being undertaken and the collected data were used to establish a geological model of the basin. In this study, we performed preliminary modelling study on the effect of impurities on the geological storage using the geological model. Using a potential compositions of impurities in CO2 streams from the steel company, we firstly calculated density and viscosity of CO2 streams as a function of various pressure and temperature conditions with CMG-WINPROP and then investigated the effect of the non-condensable gases on storage capacity, injectivity and plume migrations with CMG-GEM. Further simulations to evaluate the areal and vertical sweep efficiencies by impurities were perform in a 2D vertical cross section as well as in a 3D simulation grid. Also, pressure increases caused by the impurities and the partitioning between CO2 and other non-condensable gases were explored. In addition, the possibility of using these contaminants as a tracer were examined.

Porous Metal Organic Polyhedral Framework Containing Cuboctahedron Cages as SBUs with High Affinity for H2 and CO2 Sorptions: A Heterogeneous Catalyst for Chemical Fixation of CO2.

PubMed

Biradha, Kumar; Maity, Kartik; Karan, Chandan Kumar

2018-06-11

Development of active porous materials that can efficiently adsorb H2 and CO2 are in need due to their practical utilities. Here we present the design and synthesis of an interpenetrated Cu(II)-MOF that is thermally stable, highly porous and can act as a heterogeneous catalyst. The Cu(II)-MOF contains highly symmetric polyhedral metal cluster (Cu24) with cuboctahedron geometry as SBU. The double interpenetration of such huge cluster containing nets provides high density of open metal sites due to which it exhibits remarkable H2 storage capacity (313 cm3g-1 at 1bar and 77K) as well as high CO2 capture ability (159 cm3g-1 at 1bar and 273K). Further, its propensity towards the CO2 sorption utilized for the heterogeneous catalysis of chemical conversion of CO2 into the corresponding cyclic carbonates upon reaction with epoxides with high TON and TOF values. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Carbon Dioxide Extraction from the Atmosphere Through Engineered Chemical Sinkage: Enabling Energy and Environmental Security

NASA Astrophysics Data System (ADS)

Dubey, M. K.; Ziock, H.; Rueff, G.; Smith, W. S.; Colman, J.; Elliott, S.; Lackner, K.; Johnston, N. A.

2002-05-01

We present the case for carbon dioxide (CO2) extraction from air using engineered chemical sinks as a means of sustaining fossil energy use by avoiding climate change. Existing carbon sequestration strategies such as CO2 injection into geologic formations or the deep ocean and mineral carbonation, require a pure stream of concentrated CO2 to be viable. Furthermore, current emphasis on reducing the global CO2 emissions is on large centralized power plants. However, more than half of all emissions are from the transportation sector and small, distributed sources such as home heating, etc. Most solutions for dealing with these sources explicitly or implicitly entail completely overhauling the existing infrastructure. To solve these problems, Los Alamos National Laboratory has conceived a novel approach for directly extracting CO2 from the atmosphere. Direct extraction converts the dilute CO2 (370 parts per million) in the atmosphere into a pure CO2 stream ready for permanent sequestration. It provides the following advantages: (1) Preserves our existing energy use and fuel distribution systems, which represent a large investment, (2) Indirectly captures CO2 from the myriad of small, distributed, and mobile sources that otherwise are not accessible to sequestration, (3) Allows atmospheric CO2 levels to be restored to their pre-industrial age value, (4) Provides free transport of CO2 to suitable sequestration sites by using natural atmospheric circulation, and (5) Is relatively compact and therefore inexpensive when compared to renewable concepts. Our concept harnesses atmospheric circulation to transport CO2 to sites where the CO2 is extracted by binding it to an adsorbent. The bound CO2 is then recovered as pure gas by heating together with the solid adsorbent that is recycled. As a proof of concept, we show that an aqueous Ca(OH)2 solution efficiently converts CO2 to a CaCO3 solid that can be heated to obtain pure CO2 and recover the CaO. Even with recycling costs, CO2 extraction from air blown by wind through a 1 m2 aperture could eliminate the greenhouse gas impact of a 100 kW gasoline engine, making it more favorable than renewable sources such as solar, wind, or bio-mass. We report economic and scaling arguments, atmospheric simulations and laboratory experiments on candidate adsorbents that support pursuing air-extraction as an advanced CO2 capture technology. We assess and guide synthetic advances in tailoring zeolites, amines, carbon, and ionic fluids to adsorb CO2 selectively, rapidly, and gently enough to facilitate recovery, that promise to significantly enhance the efficiency of CO2 air extraction. This method could process today's world output of CO2 at costs of about 5 cents/liter of gasoline, a manageable scale for this massive undertaking.

Evaluation of the impact of H2O, O2, and SO2 on postcombustion CO2 capture in metal-organic frameworks.

PubMed

Yu, Jiamei; Ma, Yuguang; Balbuena, Perla B

2012-05-29

Molecular modeling methods are used to estimate the influence of impurity species: water, O(2), and SO(2) in flue gas mixtures present in postcombustion CO(2) capture using a metal organic framework, HKUST-1, as a model sorbent material. Coordinated and uncoordinated water effects on CO(2) capture are analyzed. Increase of CO(2) adsorption is observed for both cases, which can be attributed to the enhanced binding energy between CO(2) and HKUST-1 due to the introduction of a small amount of water. Density functional theory calculations indicate that the binding energy between CO(2) and HKUST-1 with coordinated water is ~1 kcal/mol higher than that without coordinated water. It is found that the improvement of CO(2)/N(2) selectivity induced by coordinated water may mainly be attributed to the increased CO(2) adsorption on the hydrated HKUST-1. On the other hand, the enhanced selectivity induced by uncoordinated water in the flue gas mixture can be explained on the basis of the competition of adsorption sites between water and CO(2) (N(2)). At low pressures, a significant CO(2)/N(2) selectivity increase is due to the increase of CO(2) adsorption and decrease of N(2) adsorption as a consequence of competition of adsorption sites between water and N(2). However, with more water molecules adsorbed at higher pressures, the competition between water and CO(2) leads to the decrease of CO(2) adsorption capacity. Therefore, high pressure operation should be avoided in HKUST-1 sorbents for CO(2) capture. In addition, the effects of O(2) and SO(2) on CO(2) capture in HKUST-1 are investigated: The CO(2)/N(2) selectivity does not change much even with relatively high concentrations of O(2) in the flue gas (up to 8%). A slightly lower CO(2)/N(2) selectivity of a CO(2)/N(2)/H(2)O/SO(2) mixture is observed compared with that in a CO(2)/N(2)/H(2)O mixture, especially at high pressures, due to the strong SO(2) binding with HKUST-1.

Simulation and experiment for oxygen-enriched combustion engine using liquid oxygen to solidify CO2

NASA Astrophysics Data System (ADS)

Liu, Yongfeng; Jia, Xiaoshe; Pei, Pucheng; Lu, Yong; Yi, Li; Shi, Yan

2016-01-01

For capturing and recycling of CO2 in the internal combustion engine, Rankle cycle engine can reduce the exhaust pollutants effectively under the condition of ensuring the engine thermal efficiency by using the techniques of spraying water in the cylinder and optimizing the ignition advance angle. However, due to the water spray nozzle need to be installed on the cylinder, which increases the cylinder head design difficulty and makes the combustion conditions become more complicated. In this paper, a new method is presented to carry out the closing inlet and exhaust system for internal combustion engines. The proposed new method uses liquid oxygen to solidify part of cooled CO2 from exhaust system into dry ice and the liquid oxygen turns into gas oxygen which is sent to inlet system. The other part of CO2 is sent to inlet system and mixed with oxygen, which can reduce the oxygen-enriched combustion detonation tendency and make combustion stable. Computing grid of the IP52FMI single-cylinder four-stroke gasoline-engine is established according to the actual shape of the combustion chamber using KIVA-3V program. The effects of exhaust gas recirculation (EGR) rate are analyzed on the temperatures, the pressures and the instantaneous heat release rates when the EGR rate is more than 8%. The possibility of enclosing intake and exhaust system for engine is verified. The carbon dioxide trapping device is designed and the IP52FMI engine is transformed and the CO2 capture experiment is carried out. The experimental results show that when the EGR rate is 36% for the optimum EGR rate. When the liquid oxygen of 35.80-437.40 g is imported into the device and last 1-20 min, respectively, 21.50-701.30 g dry ice is obtained. This research proposes a new design method which can capture CO2 for vehicular internal combustion engine.

CO2 capture from humid flue gases and humid atmosphere using a microporous coppersilicate.

PubMed

Datta, Shuvo Jit; Khumnoon, Chutharat; Lee, Zhen Hao; Moon, Won Kyung; Docao, Son; Nguyen, Thanh Huu; Hwang, In Chul; Moon, Dohyun; Oleynikov, Peter; Terasaki, Osamu; Yoon, Kyung Byung

2015-10-16

Capturing CO2 from humid flue gases and atmosphere with porous materials remains costly because prior dehydration of the gases is required. A large number of microporous materials with physical adsorption capacity have been developed as CO2-capturing materials. However, most of them suffer from CO2 sorption capacity reduction or structure decomposition that is caused by co-adsorbed H2O when exposed to humid flue gases and atmosphere. We report a highly stable microporous coppersilicate. It has H2O-specific and CO2-specific adsorption sites but does not have H2O/CO2-sharing sites. Therefore, it readily adsorbs both H2O and CO2 from the humid flue gases and atmosphere, but the adsorbing H2O does not interfere with the adsorption of CO2. It is also highly stable after adsorption of H2O and CO2 because it was synthesized hydrothermally. Copyright © 2015, American Association for the Advancement of Science.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Alptekin, Gokhan

The overall objective of the proposed research is to develop a low cost, high capacity CO{sub 2} sorbent and demonstrate its technical and economic viability for pre-combustion CO{sub 2} capture. The specific objectives supporting our research plan were to optimize the chemical structure and physical properties of the sorbent, scale-up its production using high throughput manufacturing equipment and bulk raw materials and then evaluate its performance, first in bench-scale experiments and then in slipstream tests using actual coal-derived synthesis gas. One of the objectives of the laboratory-scale evaluations was to demonstrate the life and durability of the sorbent for overmore » 10,000 cycles and to assess the impact of contaminants (such as sulfur) on its performance. In the field tests, our objective was to demonstrate the operation of the sorbent using actual coal-derived synthesis gas streams generated by air-blown and oxygen-blown commercial and pilot-scale coal gasifiers (the CO{sub 2} partial pressure in these gas streams is significantly different, which directly impacts the operating conditions hence the performance of the sorbent). To support the field demonstration work, TDA collaborated with Phillips 66 and Southern Company to carry out two separate field tests using actual coal-derived synthesis gas at the Wabash River IGCC Power Plant in Terre Haute, IN and the National Carbon Capture Center (NCCC) in Wilsonville, AL. In collaboration with the University of California, Irvine (UCI), a detailed engineering and economic analysis for the new CO{sub 2} capture system was also proposed to be carried out using Aspen PlusTM simulation software, and estimate its effect on the plant efficiency.« less

SO 2-Resistant Immobilized Amine Sorbents for CO 2 Capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tumuluri, Uma

2014-01-01

The solid amine sorbent for CO 2 capture process has advantages of simplicity and low operating cost compared to the MEA (monoethanolamine) process. Solid amine sorbents reported so far suffered from either low CO 2 capture capacity or low stability in the flue gas environment. This project is aimed at developing a SO 2-resistant solid amine sorbent for capturing CO 2 from coal–fired power plants with SCR/FGD which emits SO 2ranging from 15 to 30 ppm and NO ranging from 5 to 10 ppm. The amine sorbent we developed in a previous project degraded rapidly with 65% decrease in themore » initial capture capacity in presence of 1% SO 2. This amine sorbent was further modified by coating with polyethyleneglycol (PEG) to increase the SO 2-resistance. Polyethylene glycol (PEG) was found to decrease the SO 2-amine interaction, resulting in the decrease in the maximum SO desorption temperature (Tmax ) of amine sorbent. The PEG-coated amine sorbent exhibited higher stability with only 40% decrease in the initial capture capacity compared to un-coated amine sorbents. The cost of the solid amine sorbent developed in this project is estimated to be less than $7.00/lb; the sorbent exhibited CO 2 capture capacity more than 2.3 mmol/g. The results of this study provided the scientific basis for further development of SO 2-resistant sorbents.« less

Long-term energy and climate implications of carbon capture and storage deployment strategies in the US coal-fired electricity fleet.

PubMed

Sathre, Roger; Masanet, Eric

2012-09-04

To understand the long-term energy and climate implications of different implementation strategies for carbon capture and storage (CCS) in the US coal-fired electricity fleet, we integrate three analytical elements: scenario projection of energy supply systems, temporally explicit life cycle modeling, and time-dependent calculation of radiative forcing. Assuming continued large-scale use of coal for electricity generation, we find that aggressive implementation of CCS could reduce cumulative greenhouse gas emissions (CO(2), CH(4), and N(2)O) from the US coal-fired power fleet through 2100 by 37-58%. Cumulative radiative forcing through 2100 would be reduced by only 24-46%, due to the front-loaded time profile of the emissions and the long atmospheric residence time of CO(2). The efficiency of energy conversion and carbon capture technologies strongly affects the amount of primary energy used but has little effect on greenhouse gas emissions or radiative forcing. Delaying implementation of CCS deployment significantly increases long-term radiative forcing. This study highlights the time-dynamic nature of potential climate benefits and energy costs of different CCS deployment pathways and identifies opportunities and constraints of successful CCS implementation.

Modification of photosynthesis and growth responses to elevated CO2 by ozone in two cultivars of winter wheat with different years of release

PubMed Central

Jiang, G.M.

2013-01-01

The beneficial effects of elevated CO2 on plants are expected to be compromised by the negative effects posed by other global changes. However, little is known about ozone (O3)-induced modulation of elevated CO2 response in plants with differential sensitivity to O3. An old (Triticum aestivum cv. Beijing 6, O3 tolerant) and a modern (T. aestivum cv. Zhongmai 9, O3 sensitive) winter wheat cultivar were exposed to elevated CO2 (714 ppm) and/or O3 (72 ppb, for 7h d–1) in open-topped chambers for 21 d. Plant responses to treatments were assessed by visible leaf symptoms, simultaneous measurements of gas exchange and chlorophyll a fluorescence, in vivo biochemical properties, and growth. It was found that elevated CO2 resulted in higher growth stimulation in the modern cultivar attributed to a higher energy capture and electron transport rate compared with the old cultivar. Exposure to O3 caused a greater growth reduction in the modern cultivar due to higher O3 uptake and a greater loss of photosystem II efficiency (mature leaf) and mesophyll cell activity (young leaf) than in the old cultivar. Elevated CO2 completely protected both cultivars against the deleterious effects of O3 under elevated CO2 and O3. The modern cultivar showed a greater relative loss of elevated CO2-induced growth stimulation due to higher O3 uptake and greater O3-induced photoinhibition than the old cultivar at elevated CO2 and O3. Our findings suggest that the elevated CO2-induced growth stimulation in the modern cultivar attributed to higher energy capture and electron transport rate can be compromised by its higher O3 uptake and greater O3-induced photoinhibition under elevated CO2 and O3 exposure. PMID:23378379

Modeling and optimal design of CO2 Direct Air Capture systems in large arrays

NASA Astrophysics Data System (ADS)

Sadri Irani, Samaneh; Luzzatto-Fegiz, Paolo

2017-11-01

As noted by the 2014 IPCC report, while the rise in atmospheric CO2 would be slowed by emissions reductions, removing atmospheric CO2 is an important part of possible paths to climate stabilization. Direct Air Capture of CO2 with chemicals (DAC) is one of several proposed carbon capture technologies. There is an ongoing debate on whether DAC is an economically viable approach to alleviate climate change. In addition, like all air capture strategies, DAC is strongly constrained by the net-carbon problem, namely the need to control CO2 emissions associated with the capture process (for example, if DAC not powered by renewables). Research to date has focused on the chemistry and economics of individual DAC devices. However, the fluid mechanics of their large-scale deployment has not been examined in the literature, to the best of our knowledge. In this presentation, we develop a model for flow through an array of DAC devices, varying their lateral extent and their separation. We build on a recent theory of canopy flows, introducing terms for CO2 entrainment into the array boundary layer, and transport into the farm. In addition, we examine the possibility of driving flow passively by wind, thereby reducing energy consumption. The optimal operational design is established considering the total cost, drag force, energy consumption and total CO2 capture.

Assessment of Energy Efficiency Improvement and CO2 Emission Reduction Potentials in India's Cement Industry

DOE Office of Scientific and Technical Information (OSTI.GOV)

Morrow, III, William R.; Hasanbeigi, Ali; Xu, Tengfang

2012-12-03

India’s cement industry is the second largest in the world behind China with annual cement production of 168 Mt in 2010 which accounted for slightly greater than six percent of the world’s annual cement production in the same year. To produce that amount of cement, the industry consumed roughly 700 PJ of fuel and 14.7 TWh of electricity. We identified and analyzed 22 energy efficiency technologies and measures applicable to the processes in the Indian cement industry. The Conservation Supply Curve (CSC) used in this study is an analytical tool that captures both the engineering and the economic perspectives ofmore » energy conservation. Using a bottom-up electricity CSC model and compared to an electricity price forecast the cumulative cost-effective plant-level electricity savings potential for the Indian cement industry for 2010- 2030 is estimated to be 83 TWh, and the cumulative plant-level technical electricity saving potential is 89 TWh during the same period. The grid-level CO2 emissions reduction associated with cost-effective electricity savings is 82 Mt CO2 and the electric grid-level CO2 emission reduction associated with technical electricity saving potential is 88 Mt CO2. Compared to a fuel price forecast, an estimated cumulative cost-effective fuel savings potential of 1,029 PJ with associated CO2 emission reduction of 97 Mt CO2 during 2010-2030 is possible. In addition, a sensitivity analysis with respect to the discount rate used is conducted to assess the effect of changes in this parameter on the results. The result of this study gives a comprehensive and easy to understand perspective to the Indian cement industry and policy makers about the energy efficiency potential and its associated cost over the next twenty years.« less

Relationship between mosquito (Diptera: Culicidae) landing rates on a human subject and numbers captured using CO2-baited light traps.

PubMed

Barnard, D R; Knue, G J; Dickerson, C Z; Bernier, U R; Kline, D L

2011-06-01

Capture rates of insectary-reared female Aedes albopictus (Skuse), Anopheles quadrimaculatus Say, Culex nigripalpus Theobald, Culex quinquefasciatus Say and Aedes triseriatus (Say) in CDC-type light traps (LT) supplemented with CO2 and using the human landing (HL) collection method were observed in matched-pair experiments in outdoor screened enclosures. Mosquito responses were compared on a catch-per-unit-effort basis using regression analysis with LT and HL as the dependent and independent variables, respectively. The average number of mosquitoes captured in 1 min by LT over a 24-h period was significantly related to the average number captured in 1 min by HL only for Cx. nigripalpus and Cx. quinquefasciatus. Patterns of diel activity indicated by a comparison of the mean response to LT and HL at eight different times in a 24-h period were not superposable for any species. The capture rate efficiency of LT when compared with HL was ≤15% for all mosquitoes except Cx. quinquefasciatus (43%). Statistical models of the relationship between mosquito responses to each collection method indicate that, except for Ae. albopictus, LT and HL capture rates are significantly related only during certain times of the diel period. Estimates of mosquito activity based on observations made between sunset and sunrise were most precise in this regard for An. quadrimaculatus and Cx. nigripalpus, as were those between sunrise and sunset for Cx. quinquefasciatus and Ae. triseriatus.

Extraction of Mg(OH)2 from Mg silicate minerals with NaOH assisted with H2O: implications for CO2 capture from exhaust flue gas.

PubMed

Madeddu, Silvia; Priestnall, Michael; Godoy, Erik; Kumar, R Vasant; Raymahasay, Sugat; Evans, Michael; Wang, Ruofan; Manenye, Seabelo; Kinoshita, Hajime

2015-01-01

The utilisation of Mg(OH)2 to capture exhaust CO2 has been hindered by the limited availability of brucite, the Mg(OH)2 mineral in natural deposits. Our previous study demonstrated that Mg(OH)2 can be obtained from dunite, an ultramafic rock composed of Mg silicate minerals, in highly concentrated NaOH aqueous systems. However, the large quantity of NaOH consumed was considered an obstacle for the implementation of the technology. In the present study, Mg(OH)2 was extracted from dunite reacted in solid systems with NaOH assisted with H2O. The consumption of NaOH was reduced by 97% with respect to the NaOH aqueous systems, maintaining a comparable yield of Mg(OH)2 extraction, i.e. 64.8-66%. The capture of CO2 from a CO2-N2 gas mixture was tested at ambient conditions using a Mg(OH)2 aqueous slurry. Mg(OH)2 almost fully dissolved and reacted with dissolved CO2 by forming Mg(HCO3)2 which remained in equilibrium storing the CO2 in the aqueous solution. The CO2 balance of the process was assessed from the emissions derived from the power consumption for NaOH production and Mg(OH)2 extraction together with the CO2 captured by Mg(OH)2 derived from dunite. The process resulted as carbon neutral when dunite is reacted at 250 °C for durations of 1 and 3 hours and CO2 is captured as Mg(HCO3)2.

The Inherent Tracer Fingerprint of Captured CO2

NASA Astrophysics Data System (ADS)

Flude, Stephanie; Gyore, Domokos; Stuart, Finlay; Boyce, Adrian; Haszeldine, Stuart; Chalaturnyk, Rick; Gilfillan, Stuart

2017-04-01

Inherent tracers, the isotopic and trace gas composition of captured CO2 streams, are potentially powerful tracers for use in CCS technology [1,2]. Despite this potential, the inherent tracer fingerprint in captured CO2 streams has yet to be robustly investigated and documented [3]. Here, we will present the first high quality systematic measurements of the carbon and oxygen isotopic and noble gas fingerprints measured in anthropogenic CO2 captured from combustion power stations and fertiliser plants, using amine capture, oxyfuel and gasification processes, and derived from coal, biomass and natural gas feedstocks. We will show that δ13C values are mostly controlled by the feedstock composition, as expected. The majority of the CO2 samples exhibit δ18O values similar to atmospheric O2 although captured CO2 samples from biomass and gas feedstocks at one location in the UK are significantly higher. Our measured noble gas concentrations in captured CO2 are generally as expected [2], typically being two orders of magnitude lower in concentration than in atmospheric air. Relative noble gas elemental abundances are variable and often show an opposite trend to that of a water in contact with the atmosphere. Expected enrichments in radiogenic noble gases (4He and 40Ar) for fossil fuel derived CO2 were not always observed due to dilution with atmospheric noble gases during the CO2 generation and capture process. Many noble gas isotope ratios indicate that isotopic fractionation takes place during the CO2 generation and capture processes, resulting in isotope ratios similar to fractionated air. We conclude that phase changes associated with CO2 transport and sampling may induce noble gas elemental and isotopic fractionation, due to different noble gas solubilities between high (liquid or supercritical) and low (gaseous) density CO2. Data from the Australian CO2CRC Otway test site show that δ13C of CO2 will change once injected into the storage reservoir, but that this change is small and can be quantitatively modelled in order to determine the proportion of CO2 that has dissolved into the formation waters. Furthermore, noble gas data from the Otway storage reservoir post-injection, shows evidence of noble gas stripping of formation water and contamination with Kr and Xe related to an earlier injection experiment. Importantly, He data from SaskPower's Aquistore illustrates that injected CO2 will inherit distinctive crustal radiogenic noble gas fingerprints from the subsurface once injected into an undisturbed geological storage reservoir, meaning this could be used to identify unplanned migration of the CO2 to the surface and shallow subsurface [4]. References [1] Mayer et al., (2015) IJGGC, Vol. 37, 46-60 http://dx.doi.org/10.1016/j.ijggc.2015.02.021 [2] Gilfillan et al., (2014) Energy Procedia, Vol. 63, 4123-4133 http://dx.doi.org/10.1016/j.egypro.2014.11.443 [3] Flude et al., (2016) Environ. Sci. Technol., 50 (15), pp 7939-7955 DOI: 10.1021/acs.est.6b01548 [4] Gilfillan et al., (2011) IJGGC, Vol. 5 (6) 1507-1516 http://dx.doi.org/10.1016/j.ijggc.2011.08.008

Moisture-Stable Zn(II) Metal-Organic Framework as a Multifunctional Platform for Highly Efficient CO2 Capture and Nitro Pollutant Vapor Detection.

PubMed

Chen, Di-Ming; Tian, Jia-Yue; Chen, Min; Liu, Chun-Sen; Du, Miao

2016-07-20

A moisture-stable three-dimensional (3D) metal-organic framework (MOF), {(Me2NH2)[Zn2(bpydb)2(ATZ)](DMA)(NMF)2}n (1, where bpydb = 4,4'-(4,4'-bipyridine-2,6-diyl)dibenzoate, ATZ = deprotonated 5-aminotetrazole, DMA = N,N-dimethylacetamide, and NMF = N-methylformamide), with uncoordinated N-donor sites and charged framework skeleton was fabricated. This MOF exhibits interesting structural dynamic upon CO2 sorption at 195 K and high CO2/N2 (127) and CO2/CH4 (131) sorption selectivity at 298 K and 1 bar. Particularly, its CO2/CH4 selectivity is among the highest MOFs for selective CO2 separation. The results of Grand Canonical Monte Carlo (GCMC) simulation indicate that the polar framework contributes to the strong framework-CO2 binding at zero loading, and the tetrazole pillar contributes to the high CO2 uptake capacity at high loading. Furthermore, the solvent-responsive luminescent properties of 1 indicate that it could be utilized as a fluorescent sensor to detect trace amounts of nitrobenzene in both solvent and vapor systems.

Engineered yeast for enhanced CO2 mineralization†

PubMed Central

Barbero, Roberto; Carnelli, Lino; Simon, Anna; Kao, Albert; Monforte, Alessandra d’Arminio; Riccò, Moreno; Bianchi, Daniele; Belcher, Angela

2014-01-01

In this work, a biologically catalyzed CO2 mineralization process for the capture of CO2 from point sources was designed, constructed at a laboratory scale, and, using standard chemical process scale-up protocols, was modeled and evaluated at an industrial scale. A yeast display system in Saccharomyces cerevisae was used to screen several carbonic anhydrase isoforms and mineralization peptides for their impact on CO2 hydration, CaCO3 mineralization, and particle settling rate. Enhanced rates for each of these steps in the CaCO3 mineralization process were confirmed using quantitative techniques in lab-scale measurements. The effect of these enhanced rates on the CO2 capture cost in an industrial scale CO2 mineralization process using coal fly ash as the CaO source was evaluated. The model predicts a process using bCA2- yeast and fly ash is ~10% more cost effective per ton of CO2 captured than a process with no biological molecules, a savings not realized by wild-type yeast and high-temperature stable recombinant CA2 alone or in combination. The levelized cost of electricity for a power plant using this process was calculated and scenarios in which this process compares favorably to CO2 capture by MEA absorption process are presented. PMID:25289021

A review on wetting and water condensation - Perspectives for CO2 condensation.

PubMed

Snustad, Ingrid; Røe, Ingeborg T; Brunsvold, Amy; Ervik, Åsmund; He, Jianying; Zhang, Zhiliang

2018-06-01

Liquefaction of vapor is a necessary, but energy intensive step in several important process industries. This review identifies possible materials and surface structures for promoting dropwise condensation, known to increase efficiency of condensation heat transfer. Research on superhydrophobic and superomniphobic surfaces promoting dropwise condensation constitutes the basis of the review. In extension of this, knowledge is extrapolated to condensation of CO 2 . Global emissions of CO 2 need to be minimized in order to reduce global warming, and liquefaction of CO 2 is a necessary step in some carbon capture, transport and storage (CCS) technologies. The review is divided into three main parts: 1) An overview of recent research on superhydrophobicity and promotion of dropwise condensation of water, 2) An overview of recent research on superomniphobicity and dropwise condensation of low surface tension substances, and 3) Suggested materials and surface structures for dropwise CO 2 condensation based on the two first parts. Copyright © 2018 Elsevier B.V. All rights reserved.

Low-Energy Solvents For Carbon Dioxide Capture Enabled By A Combination Of Enzymes And Vacuum Regeneration

DOE Office of Scientific and Technical Information (OSTI.GOV)

Salmon, Sonja; House, Alan; Liu, Kun

An integrated bench-scale system combining the attributes of the bio-renewable enzyme carbonic anhydrase (CA) with low-enthalpy CO2 absorption solvents and vacuum regeneration was designed, built and operated for 500 hours using simulated flue gas. The objective was to develop a CO2 capture process with improved efficiency and sustainability when compared to NETL Case 10 monoethanolamine (MEA) scrubbing technology. The use of CA accelerates inter-conversion between dissolved CO2 and bicarbonate ion to enhance CO2 absorption, and the use of low enthalpy CO2 absorption solvents makes it possible to regenerate the solvent at lower temperatures relative to the reference MEA-based solvent. Themore » vacuum regeneration-based integrated bench-scale system operated successfully for an accumulated 500 hours using aqueous 23.5 wt% K2CO3-based solvent containing 2.5 g/L enzyme to deliver an average 84% CO2 capture when operated with a 20% enzyme replenishment rate per ~7 hour steady-state run period. The total inlet gas flow was 30 standard liters per minute with 15% CO2 and 85% N2. The absorber temperature was 40°C and the stripper operated under 35 kPa pressure with an approximate 77°C stripper bottom temperature. Tests with a 30°C absorber temperature delivered >90% capture. On- and off-line operational measurements provided a full process data set, with recirculating enzyme, that allowed for enzyme replenishment and absorption/desorption kinetic parameter calculations. Dissolved enzyme replenishment and conventional process controls were demonstrated as straightforward approaches to maintain system performance. Preliminary evaluation of a novel flow-through ultrasonically enhanced regeneration system was also conducted, yet resulted in CO2 release within the range of temperature-dependent release, and further work would be needed to validate the benefits of ultrasonic enhanced stripping. A full technology assessment was completed in which four techno-economic cases for enzyme-enhanced aqueous K2CO3 solvent with vacuum stripping were considered and a corresponding set of sensitivity studies were developed. The cases were evaluated using bench-scale and laboratory-based observations, AspenPlus® process simulation and modeling, AspenTech’s CCE® Parametric Software, current vendor quotations, and project partners’ know-how of unit operations. Overall, the DOE target of 90% CO2 capture could be met using the benign enzyme-enhanced aqueous K2CO3-based alternative to NETL Case 10. The model-predicted plant COE performance, scaled to 550 MWe net output, was 9% higher than NETL Case 10 for an enzyme-activated case with minimized technical risk and highest confidence in physical system performance utilizing commercially available equipment. A COE improvement of 2.8% versus NETL Case 10 was predicted when favorable features of improved enzyme longevity and additional power output from a very low pressure (VLP) turbine were combined, wherein corresponding high capital and operational costs limited the level of COE benefit. The environmental, health and safety (EH&S) profile of the system was found to be favorable and was compliant with the Federal EH&S legislation reviewed. Further work on a larger scale test unit is recommended to reduce the level of uncertainty inherent in extrapolating findings from a bench-scale unit to a full scale PCC plant, and to further investigate several identified opportunities for improvement. Production feasibility and suitability of carbonic anhydrases for scale-up testing was confirmed both through the current project and through parallel efforts.« less

Study of CO2 recovery in a carbonate fuel cell tri-generation plant

NASA Astrophysics Data System (ADS)

Rinaldi, Giorgio; McLarty, Dustin; Brouwer, Jack; Lanzini, Andrea; Santarelli, Massimo

2015-06-01

The possibility of separating and recovering CO2 in a biogas plant that co-produces electricity, hydrogen, and heat is investigated. Exploiting the ability of a molten carbonate fuel cell (MCFC) to concentrate CO2 in the anode exhaust stream reduces the energy consumption and complexity of CO2 separation techniques that would otherwise be required to remove dilute CO2 from combustion exhaust streams. Three potential CO2 concentrating configurations are numerically simulated to evaluate potential CO2 recovery rates: 1) anode oxidation and partial CO2 recirculation, 2) integration with exhaust from an internal combustion engine, and 3) series connection of molten carbonate cathodes initially fed with internal combustion engine (ICE) exhaust. Physical models have been calibrated with data acquired from an operating MCFC tri-generating plant. Results illustrate a high compatibility between hydrogen co-production and CO2 recovery with series connection of molten carbonate systems offering the best results for efficient CO2 recovery. In this case the carbon capture ratio (CCR) exceeds 73% for two systems in series and 90% for 3 MCFC in series. This remarkably high carbon recovery is possible with 1.4 MWe delivered by the ICE system and 0.9 MWe and about 350 kg day-1 of H2 delivered by the three MCFC.

Synthesis of Size-Tunable CO2-Philic Imprinted Polymeric Particles (MIPs) for Low-Pressure CO2 Capture Using Oil-in-Oil Suspension Polymerization.

PubMed

Nabavi, Seyed Ali; Vladisavljević, Goran T; Zhu, Yidi; Manović, Vasilije

2017-10-03

Highly selective molecularly imprinted poly[acrylamide-co-(ethylene glycol dimethacrylate)] polymer particles (MIPs) for CO 2 capture were synthesized by suspension polymerization via oil-in-oil emulsion. Creation of CO 2 -philic, amide-decorated cavities in the polymer matrix led to a high affinity to CO 2 . At 0.15 bar CO 2 partial pressure, the CO 2 /N 2 selectivity was 49 (corresponding to 91% purity of the gas stream after regeneration), and reached 97 at ultralow CO 2 partial pressures. The imprinted polymers showed considerably higher CO 2 uptakes compared to their nonimprinted counterparts, and the maximum equilibrium CO 2 capture capacity of 1.1 mmol g -1 was achieved at 273 K. The heat of adsorption was below 32 kJ mol -1 and the temperature of onset of intense thermal degradation was 351-376 °C. An increase in monomer-to-cross-linker molar ratio in the dispersed phase up to 1:2.5 led to a higher affinity toward CO 2 due to higher density of selective amide groups in the polymer network. MIPs are a promising option for industrial packed and fluidized bed CO 2 capture systems due to large particles with a diameter up to 1200 μm and irregular oblong shapes formed due to arrested coalescence during polymerization, occurring as a result of internal elasticity of the partially polymerized semisolid drops.

Bottleneck Effect of N,N-Dimethylformamide in InOF-1: Increasing CO2 Capture in Porous Coordination Polymers.

PubMed

Sánchez-González, Elí; González-Zamora, Eduardo; Martínez-Otero, Diego; Jancik, Vojtech; Ibarra, Ilich A

2017-05-15

The bottleneck effect of confined N,N-dimethylformamide (DMF) molecules was observed in InOF-1 for the first time: CO 2 capture was remarkably enhanced in samples of as-synthesized InOF-1, thermally activated in such a way that a small residual amount of DMF molecules remained confined within the pores (DMF@InOF-1). Dynamic CO 2 adsorption experiments on DMF@InOF-1 exhibited a CO 2 capture of 8.06 wt % [1.5-fold higher than that of a fully activated InOF-1 (5.24%)]. DMF@InOF-1 can reversibly adsorb/desorb 8.09% CO 2 with no loss of CO 2 capacity after 10 cycles, and the desorption is accomplished by only turning the CO 2 flow off. Static CO 2 adsorption experiments (at 196 K) demonstrated a 1.4-fold CO 2 capture increase (from 5.5 mmol·g -1 , fully activated InOF-1, to 7.5 mmol·g -1 , DMF@InOF-1). Therefore, these CO 2 capture properties are the result of the presence of residual-confined DMF molecules within the InOF-1 framework and their interactions via a very strong hydrogen bond with the In 2 (μ-OH) groups, which prevent DMF leaching. The stability of this hydrogen bond is given by a perfect fit of the DMF molecule in the "dent" around the OH group that allows a nearly ideal orientation of the DMF molecule towards the OH group.

CFD analysis of supercritical CO2 used as HTF in a solar tower receiver

NASA Astrophysics Data System (ADS)

Roldán, M. I.; Fernández-Reche, J.

2016-05-01

The relative cost of a solar receiver can be minimized by the selection of an appropriate heat transfer fluid capable of achieving high receiver efficiencies. In a conventional central receiver system, the concentrated solar energy is transferred from the receiver tube walls to the heat transfer fluid (HTF), which passes through a heat exchanger to generate steam for a Rankine cycle. Thus, higher working fluid temperature is associated with greater efficiency in receiver and power cycle. Emerging receiver designs that can enable higher efficiencies using advanced power cycles, such as supercritical CO2 (s-CO2) closed-loop Brayton cycles, include direct heating of s-CO2 in tubular receiver designs capable of withstanding high internal fluid pressures (around 20 MPa) and temperatures (900 K). Due to the high pressures required and the presence of moving components installed in pipelines (ball-joints and/or flexible connections), the use of s-CO2 presents many technical challenges due to the compatibility of seal materials and fluid leakages of the moving connections. These problems are solved in solar tower systems because the receiver is fixed. In this regard, a preliminary analysis of a tubular receiver with s-CO2 as HTF has been developed using the design of a molten-salt receiver which was previously tested at Plataforma Solar de Almería (PSA). Therefore, a simplified CFD model has been carried out in this study in order to analyze the feasibility of s-CO2 as HTF in solar towers. Simulation results showed that the heat gained by s-CO2 was around 75% greater than the one captured by molten salts (fluid inlet temperature of 715 K), but at a pressure range of 7.5-9.7 MPa. Thus, the use of s-CO2 as HTF in solar tower receivers appears to be a promising alternative, taking into account both the operating conditions required and their maintenance cost.

Recombinant thermoactive phosphoenolpyruvate carboxylase (PEPC) from Thermosynechococcus elongatus and its coupling with mesophilic/thermophilic bacterial carbonic anhydrases (CAs) for the conversion of CO2 to oxaloacetate.

PubMed

Del Prete, Sonia; De Luca, Viviana; Capasso, Clemente; Supuran, Claudiu T; Carginale, Vincenzo

2016-01-15

With the continuous increase of atmospheric CO2 in the last decades, efficient methods for carbon capture, sequestration, and utilization are urgently required. The possibility of converting CO2 into useful chemicals could be a good strategy to both decreasing the CO2 concentration and for achieving an efficient exploitation of this cheap carbon source. Recently, several single- and multi-enzyme systems for the catalytic conversion of CO2 mainly to bicarbonate have been implemented. In order to design and construct a catalytic system for the conversion of CO2 to organic molecules, we implemented an in vitro multienzyme system using mesophilic and thermophilic enzymes. The system, in fact, was constituted by a recombinant phosphoenolpyruvate carboxylase (PEPC) from the thermophilic cyanobacterium Thermosynechococcus elongatus, in combination with mesophilic/thermophilic bacterial carbonic anhydrases (CAs), for converting CO2 into oxaloacetate, a compound of potential utility in industrial processes. The catalytic procedure is in two steps: the conversion of CO2 into bicarbonate by CA, followed by the carboxylation of phosphoenolpyruvate with bicarbonate, catalyzed by PEPC, with formation of oxaloacetate (OAA). All tested CAs, belonging to α-, β-, and γ-CA classes, were able to increase OAA production compared to procedures when only PEPC was used. Interestingly, the efficiency of the CAs tested in OAA production was in good agreement with the kinetic parameters for the CO2 hydration reaction of these enzymes. This PEPC also revealed to be thermoactive and thermostable, and when coupled with the extremely thermostable CA from Sulphurhydrogenibium azorense (SazCA) the production of OAA was achieved even if the two enzymes were exposed to temperatures up to 60 °C, suggesting a possible role of the two coupled enzymes in biotechnological processes. Copyright © 2015 Elsevier Ltd. All rights reserved.

Bench Scale Process for Low Cost CO 2 Capture Using a Phase-Changing Absorbent: Final Scientific/Technical Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Westendorf, Tiffany; Buddle, Stanlee; Caraher, Joel

The objective of this project is to design and build a bench-scale process for a novel phase-changing aminosilicone-based CO 2-capture solvent. The project will establish scalability and technical and economic feasibility of using a phase-changing CO 2-capture absorbent for post-combustion capture of CO 2 from coal-fired power plants. The U.S. Department of Energy’s goal for Transformational Carbon Capture Technologies is the development of technologies available for demonstration by 2025 that can capture 90% of emitted CO 2 with at least 95% CO 2 purity for less than $40/tonne of CO 2 captured. In the first budget period of the project,more » the bench-scale phase-changing CO2 capture process was designed using data and operating experience generated under a previous project (ARPA-e project DE-AR0000084). Sizing and specification of all major unit operations was completed, including detailed process and instrumentation diagrams. The system was designed to operate over a wide range of operating conditions to allow for exploration of the effect of process variables on CO 2 capture performance. In the second budget period of the project, individual bench-scale unit operations were tested to determine the performance of each of each unit. Solids production was demonstrated in dry simulated flue gas across a wide range of absorber operating conditions, with single stage CO 2 conversion rates up to 75mol%. Desorber operation was demonstrated in batch mode, resulting in desorption performance consistent with the equilibrium isotherms for GAP-0/CO 2 reaction. Important risks associated with gas humidity impact on solids consistency and desorber temperature impact on thermal degradation were explored, and adjustments to the bench-scale process were made to address those effects. Corrosion experiments were conducted to support selection of suitable materials of construction for the major unit operations in the process. The bench scale unit operations were assembled into a continuous system to support steady state system testing. In the third budget period of the project, continuous system testing was conducted, including closed-loop operation of the absorber and desober systems. Slurries of GAP-0/GAP-0 carbamate/water mixtures produced in the absorber were pumped successfully to the desorber unit, and regenerated solvent was returned to the absorber. A techno-economic analysis, EH&S risk assessment, and solvent manufacturability study were completed.« less

CO2 Capture from the Air: Technology Assessment and Implications for Climate Policy

NASA Astrophysics Data System (ADS)

Keith, D. W.

2002-05-01

It is physically possible to capture CO2 directly from the air and immobilize it in geological structures. Today, there are no large-scale technologies that achieve air capture at reasonable cost. Yet, strong arguments suggest that it will comparatively easy to develop practical air capture technologies on the timescales relevant to climate policy [1]. This paper first analyzes the cost of air capture and then assesses the implications for climate policy. We first analyze the lower bound on the cost needed for air capture, describing the thermodynamic and physical limits to the use of energy and land. We then compare the costs of air capture to the cost of capture from combustion exhaust streams. While the intrinsic minimum energy requirement is larger for air capture, we argue that air capture has important structural advantages, such as the reduction of transport costs and the larger potential for economies of scale. These advantages suggest that, in the long-run air capture be competitive with other methods of achieving deep emissions reductions. We provide a preliminary engineering-economic analysis of an air capture system based on CaO to CaCO3 chemical looping [1]. We analyze the possibility of doing the calcination in a modified pressurized fluidized bed combustor (PFBC) burning coal in a CO2 rich atmosphere with oxygen supplied by an air separation unit. The CaCO3-to-coal ratio would be ~2:1 and the system would be nearly thermally neutral. PFBC systems have been demonstrated at capacities of over 100 MW. Such systems already include CaCO3 injection for sulfur control, and operate at suitable temperatures and pressures for calcination. We assess the potential to recover heat from the dissolution of CaO in order to reduce the overall energy requirements. We analyze the possibility of adapting existing large water/air heat exchangers for use as contacting systems to capture CO2 from the air using the calcium hydroxide solution. The implications of air capture for global climate policy are examined using DIAM [2], a stylized integrated assessment model. We find that air capture can fundamentally alter the temporal dynamics of global warming mitigation. The reason for this is that air capture differs from conventional mitigation in three key aspects. First, it removes emissions from any part of the economy with equal ease or difficulty, so its cost provides an absolute cap on the cost of mitigation. Second, it permits reduction in concentrations faster than the natural carbon cycle: the effects of irreversibility are thus partly alleviated. Third, because it is less coupled with the energy system, air capture may offer stronger economies of scale and smaller adjustment costs than the more conventional mitigation technologies. Air capture limits the total cost of a worst-case climate scenario. In an optimal sequential decision framework with uncertainty, existence of air capture decreases the need for near-term precautionary abatement. Like geoengineering, air capture thus poses a moral hazard. 1. S. Elliott, et al. Compensation of atmospheric CO2 buildup through engineered chemical sinkage. Geophys. Res. Let., 28:1235-1238, 2001. 2. Minh Ha-Duong, Michael J. Grubb, and Jean-Charles Hourcade. Influence of socioeconomic inertia and uncertainty on optimal CO2-emission abatement. Nature, 390: 270-274, 1997.

Studying the effect of CO2-induced acidification on sediment toxicity using acute amphipod toxicity test.

PubMed

Basallote, M Dolores; De Orte, Manoela R; DelValls, T Ángel; Riba, Inmaculada

2014-01-01

Carbon capture and storage is increasingly being considered one of the most efficient approaches to mitigate the increase of CO2 in the atmosphere associated with anthropogenic emissions. However, the environmental effects of potential CO2 leaks remain largely unknown. The amphipod Ampelisca brevicornis was exposed to environmental sediments collected in different areas of the Gulf of Cádiz and subjected to several pH treatments to study the effects of CO2-induced acidification on sediment toxicity. After 10 days of exposure, the results obtained indicated that high lethal effects were associated with the lowest pH treatments, except for the Ría of Huelva sediment test. The mobility of metals from sediment to the overlying seawater was correlated to a pH decrease. The data obtained revealed that CO2-related acidification would lead to lethal effects on amphipods as well as the mobility of metals, which could increase sediment toxicity.

Comparison of volatiles and mosquito capture efficacy for three carbohydrate sources in a yeast-fermentation CO2 generator

USDA-ARS?s Scientific Manuscript database

Mosquito surveillance in remote areas with limited access to canisters of CO2 or dry ice will benefit from an effective alternative CO2 source. In this study, we document the differences in mosquito and non-mosquito capture rates from CO2 baited (dry ice or yeast fermentation of carbohydrates) CDC t...

An Uncommon Carboxyl-Decorated Metal-Organic Framework with Selective Gas Adsorption and Catalytic Conversion of CO2.

PubMed

Li, Yong-Zhi; Wang, Hai-Hua; Yang, Hong-Yun; Hou, Lei; Wang, Yao-Yu; Zhu, Zhonghua

2018-01-19

A new three-dimensional (3D) framework, [Ni(btzip)(H 2 btzip)]⋅2 DMF⋅2 H 2 O (1) (H 2 btzip=4,6-bis(triazol-1-yl)isophthalic acid) as an acidic heterogeneous catalyst was constructed by the reaction of nickel wire and a triazolyl-carboxyl linker. Framework 1 possesses intersected 2D channels decorated by free COOH groups and uncoordinated triazolyl N atoms, leading to not only high CO 2 and C 2 H 6 adsorption capacity but also significant selective capture for CO 2 and C 2 H 6 over CH 4 and CO in 273-333 K. Moreover, 1 reveals chemical stability toward water. Grand Canonical Monte Carlo simulations confirmed the multiple CO 2 - and C 2 H 6 -philic sites. As a result of the presence of accessible Brønsted acidic COOH groups in the channels, the activated framework demonstrates highly efficient catalytic activity in the cycloaddition reaction of CO 2 with propylene oxide/4-chloromethyl-1,3-dioxolan-2-one/3-butoxy-1,2-epoxypropane into cyclic carbonates. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Tandem mass spectrometry measurement of the collision products of carbamate anions derived from CO2 capture sorbents: paving the way for accurate quantitation.

PubMed

Jackson, Phil; Fisher, Keith J; Attalla, Moetaz Ibrahim

2011-08-01

The reaction between CO(2) and aqueous amines to produce a charged carbamate product plays a crucial role in post-combustion capture chemistry when primary and secondary amines are used. In this paper, we report the low energy negative-ion CID results for several anionic carbamates derived from primary and secondary amines commonly used as post-combustion capture solvents. The study was performed using the modern equivalent of a triple quadrupole instrument equipped with a T-wave collision cell. Deuterium labeling of 2-aminoethanol (1,1,2,2,-d(4)-2-aminoethanol) and computations at the M06-2X/6-311++G(d,p) level were used to confirm the identity of the fragmentation products for 2-hydroxyethylcarbamate (derived from 2-aminoethanol), in particular the ions CN(-), NCO(-) and facile neutral losses of CO(2) and water; there is precedent for the latter in condensed phase isocyanate chemistry. The fragmentations of 2-hydroxyethylcarbamate were generalized for carbamate anions derived from other capture amines, including ethylenediamine, diethanolamine, and piperazine. We also report unequivocal evidence for the existence of carbamate anions derived from sterically hindered amines (Tris(2-hydroxymethyl)aminomethane and 2-methyl-2-aminopropanol). For the suite of carbamates investigated, diagnostic losses include the decarboxylation product (-CO(2), 44 mass units), loss of 46 mass units and the fragments NCO(-) (m/z 42) and CN(-) (m/z 26). We also report low energy CID results for the dicarbamate dianion ((-)O(2)CNHC(2)H(4)NHCO(2)(-)) commonly encountered in CO(2) capture solution utilizing ethylenediamine. Finally, we demonstrate a promising ion chromatography-MS based procedure for the separation and quantitation of aqueous anionic carbamates, which is based on the reported CID findings. The availability of accurate quantitation methods for ionic CO(2) capture products could lead to dynamic operational tuning of CO(2) capture-plants and, thus, cost-savings via real-time manipulation of solvent regeneration energies.

A 490 W transversely excited atmospheric CO2 spark gap laser with added H2

NASA Astrophysics Data System (ADS)

Zand, M.; Koushki, A. M.; Neshati, R.; Kia, B.; Khorasani, K.

2018-02-01

In this paper we present a new design for a high pulse repetition rate transversely excited atmospheric CO2 laser with ultraviolet pre-ionization. A new method of fast thyristor capacitor charging and discharging by a spark gap is used. The effect of H2 gas addition on the output and stability of a transversely excited atmospheric laser operating with a basic mixture of CO2, N2 and He is investigated. The output power was increased by adding H2 to the gas mixture ratio of CO2:N2:He:H2  =  1:1:8:0.5 at total pressure of 850 mbar. An average power of 490 W at 110 Hz with 4.5 J per pulse was obtained. The laser efficiency was 11.2% and oxygen gas was used in the spark gap for electron capture to reduce the recovery time and increase the repetition rate.

Micro-scale thermal imaging of CO2 absorption in the thermochemical energy storage of Li metal oxides at high temperature

NASA Astrophysics Data System (ADS)

Morikawa, Junko; Takasu, Hiroki; Zamengo, Massimiliano; Kato, Yukitaka

2017-05-01

Li-Metal oxides (typical example: lithium ortho-silicate Li4SiO4) are regarded as a novel solid carbon dioxide CO2 absorbent accompanied by an exothermic reaction. At temperatures above 700°C the sorbent is regenerated with the release of the captured CO2 in an endothermic reaction. As the reaction equilibrium of this reversible chemical reaction is controllable only by the partial pressure of CO2, the system is regarded as a potential candidate for chemical heat storage at high temperatures. In this study, we applied our recent developed mobile type instrumentation of micro-scale infrared thermal imaging system to observe the heat of chemical reaction of Li4SiO4 and CO2 at temperature higher than 600°C or higher. In order to quantify the micro-scale heat transfer and heat exchange in the chemical reaction, the superimpose signal processing system is setup to determine the precise temperature. Under an ambient flow of carbon dioxide, a powder of Li4SiO4 with a diameter 50 micron started to shine caused by an exothermic chemical reaction heat above 600°C. The phenomena was accelerated with increasing temperature up to 700°C. At the same time, the reaction product lithium carbonate (Li2CO3) started to melt with endothermic phase change above 700°C, and these thermal behaviors were captured by the method of thermal imaging. The direct measurement of multiple thermal phenomena at high temperatures is significant to promote an efficient design of chemical heat storage materials. This is the first observation of the exothermic heat of the reaction of Li4SiO4 and CO2 at around 700°C by the thermal imaging method.

Salinity-gradient energy driven microbial electrosynthesis of value-added chemicals from CO2 reduction.

PubMed

Li, Xiaohu; Angelidaki, Irini; Zhang, Yifeng

2018-06-14

Biological conversion of CO 2 to value-added chemicals and biofuels has emerged as an attractive strategy to address the energy and environmental concerns caused by the over-reliance on fossil fuels. In this study, an innovative microbial reverse-electrodialysis electrolysis cell (MREC), which combines the strengths of reverse electrodialysis (RED) and microbial electrosynthesis technology platforms, was developed to achieve efficient CO 2 -to-value chemicals bioconversion by using the salinity gradient energy as driven energy sources. In the MREC, maximum acetate and ethanol concentrations of 477.5 ± 33.2 and 46.2 ± 8.2 mg L -1 were obtained at the cathode, catalyzed by Sporomusa ovata with production rates of 165.79 ± 11.52 and 25.11 ± 4.46 mmol m -2 d -1 , respectively. Electron balance analysis indicates that 94.4 ± 3.9% of the electrons derived from wastewater and salinity gradient were recovered in acetate and ethanol. This work for the first time proved the potential of innovative MREC configuration has the potential as an efficient technology platform for simultaneous CO 2 capture and electrosynthesis of valuable chemicals. Copyright © 2018 Elsevier Ltd. All rights reserved.

Recovery Act: Innovative CO 2 Sequestration from Flue Gas Using Industrial Sources and Innovative Concept for Beneficial CO 2 Use

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dando, Neal; Gershenzon, Mike; Ghosh, Rajat

2012-07-31

The overall goal of this DOE Phase 2 project was to further develop and conduct pilot-scale and field testing of a biomimetic in-duct scrubbing system for the capture of gaseous CO 2 coupled with sequestration of captured carbon by carbonation of alkaline industrial wastes. The Phase 2 project, reported on here, combined efforts in enzyme development, scrubber optimization, and sequestrant evaluations to perform an economic feasibility study of technology deployment. The optimization of carbonic anhydrase (CA) enzyme reactivity and stability are critical steps in deployment of this technology. A variety of CA enzyme variants were evaluated for reactivity and stabilitymore » in both bench scale and in laboratory pilot scale testing to determine current limits in enzyme performance. Optimization of scrubber design allowed for improved process economics while maintaining desired capture efficiencies. A range of configurations, materials, and operating conditions were examined at the Alcoa Technical Center on a pilot scale scrubber. This work indicated that a cross current flow utilizing a specialized gas-liquid contactor offered the lowest system operating energy. Various industrial waste materials were evaluated as sources of alkalinity for the scrubber feed solution and as sources of calcium for precipitation of carbonate. Solids were mixed with a simulated sodium bicarbonate scrubber blowdown to comparatively examine reactivity. Supernatant solutions and post-test solids were analyzed to quantify and model the sequestration reactions. The best performing solids were found to sequester between 2.3 and 2.9 moles of CO 2 per kg of dry solid in 1-4 hours of reaction time. These best performing solids were cement kiln dust, circulating dry scrubber ash, and spray dryer absorber ash. A techno-economic analysis was performed to evaluate the commercial viability of the proposed carbon capture and sequestration process in full-scale at an aluminum smelter and a refinery location. For both cases the in-duct scrubber technology was compared to traditional amine- based capture. Incorporation of the laboratory results showed that for the application at the aluminum smelter, the in-duct scrubber system is more economical than traditional methods. However, the reverse is true for the refinery case, where the bauxite residue is not effective enough as a sequestrant, combined with challenges related to contaminants in the bauxite residue accumulating in and fouling the scrubber absorbent. Sensitivity analyses showed that the critical variables by which process economics could be improved are enzyme concentration, efficiency, and half-life. At the end of the first part of the Phase 2 project, a gate review (DOE Decision Zero Gate Point) was conducted to decide on the next stages of the project. The original plan was to follow the pre-testing phase with a detailed design for the field testing. Unfavorable process economics, however, resulted in a decision to conclude the project before moving to field testing. It is noted that CO 2 Solutions proposed an initial solution to reduce process costs through more advanced enzyme management, however, DOE program requirements restricting any technology development extending beyond 2014 as commercial deployment timeline did not allow this solution to be undertaken.« less

Evaluation of Solid Sorbents as a Retrofit Technology for CO 2 Capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sjostrom, Sharon

2016-06-02

ADA completed a DOE-sponsored program titled Evaluation of Solid Sorbents as a Retrofit Technology for CO 2 Capture under program DE-FE0004343. During this program, sorbents were analyzed for use in a post-combustion CO 2 capture process. A supported amine sorbent was selected based upon superior performance to adsorb a greater amount of CO 2 than the activated carbon sorbents tested. When the most ideal sorbent at the time was selected, it was characterized and used to create a preliminary techno-economic analysis (TEA). A preliminary 550 MW coal-fired power plant using Illinois #6 bituminous coal was designed with a solid sorbentmore » CO 2 capture system using the selected supported amine sorbent to both facilitate the TEA and to create the necessary framework to scale down the design to a 1 MWe equivalent slipstream pilot facility. The preliminary techno-economic analysis showed promising results and potential for improved performance for CO 2 capture compared to conventional MEA systems. As a result, a 1 MWe equivalent solid sorbent system was designed, constructed, and then installed at a coal-fired power plant in Alabama. The pilot was designed to capture 90% of the CO 2 from the incoming flue gas at 1 MWe net electrical generating equivalent. Testing was not possible at the design conditions due to changes in sorbent handling characteristics at post-regenerator temperatures that were not properly incorporated into the pilot design. Thus, severe pluggage occurred at nominally 60% of the design sorbent circulation rate with heated sorbent, although no handling issues were noted when the system was operated prior to bringing the regenerator to operating temperature. Testing within the constraints of the pilot plant resulted in 90% capture of the incoming CO 2 at a flow rate equivalent of 0.2 to 0.25 MWe net electrical generating equivalent. The reduction in equivalent flow rate at 90% capture was primarily the result of sorbent circulation limitations at operating temperatures combined with pre-loading of the sorbent with CO 2 prior to entering the adsorber. Specifically, CO 2-rich gas was utilized to convey sorbent from the regenerator to the adsorber. This gas was nominally 45°C below the regenerator temperature during testing. ADA’s post-combustion capture system with modifications to overcome pilot constraints, in conjunction with incorporating a sorbent with CO 2 working capacity of 15 g CO 2/100 g sorbent and a contact time of 10 to 15 minutes or less with flue gas could provide significant cost and performance benefits when compared to an MEA system.« less

Alkyl amine and vegetable oil mixture-a viable candidate for CO2 capture and utilization.

PubMed

Uma Maheswari, A; Palanivelu, K

2017-02-01

In this present work, the absorption of CO 2 in alkyl amines and vegetable oil mixture has been evaluated. The results showed that the absorption is higher in alkyl amines and vegetable oil mixture compared with the aqueous alkyl amines. In addition to that, by employing the greener and non-toxic vegetable oil media, the CO 2 gas has been captured as well as converted into value-added products, such as carbamates of ethylenediamine, diethylenetriamine, and triethylenetetramine. The carbamates have been isolated and characterized by Fourier transform infrared and 1 H and 13 C nuclear magnetic resonance spectroscopic techniques. The formation of these products in precipitate form has not been observed in the case of aqueous medium. Among the various alkyl amine and vegetable oil combinations, triethylenetetramine in coconut oil medium showed the maximum CO 2 capture capacity of 72%. The coconut oil used for the process has been recovered, recycled, and reused for 3 cycles. Thus, this novel scheme seems to be a better alternative to conquer the drawback of aqueous amine-based CO 2 capture as well as for the capture and utilization of the CO 2 gas to gain the value-added products.

Evaluation of CDC light traps for mosquito surveillance in a malaria endemic area on the Thai-Myanmar border.

PubMed

Sriwichai, Patchara; Karl, Stephan; Samung, Yudthana; Sumruayphol, Suchada; Kiattibutr, Kirakorn; Payakkapol, Anon; Mueller, Ivo; Yan, Guiyun; Cui, Liwang; Sattabongkot, Jetsumon

2015-12-15

Centers for Disease Control and Prevention miniature light traps (CDC-LT) baited with CO2 are a routine tool for adult mosquito sampling used in entomological surveys, and for monitoring and surveillance of disease vectors. The present study was aimed at evaluating the performance of baited and unbaited CDC-LT for indoor and outdoor trapping of endemic mosquito species in northwestern Thailand. CDC-LT (n = 112) with and without dry ice baits were set both indoors and outdoors in 88 selected houses for stretches of 5 consecutive nights per month in 7 villages in Tha Song Yang district, Tak province between January 2011 and March 2013. Individual traps were repeatedly placed in the same location for a median of 6 (range 1-10) times. Mosquitoes were identified by morphological characteristics and classified into blood-fed, empty, male/female and gravid. Absolute mosquito numbers were converted to capture rates (i.e., mosquitoes per trap and year). Capture rates were compared using multilevel negative binomial regression to account for multiple trap placements and adjust for regional and seasonal differences. A total of 6,668 mosquitoes from 9 genera were collected from 576 individual CDC-LT placements. Culex was the predominant captured genus (46%), followed by anopheline mosquitoes (45%). Overall, CO2 baited traps captured significantly more Culex (especially Culex vishnui Theobald) and Anopheles mosquitoes per unit time (adjusted capture rate ratio (aCRR) 1.64 and 1.38, respectively). Armigeres spp. mosquitoes were trapped in outdoor traps with significantly higher frequency (aCRR: 1.50), whereas Aedes albopictus (Skuse) had a tendency to be trapped more frequently indoors (aCRR: 1.89, p = 0.07). Furthermore, capture rate ratios between CO2 baited and non-baited CDC-LT were significantly influenced by seasonality and indoor vs. outdoor trap placement. The present study shows that CDC-LT with CO2 baiting capture significantly more Culex and Anopheles mosquitoes, some of which (e.g., Cx. vishnui, Cx. quinquefasciatus Say, An. minimus s.l. Theobald, An. maculatus s.l. Theobald) represent important disease vectors in Thailand. This study also shows significant differences in the capture efficiency of CDC-LT when placed indoors or outdoors and in different seasons. Our study thus provides important guidelines for more targeted future vector trapping studies on the Thai-Myanmar border, which is an important cross-border malaria transmission region in Thailand.

Opportunities for increasing CO 2 storage in deep, saline formations by active reservoir management and treatment of extracted formation water: Case study at the GreenGen IGCC facility, Tianjin, PR China

DOE PAGES

Ziemkiewicz, Paul; Stauffer, Philip H.; Sullivan-Graham, Jeri; ...

2016-08-04

Carbon capture, utilization and storage (CCUS) seeks beneficial applications for CO 2 recovered from fossil fuel combustion. This study evaluated the potential for removing formation water to create additional storage capacity for CO 2, while simultaneously treating the produced water for beneficial use. Furthermore, the process would control pressures within the target formation, lessen the risk of caprock failure, and better control the movement of CO 2 within that formation. The project plans to highlight the method of using individual wells to produce formation water prior to injecting CO 2 as an efficient means of managing reservoir pressure. Because themore » pressure drawdown resulting from pre-injection formation water production will inversely correlate with pressure buildup resulting from CO 2 injection, it can be proactively used to estimate CO 2 storage capacity and to plan well-field operations. The project studied the GreenGen site in Tianjin, China where Huaneng Corporation is capturing CO 2 at a coal fired IGCC power plant. Known as the Tianjin Enhanced Water Recovery (EWR) project, local rock units were evaluated for CO 2 storage potential and produced water treatment options were then developed. Average treatment cost for produced water with a cooling water treatment goal ranged from 2.27 to 2.96 US$/m 3 (recovery 95.25%), and for a boiler water treatment goal ranged from 2.37 to 3.18 US$/m 3 (recovery 92.78%). Importance analysis indicated that water quality parameters and transportation are significant cost factors as the injection-extraction system is managed over time. Our study found that in a broad sense, active reservoir management in the context of CCUS/EWR is technically feasible. In addition, criteria for evaluating suitable vs. unsuitable reservoir properties, reservoir storage (caprock) integrity, a recommended injection/withdrawal strategy and cost estimates for water treatment and reservoir management are proposed.« less

Opportunities for increasing CO 2 storage in deep, saline formations by active reservoir management and treatment of extracted formation water: Case study at the GreenGen IGCC facility, Tianjin, PR China

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ziemkiewicz, Paul; Stauffer, Philip H.; Sullivan-Graham, Jeri

Carbon capture, utilization and storage (CCUS) seeks beneficial applications for CO 2 recovered from fossil fuel combustion. This study evaluated the potential for removing formation water to create additional storage capacity for CO 2, while simultaneously treating the produced water for beneficial use. Furthermore, the process would control pressures within the target formation, lessen the risk of caprock failure, and better control the movement of CO 2 within that formation. The project plans to highlight the method of using individual wells to produce formation water prior to injecting CO 2 as an efficient means of managing reservoir pressure. Because themore » pressure drawdown resulting from pre-injection formation water production will inversely correlate with pressure buildup resulting from CO 2 injection, it can be proactively used to estimate CO 2 storage capacity and to plan well-field operations. The project studied the GreenGen site in Tianjin, China where Huaneng Corporation is capturing CO 2 at a coal fired IGCC power plant. Known as the Tianjin Enhanced Water Recovery (EWR) project, local rock units were evaluated for CO 2 storage potential and produced water treatment options were then developed. Average treatment cost for produced water with a cooling water treatment goal ranged from 2.27 to 2.96 US$/m 3 (recovery 95.25%), and for a boiler water treatment goal ranged from 2.37 to 3.18 US$/m 3 (recovery 92.78%). Importance analysis indicated that water quality parameters and transportation are significant cost factors as the injection-extraction system is managed over time. Our study found that in a broad sense, active reservoir management in the context of CCUS/EWR is technically feasible. In addition, criteria for evaluating suitable vs. unsuitable reservoir properties, reservoir storage (caprock) integrity, a recommended injection/withdrawal strategy and cost estimates for water treatment and reservoir management are proposed.« less

Secondary scintillation yield of xenon with sub-percent levels of CO 2 additive for rare-event detection

DOE PAGES

Henriques, C. A. O.; Freitas, E. D. C.; Azevedo, C. D. R.; ...

2017-09-12

Xe–CO 2 mixtures are important alternatives to pure xenon in Time Projection Chambers (TPC) based on secondary scintillation (electroluminescence) signal amplification with applications in the important field of rare event detection such as directional dark matter, double electron capture and double beta decay detection. The addition of CO 2 to pure xenon at the level of 0.05–0.1% can reduce significantly the scale of electron diffusion from 10 mm / √m to 2.5mm / √m, with high impact on the discrimination efficiency of the events through pattern recognition of the topology of primary ionization trails. We have measured the electroluminescence (EL)more » yield of Xe–CO 2 mixtures, with sub-percent CO 2 concentrations. We demonstrate that the EL production is still high in these mixtures, 70% and 35% relative to that produced in pure xenon, for CO 2 concentrations around 0.05% and 0.1%, respectively. In conclusion, the contribution of the statistical fluctuations in EL production to the energy resolution increases with increasing CO 2 concentration, being smaller than the contribution of the Fano factor for concentrations below 0.1% CO 2.« less

Secondary scintillation yield of xenon with sub-percent levels of CO2 additive for rare-event detection

NASA Astrophysics Data System (ADS)

Henriques, C. A. O.; Freitas, E. D. C.; Azevedo, C. D. R.; González-Díaz, D.; Mano, R. D. P.; Jorge, M. R.; Fernandes, L. M. P.; Monteiro, C. M. B.; Gómez-Cadenas, J. J.; Álvarez, V.; Benlloch-Rodríguez, J. M.; Borges, F. I. G. M.; Botas, A.; Cárcel, S.; Carríon, J. V.; Cebrían, S.; Conde, C. A. N.; Díaz, J.; Diesburg, M.; Esteve, R.; Felkai, R.; Ferrario, P.; Ferreira, A. L.; Goldschmidt, A.; Gutiérrez, R. M.; Hauptman, J.; Hernandez, A. I.; Hernando Morata, J. A.; Herrero, V.; Jones, B. J. P.; Labarga, L.; Laing, A.; Lebrun, P.; Liubarsky, I.; López-March, N.; Losada, M.; Martín-Albo, J.; Martínez-Lema, G.; Martínez, A.; McDonald, A. D.; Monrabal, F.; Mora, F. J.; Moutinho, L. M.; Muñoz Vidal, J.; Musti, M.; Nebot-Guinot, M.; Novella, P.; Nygren, D. R.; Palmeiro, B.; Para, A.; Pérez, J.; Querol, M.; Renner, J.; Ripoll, L.; Rodríguez, J.; Rogers, L.; Santos, F. P.; dos Santos, J. M. F.; Simón, A.; Sofka, C.; Sorel, M.; Stiegler, T.; Toledo, J. F.; Torrent, J.; Tsamalaidze, Z.; Veloso, J. F. C. A.; Webb, R.; White, J. T.; Yahlali, N.; NEXT Collaboration

2017-10-01

Xe-CO2 mixtures are important alternatives to pure xenon in Time Projection Chambers (TPC) based on secondary scintillation (electroluminescence) signal amplification with applications in the important field of rare event detection such as directional dark matter, double electron capture and double beta decay detection. The addition of CO2 to pure xenon at the level of 0.05-0.1% can reduce significantly the scale of electron diffusion from 10 mm /√{m} to 2.5 mm /√{m}, with high impact on the discrimination efficiency of the events through pattern recognition of the topology of primary ionization trails. We have measured the electroluminescence (EL) yield of Xe-CO2 mixtures, with sub-percent CO2 concentrations. We demonstrate that the EL production is still high in these mixtures, 70% and 35% relative to that produced in pure xenon, for CO2 concentrations around 0.05% and 0.1%, respectively. The contribution of the statistical fluctuations in EL production to the energy resolution increases with increasing CO2 concentration, being smaller than the contribution of the Fano factor for concentrations below 0.1% CO2.

Secondary scintillation yield of xenon with sub-percent levels of CO 2 additive for rare-event detection

DOE Office of Scientific and Technical Information (OSTI.GOV)

Henriques, C. A. O.; Freitas, E. D. C.; Azevedo, C. D. R.

Xe–CO 2 mixtures are important alternatives to pure xenon in Time Projection Chambers (TPC) based on secondary scintillation (electroluminescence) signal amplification with applications in the important field of rare event detection such as directional dark matter, double electron capture and double beta decay detection. The addition of CO 2 to pure xenon at the level of 0.05–0.1% can reduce significantly the scale of electron diffusion from 10 mm / √m to 2.5mm / √m, with high impact on the discrimination efficiency of the events through pattern recognition of the topology of primary ionization trails. We have measured the electroluminescence (EL)more » yield of Xe–CO 2 mixtures, with sub-percent CO 2 concentrations. We demonstrate that the EL production is still high in these mixtures, 70% and 35% relative to that produced in pure xenon, for CO 2 concentrations around 0.05% and 0.1%, respectively. In conclusion, the contribution of the statistical fluctuations in EL production to the energy resolution increases with increasing CO 2 concentration, being smaller than the contribution of the Fano factor for concentrations below 0.1% CO 2.« less

Particle-scale CO2 adsorption kinetics modeling considering three reaction mechanisms

DOE Office of Scientific and Technical Information (OSTI.GOV)

Suh, Dong-Myung; Sun, Xin

2013-09-01

In the presence of water (H2O), dry and wet adsorptions of carbon dioxide (CO2) and physical adsorption of H2O happen concurrently in a sorbent particle. The three reactions depend on each other and have a complicated, but important, effect on CO2 capturing via a solid sorbent. In this study, transport phenomena in the sorbent were modeled, including the tree reactions, and a numerical solving procedure for the model also was explained. The reaction variable distribution in the sorbent and their average values were calculated, and simulation results were compared with experimental data to validate the proposed model. Some differences, causedmore » by thermodynamic parameters, were observed between them. However, the developed model reasonably simulated the adsorption behaviors of a sorbent. The weight gained by each adsorbed species, CO2 and H2O, is difficult to determine experimentally. It is known that more CO2 can be captured in the presence of water. Still, it is not yet known quantitatively how much more CO2 the sorbent can capture, nor is it known how much dry and wet adsorptions separately account for CO2 capture. This study addresses those questions by modeling CO2 adsorption in a particle and simulating the adsorption process using the model. As adsorption temperature changed into several values, the adsorbed amount of each species was calculated. The captured CO2 in the sorbent particle was compared quantitatively between dry and wet conditions. As the adsorption temperature decreased, wet adsorption increased. However, dry adsorption was reduced.« less

A Life Cycle Assessment Case Study of Coal-Fired Electricity Generation with Humidity Swing Direct Air Capture of CO2 versus MEA-Based Postcombustion Capture.

PubMed

van der Giesen, Coen; Meinrenken, Christoph J; Kleijn, René; Sprecher, Benjamin; Lackner, Klaus S; Kramer, Gert Jan

2017-01-17

Most carbon capture and storage (CCS) envisions capturing CO 2 from flue gas. Direct air capture (DAC) of CO 2 has hitherto been deemed unviable because of the higher energy associated with capture at low atmospheric concentrations. We present a Life Cycle Assessment of coal-fired electricity generation that compares monoethanolamine (MEA)-based postcombustion capture (PCC) of CO 2 with distributed, humidity-swing-based direct air capture (HS-DAC). Given suitable temperature, humidity, wind, and water availability, HS-DAC can be largely passive. Comparing energy requirements of HS-DAC and MEA-PCC, we find that the parasitic load of HS-DAC is less than twice that of MEA-PCC (60-72 kJ/mol versus 33-46 kJ/mol, respectively). We also compare other environmental impacts as a function of net greenhouse gas (GHG) mitigation: To achieve the same 73% mitigation as MEA-PCC, HS-DAC would increase nine other environmental impacts by on average 38%, whereas MEA-PCC would increase them by 31%. Powering distributed HS-DAC with photovoltaics (instead of coal) while including recapture of all background GHG, reduces this increase to 18%, hypothetically enabling coal-based electricity with net-zero life-cycle GHG. We conclude that, in suitable geographies, HS-DAC can complement MEA-PCC to enable CO 2 capture independent of time and location of emissions and recapture background GHG from fossil-based electricity beyond flue stack emissions.

Computational Modeling of the Geologic Sequestration of Carbon Dioxide

EPA Science Inventory

Geologic sequestration of CO2 is a component of C capture and storage (CCS), an emerging technology for reducing CO2 emissions to the atmosphere, and involves injection of captured CO2 into deep subsurface formations. Similar to the injection of hazardous wastes, before injection...

Porous materials with pre-designed single-molecule traps for CO2 selective adsorption

DOE Office of Scientific and Technical Information (OSTI.GOV)

Li, JR; Yu, JM; Lu, WG

2013-02-26

Despite tremendous efforts, precise control in the synthesis of porous materials with pre-designed pore properties for desired applications remains challenging. Newly emerged porous metal-organic materials, such as metal-organic polyhedra and metal-organic frameworks, are amenable to design and property tuning, enabling precise control of functionality by accurate design of structures at the molecular level. Here we propose and validate, both experimentally and computationally, a precisely designed cavity, termed a 'single-molecule trap', with the desired size and properties suitable for trapping target CO2 molecules. Such a single-molecule trap can strengthen CO2-host interactions without evoking chemical bonding, thus showing potential for CO2 capture.more » Molecular single-molecule traps in the form of metal-organic polyhedra are designed, synthesised and tested for selective adsorption of CO2 over N-2 and CH4, demonstrating the trapping effect. Building these pre-designed single-molecule traps into extended frameworks yields metal-organic frameworks with efficient mass transfer, whereas the CO2 selective adsorption nature of single-molecule traps is preserved.« less

Hydrogen-based power generation from bioethanol steam reforming

NASA Astrophysics Data System (ADS)

Tasnadi-Asztalos, Zs.; Cormos, C. C.; Agachi, P. S.

2015-12-01

This paper is evaluating two power generation concepts based on hydrogen produced from bioethanol steam reforming at industrial scale without and with carbon capture. The power generation from bioethanol conversion is based on two important steps: hydrogen production from bioethanol catalytic steam reforming and electricity generation using a hydrogen-fuelled gas turbine. As carbon capture method to be assessed in hydrogen-based power generation from bioethanol steam reforming, the gas-liquid absorption using methyl-di-ethanol-amine (MDEA) was used. Bioethanol is a renewable energy carrier mainly produced from biomass fermentation. Steam reforming of bioethanol (SRE) provides a promising method for hydrogen and power production from renewable resources. SRE is performed at high temperatures (e.g. 800-900°C) to reduce the reforming by-products (e.g. ethane, ethene). The power generation from hydrogen was done with M701G2 gas turbine (334 MW net power output). Hydrogen was obtained through catalytic steam reforming of bioethanol without and with carbon capture. For the evaluated plant concepts the following key performance indicators were assessed: fuel consumption, gross and net power outputs, net electrical efficiency, ancillary consumptions, carbon capture rate, specific CO2 emission etc. As the results show, the power generation based on bioethanol conversion has high energy efficiency and low carbon footprint.

Hydrogen-based power generation from bioethanol steam reforming

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tasnadi-Asztalos, Zs., E-mail: tazsolt@chem.ubbcluj.ro; Cormos, C. C., E-mail: cormos@chem.ubbcluj.ro; Agachi, P. S.

This paper is evaluating two power generation concepts based on hydrogen produced from bioethanol steam reforming at industrial scale without and with carbon capture. The power generation from bioethanol conversion is based on two important steps: hydrogen production from bioethanol catalytic steam reforming and electricity generation using a hydrogen-fuelled gas turbine. As carbon capture method to be assessed in hydrogen-based power generation from bioethanol steam reforming, the gas-liquid absorption using methyl-di-ethanol-amine (MDEA) was used. Bioethanol is a renewable energy carrier mainly produced from biomass fermentation. Steam reforming of bioethanol (SRE) provides a promising method for hydrogen and power production frommore » renewable resources. SRE is performed at high temperatures (e.g. 800-900°C) to reduce the reforming by-products (e.g. ethane, ethene). The power generation from hydrogen was done with M701G2 gas turbine (334 MW net power output). Hydrogen was obtained through catalytic steam reforming of bioethanol without and with carbon capture. For the evaluated plant concepts the following key performance indicators were assessed: fuel consumption, gross and net power outputs, net electrical efficiency, ancillary consumptions, carbon capture rate, specific CO{sub 2} emission etc. As the results show, the power generation based on bioethanol conversion has high energy efficiency and low carbon footprint.« less

Evaluation of Mars CO2 Capture and Gas Separation Technologies

NASA Technical Reports Server (NTRS)

Muscatello, Anthony C.; Santiago-Maldonado, Edgardo; Gibson, Tracy; Devor, Robert; Captain, James

2011-01-01

Recent national policy statements have established that the ultimate destination of NASA's human exploration program is Mars. In Situ Resource Utilization (ISRU) is a key technology required to ,enable such missions and it is appropriate to review progress in this area and continue to advance the systems required to produce rocket propellant, oxygen, and other consumables on Mars using the carbon dioxide atmosphere and other potential resources. The Mars Atmospheric Capture and Gas separation project is selecting, developing, and demonstrating techniques to capture and purify Martian atmospheric gases for their utilization for the production of hydrocarbons, oxygen, and water in ISRU systems. Trace gases will be required to be separated from Martian atmospheric gases to provide pure CO2 to processing elements. In addition, other Martian gases, such as nitrogen and argon, occur in concentrations high enough to be useful as buffer gas and should be captured as well. To achieve these goals, highly efficient gas separation processes will be required. These gas separation techniques are also required across various areas within the ISRU project to support various consumable production processes. The development of innovative gas separation techniques will evaluate the current state-of-the-art for the gas separation required, with the objective to demonstrate and develop light-weight, low-power methods for gas separation. Gas separation requirements include, but are not limited to the selective separation of: (1) methane and water from unreacted carbon oxides (C02-CO) and hydrogen typical of a Sabatier-type process, (2) carbon oxides and water from unreacted hydrogen from a Reverse Water-Gas Shift process, (3)/carbon oxides from oxygen from a trash/waste processing reaction, and (4) helium from hydrogen or oxygen from a propellant scavenging process. Potential technologies for the separations include' freezers, selective membranes, selective solvents, polymeric sorbents, zeolites, and new technologies. This paper summarizes the results of an extensive literature review of candidate technologies for the capture and separation of CO2 and other relevant gases. This information will be used to prioritize the technologies to be developed further during this and other ISRU projects.

Carbon dioxide capture using Sodium bicarbonate/Sodium carbonate supported on nanoporous Iron(III) oxide

NASA Astrophysics Data System (ADS)

Dutcher, Bryce

Strong evidence exists suggesting that anthropogenic emissions of CO 2, primarily from the combustion of fossil fuels, have been contributing to global climate change, including warming of the atmosphere and acidification of the oceans. These, in turn, lead to other effects such as melting of ice and snow cover, rising sea levels, severe weather patterns, and extinction of life forms. With these detrimental shifts in ecosystems already being observed, it becomes imperative to mitigate anthropogenic CO2. CO2 capture is typically a costly operation, usually due to the energy required for regeneration of the capture medium. Na2CO3 is one potential capture medium with the potential to decrease this energy requirement. Extensively researched as a potential sorbent for CO2, Na2CO3 is well known for its theoretically low energy requirement, due largely to its relatively low heat of reaction compared to other capture technologies. Its primary pitfalls, however, are its extremely low reaction rate during sorption and slow regeneration of Na2CO 3. Before Na2CO3 can be used as a CO2 sorbent, then, it is critical to increase its reaction rate. In order to do so, this project studied nanoporous FeOOH as a potential supporting material for Na2CO3. Because regeneration of the sorbent is the most energy-intensive step when using Na2CO3 for CO 2 sorption, this project focused on the decomposition of NaHCO 3, which is equivalent to CO2 desorption. Using BET, FTIR, XRD, XPS, SEM, TEM, magnetic susceptibility tests, and Mossbauer spectroscopy, we show FeOOH to be thermally stable both with and without the presence of NaHCO3 at temperatures necessary for sorption and regeneration, up to about 200°C. More significantly, we observe that FeOOH not only increases the surface area of NaHCO3, but also has a catalytic effect on the decomposition of NaHCO3, reducing activation energy from 80 kJ/mol to 44 kJ/mol. This reduction in activation energy leads to a significant increase in the reaction rate by a factor of nearly 50, which could translate into a substantial decrease in the cost of using Na2 CO3 for CO2 capture.

Mimic Carbonic Anhydrase Using Metal-Organic Frameworks for CO2 Capture and Conversion.

PubMed

Jin, Chaonan; Zhang, Sainan; Zhang, Zhenjie; Chen, Yao

2018-02-19

Carbonic anhydrase (CA) is a zinc-containing metalloprotein, in which the Zn active center plays the key role to transform CO 2 into carbonate. Inspired by nature, herein we used metal-organic frameworks (MOFs) to mimic CA for CO 2 conversion, on the basis of the structural similarity between the Zn coordination in MOFs and CA active center. The biomimetic activity of MOFs was investigated by detecting the hydrolysis of para-nitrophenyl acetate, which is a model reaction used to evaluate CA activity. The biomimetic materials (e.g., CFA-1) showed good catalytic activity, and excellent reusability, and solvent and thermal stability, which is very important for practical applications. In addition, ZIF-100 and CFA-1 were used to mimic CA to convert CO 2 gas, and exhibited good efficiency on CO 2 conversion compared with those of other porous materials (e.g., MCM-41, active carbon). This biomimetic study revealed a novel CO 2 treatment method. Instead of simply using MOFs to absorb CO 2 , ZIF-100 and CFA-1 were used to mimic CA for in situ CO 2 conversion, which provides a new prospect in the biological and industrial applications of MOFs.

Ultrafast and Stable CO2 Capture Using Alkali Metal Salt-Promoted MgO-CaCO3 Sorbents.

PubMed

Cui, Hongjie; Zhang, Qiming; Hu, Yuanwu; Peng, Chong; Fang, Xiangchen; Cheng, Zhenmin; Galvita, Vladimir V; Zhou, Zhiming

2018-06-20

As a potential candidate for precombustion CO 2 capture at intermediate temperatures (200-400 °C), MgO-based sorbents usually suffer from low kinetics and poor cyclic stability. Herein, a general and facile approach is proposed for the fabrication of high-performance MgO-based sorbents via incorporation of CaCO 3 into MgO followed by deposition of a mixed alkali metal salt (AMS). The AMS-promoted MgO-CaCO 3 sorbents are capable of adsorbing CO 2 at an ultrafast rate, high capacity, and good stability. The CO 2 uptake of sorbent can reach as high as above 0.5 g CO 2 g sorbent -1 after only 5 min of sorption at 350 °C, accounting for vast majority of the total uptake. In addition, the sorbents are very stable even under severe but more realistic conditions (desorption in CO 2 at 500 °C), where the CO 2 uptake of the best sorbent is stabilized at 0.58 g CO 2 g sorbent -1 in 20 consecutive cycles. The excellent CO 2 capture performance of the sorbent is mainly due to the promoting effect of molten AMS, the rapid formation of CaMg(CO 3 ) 2 , and the plate-like structure of sorbent. The exceptional ultrafast rate and the good stability of the AMS-promoted MgO-CaCO 3 sorbents promise high potential for practical applications, such as precombustion CO 2 capture from integrated gasification combined cycle plants and sorption-enhanced water gas shift process.

Field Testing of Cryogenic Carbon Capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sayre, Aaron; Frankman, Dave; Baxter, Andrew

Sustainable Energy Solutions has been developing Cryogenic Carbon Capture™ (CCC) since 2008. In that time two processes have been developed, the External Cooling Loop and Compressed Flue Gas Cryogenic Carbon Capture processes (CCC ECL™ and CCC CFG™ respectively). The CCC ECL™ process has been scaled up to a 1TPD CO2 system. In this process the flue gas is cooled by an external refrigerant loop. SES has tested CCC ECL™ on real flue gas slip streams from subbituminous coal, bituminous coal, biomass, natural gas, shredded tires, and municipal waste fuels at field sites that include utility power stations, heating plants, cementmore » kilns, and pilot-scale research reactors. The CO2 concentrations from these tests ranged from 5 to 22% on a dry basis. CO2 capture ranged from 95-99+% during these tests. Several other condensable species were also captured including NO2, SO2 and PMxx at 95+%. NO was also captured at a modest rate. The CCC CFG™ process has been scaled up to a .25 ton per day system. This system has been tested on real flue gas streams including subbituminous coal, bituminous coal and natural gas at field sites that include utility power stations, heating plants, and pilot-scale research reactors. CO2 concentrations for these tests ranged from 5 to 15% on a dry basis. CO2 capture ranged from 95-99+% during these tests. Several other condensable species were also captured including NO2, SO2 and PMxx at 95+%. NO was also captured at 90+%. Hg capture was also verified and the resulting effluent from CCC CFG™ was below a 1ppt concentration. This paper will focus on discussion of the capabilities of CCC, the results of field testing and the future steps surrounding the development of this technology.« less

The Concept and Experimental Investigation of CO2 and Steam Co-electrolysis for Resource Utilization in Space Exploration

NASA Technical Reports Server (NTRS)

Stoots, Carl; Mulloth, Lila M.; Luna, Bernadette; Varghese, Mini M.

2009-01-01

CO2 acquisition and utilization technologies will have a vital role in determining sustained and affordable life support and in-situ fuel production architectures for human and robotic exploration of Moon and Mars. For long-term human exploration to be practical, reliable technologies have to be implemented to capture and chemically reduce the metabolic CO2 from the cabin air to restitute oxygen consumption. Technologies that facilitate the in-situ capture and conversion of atmospheric CO2 to fuel are essential for a viable human mission to Mars and their demonstration on the moon is critical as well. This paper describes the concept and experimental investigation of a CO2 capture and reduction system that comprises an adsorption compressor and a CO2 and steam co-electrolysis unit. The process products include oxygen for life support and Syngas (CO and H2) for synthetic fuel production. Electrochemical performance in terms of CO2 conversion, oxygen production, and power consumption of a system with a capacity to process 1kg CO2 per day (1-person equivalent) will be discussed.

Cycle development and design for CO{sub 2} capture from flue gas by vacuum swing adsorption

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jun Zhang; Paul A. Webley

CO{sub 2} capture and storage is an important component in the development of clean power generation processes. One CO{sub 2} capture technology is gas-phase adsorption, specifically pressure (or vacuum) swing adsorption. The complexity of these processes makes evaluation and assessment of new adsorbents difficult and time-consuming. In this study, we have developed a simple model specifically targeted at CO{sub 2} capture by pressure swing adsorption and validated our model by comparison with data from a fully instrumented pilot-scale pressure swing adsorption process. The model captures non-isothermal effects as well as nonlinear adsorption and nitrogen coadsorption. Using the model and ourmore » apparatus, we have designed and studied a large number of cycles for CO{sub 2} capture. We demonstrate that by careful management of adsorption fronts and assembly of cycles based on understanding of the roles of individual steps, we are able to quickly assess the effect of adsorbents and process parameters on capture performance and identify optimal operating regimes and cycles. We recommend this approach in contrast to exhaustive parametric studies which tend to depend on specifics of the chosen cycle and adsorbent. We show that appropriate combinations of process steps can yield excellent process performance and demonstrate how the pressure drop, and heat loss, etc. affect process performance through their effect on adsorption fronts and profiles. Finally, cyclic temperature profiles along the adsorption column can be readily used to infer concentration profiles - this has proved to be a very useful tool in cyclic function definition. Our research reveals excellent promise for the application of pressure/vacuum swing adsorption technology in the arena of CO{sub 2} capture from flue gases. 20 refs., 6 figs., 2 tabs.« less

Stuart Cohen | NREL

Science.gov Websites

;Optimizing post-combustion CO2 capture in response to volatile electricity prices." International , S.M., H.L. Chalmers, M.E. Webber, C.W. King, and J. Gibbins. "Comparing post-combustion CO2 ., G.T. Rochelle, and M.E. Webber. "Optimal operation of flexible post- combustion CO2 capture in

BioCO2 - a multidisciplinary, biological approach using solar energy to capture CO2 while producing H2 and high value products.

PubMed

Skjånes, Kari; Lindblad, Peter; Muller, Jiri

2007-10-01

Many areas of algae technology have developed over the last decades, and there is an established market for products derived from algae, dominated by health food and aquaculture. In addition, the interest for active biomolecules from algae is increasing rapidly. The need for CO(2) management, in particular capture and storage is currently an important technological, economical and global political issue and will continue to be so until alternative energy sources and energy carriers diminish the need for fossil fuels. This review summarizes in an integrated manner different technologies for use of algae, demonstrating the possibility of combining different areas of algae technology to capture CO(2) and using the obtained algal biomass for various industrial applications thus bringing added value to the capturing and storage processes. Furthermore, we emphasize the use of algae in a novel biological process which produces H(2) directly from solar energy in contrast to the conventional CO(2) neutral biological methods. This biological process is a part of the proposed integrated CO(2) management scheme.

Hierarchically Mesoporous o-Hydroxyazobenzene Polymers: Synthesis and Their Applications in CO2 Capture and Conversion.

PubMed

Ji, Guipeng; Yang, Zhenzhen; Zhang, Hongye; Zhao, Yanfei; Yu, Bo; Ma, Zhishuang; Liu, Zhimin

2016-08-08

The synthesis of hierarchically mesoporous polymers with multiple functionalities is challenging. Herein we reported a template-free strategy for synthesis of phenolic azo-polymers with hierarchical porous structures based on diazo-coupling reaction in aqueous solution under mild conditions. The resultant polymers have surface areas up to 593 m(2)  g(-1) with the mesopore ratio of >80 %, and a good ability to complex with metal ions, such as Cu(2+) , Zn(2+) ,Ni(2+) , achieving a metal loading up to 26.24 wt %. Moreover, the polymers complexed with Zn showed excellent performance for catalyzing the reaction of CO2 with epoxide, affording a TOF of 2570 h(-1) in the presence of tetrabutyl ammonium bromide (7.2 mol %). The polymer complexed with Cu could catalyze the oxidation of alcohol with high efficiency. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Enhancement of CO Evolution by Modification of Ga2O3 with Rare-Earth Elements for the Photocatalytic Conversion of CO2 by H2O.

PubMed

Tatsumi, Hiroyuki; Teramura, Kentaro; Huang, Zeai; Wang, Zheng; Asakura, Hiroyuki; Hosokawa, Saburo; Tanaka, Tsunehiro

2017-12-12

Modification of the surface of Ga 2 O 3 with rare-earth elements enhanced the evolution of CO as a reduction product in the photocatalytic conversion of CO 2 using H 2 O as an electron donor under UV irradiation in aqueous NaHCO 3 as a pH buffer, with the rare-earth species functioning as a CO 2 capture and storage material. Isotope experiments using 13 CO 2 as a substrate clearly revealed that CO was generated from the introduced gaseous CO 2 . In the presence of the NaHCO 3 additive, the rare-earth (RE) species on the Ga 2 O 3 surface are transformed into carbonate hydrates (RE 2 (CO 3 ) 3 ·nH 2 O) and/or hydroxycarbonates (RE 2 (OH) 2(3-x) (CO 3 ) x ) which are decomposed upon photoirradiation. Consequently, Ag-loaded Yb-modified Ga 2 O 3 exhibits much higher activity (209 μmol h -1 of CO) than the pristine Ag-loaded Ga 2 O 3 . The further modification of the surface of the Yb-modified Ga 2 O 3 with Zn afforded a selectivity toward CO evolution of 80%. Thus, we successfully achieved an efficient Ag-loaded Yb- and Zn-modified Ga 2 O 3 photocatalyst with high activity and controllable selectivity, suitable for use in artificial photosynthesis.

CO2-Binding-Organic-Liquids-Enhanced CO2 Capture using Polarity-Swing-Assisted Regeneration

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Jian; Kutnyakov, Igor; Koech, Phillip K.

A new solvent-based CO2 capture process couples the unique attributes of non-aqueous, CO2-binding organic liquids (CO2BOLs) with the newly discovered polarity-swing-assisted regeneration (PSAR) process that is unique to switchable ionic liquids. Laboratory measurements with PSAR indicate the ability to achieve a regeneration effect at 75°C comparable to that at 120°C using thermal regeneration only. Initial measurements also indicate that the kinetic behavior of CO2 release is also improved with PSAR. Abstract cleared PNWD-SA-9743

Modeling Energy Efficiency As A Green Logistics Component In Vehicle Assembly Line

NASA Astrophysics Data System (ADS)

Oumer, Abduaziz; Mekbib Atnaw, Samson; Kie Cheng, Jack; Singh, Lakveer

2016-11-01

This paper uses System Dynamics (SD) simulation to investigate the concept green logistics in terms of energy efficiency in automotive industry. The car manufacturing industry is considered to be one of the highest energy consuming industries. An efficient decision making model is proposed that capture the impacts of strategic decisions on energy consumption and environmental sustainability. The sources of energy considered in this research are electricity and fuel; which are the two main types of energy sources used in a typical vehicle assembly plant. The model depicts the performance measurement for process- specific energy measures of painting, welding, and assembling processes. SD is the chosen simulation method and the main green logistics issues considered are Carbon Dioxide (CO2) emission and energy utilization. The model will assist decision makers acquire an in-depth understanding of relationship between high level planning and low level operation activities on production, environmental impacts and costs associated. The results of the SD model signify the existence of positive trade-offs between green practices of energy efficiency and the reduction of CO2 emission.

Polyethylenimine-incorporated zeolite 13X with mesoporosity for post-combustion CO2 capture

NASA Astrophysics Data System (ADS)

Chen, Chao; Kim, Su-Sung; Cho, Won-Seung; Ahn, Wha-Seung

2015-03-01

X-type zeolite with mesoporosity (Meso-13X) was prepared by using dimethyloctadecyl[3-(trimethoxysilyl)propyl]ammonium chloride as a mesopore-generating agent, and then modified with polyethylenimine (PEI) through a physical impregnation method to form a hybrid material (Meso-13X-PEI). Meso-13X with and without PEI was characterized by X-ray powder diffraction (XRD), N2 adsorption-desorption isotherm at 77 K, scanning electron microscopy (SEM), and thermogravimetric analysis (TGA). Meso-13X-PEI exhibited higher CO2 capture capacity than PEI-modified zeolite 13X owing to its larger pore volume that accommodates more amine species inside the pore structure, and the mesoporosity also can facilitate dispersion of PEI molecules inside the pore channels. Compared to zeolite 13X, Meso-13X-PEI showed much higher CO2 capture selectivity (against N2) as well as higher CO2 capture capacity at relatively high temperature (e.g. 100 °C) and dilute CO2 concentration relevant to post-combustion conditions.

Subsurface capture of carbon dioxide

DOEpatents

Blount, Gerald; Siddal, Alvin A.; Falta, Ronald W.

2014-07-22

A process and apparatus of separating CO.sub.2 gas from industrial off-gas source in which the CO.sub.2 containing off-gas is introduced deep within an injection well. The CO.sub.2 gases are dissolved in the, liquid within the injection well while non-CO.sub.2 gases, typically being insoluble in water or brine, are returned to the surface. Once the CO.sub.2 saturated liquid is present within the injection well, the injection well may be used for long-term geologic storage of CO.sub.2 or the CO.sub.2 saturated liquid can be returned to the surface for capturing a purified CO.sub.2 gas.

Comparative Study of Molecular Basket Sorbents Consisting of Polyallylamine and Polyethylenimine Functionalized SBA-15 for CO2 Capture from Flue Gas.

PubMed

Wang, Dongxiang; Wang, Xiaoxing; Song, Chunshan

2017-11-17

Polyallylamine (PAA)-based molecular basket sorbents (MBS) have been studied for CO 2 capture in comparison with polyethylenimine (PEI)-based MBS. The characterizations including N 2 physisorption, diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), and thermogravimetric analysis (TGA) showed that PAA (M n =15 000) is more rigid and has more steric hindrance inside SBA-15 pores than PEI owing mainly to its different polymer structure. The effects of temperature and PAA loading on the CO 2 sorption capacity of PAA-based MBS have been examined by TGA by using 100 % CO 2 gas stream and compared with PEI/SBA-15. It was found that the capacity of the PAA/SBA-15 sorbent increased with increasing temperature. The optimum capacity of 88 mg CO2  g sorb -1 was obtained at 140 °C for PAA(50)/SBA-15 whereas the optimum sorption temperature was 75 and 90 °C for PEI-I(50)/SBA-15 (PEI-I, M n =423) and PEI-II(50)/SBA-15 (PEI-II, M n =25 000), respectively. The capacity initially increased with the increase of PAA loading and then dropped at high amine contents, owing to the increased diffusion barrier. The highest CO 2 capacity of 109 mg CO2  g sorb -1 was obtained at a PAA loading of 65 wt %, whereas the PAA(50)/SBA-15 sorbent gave the best amine efficiency of 0.23 mol CO2  mol N -1 . The effect of moisture was examined in a fixed-bed flow system with simulated flue gas containing 15 % CO 2 and 4.5 % O 2 in N 2 . It was found that the presence of moisture significantly enhanced CO 2 sorption over PAA(50)/SBA-15 and greatly improved its cyclic stability and regenerability. Compared with PEI/SBA-15, PAA/SBA-15 possesses a better thermal stability and higher resistance to oxidative degradation. However, the CO 2 sorption rate over the PAA(50)/SBA-15 sorbent was much slower. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Advanced Amine Solvent Formulations and Process Integration for Near-Term CO2 Capture Success

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fisher, Kevin S.; Searcy, Katherine; Rochelle, Gary T.

2007-06-28

This Phase I SBIR project investigated the economic and technical feasibility of advanced amine scrubbing systems for post-combustion CO2 capture at coal-fired power plants. Numerous combinations of advanced solvent formulations and process configurations were screened for energy requirements, and three cases were selected for detailed analysis: a monoethanolamine (MEA) base case and two “advanced” cases: an MEA/Piperazine (PZ) case, and a methyldiethanolamine (MDEA) / PZ case. The MEA/PZ and MDEA/PZ cases employed an advanced “double matrix” stripper configuration. The basis for calculations was a model plant with a gross capacity of 500 MWe. Results indicated that CO2 capture increased themore » base cost of electricity from 5 cents/kWh to 10.7 c/kWh for the MEA base case, 10.1 c/kWh for the MEA / PZ double matrix, and 9.7 c/kWh for the MDEA / PZ double matrix. The corresponding cost per metric tonne CO2 avoided was 67.20 $/tonne CO2, 60.19 $/tonne CO2, and 55.05 $/tonne CO2, respectively. Derated capacities, including base plant auxiliary load of 29 MWe, were 339 MWe for the base case, 356 MWe for the MEA/PZ double matrix, and 378 MWe for the MDEA / PZ double matrix. When compared to the base case, systems employing advanced solvent formulations and process configurations were estimated to reduce reboiler steam requirements by 20 to 44%, to reduce derating due to CO2 capture by 13 to 30%, and to reduce the cost of CO2 avoided by 10 to 18%. These results demonstrate the potential for significant improvements in the overall economics of CO2 capture via advanced solvent formulations and process configurations.« less

Bench Scale Development and Testing of Aerogel Sorbents for CO 2 Capture Final Technical Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Begag, Redouane

The primary objective of this project was scaling up and evaluating a novel Amine Functionalized Aerogel (AFA) sorbent in a bench scale fluidized bed reactor. The project team (Aspen Aerogels, University of Akron, ADA-ES, and Longtail Consulting) has carried out numerous tests and optimization studies to demonstrate the CO 2 capture performance of the AFA sorbent in all its forms: powder, pellet, and bead. The CO 2 capture target performance of the AFA sorbent (all forms) were set at > 12 wt.% and > 6 wt.% for total and working CO 2 capacity, respectively (@ 40 °C adsorption / 100more » – 120 °C desorption). The optimized AFA powders outperformed the performance targets by more than 30%, for the total CO 2 capacity (14 - 20 wt.%), and an average of 10 % more for working CO 2 capacity (6.6 – 7.0 wt.%, and could be as high as 9.6 wt. % when desorbed at 120 °C). The University of Akron developed binder formulations, pellet production methods, and post treatment technology for increased resistance to attrition and flue gas contaminants. In pellet form the AFA total CO 2 capacity was ~ 12 wt.% (over 85% capacity retention of that of the powder), and there was less than 13% degradation in CO 2 capture capacity after 20 cycles in the presence of 40 ppm SO 2. ADA-ES assessed the performance of the AFA powder, pellet, and bead by analyzing sorption isotherms, water uptake analysis, cycling stability, jet cup attrition and crush tests. At bench scale, the hydrodynamic and heat transfer properties of the AFA sorbent pellet in fluidized bed conditions were evaluated at Particulate Solid Research, Inc. (PSRI). After the process design requirements were completed, by Longtail Consulting LLC, a techno-economic analysis was achieved using guidance from The National Energy Technology Laboratory (NETL) report. This report provides the necessary framework to estimate costs for a temperature swing post combustion CO 2 capture process using a bituminous coal fired, super-critical steam cycle power plant producing 550 MWe net generation with 90% CO 2 capture using a methylethylamine (MEA) solvent. Using the NETL report as guidance, the designed CO 2 capture system was analyzed on a cost basis to determine relative cost estimates between the benchmark MEA system and the AFA sorbent system.« less

Cycle development and design for CO2 capture from flue gas by vacuum swing adsorption.

PubMed

Zhang, Jun; Webley, Paul A

2008-01-15

CO2 capture and storage is an important component in the development of clean power generation processes. One CO2 capture technology is gas-phase adsorption, specifically pressure (or vacuum) swing adsorption. The complexity of these processes makes evaluation and assessment of new adsorbents difficult and time-consuming. In this study, we have developed a simple model specifically targeted at CO2 capture by pressure swing adsorption and validated our model by comparison with data from a fully instrumented pilot-scale pressure swing adsorption process. The model captures nonisothermal effects as well as nonlinear adsorption and nitrogen coadsorption. Using the model and our apparatus, we have designed and studied a large number of cycles for CO2 capture. We demonstrate that by careful management of adsorption fronts and assembly of cycles based on understanding of the roles of individual steps, we are able to quickly assess the effect of adsorbents and process parameters on capture performance and identify optimal operating regimes and cycles. We recommend this approach in contrast to exhaustive parametric studies which tend to depend on specifics of the chosen cycle and adsorbent. We show that appropriate combinations of process steps can yield excellent process performance and demonstrate how the pressure drop, and heat loss, etc. affect process performance through their effect on adsorption fronts and profiles. Finally, cyclic temperature profiles along the adsorption column can be readily used to infer concentration profiles-this has proved to be a very useful tool in cyclic function definition. Our research reveals excellent promise for the application of pressure/vacuum swing adsorption technology in the arena of CO2 capture from flue gases.

Development of a cost-effective CO2 adsorbent from petroleum coke via KOH activation

NASA Astrophysics Data System (ADS)

Jang, Eunji; Choi, Seung Wan; Hong, Seok-Min; Shin, Sangcheol; Lee, Ki Bong

2018-01-01

The capture of CO2 via adsorption is considered an effective technology for decreasing global warming issues; hence, adsorbents for CO2 capture have been actively developed. Taking into account cost-effectiveness and environmental concerns, the development of CO2 adsorbents from waste materials is attracting considerable attention. In this study, petroleum coke (PC), which is the carbon residue remaining after heavy oil upgrading, was used to produce high-value-added porous carbon for CO2 capture. Porous carbon materials were prepared by KOH activation using different weight ratios of KOH/PC (1:1, 2:1, 3:1, and 4:1) and activation temperatures (600, 700, and 800 °C). The specific surface area and total pore volume of resulting porous carbon materials increased with KOH amount, reaching up to 2433 m2/g and 1.11 cm3/g, respectively. The sample prepared under moderate conditions with a KOH/PC weight ratio of 2:1 and activation temperature of 700 °C exhibited the highest CO2 adsorption uptake of 3.68 mmol/g at 25 °C and 1 bar. Interestingly, CO2 adsorption uptake was linearly correlated with the volume of micropores less than 0.8 nm, indicating that narrow micropore volume is crucial for CO2 adsorption. The prepared porous carbon materials also exhibited good selectivity for CO2 over N2, rapid adsorption, facile regeneration, and stable adsorption-desorption cyclic performance, demonstrating potential as a candidate for CO2 capture.

Application of ultraviolet, ozone, and advanced oxidation treatments to washwaters to destroy nitrosamines, nitramines, amines, and aldehydes formed during amine-based carbon capture.

PubMed

Shah, Amisha D; Dai, Ning; Mitch, William A

2013-03-19

Although amine-based CO(2) absorption is a leading contender for full-scale postcombustion CO(2) capture at power plants, concerns have been raised about the potential release of carcinogenic N-nitrosamines and N-nitramines formed by reaction of exhaust gas NO(x) with the amines. Experiments with a laboratory-scale pilot unit suggested that washwater units meant to scrub contaminants from absorber unit exhaust could potentially serve as a source of N-nitrosamines via reactions of residual NO(x) with amines accumulating in the washwater. Dosage requirements for the continuous treatment of the washwater recycle line with ultraviolet (UV) light for destruction of N-nitrosamines and N-nitramines, and with ozone or hydroxyl radical-based advanced oxidation processes (AOPs) for destruction of amines and aldehydes, were evaluated. Although <1000 mJ/cm(2) UV fluence was generally needed for 90% removal of a series of model N-nitrosamines and N-nitramines, 280-1000 mJ/cm(2) average fluence was needed for 90% removal of total N-nitrosamines in pilot washwaters associated with two different solvents. While AOPs were somewhat more efficient than ozone for acetaldehyde destruction, ozone was more efficient for amine destruction. Ozone achieved 90% amine removal in washwaters at 5-12 molar excess of ozone, indicating transferred dosage levels of ∼100 mg/L for 90% removal in a first-stage washwater unit, but likely only ∼10 mg/L if applied to a second-stage washwater. Accurate dosage and cost estimates would require pilot testing to capture synergies between UV and ozone treatments.

Directed evolution of an ultrastable carbonic anhydrase for highly efficient carbon capture from flue gas

DOE PAGES

Alvizo, Oscar; Nguyen, Luan J.; Savile, Christopher K.; ...

2014-11-03

Carbonic anhydrase (CA) is one of nature’s fastest enzymes and can dramatically improve the economics of carbon capture under demanding environments such as coal-fired power plants. The use of CA to accelerate carbon capture is limited by the enzyme’s sensitivity to the harsh process conditions. Using directed evolution, the properties of a β-class CA from Desulfovibrio vulgaris were dramatically enhanced. Iterative rounds of library design, library generation, and high-throughput screening identified highly stable CA variants that tolerate temperatures of up to 107 °C in the presence of 4.2 M alkaline amine solvent at pH >10.0. This increase in thermostability andmore » alkali tolerance translates to a 4,000,000-fold improvement over the natural enzyme. In conclusion, at pilot scale, the evolved catalyst enhanced the rate of CO2 absorption 25-fold compared with the noncatalyzed reaction.« less

Directed evolution of an ultrastable carbonic anhydrase for highly efficient carbon capture from flue gas

PubMed Central

Alvizo, Oscar; Nguyen, Luan J.; Savile, Christopher K.; Bresson, Jamie A.; Lakhapatri, Satish L.; Solis, Earl O. P.; Fox, Richard J.; Broering, James M.; Benoit, Michael R.; Zimmerman, Sabrina A.; Novick, Scott J.; Liang, Jack; Lalonde, James J.

2014-01-01

Carbonic anhydrase (CA) is one of nature’s fastest enzymes and can dramatically improve the economics of carbon capture under demanding environments such as coal-fired power plants. The use of CA to accelerate carbon capture is limited by the enzyme’s sensitivity to the harsh process conditions. Using directed evolution, the properties of a β-class CA from Desulfovibrio vulgaris were dramatically enhanced. Iterative rounds of library design, library generation, and high-throughput screening identified highly stable CA variants that tolerate temperatures of up to 107 °C in the presence of 4.2 M alkaline amine solvent at pH >10.0. This increase in thermostability and alkali tolerance translates to a 4,000,000-fold improvement over the natural enzyme. At pilot scale, the evolved catalyst enhanced the rate of CO2 absorption 25-fold compared with the noncatalyzed reaction. PMID:25368146

Process modeling of an advanced NH₃ abatement and recycling technology in the ammonia-based CO₂ capture process.

PubMed

Li, Kangkang; Yu, Hai; Tade, Moses; Feron, Paul; Yu, Jingwen; Wang, Shujuan

2014-06-17

An advanced NH3 abatement and recycling process that makes great use of the waste heat in flue gas was proposed to solve the problems of ammonia slip, NH3 makeup, and flue gas cooling in the ammonia-based CO2 capture process. The rigorous rate-based model, RateFrac in Aspen Plus, was thermodynamically and kinetically validated by experimental data from open literature and CSIRO pilot trials at Munmorah Power Station, Australia, respectively. After a thorough sensitivity analysis and process improvement, the NH3 recycling efficiency reached as high as 99.87%, and the NH3 exhaust concentration was only 15.4 ppmv. Most importantly, the energy consumption of the NH3 abatement and recycling system was only 59.34 kJ/kg CO2 of electricity. The evaluation of mass balance and temperature steady shows that this NH3 recovery process was technically effective and feasible. This process therefore is a promising prospect toward industrial application.

Earth 2075 (CO2) - can Ocean-Amplified Carbon Capture (oacc) Impart Atmospheric CO2-SINKING Ability to CCS Fossil Energy?

NASA Astrophysics Data System (ADS)

Fry, R.; Routh, M.; Chaudhuri, S.; Fry, S.; Ison, M.; Hughes, S.; Komor, C.; Klabunde, K.; Sethi, V.; Collins, D.; Polkinghorn, W.; Wroobel, B.; Hughes, J.; Gower, G.; Shkolnik, J.

2017-12-01

Previous attempts to capture atmospheric CO2 by algal blooming were stalled by ocean viruses, zooplankton feeding, and/or bacterial decomposition of surface blooms, re-releasing captured CO2 instead of exporting it to seafloor. CCS fossil energy coupling could bypass algal bloom limits—enabling capture of 10 GtC/yr atmospheric CO2 by selective emiliania huxleyi (EHUX) blooming in mid-latitude open oceans, far from coastal waters and polar seas. This could enable a 500 GtC drawdown, 350 ppm restoration by 2050, 280 ppm CO2 by 2075, and ocean pH 8.2. White EHUX blooms could also reflect sunlight back into outer space and seed extra ocean cloud cover, via DMS release, to raise albedo 1.8%—restoring preindustrial temperature (ΔT = 0°C) by 2030. Open oceans would avoid post-bloom anoxia, exclusively a coastal water phenomenon. The EHUX calcification reaction initially sources CO2, but net sinking prevails in follow-up equilibration reactions. Heavier-than-water EHUX sink captured CO2 to the sea floor before surface decomposition occurs. Seeding EHUX high on their nonlinear growth curve could accelerate short-cycle secondary open-ocean blooming—overwhelming mid-latitude viruses, zooplankton, and competition from other algae. Mid-latitude "ocean deserts" exhibit low viral, zooplankton, and bacterial counts. Thermocline prevents nutrient upwelling that would otherwise promote competing algae. Adding nitrogen nutrient would foster exclusive EHUX blooming. Elevated EHUX seed levels could arise from sealed, pH-buffered, floating, seed-production bioreactors infused with 10% CO2 from carbon feedstock supplied by inland CCS fossil power plants capturing 90% of emissions as liquid CO2. Deep-water SPAR platforms extract natural gas from beneath the sea floor. On-platform Haber and pH processing could convert extracted CH4 to buffered NH4+ nutrient, enabling ≥0.7 GtC/yr of bioreactor seed production and 10 GtC/yr of amplified secondary open-ocean CO2 capture—making CCS fossil energy 1400% carbon negative.

Modeling Amorphous Microporous Polymers for CO2 Capture and Separations.

PubMed

Kupgan, Grit; Abbott, Lauren J; Hart, Kyle E; Colina, Coray M

2018-06-13

This review concentrates on the advances of atomistic molecular simulations to design and evaluate amorphous microporous polymeric materials for CO 2 capture and separations. A description of atomistic molecular simulations is provided, including simulation techniques, structural generation approaches, relaxation and equilibration methodologies, and considerations needed for validation of simulated samples. The review provides general guidelines and a comprehensive update of the recent literature (since 2007) to promote the acceleration of the discovery and screening of amorphous microporous polymers for CO 2 capture and separation processes.

Hierarchically Porous Carbon Materials for CO 2 Capture: The Role of Pore Structure

DOE Office of Scientific and Technical Information (OSTI.GOV)

Estevez, Luis; Barpaga, Dushyant; Zheng, Jian

2018-01-17

With advances in porous carbon synthesis techniques, hierarchically porous carbon (HPC) materials are being utilized as relatively new porous carbon sorbents for CO2 capture applications. These HPC materials were used as a platform to prepare samples with differing textural properties and morphologies to elucidate structure-property relationships. It was found that high microporous content, rather than overall surface area was of primary importance for predicting good CO2 capture performance. Two HPC materials were analyzed, each with near identical high surface area (~2700 m2/g) and colossally high pore volume (~10 cm3/g), but with different microporous content and pore size distributions, which ledmore » to dramatically different CO2 capture performance. Overall, large pore volumes obtained from distinct mesopores were found to significantly impact adsorption performance. From these results, an optimized HPC material was synthesized that achieved a high CO2 capacity of ~3.7 mmol/g at 25°C and 1 bar.« less

Novel Supercritical Carbon Dioxide Power Cycle Utilizing Pressured Oxy-combustion in Conjunction with Cryogenic Compression

DOE Office of Scientific and Technical Information (OSTI.GOV)

Brun, Klaus; McClung, Aaron; Davis, John

2014-03-31

The team of Southwest Research Institute® (SwRI) and Thar Energy LLC (Thar) applied technology engineering and economic analysis to evaluate two advanced oxy-combustion power cycles, the Cryogenic Pressurized Oxy-combustion Cycle (CPOC), and the Supercritical Oxy-combustion Cycle. This assessment evaluated the performance and economic cost of the two proposed cycles with carbon capture, and included a technology gap analysis of the proposed technologies to determine the technology readiness level of the cycle and the cycle components. The results of the engineering and economic analysis and the technology gap analysis were used to identify the next steps along the technology development roadmapmore » for the selected cycle. The project objectives, as outlined in the FOA, were 90% CO{sub 2} removal at no more than a 35% increase in cost of electricity (COE) as compared to a Supercritical Pulverized Coal Plant without CO{sub 2} capture. The supercritical oxy-combustion power cycle with 99% carbon capture achieves a COE of $121/MWe. This revised COE represents a 21% reduction in cost as compared to supercritical steam with 90% carbon capture ($137/MWe). However, this represents a 49% increase in the COE over supercritical steam without carbon capture ($80.95/MWe), exceeding the 35% target. The supercritical oxy-combustion cycle with 99% carbon capture achieved a 37.9% HHV plant efficiency (39.3% LHV plant efficiency), when coupling a supercritical oxy-combustion thermal loop to an indirect supercritical CO{sub 2} (sCO{sub 2}) power block. In this configuration, the power block achieved 48% thermal efficiency for turbine inlet conditions of 650°C and 290 atm. Power block efficiencies near 60% are feasible with higher turbine inlet temperatures, however a design tradeoff to limit firing temperature to 650°C was made in order to use austenitic stainless steels for the high temperature pressure vessels and piping and to minimize the need for advanced turbomachinery features such as blade cooling. The overall technical readiness of the supercritical oxy-combustion cycle is TRL 2, Technology Concept, due to the maturity level of the supercritical oxy-combustor for solid fuels, and several critical supporting components, as identified in the Technical Gap Analysis. The supercritical oxycombustor for solid fuels operating at pressures near 100 atm is a unique component of the supercritical oxy-combustion cycle. In addition to the low TRL supercritical oxy-combustor, secondary systems were identified that would require adaptation for use with the supercritical oxycombustion cycle. These secondary systems include the high pressure pulverized coal feed, high temperature cyclone, removal of post-combustion particulates from the high pressure cyclone underflow stream, and micro-channel heat exchangers tolerant of particulate loading. Bench scale testing was utilized to measure coal combustion properties at elevated pressures in a CO{sub 2} environment. This testing included coal slurry preparation, visualization of coal injection into a high pressure fluid, and modification of existing test equipment to facilitate the combustion properties testing. Additional bench scale testing evaluated the effectiveness of a rotary atomizer for injecting a coal-water slurry into a fluid with similar densities, as opposed to the typical application where the high density fluid is injected into a low density fluid. The swirl type supercritical oxy-combustor was developed from initial concept to an advanced design stage through numerical simulation using FLUENT and Chemkin to model the flow through the combustor and provide initial assessment of the coal combustion reactions in the flow path. This effort enabled the initial combustor mechanical layout, initial pressure vessel design, and the conceptual layout of a pilot scale test loop. A pilot scale demonstration of the supercritical oxy-combustion cycle is proposed as the next step in the technology development. This demonstration would advance the supercritical oxy-combustion cycle and the supercritical oxy-combustor from a current TRL of 2, Technology Concept, to TRL 6, Pilot Scale System Demonstrated in a Relevant Environment, and enable the evaluation and continued refinement of the supercritical oxy-combustor and critical secondary systems.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Johnson, Terry Alan; Hogan, Roy E., Jr.; McDaniel, Anthony H.

Two of the most daunting problems facing humankind in the twenty-first century are energy security and climate change. This report summarizes work accomplished towards addressing these problems through the execution of a Grand Challenge LDRD project (FY09-11). The vision of Sunshine to Petrol is captured in one deceptively simple chemical equation: Solar Energy + xCO{sub 2} + (x+1)H{sub 2}O {yields} C{sub x}H{sub 2x+2}(liquid fuel) + (1.5x+.5)O{sub 2} Practical implementation of this equation may seem far-fetched, since it effectively describes the use of solar energy to reverse combustion. However, it is also representative of the photosynthetic processes responsible for much ofmore » life on earth and, as such, summarizes the biomass approach to fuels production. It is our contention that an alternative approach, one that is not limited by efficiency of photosynthesis and more directly leads to a liquid fuel, is desirable. The development of a process that efficiently, cost effectively, and sustainably reenergizes thermodynamically spent feedstocks to create reactive fuel intermediates would be an unparalleled achievement and is the key challenge that must be surmounted to solve the intertwined problems of accelerating energy demand and climate change. We proposed that the direct thermochemical conversion of CO{sub 2} and H{sub 2}O to CO and H{sub 2}, which are the universal building blocks for synthetic fuels, serve as the basis for this revolutionary process. To realize this concept, we addressed complex chemical, materials science, and engineering problems associated with thermochemical heat engines and the crucial metal-oxide working-materials deployed therein. By project's end, we had demonstrated solar-driven conversion of CO{sub 2} to CO, a key energetic synthetic fuel intermediate, at 1.7% efficiency.« less

Human health risk assessment of nitrosamines and nitramines for potential application in CO2 capture.

PubMed

Ravnum, S; Rundén-Pran, E; Fjellsbø, L M; Dusinska, M

2014-07-01

Emission and accumulation of carbon dioxide (CO2) in the atmosphere exert an environmental and climate change challenge. An attempt to deal with this challenge is made at Mongstad by application of amines for CO2 capture and storage (CO2 capture Mongstad (CCM) project). As part of the CO2 capture process, nitrosamines and nitramines may be emitted. Toxicological testing of nitrosamines and nitramines indicate a genotoxic potential of these substances. Here we present a risk characterization and assessment for five nitrosamines (N-Nitrosodi-methylamine (NDMA) N-Nitrosodi-ethylamine (NDEA), N-Nitroso-morpholine (NNM), N-Nitroso-piperidine (NPIP), and Dinitroso-piperazine (DNP)) and two nitramines (N-Methyl-nitramine (NTMA), Dimethyl-nitramine (NDTMA)), which are potentially emitted from the CO2 capture plant (CCP). Human health risk assessment of genotoxic non-threshold substances is a heavily debated topic, and no consensus methodology exists internationally. Extrapolation modeling from high-dose animal exposures to low-dose human exposures can be crucial for the final risk calculation. In the work presented here, different extrapolation models are discussed, and suggestions on applications are given. Then, preferred methods for calculating derived minimal effect level (DMEL) are presented with the selected nitrosamines and nitramines. Copyright © 2014 Elsevier Inc. All rights reserved.

Performance, cost and environmental assessment of gasification-based electricity in India: A preliminary analysis

NASA Astrophysics Data System (ADS)

Rani, Abha; Singh, Udayan; Jayant; Singh, Ajay K.; Sankar Mahapatra, Siba

2017-07-01

Coal gasification processes are crucial to decarbonisation in the power sector. While underground coal gasification (UCG) and integrated gasification combined cycle (IGCC) are different in terms of the site of gasification, they have considerable similarities in terms of the types of gasifiers used. Of course, UCG offers some additional advantages such as reduction of the fugitive methane emissions accompanying the coal mining process. Nevertheless, simulation of IGCC plants involving surface coal gasification is likely to give reasonable indication of the 3E (efficiency, economics and emissions) prospects of the gasification pathway towards electricity. This paper will aim at Estimating 3E impacts (efficiency, environment, economics) of gasification processes using simulation carried out in the Integrated Environmental Control Model (IECM) software framework. Key plant level controls which will be studied in this paper will be based on Indian financial regulations and operating costs which are specific to the country. Also, impacts of CO2 capture and storage (CCS) in these plants will be studied. The various parameters that can be studied are plant load factor, impact of coal quality and price, type of CO2 capture process, capital costs etc. It is hoped that relevant insights into electricity generation from gasification may be obtained with this paper.

Influence of periodically changing oxidizing and reducing environment on sulfur capture under PFBC conditions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yrjas, P.; Hupa, M.

1997-12-31

In the literature it has been reported that sulfur capture with limestone (CaCO{sub 3}) under atmospheric fluidized bed combustion conditions reaches a maximum at about 850 C. Previously, the maximum has been attributed to the sintering of the sorbent particles which decreases the reactive surface area. Lately, also another explanation has been reported. In this case the sulfur capture decrease at higher temperatures was concluded to be due to fluctuating oxidizing/reducing conditions in the atmospheric combustor. In this paper the influence of alternating oxidizing/reducing conditions on SO{sub 2} capture at atmospheric and elevated pressure (15 bar) is reported. In themore » pressurized case, the CO{sub 2} partial pressure was kept high enough to prevent CaCO{sub 3} from calcining and therefore the CaSO{sub 4} would not form CaO but CaCO{sub 3} from calcining and therefore the CaSO{sub 4} would not form CaO but CaCO{sub 3} under reducing conditions. The experiments were done with a pressurized TGA by periodically changing the gas environment between oxidizing (O{sub 2}, SO{sub 2}, CO{sub 2} and N{sub 2}) and slightly reducing (CO, SO{sub 2}, CO{sub 2} and N{sub 2}) gas mixtures at different temperatures. The results showed that under normal pressure and slightly reducing conditions CaO formation from CaSO{sub 4} increased with temperature as expected. However, no significant amounts of CaCO{sub 3} were formed from CaSO{sub 4} at elevated pressure. It was also concluded that since the formation of CaO from CaSO{sub 4} was relatively slow it could not explain the sharp sulfur capture maximum at about 850 C. Therefore, it was assumed that the strongly reducing zones, where CaS thermodynamically is the stable compound, may play a more important role than the slightly reducing zones, concerning the sulfur capture in fluidized bed combustors.« less

The long-run effects of economic, demographic, and political indices on actual and potential CO2 emissions.

PubMed

Adom, Philip Kofi; Kwakwa, Paul Adjei; Amankwaa, Afua

2018-07-15

This study examines the long-run drivers of potential and actual CO 2 emissions in Ghana, a sub-Saharan Africa country. The use of the former helps address the reverse causality problem and capture the true long-run effects. The Stock-Watson dynamic OLS is used with data from 1970 to 2014. The result shows that potential CO 2 emissions improve model efficiency. Income (except in "other sector") and financial development (except in manufacturing and construction sector) have compelling positive and negative effects on actual and potential CO 2 emissions, respectively. A higher price (oil and electricity) reduces actual and potential CO 2 emissions, but electricity price is more vital in residential, buildings and commercial and public services sector, while oil price is crucial in the transport sector. Democracy lowers actual and potential CO 2 emissions in the aggregate (insignificant) and transport sectors but raises it in the manufacturing and construction sector. The effect is, however, inconsistent for the remaining sectors. Urbanization raises aggregate actual and potential CO 2 emissions, but the effect is inconsistent for the transport sector. The findings have important implications for policy formulation. Copyright © 2018 Elsevier Ltd. All rights reserved.

Computational materials chemistry for carbon capture using porous materials

NASA Astrophysics Data System (ADS)

Sharma, Abhishek; Huang, Runhong; Malani, Ateeque; Babarao, Ravichandar

2017-11-01

Control over carbon dioxide (CO2) release is extremely important to decrease its hazardous effects on the environment such as global warming, ocean acidification, etc. For CO2 capture and storage at industrial point sources, nanoporous materials offer an energetically viable and economically feasible approach compared to chemisorption in amines. There is a growing need to design and synthesize new nanoporous materials with enhanced capability for carbon capture. Computational materials chemistry offers tools to screen and design cost-effective materials for CO2 separation and storage, and it is less time consuming compared to trial and error experimental synthesis. It also provides a guide to synthesize new materials with better properties for real world applications. In this review, we briefly highlight the various carbon capture technologies and the need of computational materials design for carbon capture. This review discusses the commonly used computational chemistry-based simulation methods for structural characterization and prediction of thermodynamic properties of adsorbed gases in porous materials. Finally, simulation studies reported on various potential porous materials, such as zeolites, porous carbon, metal organic frameworks (MOFs) and covalent organic frameworks (COFs), for CO2 capture are discussed.

Reinventing Design Principles for Developing Low-Viscosity Carbon Dioxide-Binding Organic Liquids for Flue Gas Clean Up.

PubMed

Malhotra, Deepika; Koech, Phillip K; Heldebrant, David J; Cantu, David C; Zheng, Feng; Glezakou, Vassiliki-Alexandra; Rousseau, Roger

2017-02-08

Anthropogenic CO 2 emissions from point sources (e.g., coal fired-power plants) account for the majority of the greenhouse gases in the atmosphere. Water-lean solvent systems such as CO 2 -binding organic liquids (CO 2 BOLs) are being developed to reduce the energy requirement for CO 2 capture. Many water-lean solvents such as CO 2 BOLs are currently limited by the high viscosities of concentrated electrolyte solvents, thus many of these solvents have yet to move toward commercialization. Conventional standard trial-and-error approaches for viscosity reduction, while effective, are time consuming and economically expensive. We rethink the metrics and design principles of low-viscosity CO 2 -capture solvents using a combined synthesis and computational modeling approach. We critically study the effects of viscosity reducing factors such as orientation of hydrogen bonding, introduction of higher degrees of freedom, and cation or anion charge solvation, and assess whether or how each factor affects viscosity of CO 2 BOL CO 2 capture solvents. Ultimately, we found that hydrogen bond orientation and strength is the predominant factor influencing the viscosity in CO 2 BOL solvents. With this knowledge, a new CO 2 BOL variant, 1-MEIPADM-2-BOL, was synthesized and tested, resulting in a solvent that is approximately 60 % less viscous at 25 mol % CO 2 loading than our base compound 1-IPADM-2-BOL. The insights gained from the current study redefine the fundamental concepts and understanding of what influences viscosity in concentrated organic CO 2 -capture solvents. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Multi-Fluid Geothermal Energy Systems: Using CO2 for Dispatchable Renewable Power Generation and Grid Stabilization

NASA Astrophysics Data System (ADS)

Buscheck, T. A.; Bielicki, J. M.; Randolph, J.; Chen, M.; Hao, Y.; Sun, Y.

2013-12-01

Abstract We present an approach to use CO2 to (1) generate dispatchable renewable power that can quickly respond to grid fluctuations and be cost-competitive with natural gas, (2) stabilize the grid by efficiently storing large quantities of energy, (3) enable seasonal storage of solar thermal energy for grid integration, (4) produce brine for power-plant cooling, all which (5) increase CO2 value, rendering CO2 capture to be commerically viable, while (6) sequestering huge quantities of CO2. These attributes reduce carbon intensity of electric power, and enable cost-competitive, dispatchable power from major sources of renewable energy: wind, solar, and geothermal. Conventional geothermal power systems circulate brine as the working fluid to extract heat, but the parasitic power load for this circulation can consume a large portion of gross power output. Recently, CO2 has been considered as a working fluid because its advantageous properties reduce this parasitic loss. We expand on this idea by using multiple working fluids: brine, CO2, and N2. N2 can be separated from air at lower cost than captured CO2, it is not corrosive, and it will not react with the formation. N2 also can improve the economics of energy production and enable energy storage, while reducing operational risk. Extracting heat from geothermal reservoirs often requires submersible pumps to lift brine, but these pumps consume much of the generated electricity. In contrast, our approach drives fluid circulation by injecting supplemental, compressible fluids (CO2, and N2) with high coefficients of thermal expansion. These fluids augment reservoir pressure, produce artesian flow at the producers, and reduce the parasitic load. Pressure augmentation is improved by the thermosiphon effect that results from injecting cold/dense CO2 and N2. These fluids are heated to reservoir temperature, greatly expand, and increase the artesian flow of brine and supplemental fluid at the producers. Rather than using pumps, the thermosiphon directly converts reservoir thermal energy into mechanical energy for fluid circulation. Because stored pressure drives fluid production, the response time is faster than that of conventional geothermal power, already considered to be dispatchable. For conventional geothermal, the parasitic power load is in phase with gross power output. In contrast, our approach can time-shift much of the parasitic power load, which is dominated by the power required to separate N2 from air and compress it for injection. Because N2 is readily available, it can be injected intermittently. Thus, most of the parasitic power load can be shifted to coincide with minimum power demand or when there is a surplus of renewable power. Such a time-shift also allows net power output to be nearly equal to gross power output during peak demand. Energy storage can be almost 100 percent efficient because it is achieved by shifting the parasitic load, which is more efficient than other methods used to store energy and stabilize the grid. This work was performed under the auspices of the U.S. DOE by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344.

High CO2 absorption capacity by chemisorption at cations and anions in choline-based ionic liquids.

PubMed

Bhattacharyya, Shubhankar; Filippov, Andrei; Shah, Faiz Ullah

2017-11-29

The effect of CO 2 absorption on the aromaticity and hydrogen bonding in ionic liquids is investigated. Five different ionic liquids with choline based cations and aprotic N-heterocyclic anions were synthesized. Purity and structures of the synthesized ionic liquids were characterized by 1 H and 13 C NMR spectroscopy. CO 2 capture performance was studied at 20 °C and 40 °C under three different pressures (1, 3, 6 bar). The IL [N 1,1,6,2OH ][4-Triz] showed the highest CO 2 capture capacity (28.6 wt%, 1.57 mol of CO 2 per mol of the IL, 6.48 mol of CO 2 per kg of the ionic liquid) at 20 °C and 1 bar. The high CO 2 capture capacity of the [N 1,1,6,2OH ][4-Triz] IL is due to the formation of carbonic acid (-OCO 2 H) together with carbamate by participation of the -OH group of the [N 1,1,6,2OH ] + cation in the CO 2 capture process. The structure of the adduct formed by CO 2 reaction with the IL [N 1,1,6,2OH ][4-Triz] was probed by using IR, 13 C NMR and 1 H- 13 C HMBC NMR experiments utilizing 13 C labeled CO 2 gas. 1 H and 13 C PFG NMR studies were performed before and after CO 2 absorption to explore the effect of cation-anion structures on the microscopic ion dynamics in ILs. The ionic mobility was significantly increased after CO 2 reaction due to lowering of aromaticity in the case of ILs with aromatic N-heterocyclic anions.

Biorefineries of carbon dioxide: From carbon capture and storage (CCS) to bioenergies production.

PubMed

Cheah, Wai Yan; Ling, Tau Chuan; Juan, Joon Ching; Lee, Duu-Jong; Chang, Jo-Shu; Show, Pau Loke

2016-09-01

Greenhouse gas emissions have several adverse environmental effects, like pollution and climate change. Currently applied carbon capture and storage (CCS) methods are not cost effective and have not been proven safe for long term sequestration. Another attractive approach is CO2 valorization, whereby CO2 can be captured in the form of biomass via photosynthesis and is subsequently converted into various form of bioenergy. This article summarizes the current carbon sequestration and utilization technologies, while emphasizing the value of bioconversion of CO2. In particular, CO2 sequestration by terrestrial plants, microalgae and other microorganisms are discussed. Prospects and challenges for CO2 conversion are addressed. The aim of this review is to provide comprehensive knowledge and updated information on the current advances in biological CO2 sequestration and valorization, which are essential if this approach is to achieve environmental sustainability and economic feasibility. Copyright © 2016 Elsevier Ltd. All rights reserved.

Feasibility Study of Regenerative Burners in Aluminum Holding Furnaces

NASA Astrophysics Data System (ADS)

Hassan, Mohamed I.; Al Kindi, Rashid

2014-09-01

Gas-fired aluminum holding reverberatory furnaces are currently considered to be the lowest efficiency fossil fuel system. A considerable volume of gas is consumed to hold the molten metal at temperature that is much lower than the flame temperature. This will lead to more effort and energy consumption to capture the excessive production of the CO2. The concern of this study is to investigate the feasibility of the regenerative-burners' furnaces to increase the furnace efficiency to reduce gas consumption per production and hence result in less CO2 production. Energy assessments for metal holding furnaces are considered at different operation conditions. Onsite measurements, supervisory control and data acquisition data, and thermodynamics analysis are performed to provide feasible information about the gas consumption and CO2 production as well as area of improvements. In this study, onsite measurements are used with thermodynamics modeling to assess a 130 MT rectangular furnace with two regenerative burners and one cold-air holding burner. The assessment showed that the regenerative burner furnaces are not profitable in saving energy, in addition to the negative impact on the furnace life. However, reducing the holding and door opening time would significantly increase the operation efficiency and hence gain the benefit of the regenerative technology.

Improved Mapping of Carbon, Water and Energy Land-Surface Fluxes Using Remotely Sensed Indicators of Canopy Light Use Efficiency

NASA Astrophysics Data System (ADS)

Schull, M. A.; Anderson, M. C.; Kustas, W.; Cammalleri, C.; Houborg, R.

2012-12-01

A light-use-efficiency (LUE) based model of canopy resistance has been embedded into a thermal-based Two-Source Energy Balance (TSEB) model to facilitate coupled simulations of transpiration and carbon assimilation. The model assumes that deviations of the observed canopy LUE from a nominal stand-level value (LUEn - typically indexed by vegetation class) are due to varying conditions of light, humidity, CO2 concentration and leaf temperature. The deviations are accommodated by adjusting an effective LUE that responds to the varying conditions. The challenge to monitoring fluxes on a larger scale is to capture the physiological responses due to changing conditions. This challenge can be met using remotely sensed leaf chlorophyll (Cab). Since Cab is a vital pigment for absorbing light for use in photosynthesis, it has been recognized as a key parameter for quantifying photosynthetic functioning that are sensitive to these conditions. Recent studies have shown that it is sensitive to changes in LUE, which defines how efficiently a plant can assimilate carbon dioxide (CO2) given the absorbed Photosynthetically Active Radiation (PAR) and is therefore useful for monitoring carbon fluxes. We investigate the feasibility of leaf chlorophyll to capture these variations in LUEn using remotely sensed data. To retrieve Cab from remotely sensed data we use REGFLEC, a physically based tool that translates at-sensor radiances in the green, red and NIR spectral regions from multiple satellite sensors into realistic maps of LAI and Cab. Initial results show that Cab is exponentially correlated to light use efficiency. Incorporating nominal light use efficiency estimated from Cab is shown to improve fluxes of carbon, water and energy most notably in times of stressed vegetation. The result illustrates that Cab is sensitive to changes in plant physiology and can capture plant stress needed for improved estimation of fluxes. The observed relationship and initial results demonstrate the need for integrating remotely sensed Cab to facilitate improved mapping of coupled carbon, water, and energy fluxes across vegetated landscapes.

The U. S. DOE Carbon Storage Program: Status and Future Directions

NASA Astrophysics Data System (ADS)

Damiani, D.

2016-12-01

The U.S. Department of Energy (DOE) is taking steps to reduce carbon dioxide (CO2) emissions through clean energy innovation, including carbon capture and storage (CCS) research. The Office of Fossil Energy Carbon Storage Program is focused on ensuring the safe and permanent storage and/or utilization of CO2 captured from stationary sources. The Program is developing and advancing geologic storage technologies both onshore and offshore that will significantly improve the effectiveness of CCS, reduce the cost of implementation, and be ready for widespread commercial deployment in the 2025-2035 timeframe. The technology development and field testing conducted through this Program will be used to benefit the existing and future fleet of fossil fuel power generating and industrial facilities by creating tools to increase our understanding of geologic reservoirs appropriate for CO2 storage and the behavior of CO2 in the subsurface. The Program is evaluating the potential for storage in depleted oil and gas reservoirs, saline formations, unmineable coal, organic-rich shale formations, and basalt formations. Since 1997, DOE's Carbon Storage Program has significantly advanced the CCS knowledge base through a diverse portfolio of applied research projects. The Core Storage R&D research component focuses on analytic studies, laboratory, and pilot- scale research to develop technologies that can improve wellbore integrity, increase reservoir storage efficiency, improve management of reservoir pressure, ensure storage permanence, quantitatively assess risks, and identify and mitigate potential release of CO2 in all types of storage formations. The Storage Field Management component focuses on scale-up of CCS and involves field validation of technology options, including large-volume injection field projects at pre-commercial scale to confirm system performance and economics. Future research involves commercial-scale characterization for regionally significant storage locations capable of storing from 50 to 100 million metric tons of CO2 in a saline formation. These projects will lay the foundation for fully integrated carbon capture and storage demonstrations of future first of a kind (FOAK) coal power projects. Future research will also bring added focus on offshore CCS.

C3 and C4 biomass allocation responses to elevated CO2 and nitrogen: contrasting resource capture strategies

USGS Publications Warehouse

White, K.P.; Langley, J.A.; Cahoon, D.R.; Megonigal, J.P.

2012-01-01

Plants alter biomass allocation to optimize resource capture. Plant strategy for resource capture may have important implications in intertidal marshes, where soil nitrogen (N) levels and atmospheric carbon dioxide (CO2) are changing. We conducted a factorial manipulation of atmospheric CO2 (ambient and ambient + 340 ppm) and soil N (ambient and ambient + 25 g m-2 year-1) in an intertidal marsh composed of common North Atlantic C3 and C4 species. Estimation of C3 stem turnover was used to adjust aboveground C3 productivity, and fine root productivity was partitioned into C3-C4 functional groups by isotopic analysis. The results suggest that the plants follow resource capture theory. The C3 species increased aboveground productivity under the added N and elevated CO2 treatment (P 2 alone. C3 fine root production decreased with added N (P 2 (P = 0.0481). The C4 species increased growth under high N availability both above- and belowground, but that stimulation was diminished under elevated CO2. The results suggest that the marsh vegetation allocates biomass according to resource capture at the individual plant level rather than for optimal ecosystem viability in regards to biomass influence over the processes that maintain soil surface elevation in equilibrium with sea level.

Microporous metal organic framework [M2(hfipbb)2(ted)] (M=Zn, Co; H2hfipbb=4,4-(hexafluoroisopropylidene)-bis(benzoic acid); ted=triethylenediamine): Synthesis, structure analysis, pore characterization, small gas adsorption and CO2/N2 separation properties

NASA Astrophysics Data System (ADS)

Xu, William W.; Pramanik, Sanhita; Zhang, Zhijuan; Emge, Thomas J.; Li, Jing

2013-04-01

Carbon dioxide is a greenhouse gas that is a major contributor to global warming. Developing methods that can effectively capture CO2 is the key to reduce its emission to the atmosphere. Recent research shows that microporous metal organic frameworks (MOFs) are emerging as a promising family of adsorbents that may be promising for use in adsorption based capture and separation of CO2 from power plant waste gases. In this work we report the synthesis, crystal structure analysis and pore characterization of two microporous MOF structures, [M2(hfipbb)2(ted)] (M=Zn (1), Co (2); H2hfipbb=4,4-(hexafluoroisopropylidene)-bis(benzoic acid); ted=triethylenediamine). The CO2 and N2 adsorption experiments and IAST calculations are carried out on [Zn2(hfipbb)2(ted)] under conditions that mimic post-combustion flue gas mixtures emitted from power plants. The results show that the framework interacts with CO2 strongly, giving rise to relatively high isosteric heats of adsorption (up to 28 kJ/mol), and high adsorption selectivity for CO2 over N2, making it promising for capturing and separating CO2 from CO2/N2 mixtures.

Amine-impregnated silica monolith with a hierarchical pore structure: enhancement of CO2 capture capacity.

PubMed

Chen, Chao; Yang, Seung-Tae; Ahn, Wha-Seung; Ryoo, Ryong

2009-06-28

A polyethylenimine-impregnated hierarchical silica monolith exhibited significantly higher CO(2) capturing capacity than other silica-supported amine sorbents, and produced a reversible and durable sorption performance.

Novel Inorganic/Polymer Composite Membranes for CO 2 Capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ho, W.S. Winston; Dutta, Prabir K.; Schmit, Steve J.

The objective of this project is to develop a cost-effective design and manufacturing process for new membrane modules that capture CO 2 from flue gas in coal-fired power plants. The membrane consisted of a thin selective layer including inorganic (zeolite) embedded in a polymer structure so that it can be made in a continuous manufacturing process. The membrane was incorporated in spiral-wound modules for the field test with actual flue gas at the National Carbon Capture Center (NCCC) in Wilsonville, AL and bench scale tests with simulated flue gas at the Ohio State University (OSU). Using the modules for post-combustionmore » CO 2 capture is expected to achieve the DOE target of $40/tonne CO 2 captured (in 2007 dollar) for 2025. Membranes with the amine-containing polymer cover layer on zeolite-Y (ZY) nanoparticles deposited on the polyethersulfone (PES) substrate were successfully synthesized. The membranes showed a high CO 2 permeance of about 1100 GPU (gas permeation unit, 1 GPU = 10 -6 cm 3 (STP)/(cm 2 • s • cm Hg), 3000 GPU = 10-6 mol/(m 2 • s • Pa)) with a high CO 2/N 2 selectivity of > 200 at the typical flue gas conditions at 57°C (about 17% water vapor in feed gas) and > 1400 GPU CO 2 permeance with > 500 CO 2/N 2 selectivity at 102°C (~ 80% water vapor). The synthesis of ZY nanoparticles was successfully scaled up, and the pilot-scale membranes were also successfully fabricated using the continuous membrane machine at OSU. The transport performance of the pilot-scale membranes agreed reasonably well with the lab-scale membranes. The results from both the lab-scale and scale-up membranes were used for the techno-economic analysis. The scale-up membranes were fabricated into prototype spiral-wound membrane modules for continuous testing with simulated or real flue gas. For real flue gas testing, we worked with NCCC, in consultation with TriSep Corporation, Gradient Technology and American Electric Power (AEP). The membrane module demonstrated > 800 GPU of CO 2 permeance and > 150 CO 2/N 2 selectivity when tested with real flue gas at NCCC. The results obtained were used to update the techno-economic analysis. In addition, the EH&S assessment of the membranes for post-combustion CO 2 capture was conducted.« less

Humidity-swing mechanism for CO2 capture from ambient air.

PubMed

Yang, Hao; Singh, Manmilan; Schaefer, Jacob

2018-05-10

A humidity-swing polymeric sorbent captures CO2 from ambient air at room temperature simply by changing the humidity level. To date there has been no direct experimental evidence to characterize the chemical mechanism for this process. In this report we describe the use of solid-state NMR to study the humidity-swing CO2 absorption/desorption cycle directly. We find that at low humidity levels CO2 is absorbed as HCO3-. At high humidity levels, HCO3- is replaced by hydrated OH- and the absorbed CO2 is released.

Pre-combustion CO2 capture by transition metal ions embedded in phthalocyanine sheets

NASA Astrophysics Data System (ADS)

Lü, Kun; Zhou, Jian; Zhou, Le; Chen, X. S.; Chan, Siew Hwa; Sun, Qiang

2012-06-01

Transition metal (TM) embedded two-dimensional phthalocyanine (Pc) sheets have been recently synthesized in experiments [M. Abel, S. Clair, O. Ourdjini, M. Mossoyan, and L. Porte, J. Am. Chem. Soc. 133, 1203 (2010)], 10.1021/ja108628r, where the transition metal ions are uniformly distributed in porous structures, providing the possibility of capturing gas molecules. Using first principles and grand canonical Monte Carlo simulations, TMPc sheets (TM = Sc, Ti, and Fe) are studied for pre-combustion CO2 capture by considering the adsorptions of H2/CO2 gas mixtures. It is found that ScPc sheet shows a good selectivity for CO2, and the excess uptake capacity of single-component CO2 on ScPc sheet at 298 K and 50 bar is found to be 2949 mg/g, larger than that of any other reported porous materials. Furthermore, electrostatic potential and natural bond orbital analyses are performed to reveal the underlying interaction mechanisms, showing that electrostatic interactions as well as the donation and back donation of electrons between the transition metal ions and the CO2 molecules play a key role in the capture.

Potassium-based sorbents from fly ash for high-temperature CO2 capture.

PubMed

Sanna, Aimaro; Maroto-Valer, M Mercedes

2016-11-01

Potassium-fly ash (K-FA) sorbents were investigated for high-temperature CO 2 sorption. K-FAs were synthesised using coal fly ash as source of silica and aluminium. The synthesised materials were also mixed with Li 2 CO 3 and Ca(OH) 2 to evaluate their effect on CO 2 capture. Temperature strongly affected the performance of the K-FA sorbents, resulting in a CO 2 uptake of 1.45 mmol CO 2 /g sorbent for K-FA 1:1 at 700 °C. The CO 2 sorption was enhanced by the presence of Li 2 CO 3 (10 wt%), with the K-FA 1:1 capturing 2.38 mmol CO 2 /g sorbent at 700 °C in 5 min. This sorption was found to be similar to previously developed Li-Na-FA (2.54 mmol/g) and Li-FA (2.4 mmol/g) sorbents. The presence of 10 % Li 2 CO 3 also accelerated sorption and desorption. The results suggest that the increased uptake of CO 2 and faster reaction rates in presence of K-FA can be ascribed to the formation of K-Li eutectic phase, which favours the diffusion of potassium and CO 2 in the material matrix. The cyclic experiments showed that the K-FA materials maintained stable CO 2 uptake and reaction rates over 10 cycles.

Sequential capture of CO2 and SO2 in a pressurized TGA simulating FBC conditions.

PubMed

Sun, Ping; Grace, John R; Lim, C Jim; Anthony, Edward J

2007-04-15

Four FBC-based processes were investigated as possible means of sequentially capturing SO2 and CO2. Sorbent performance is the key to their technical feasibility. Two sorbents (a limestone and a dolomite) were tested in a pressurized thermogravimetric analyzer (PTGA). The sorbent behaviors were explained based on complex interaction between carbonation, sulfation, and direct sulfation. The best option involved using limestone or dolomite as a SO2-sorbent in a FBC combustor following cyclic CO2 capture. Highly sintered limestone is a good sorbent for SO2 because of the generation of macropores during calcination/carbonation cycling.

Synergistic effect of Fe2O3/Ho2O3 Co-modified 2D-titanate heterojunctions on enhanced photocatalytic degradation

NASA Astrophysics Data System (ADS)

Zhao, Xiaona; Liu, Xinzhao; Lu, Dingze; Wu, Pei; Yan, Qiuyang; Liu, Min; Fang, Pengfei

2017-01-01

TiO2-based nanosheets (TNSs) co-modified by Fe2O3 and Ho2O3 were synthesized by one-pot hydrothermal method using Fe(NO3)3 and Ho(NO3)3 as precursors compositing with TiO2. The Fe2O3/Ho2O3-TNSs heterojunctions possessed a thickness of approximately 3-4 nm, large specific surface area of 210-310 cm2/g, with Fe2O3 and Ho2O3 nanoparticles highly dispersed over the surface of the nanosheets. The crystallization of the samples gradually increased with the amount of Fe2O3 nanoparticles, which was confirmed by the XRD, BET and Raman spectra, indicating that Ho2O3 and Fe2O3 influenced the crystallinity and structure evolution of the TNSs, besides, led to an improved the visible-light absorption. Surface photocurrent and fluorescence spectral studies revealed that the photo-generated charge carrier separation efficiency could be efficiently improved by an appropriate amount of modification. The Fe2O3/Ho2O3-TNSs exhibited synergistic effect on photocatalytic degradation of RhB as well as MO under visible light. The highest efficiency was obtained by 0.05%-Fe2O3/Ho2O3-TNSs (Fe:Ho:Ti = 0.05:1:100), which was 8.86 and 6.72 times than that of individual 1.0%-Ho2O3-TNSs (Ho:Ti = 1:100) and 0.05%-Fe2O3-TNSs (Fe:Ti = 0.05:100), respectively. The possible mechanism for enhanced visible-light-induced photocatalytic activity was proposed. Ho2O3 introduced in the photocatalysts may act as the hole capture while Fe2O3 may share the same Fermi levels with TNSs and serve as the electron capture center in the n-n-p system, which reduced the recombination rate of photo-induced electron-hole pairs.

Microwave-assisted nitric acid treatment of sepiolite and functionalization with polyethylenimine applied to CO2 capture and CO2/N2 separation

NASA Astrophysics Data System (ADS)

Vilarrasa-García, E.; Cecilia, J. A.; Bastos-Neto, M.; Cavalcante, C. L.; Azevedo, D. C. S.; Rodríguez-Castellón, E.

2017-07-01

Sepiolite was treated in HNO3 solutions with the assistance of microwave radiation. This treatment caused the progressive depletion of Mg2+, the gradual degradation of the sepiolite structure and the formation of an amorphous silica phase, which contributes to a noticeable increase of the surface area. The use of microwaves during acid treatment, after few minutes, led to materials with similar SBET to those obtained after 48 h with conventional heating methods. The influence of mineralogical impurities, crystallinity and chemical composition in the reactivity of sepiolite to this treatment was also studied. The obtained materials were impregnated with polyethylenimine and assessed for CO2 capture and CO2/N2 selectivity at different temperatures. Experimental equilibrium data were fitted to Langmuir and Sips models. The adsorption data revealed that sepiolite can be an interesting adsorbent for CO2 capture, achieving a capacity of 1.70 mmol g-1 at 338 K and 1 bar, providing a high CO2/N2 selectivity (440 mol CO2/mol N2).

Using infrastructure optimization to reduce greenhouse gas emissions from oil sands extraction and processing.

PubMed

Middleton, Richard S; Brandt, Adam R

2013-02-05

The Alberta oil sands are a significant source of oil production and greenhouse gas emissions, and their importance will grow as the region is poised for decades of growth. We present an integrated framework that simultaneously considers economic and engineering decisions for the capture, transport, and storage of oil sands CO(2) emissions. The model optimizes CO(2) management infrastructure at a variety of carbon prices for the oil sands industry. Our study reveals several key findings. We find that the oil sands industry lends itself well to development of CO(2) trunk lines due to geographic coincidence of sources and sinks. This reduces the relative importance of transport costs compared to nonintegrated transport systems. Also, the amount of managed oil sands CO(2) emissions, and therefore the CCS infrastructure, is very sensitive to the carbon price; significant capture and storage occurs only above 110$/tonne CO(2) in our simulations. Deployment of infrastructure is also sensitive to CO(2) capture decisions and technology, particularly the fraction of capturable CO(2) from oil sands upgrading and steam generation facilities. The framework will help stakeholders and policy makers understand how CCS infrastructure, including an extensive pipeline system, can be safely and cost-effectively deployed.

Bioinspired Pollen-Like Hierarchical Surface for Efficient Recognition of Target Cancer Cells.

PubMed

Wang, Wenshuo; Yang, Gao; Cui, Haijun; Meng, Jingxin; Wang, Shutao; Jiang, Lei

2017-08-01

The efficient recognition and isolation of rare cancer cells holds great promise for cancer diagnosis and prognosis. In nature, pollens exploit spiky structures to realize recognition and adhesion to stigma. Herein, a bioinspired pollen-like hierarchical surface is developed by replicating the assembly of pollen grains, and efficient and specific recognition to target cancer cells is achieved. The pollen-like surface is fabricated by combining filtering-assisted assembly and soft lithography-based replication of pollen grains of wild chrysanthemum. After modification with a capture agent specific to cancer cells, the pollen-like surface enables the capture of target cancer cells with high efficiency and specificity. In addition, the pollen-like surface not only assures high viability of captured cells but also performs well in cell mixture system and at low cell density. This study represents a good example of constructing cell recognition biointerfaces inspired by pollen-stigma adhesion. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

CO₂ uptake performance and life cycle assessment of CaO-based sorbents prepared from waste oyster shells blended with PMMA nanosphere scaffolds.

PubMed

Wang, Tsinghai; Xiao, Da-Cheng; Huang, Chih-Hung; Hsieh, Yi-Kong; Tan, Chung-Sung; Wang, Chu-Fang

2014-04-15

In this paper, we demonstrate a means of simultaneously solving two serious environmental issues by reutilization of calcinated mixture of pulverized waste oyster shells blending with poly(methyl methacrylate) (PMMA) nanospheres to prepare CaO-based sorbents for CO2 capture. After 10 cycles of isothermal carbonation/calcination at 750°C, the greatest CO2 uptake (0.19 g CO2/g sorbent) was that for the sorbent featuring 70 wt% of PMMA, which was almost three times higher than that (0.07 g CO2/g sorbent) of untreated waste oyster shell. The greater CO2 uptake was likely a result of particle size reduction and afterwards surface basicity enhancement and an increase in the volume of mesopores and macropores. Following simplified life cycle assessment, whose all input values were collected from our experimental results, suggested that a significant CO2 emission reduction along with lesser human health and ecosystems impacts would be achieved immediately once waste is reutilized. Most importantly, the CO2 uptake efficiency must be greater than 20% or sorbents prepared from limestone mining would eventually produce a net positive CO2 emission. Copyright © 2014 Elsevier B.V. All rights reserved.

Closing CO2 Loop in Biogas Production: Recycling Ammonia As Fertilizer.

PubMed

He, Qingyao; Yu, Ge; Tu, Te; Yan, Shuiping; Zhang, Yanlin; Zhao, Shuaifei

2017-08-01

We propose and demonstrate a novel system for simultaneous ammonia recovery, carbon capture, biogas upgrading, and fertilizer production in biogas production. Biogas slurry pretreatment (adjusting the solution pH, turbidity, and chemical oxygen demand) plays an important role in the system as it significantly affects the performance of ammonia recovery. Vacuum membrane distillation is used to recover ammonia from biogas slurry at various conditions. The ammonia removal efficiency in vacuum membrane distillation is around 75% regardless of the ammonia concentration of the biogas slurry. The recovered ammonia is used for CO 2 absorption to realize simultaneous biogas upgrading and fertilizer generation. CO 2 absorption performance of the recovered ammonia (absorption capacity and rate) is compared with a conventional model absorbent. Theoretical results on biogas upgrading are also provided. After ammonia recovery, the treated biogas slurry has significantly reduced phytotoxicity, improving the applicability for agricultural irrigation. The novel concept demonstrated in this study shows great potential in closing the CO 2 loop in biogas production by recycling ammonia as an absorbent for CO 2 absorption associated with producing fertilizers.

Highly specific fiber optic immunosensor coupled with immunomagnetic separation for detection of low levels of Listeria monocytogenes and L. ivanovii

PubMed Central

2012-01-01

Background Immunomagnetic separation (IMS) and immunoassays are widely used for pathogen detection. However, novel technology platforms with highly selective antibodies are essential to improve detection sensitivity, specificity and performance. In this study, monoclonal antibodies (MAbs) against Internalin A (InlA) and p30 were generated and used on paramagnetic beads of varying diameters for concentration, as well as on fiber-optic sensor for detection. Results Anti-InlA MAb-2D12 (IgG2a subclass) was specific for Listeria monocytogenes and L. ivanovii, and p30-specific MAb-3F8 (IgM) was specific for the genus Listeria. At all bacterial concentrations (103–108 CFU/mL) tested in the IMS assay; the 1-μm diameter MyOne beads had significantly higher capture efficiency (P < 0.05) than the 2.8-μm diameter M-280 beads with both antibodies. The highest capture efficiency for MyOne-2D12 (49.2% for 105 CFU/mL) was significantly higher (P < 0.05) than that of MyOne-3F8 (16.6 %) and Dynabeads anti-Listeria antibody (9 %). Furthermore, capture efficiency for MyOne-2D12 was highly specific for L. monocytogenes and L. ivanovii. Subsequently, we captured L. monocytogenes by MyOne-2D12 and MyOne-3F8 from hotdogs inoculated with mono- or co-cultures of L. monocytogenes and L. innocua (10–40 CFU/g), enriched for 18 h and detected by fiber-optic sensor and confirmed by plating, light-scattering, and qPCR assays. The detection limit for L. monocytogenes and L. ivanovii by the fiber-optic immunosensor was 3 × 102 CFU/mL using MAb-2D12 as capture and reporter antibody. Selective media plating, light-scattering, and qPCR assays confirmed the IMS and fiber-optic results. Conclusions IMS coupled with a fiber-optic sensor using anti-InlA MAb is highly specific for L. monocytogenes and L. ivanovii and enabled detection of these pathogens at low levels from buffer or food. PMID:23176167

Tethered catalysts for the hydration of carbon dioxide

DOEpatents

Valdez, Carlos A; Satcher, Jr., Joe H; Aines, Roger D; Wong, Sergio E; Baker, Sarah E; Lightstone, Felice C; Stolaroff, Joshuah K

2014-11-04

A system is provided that substantially increases the efficiency of CO.sub.2 capture and removal by positioning a catalyst within an optimal distance from the air-liquid interface. The catalyst is positioned within the layer determined to be the highest concentration of carbon dioxide. A hydrophobic tether is attached to the catalyst and the hydrophobic tether modulates the position of the catalyst within the liquid layer containing the highest concentration of carbon dioxide.

Ammonia modification of activated carbon to enhance carbon dioxide adsorption: Effect of pre-oxidation

NASA Astrophysics Data System (ADS)

Shafeeyan, Mohammad Saleh; Daud, Wan Mohd Ashri Wan; Houshmand, Amirhossein; Arami-Niya, Arash

2011-02-01

A commercial granular activated carbon (GAC) was subjected to thermal treatment with ammonia for obtaining an efficient carbon dioxide (CO2) adsorbent. In general, CO2 adsorption capacity of activated carbon can be increased by introduction of basic nitrogen functionalities onto the carbon surface. In this work, the effect of oxygen surface groups before introduction of basic nitrogen functionalities to the carbon surface on CO2 adsorption capacity was investigated. For this purpose two different approaches of ammonia treatment without preliminary oxidation and amination of oxidized samples were studied. Modified carbons were characterized by elemental analysis and Fourier Transform Infrared spectroscopy (FT-IR) to study the impact of changes in surface chemistry and formation of specific surface groups on adsorption properties. The texture of the samples was characterized by conducting N2 adsorption/desorption at -196 °C. CO2 capture performance of the samples was investigated using a thermogravimetric analysis (TGA). It was found that in both modification techniques, the presence of nitrogen functionalities on carbon surface generally increased the CO2 adsorption capacity. The results indicated that oxidation followed by high temperature ammonia treatment (800 °C) considerably enhanced the CO2 uptake at higher temperatures.

Joint Evaluation of Copernicus Atmosphere Monitoring Service (CAMS) High-resolution Global Near-Real Time CO and CO2 Forecasts during KORUS-AQ Field Campaign

NASA Astrophysics Data System (ADS)

Tang, W.; Arellano, A. F., Jr.; Choi, Y.; DiGangi, J. P.; Woo, J. H.; Diskin, G. S.; Agusti-panareda, A.; Parrington, M.; Massart, S.; Lee, M.; Kanaya, Y.; Jang, J.; Lee, Y.; Hong, J.; Flynn, J. H., III; Thompson, A. M.; Kim, D. B.

2017-12-01

Anthropogenic combustion has significant impacts on air quality and climate. To understand anthropogenic combustion, it is critical to model CO2 and CO (key combustion signatures) and their relationships. In this study, we jointly evaluate the Copernicus Atmosphere Monitoring Service (CAMS) free-running 16-km forecast, 9-km forecast initialized with CAMS analysis, and analysis products of CO (80km) and CO2 (40km) to understand how well combustion-related processes and constituent transport are represented in the current system. We use measurements from aircraft, ground sites, and ships during the KORUS-AQ field campaign (May - June 2016), along with satellite observations (MOPITT, IASI, OCO-2, and GOSAT). Airborne measurements by the DC-8 aircraft are classified into five regions: Seoul metropolitan, Taehwa, West Sea, Seoul-Jeju jetway, and Seoul-Busan jetway. The observed CO2, CO, and their relationships varies significantly, and the performance of CAMS products also varies across regions. The three CAMS products perform reasonably well in simulating anthropogenic combustion processes. Overall, CO2 is overestimated while CO is underestimated by CAMS. The 9km forecast product generally has a better performance than the other two, because of its higher model resolution and better initialization conditions. The analysis product also performs better than the 16km forecast. China outflow over West Sea is captured, but CO2 and CO is underestimated in the outflow. According to CAMS, is 10-15 (ppbv/ppmv) for Korea and about 30 for China outflow, indicating anthropogenic combustion in Seoul is more efficient than it is in China. This agrees well with DC-8 aircraft observations. As for ground sites, we find that CO and CO2 measured by the Olympic park and Yonsei (Seoul metropolitan sites) have more regularity in diurnal cycle, and such periodical change is well captured by CAMS. The time series for CO from Baengnyeong, and Fukue (remote sites) are irregular and episodic, which are more related to transport rather than local emissions. CAMS performances over Taehwa site are impacted by both local processes and transport. These comparisons indicate vertical mixing near sources may be an issue for CAMS. Compared to satellite observations, CO analyses show a better agreement, while for CO2, the forecasts are better.

Commercialization Development of Oxygen Fired CFB for Greenhouse Gas Control

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nsakala ya Nsakala; Gregory N. Liljedahl; David G. Turek

2007-03-31

Given that fossil fuel fired power plants are among the largest and most concentrated producers of CO{sub 2} emissions, recovery and sequestration of CO{sub 2} from the flue gas of such plants has been identified as one of the primary means for reducing anthropogenic (i.e., man-made) CO{sub 2} emissions. In 2001, ALSTOM Power Inc. (ALSTOM) began a two-phase program to investigate the feasibility of various carbon capture technologies. This program was sponsored under a Cooperative Agreement from the US Department of Energy's National Energy Technology Laboratory (DOE). The first phase entailed a comprehensive study evaluating the technical feasibility and economicsmore » of alternate CO{sub 2} capture technologies applied to Greenfield US coal-fired electric generation power plants. Thirteen cases, representing various levels of technology development, were evaluated. Seven cases represented coal combustion in CFB type equipment. Four cases represented Integrated Gasification Combined Cycle (IGCC) systems. Two cases represented advanced Chemical Looping Combined Cycle systems. Marion, et al. reported the details of this work in 2003. One of the thirteen cases studied utilized an oxygen-fired circulating fluidized bed (CFB) boiler. In this concept, the fuel is fired with a mixture of oxygen and recirculated flue gas (mainly CO{sub 2}). This combustion process yields a flue gas containing over 80 percent (by volume) CO{sub 2}. This flue gas can be processed relatively easily to enrich the CO{sub 2} content to over 96 percent for use in enhanced oil or gas recovery (EOR or EGR) or simply dried for sequestration. The Phase I study identified the O{sub 2}-fired CFB as having a near term development potential, because it uses conventional commercial CFB technology and commercially available CO{sub 2} capture enabling technologies such as cryogenic air separation and simple rectification or distillation gas processing systems. In the long term, air separation technology advancements offer significant reductions in power requirements, which would improve plant efficiency and economics for the oxygen-fired technology. The second phase consisted of pilot-scale testing followed by a refined performance and economic evaluation of the O{sub 2} fired CFB concept. As a part of this workscope, ALSTOM modified its 3 MW{sub th} (9.9 MMBtu/hr) Multiuse Test Facility (MTF) pilot plant to operate with O{sub 2}/CO{sub 2} mixtures of up to 70 percent O{sub 2} by volume. Tests were conducted with coal and petroleum coke. The test objectives were to determine the impacts of oxygen firing on heat transfer, bed dynamics, potential agglomeration, and gaseous and particulate emissions. The test data results were used to refine the design, performance, costs, and economic models developed in Phase-I for the O{sub 2}-fired CFB with CO{sub 2} capture. Nsakala, Liljedahl, and Turek reported results from this study in 2004. ALSTOM identified several items needing further investigation in preparation for large scale demonstration of the oxygen-fired CFB concept, namely: (1) Operation and performance of the moving bed heat exchanger (MBHE) to avoid recarbonation and also for cost savings compared to the standard bubbling fluid bed heat exchanger (FBHE); (2) Performance of the back-end flash dryer absorber (FDA) for sulfur capture under high CO{sub 2}/high moisture flue gas environment using calcined limestone in the fly ash and using fresh commercial lime directly in the FDA; (3) Determination of the effect of recarbonation on fouling in the convective pass; (4) Assessment of the impact of oxygen firing on the mercury, other trace elements, and volatile organic compound (VOC) emissions; and (5) Develop a proposal-level oxygen-fired retrofit design for a relatively small existing CFB steam power plant in preparation for a large-scale demonstration of the O{sub 2} fired CFB concept. Hence, ALSTOM responded to a DOE Solicitation to address all these issues with further O{sub 2} fired MTF pilot testing and a subsequent retrofit design study of oxygen firing and CO{sub 2} capture on an existing air-fired CFB plant. ALSTOM received a contract award from the DOE to conduct a project entitled 'Commercialization Development of Oxygen Fired CFB for Greenhouse Gas Control', under Cooperative Agreement DE-FC26-04NT42205 that is the subject of this topical report.« less

Screening of metal-organic frameworks for carbon dioxide capture from flue gas using a combined experimental and modeling approach.

PubMed

Yazaydin, A Ozgür; Snurr, Randall Q; Park, Tae-Hong; Koh, Kyoungmoo; Liu, Jian; Levan, M Douglas; Benin, Annabelle I; Jakubczak, Paulina; Lanuza, Mary; Galloway, Douglas B; Low, John J; Willis, Richard R

2009-12-30

A diverse collection of 14 metal-organic frameworks (MOFs) was screened for CO(2) capture from flue gas using a combined experimental and modeling approach. Adsorption measurements are reported for the screened MOFs at room temperature up to 1 bar. These data are used to validate a generalized strategy for molecular modeling of CO(2) and other small molecules in MOFs. MOFs possessing a high density of open metal sites are found to adsorb significant amounts of CO(2) even at low pressure. An excellent correlation is found between the heat of adsorption and the amount of CO(2) adsorbed below 1 bar. Molecular modeling can aid in selection of adsorbents for CO(2) capture from flue gas by screening a large number of MOFs.

CO2 dynamics on three habitats of mangrove ecosystem in Bintan Island, Indonesia

NASA Astrophysics Data System (ADS)

Dharmawan, I. W. E.

2018-02-01

Atmospheric carbon dioxide (CO2) has increased over time, implied on global warming and climate change. Blue carbon is one of interesting options to reduce CO2 concentration in the atmosphere. Indonesia has the largest mangrove area in the world which would be potential to mitigate elevated CO2 concentrations. A quantitative study on CO2 dynamic was conducted in the habitat-variable and pristine mangrove of Bintan island. The study was aimed to estimate CO2 flux on three different mangrove habitats, i.e., lagoon, oceanic and riverine. Even though all habitats were dominated by Rhizophora sp, they were significantly differed one another by species composition, density, and soil characteristics. Averagely, CO2 dynamics had the positive budget by ∼0.668 Mmol/ha (82.47%) which consisted of sequestration, decomposition, and soil efflux at 0.810 Mmol/ha/y, -0.125 Mmol/ha/y and -0.017 Mmol/ha/y, respectively. The study found that the fringing habitat had the highest CO2 capturing rate and the lowest rate of litter decomposition which was contrast to the riverine site. Therefore, oceanic mangrove was more efficient in controlling CO2 dynamics due to higher carbon storage on their biomass. A recent study also found that soil density and organic matter had a significant impact on CO2 dynamics.

Early opportunities of CO2 geological storage deployment in coal chemical industry in China

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wei, Ning; Li, Xiaochun; Liu, Shengnan

2014-11-12

Abstract: Carbon dioxide capture and geological storage (CCS) is regarded as a promising option for climate change mitigation; however, the high capture cost is the major barrier to large-scale deployment of CCS technologies. High-purity CO2 emission sources can reduce or even avoid the capture requirements and costs. Among these high-purity CO2 sources, certain coal chemical industry processes are very important, especially in China. In this paper, the basic characteristics of coal chemical industries in China is investigated and analyzed. As of 2013 there were more than 100 coal chemical plants in operation or in late planning stages. These emission sourcesmore » together emit 430 million tons CO2 per year, of which about 30% are emit high-purity and pure CO2 (CO2 concentration >80% and >99% respectively).Four typical source-sink pairs are studied by a techno-economic evaluation, including site screening and selection, source-sink matching, concept design, and experienced economic evaluation. The technical-economic evaluation shows that the levelized cost of a CO2 capture and aquifer storage project in the coal chemistry industry ranges from 14 USD/t to 17 USD/t CO2. When a 15USD/t CO2 tax and 15USD/t for CO2 sold to EOR are considered, the levelized cost of CCS project are negative, which suggests a net economic benefit from some of these CCS projects. This might provide China early opportunities to deploy and scale-up CCS projects in the near future.« less

Nitrosamines and Nitramines in Amine-Based Carbon Dioxide Capture Systems: Fundamentals, Engineering Implications, and Knowledge Gaps.

PubMed

Yu, Kun; Mitch, William A; Dai, Ning

2017-10-17

Amine-based absorption is the primary contender for postcombustion CO 2 capture from fossil fuel-fired power plants. However, significant concerns have arisen regarding the formation and emission of toxic nitrosamine and nitramine byproducts from amine-based systems. This paper reviews the current knowledge regarding these byproducts in CO 2 capture systems. In the absorber, flue gas NO x drives nitrosamine and nitramine formation after its dissolution into the amine solvent. The reaction mechanisms are reviewed based on CO 2 capture literature as well as biological and atmospheric chemistry studies. In the desorber, nitrosamines are formed under high temperatures by amines reacting with nitrite (a hydrolysis product of NO x ), but they can also thermally decompose following pseudo-first order kinetics. The effects of amine structure, primarily amine order, on nitrosamine formation and the corresponding mechanisms are discussed. Washwater units, although intended to control emissions from the absorber, can contribute to additional nitrosamine formation when accumulated amines react with residual NO x . Nitramines are much less studied than nitrosamines in CO 2 capture systems. Mitigation strategies based on the reaction mechanisms in each unit of the CO 2 capture systems are reviewed. Lastly, we highlight research needs in clarifying reaction mechanisms, developing analytical methods for both liquid and gas phases, and integrating different units to quantitatively predict the accumulation and emission of nitrosamines and nitramines.

Doping Li and K into Na2ZrO3 Sorbent to Improve Its CO2 Capture Capability

NASA Astrophysics Data System (ADS)

Duan, Yuhua

Carbon dioxide is one of the major combustion products which once released into the air can contribute to global climate change. Solid sorbents have been reported in several previous studies to be promising candidates for CO2 sorbent applications due to their high CO2 absorption capacities at moderate working temperatures. However, at a given CO2 pressure, the turnover temperature (Tt) of an individual solid capture CO2 reaction is fixed and may be outside the operating temperature range (ΔTo) for a particularly capture technology. In order to shift such Tt for a solid into the range of ΔTo, its corresponding thermodynamic property must be changed by changing its structure by reacting (mixing) with other materials or doping with other elements. As an example, by combining thermodynamic database searching with ab initio thermodynamics calculations, in this work, we explored the Li- and K-doping effects on the Tt shifts of Na2ZrO3 at different doping levels. The obtained results showed that compared to pure Na2ZrO3, the Li- and K-doped mixtures Na2-αMαZrO3 (M =Li, K) have lower Tt and higher CO2 capture capacities.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Doug Cathro

The Lake Charles CCS Project is a large-scale industrial carbon capture and sequestration (CCS) project which will demonstrate advanced technologies that capture and sequester carbon dioxide (CO{sub 2}) emissions from industrial sources into underground formations. Specifically the Lake Charles CCS Project will accelerate commercialization of large-scale CO{sub 2} storage from industrial sources by leveraging synergy between a proposed petroleum coke to chemicals plant (the LCC Gasification Project) and the largest integrated anthropogenic CO{sub 2} capture, transport, and monitored sequestration program in the U.S. Gulf Coast Region. The Lake Charles CCS Project will promote the expansion of EOR in Texas andmore » Louisiana and supply greater energy security by expanding domestic energy supplies. The capture, compression, pipeline, injection, and monitoring infrastructure will continue to sequester CO{sub 2} for many years after the completion of the term of the DOE agreement. The objectives of this project are expected to be fulfilled by working through two distinct phases. The overall objective of Phase 1 was to develop a fully definitive project basis for a competitive Renewal Application process to proceed into Phase 2 - Design, Construction and Operations. Phase 1 includes the studies attached hereto that will establish: the engineering design basis for the capture, compression and transportation of CO{sub 2} from the LCC Gasification Project, and the criteria and specifications for a monitoring, verification and accounting (MVA) plan at the Hastings oil field in Texas. The overall objective of Phase 2, provided a successful competitive down-selection, is to execute design, construction and operations of three capital projects: (1) the CO{sub 2} capture and compression equipment, (2) a Connector Pipeline from the LLC Gasification Project to the Green Pipeline owned by Denbury and an affiliate of Denbury, and (3) a comprehensive MVA system at the Hastings oil field.« less

From Zn(II)-Carboxylate to Double-Walled Zn(II)-Carboxylato Phosphate MOF: Change in the Framework Topology, Capture and Conversion of CO2, and Catalysis of Strecker Reaction.

PubMed

Gupta, Mayank; De, Dinesh; Tomar, Kapil; Bharadwaj, Parimal K

2017-12-04

The ligand H 2 L has been built by linking an imidazole moiety to the 5-position of isophthalic acid. It forms two types of porous frameworks, {[Zn(L)]·2DMF·2H 2 O} n (1) and {[(CH 3 ) 2 NH 2 ][Zn 2 (L)(H 2 O)PO 4 ]·2DMF} n (2). 1 is a porous neutral framework and has rtl rutile 3,6-conn topology, while 2 is an organo-metallophosphate anionic porous framework with double-walled hexagonal channels. Framework 1' (desolvated) exhibits moderate CO 2 adsorption (58 cc g -1 at 273 K, 1 bar), whereas 2' (desolvated) shows a microporous nature with a high adsorption of CO 2 (111.7 cc g -1 or 22 wt % at 273 K, 1 bar). Interestingly, this adsorbed CO 2 could be converted very efficiently to cyclic carbonates under mild conditions using 2' as the catalyst in the presence of tetrabutylammonium bromide as the cocatalyst. The presence of open metal sites in 2' makes it an efficient heterogeneous catalyst for solvent-free three-component Strecker reaction using various aldehydes/ketones together with amines and trimethylsilyl cyanide in high yields at room temperature. The straightforward experimental and product isolation procedure along with easy recovery and reusability of the catalyst provided an attractive route for the synthesis of α-amino nitriles.

Supersonic Post-Combustion Inertial CO 2 Extraction System Final Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Balepin, Vladimir

This report summarizes the effort carried out under NETL contract DE- FE0013122 from 1 October 2013 to 31 March 2017. As described in this document, technical challenges realized during the performance of this project resulted in completion of only the first two of three planned budget periods. Despite this outcome, substantial progress was made toward understanding and maturing the CO 2 capture technology under consideration and considerable future promise remains for applications requiring lower CO 2 capture and/or lower CO 2.

Preparation Methods of Metal Organic Frameworks and Their Capture of CO2

NASA Astrophysics Data System (ADS)

Zhang, Linjian; Liand, Fangqin; Luo, Liangfei

2018-01-01

The increasingly serious greenhouse effect makes people pay more attention to the capture and storage technology of CO2. Metal organic frameworks (MOFs) have the advantages of high specific surface area, porous structure and controllable structure, and become the research focus of CO2 emission reduction technology in recent years. In this paper, the characteristics, preparation methods and application of MOFs in the field of CO2 adsorption and separation are discussed, especially the application of flue gas environment in power plants.

Improved Structural Design and CO 2 Capture of Porous Hydroxy-Rich Polymeric Organic Frameworks

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kidder, Michelle K.; Earl, Lyndsey D.; de Almeida, Valmor F.

2016-04-16

Polymeric organic frameworks (POFs) are tunable and robust porous materials with potential applications for gas capture, catalysis, and separations technologies. A series of new porous POFs have been synthesized from the reaction of phloroglucinol or resorcinol derivatives with aryl aldehyde precursors. The monomers have various molecular shapes including linear, bent, trigonal, and tetrahedral geometries. Depending on the size and geometric matching of the monomers, the polymers are dominantly microporous with some mesoporous character or they are non-porous. In addition to standard spectroscopic and surface characterization, the materials were screened as adsorbents for carbon dioxide capture at low pressure (0-1 bar).more » The best performing material (POF 1D) has a CO 2 capture capacity of 9.0 wt. % (2.04 mmol g -1) at 298 K and 1 bar which is comparable to other polymeric organic frameworks. Isosteric heats of adsorption for POF 1A, POF 2A, and POF 2B were found to be dependent on the weight percent of CO 2 adsorbed: this suggests there are both chemisorptive and physisorptive components of CO 2 capture by the POFs.« less

Sequestering CO2 in the Ocean: Options and Consequences

NASA Astrophysics Data System (ADS)

Rau, G. H.; Caldeira, K.

2002-12-01

The likelihood of negative climate and environmental impacts associated with increasing atmospheric CO2 has prompted serious consideration of various CO2 mitigation strategies. Among these are methods of capturing and storing of CO2 in the ocean. Two approaches that have received the most attention in this regard have been i) ocean fertilization to enhanced biological uptake and fixation of CO2, and ii) the chemical/mechanical capture and injection of CO2 into the deep ocean. Both methods seek to enhance or speed up natural mechanisms of CO2 uptake and storage by the ocean, namely i) the biological CO2 "pump" or ii) the passive diffusion of CO2 into the surface ocean and subsequent mixing into the deep sea. However, as will be reviewed, concerns about the capacity and effectiveness of either strategy in long-term CO2 sequestration have been raised. Both methods are not without potentially significant environmental impacts, and the costs of CO2 capture and injection (option ii) are currently prohibitive. An alternate method of ocean CO2 sequestration would be to react and hydrate CO2 rich waste gases (e.g., power plant flue gas) with seawater and to subsequently neutralize the resulting carbonic acid with limestone to produce calcium and bicarbonate ions in solution. This approach would simply speed up the CO2 uptake and sequestration that naturally (but very slowly) occurs via global carbonate weathering. This would avoid much of the increased acidity associated with direct CO2 injection while obviating the need for costly CO2 separation and capture. The addition of the resulting bicarbonate- and carbonate-rich solution to the ocean would help to counter the decrease in pH and carbonate ion concentration, and hence loss of biological calcification that is presently occurring as anthropogenic CO2 invades the ocean from the atmosphere. However, as with any approach to CO2 mitigation, the costs, impacts, risks, and benefits of this method need to be better understood and weighed against those of alternative strategies, including business as usual.

Real-Time Imaging of Ground Cover: Relationships with Radiation Capture, Canopy Photosynthesis, and Daily Growth Rate

NASA Technical Reports Server (NTRS)

Klassen, S. P.; Ritchie, G.; Frantz, J. M.; Pinnock, D.; Bugbee, B.

2003-01-01

Cumulative absorbed radiation is highly correlated with crop biomass and yield. In this chapter we describe the use of a digital camera and commercial imaging software for estimating daily radiation capture, canopy photosynthesis, and relative growth rate. Digital images were used to determine percentage of ground cover of lettuce (Lactuca sativa L.) communities grown at five temperatures. Plants were grown in a steady-state, 10-chamber CO2 gas exchange system, which was used to measure canopy photosynthesis and daily carbon gain. Daily measurements of percentage of ground cover were highly correlated with daily measurements of both absorbed radiation (r(sup 2) = 0.99) and daily carbon gain (r(sup 2) = 0.99). Differences among temperature treatments indicated that these relationships were influenced by leaf angle, leaf area index, and chlorophyll content. An analysis of the daily images also provided good estimates of relative growth rates, which were verified by gas exchange measurements of daily carbon gain. In a separate study we found that images taken at hourly intervals were effective for monitoring real-time growth. Our data suggests that hourly images can be used for early detection of plant stress. Applications, limitations, and potential errors are discussed. We have long known that crop yield is determined by the efficiency of four component processes: (i) radiation capture, (ii) quantum yield, (iii) carbon use efficiency, and (iv) carbon partitioning efficiency (Charles-Edwards, 1982; Penning de Vries & van Laar, 1982; Thornley, 1976). More than one-half century ago, Watson (1947, 1952) showed that variation in radiation capture accounted for almost all of the variation in yield between sites in temperate regions, because the three other components are relatively constant when the crop is not severely stressed. More recently, Monteith (1977) reviewed the literature on the close correlation between radiation capture and yield. Bugbee and Monje (1992) demonstrated the close relationship between absorbed radiation and yield in an optimal environment.

CO 2 Capture by Cold Membrane Operation with Actual Power Plant Flue Gas

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chaubey, Trapti; Kulkarni, Sudhir; Hasse, David

The main objective of the project was to develop a post-combustion CO 2 capture process based on the hybrid cold temperature membrane operation. The CO 2 in the flue gas from coal fired power plant is pre-concentrated to >60% CO 2 in the first stage membrane operation followed by further liquefaction of permeate stream to achieve >99% CO 2 purity. The aim of the project was based on DOE program goal of 90% CO 2 capture with >95% CO 2 purity from Pulverized Coal (PC) fired power plants with $40/tonne of carbon capture cost by 2025. The project moves themore » technology from TRL 4 to TRL 5. The project involved optimization of Air Liquide commercial 12” PI-1 bundle to improve the bundle productivity by >30% compared to the previous baseline (DE-FE0004278) using computational fluid dynamics (CFD) modeling and bundle testing with synthetic flue gas at 0.1 MWe bench scale skid located at Delaware Research and Technology Center (DRTC). In parallel, the next generation polyimide based novel PI-2 membrane was developed with 10 times CO 2 permeance compared to the commercial PI-1 membrane. The novel PI-2 membrane was scaled from mini-permeator to 1” permeator and 1” bundle for testing. Bundle development was conducted with a Development Spin Unit (DSU) installed at MEDAL. Air Liquide’s cold membrane technology was demonstrated with real coal fired flue gas at the National Carbon Capture Center (NCCC) with a 0.3 MWe field-test unit (FTU). The FTU was designed to incorporate testing of two PI-1 commercial membrane bundles (12” or 6” diameter) in parallel or series. A slip stream was sent to the next generation PI-2 membrane for testing with real flue gas. The system exceeded performance targets with stable PI-1 membrane operation for over 500 hours of single bundle, steady state testing. The 12” PI-1 bundle exceeded the productivity target by achieving ~600 Nm3/hr, where the target was set at ~455 Nm3/hr at 90% capture rate. The cost of 90% CO 2 capture from a 550 MWe net coal power plant was estimated between 40 and $45/tonne. A 6” PI-1 bundle exhibited superior bundle performance compared to the 12” PI-1 bundle. However, the carbon capture cost was not lower with the 6” PI-1 bundle due to the higher bundle installed cost. A 1” PI-1 bundle was tested to compare bundles with different length / diameter ratios. This bundle exhibited the lowest performance due to the different fiber winding pattern and increased bundle non-ideality. Several long-term and parametric tests were conducted with 3,200 hours of total run-time at NCCC. Finally, the new PI-2 membrane fiber was tested at a small scale (1” modules) in real flue gas and exhibited up to 10 times the CO 2 permeance and slightly lower CO 2/N 2 selectivity as the commercial PI-1 fiber. This corresponded to a projected 4 - 5 times increase in the productivity per bundle and a potential cost reduction of $3/tonne for CO2 capture, as compared with PI-1. An analytical campaign was conducted to trace different impurities such as NOx, mercury, Arsenic, Selenium in gas and liquid samples through the carbon capture system. An Environmental, Health and Safety (EH&S) analysis was completed to estimate emissions from a 550 MWe net power plant with carbon capture using cold membrane. A preliminary design and cost analysis was completed for 550 tpd (~25 MWe) plant to assess the capital investment and carbon capture cost for PI-1 and PI-2 membrane solutions from coal fired flue gas. A comparison was made with an amine based solution with significant cost advantage for the membrane at this scale. Additional preliminary design and cost analysis was completed between coal, natural gas and SMR flue gas for carbon capture at 550 tpd (~25 MWe) plant.« less

CO 2 Absorption and Magnesium Carbonate Precipitation in MgCl 2–NH 3–NH 4Cl Solutions: Implications for Carbon Capture and Storage

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhu, Chen; Wang, Han; Li, Gen

CO 2 absorption and carbonate precipitation are the two core processes controlling the reaction rate and path of CO 2 mineral sequestration. Whereas previous studies have focused on testing reactive crystallization and precipitation kinetics, much less attention has been paid to absorption, the key process determining the removal efficiency of CO 2. In this study, adopting a novel wetted wall column reactor, we systematically explore the rates and mechanisms of carbon transformation from CO 2 gas to carbonates in MgCl 2–NH 3–NH 4Cl solutions. We find that reactive diffusion in liquid film of the wetted wall column is the rate-limitingmore » step of CO 2 absorption when proceeding chiefly through interactions between CO 2(aq) and NH 3(aq). We further quantified the reaction kinetic constant of the CO 2–NH 3 reaction. Our results indicate that higher initial concentration of NH 4Cl ( ≥2mol∙L -1) leads to the precipitation of roguinite [(NH 4) 2Mg(CO 3) 2∙4H 2O], while nesquehonite appears to be the dominant Mg-carbonate without NH 4Cl addition. We also noticed dypingite formation via phase transformation in hot water. This study provides new insight into the reaction kinetics of CO 2 mineral carbonation that indicates the potential of this technique for future application to industrial-scale CO 2 sequestration.« less

CO 2 Absorption and Magnesium Carbonate Precipitation in MgCl 2–NH 3–NH 4Cl Solutions: Implications for Carbon Capture and Storage

DOE PAGES

Zhu, Chen; Wang, Han; Li, Gen; ...

2017-09-19

CO 2 absorption and carbonate precipitation are the two core processes controlling the reaction rate and path of CO 2 mineral sequestration. Whereas previous studies have focused on testing reactive crystallization and precipitation kinetics, much less attention has been paid to absorption, the key process determining the removal efficiency of CO 2. In this study, adopting a novel wetted wall column reactor, we systematically explore the rates and mechanisms of carbon transformation from CO 2 gas to carbonates in MgCl 2–NH 3–NH 4Cl solutions. We find that reactive diffusion in liquid film of the wetted wall column is the rate-limitingmore » step of CO 2 absorption when proceeding chiefly through interactions between CO 2(aq) and NH 3(aq). We further quantified the reaction kinetic constant of the CO 2–NH 3 reaction. Our results indicate that higher initial concentration of NH 4Cl ( ≥2mol∙L -1) leads to the precipitation of roguinite [(NH 4) 2Mg(CO 3) 2∙4H 2O], while nesquehonite appears to be the dominant Mg-carbonate without NH 4Cl addition. We also noticed dypingite formation via phase transformation in hot water. This study provides new insight into the reaction kinetics of CO 2 mineral carbonation that indicates the potential of this technique for future application to industrial-scale CO 2 sequestration.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wareing, Christopher J.; School of Physics and Astronomy, University of Leeds, Leeds, LS2 9JT; Fairweather, Michael

Predicting the correct multi-phase fluid flow behaviour during the discharge process in the near-field of sonic CO{sub 2} jets is of particular importance in assessing the risks associated with transport aspects of carbon capture and storage schemes, given the very different hazard profiles of CO{sub 2} in the gaseous and solid states. In this paper, we apply our state-of-the-art mathematical model implemented in an efficient computational method to available data. Compared to previous applications, an improved equation of state is used. We also compare to all the available data, rather than just subsets as previously, and demonstrate both the improvedmore » performance of the fluid flow model and the variation between the available datasets. The condensed phase fraction at the vent, puncture or rupture release point is revealed to be of key importance in understanding the near-field dispersion of sonic CO{sub 2}.« less

Biocapture of CO2 by Different Microalgal-Based Technologies for Biogas Upgrading and Simultaneous Biogas Slurry Purification under Various Light Intensities and Photoperiods

PubMed Central

Guo, Pengfei; Zhang, Yuejin; Zhao, Yongjun

2018-01-01

Co-cultivation of microalgae and microbes for pollutant removal from sewage is considered as an effective wastewater treatment method. The aim of this study is to screen the optimal photoperiod, light intensity and microalgae co-cultivation method for simultaneously removing nutrients in biogas slurry and capturing CO2 in biogas. The microalgae–fungi pellets are deemed to be a viable option because of their high specific growth rate and nutrient and CO2 removal efficiency under the photoperiod of 14 h light:10 h dark. The order of both the biogas slurry purification and biogas upgrading is ranked the same, that is Chlorella vulgaris–Ganoderma lucidum > Chlorella vulgaris–activated sludge > Chlorella vulgaris under different light intensities. For all cultivation methods, the moderate light intensity of 450 μmol m−2 s−1 is regarded as the best choice. This research revealed that the control of photoperiod and light intensity can promote the biological treatment process of biogas slurry purification and biogas upgrading using microalgal-based technology. PMID:29543784

CESM-simulated 21st Century Changes in Large Scale Crop Water Requirements and Yields

NASA Astrophysics Data System (ADS)

Levis, S.; Badger, A.; Drewniak, B. A.; O'Neill, B. C.; Ren, X.

2014-12-01

We assess potential changes in crop water requirements and corresponding yields relative to the late 20th century in major crop producing regions of the world by using the Community Land Model (CLM) driven with 21st century meteorology from RCP8.5 and RCP4.5 Community Earth System Model (CESM) simulations. The RCP4.5 simulation allows us to explore the potential for averted societal impacts when compared to the RCP8.5 simulation. We consider the possibility for increased yields and improved water use efficiency under conditions of elevated atmospheric CO2 due to the CO2 fertilization effect (also known as concentration-carbon feedback). We address uncertainty in the current understanding of plant CO2 fertilization by repeating the simulations with and without the CO2 fertilization effect. Simulations without CO2 fertilization represent the radiative effect of elevated CO2 (i.e., warming) without representing the physiological effect of elevated CO2 (enhanced carbon uptake and increased water use efficiency by plants during photosynthesis). Preliminary results suggest that some plants may suffer from increasing heat and drought in much of the world without the CO2 fertilization effect. On the other hand plants (especially C3) tend to grow more with less water when models include the CO2 fertilization effect. Performing 21st century simulations with and without the CO2 fertilization effect brackets the potential range of outcomes. In this work we use the CLM crop model, which includes specific crop types that differ from the model's default plant functional types in that the crops get planted, harvested, and potentially fertilized and irrigated according to algorithms that attempt to capture human management decisions. We use an updated version of the CLM4.5 that includes cotton, rice, and sugarcane, spring wheat, spring barley, and spring rye, as well as temperate and tropical maize and soybean.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lai, Canhai; Xu, Zhijie; Li, Tingwen

In virtual design and scale up of pilot-scale carbon capture systems, the coupled reactive multiphase flow problem must be solved to predict the adsorber’s performance and capture efficiency under various operation conditions. This paper focuses on the detailed computational fluid dynamics (CFD) modeling of a pilot-scale fluidized bed adsorber equipped with vertical cooling tubes. Multiphase Flow with Interphase eXchanges (MFiX), an open-source multiphase flow CFD solver, is used for the simulations with custom code to simulate the chemical reactions and filtered models to capture the effect of the unresolved details in the coarser mesh for simulations with reasonable simulations andmore » manageable computational effort. Previously developed two filtered models for horizontal cylinder drag, heat transfer, and reaction kinetics have been modified to derive the 2D filtered models representing vertical cylinders in the coarse-grid CFD simulations. The effects of the heat exchanger configurations (i.e., horizontal or vertical) on the adsorber’s hydrodynamics and CO2 capture performance are then examined. The simulation result subsequently is compared and contrasted with another predicted by a one-dimensional three-region process model.« less

Measurement of carbon capture efficiency and stored carbon leakage

DOEpatents

Keeling, Ralph F.; Dubey, Manvendra K.

2013-01-29

Data representative of a measured carbon dioxide (CO.sub.2) concentration and of a measured oxygen (O.sub.2) concentration at a measurement location can be used to determine whether the measured carbon dioxide concentration at the measurement location is elevated relative to a baseline carbon dioxide concentration due to escape of carbon dioxide from a source associated with a carbon capture and storage process. Optionally, the data can be used to quantify a carbon dioxide concentration increase at the first location that is attributable to escape of carbon dioxide from the source and to calculate a rate of escape of carbon dioxide from the source by executing a model of gas-phase transport using at least the first carbon dioxide concentration increase. Related systems, methods, and articles of manufacture are also described.

Optimized Solvent for Energy-Efficient, Environmentally-Friendly Capture of CO{sub 2} at Coal-Fired Power Plants

DOE Office of Scientific and Technical Information (OSTI.GOV)

Farthing, G. A.; Rimpf, L. M.

The overall goal of this project, as originally proposed, was to optimize the formulation of a novel solvent as a critical enabler for the cost-effective, energy-efficient, environmentally-friendly capture of CO{sub 2} at coal-fired utility plants. Aqueous blends of concentrated piperazine (PZ) with other compounds had been shown to exhibit high rates of CO{sub 2} absorption, low regeneration energy, and other desirable performance characteristics during an earlier 5-year development program conducted by B&W. The specific objective of this project was to identify PZ-based solvent formulations that globally optimize the performance of coal-fired power plants equipped with CO{sub 2} scrubbing systems. Whilemore » previous solvent development studies have tended to focus on energy consumption and absorber size, important issues to be sure, the current work seeks to explore, understand, and optimize solvent formulation across the full gamut of issues related to commercial application of the technology: capital and operating costs, operability, reliability, environmental, health and safety (EH&S), etc. Work on the project was intended to be performed under four budget periods. The objective of the work in the first budget period has been to identify several candidate formulations of a concentrated PZ-based solvent for detailed characterization and evaluation. Work in the second budget period would generate reliable and comprehensive property and performance data for the identified formulations. Work in the third budget period would quantify the expected performance of the selected formulations in a commercial CO{sub 2} scrubbing process. Finally, work in the fourth budget period would provide a final technology feasibility study and a preliminary technology EH&S assessment. Due to other business priorities, however, B&W has requested that this project be terminated at the end of the first budget period. This document therefore serves as the final report for this project. It is the first volume of the two-volume final report and summarizes Budget Period 1 accomplishments under Tasks 1-5 of the project, including the selection of four solvent formulations for further study.« less

CaO-based CO2 sorbents: from fundamentals to the development of new, highly effective materials.

PubMed

Kierzkowska, Agnieszka M; Pacciani, Roberta; Müller, Christoph R

2013-07-01

The enormous anthropogenic emission of the greenhouse gas CO2 is most likely the main reason for climate change. Considering the continuing and indeed growing utilisation of fossil fuels for electricity generation and transportation purposes, development and implementation of processes that avoid the associated emissions of CO2 are urgently needed. CO2 capture and storage, commonly termed CCS, would be a possible mid-term solution to reduce the emissions of CO2 into the atmosphere. However, the costs associated with the currently available CO2 capture technology, that is, amine scrubbing, are prohibitively high, thus making the development of new CO2 sorbents a highly important research challenge. Indeed, CaO, readily obtained through the calcination of naturally occurring limestone, has been proposed as an alternative CO2 sorbent that could substantially reduce the costs of CO2 capture. However, one of the major drawbacks of using CaO derived from natural sources is its rapidly decreasing CO2 uptake capacity with repeated carbonation-calcination reactions. Here, we review the current understanding of fundamental aspects of the cyclic carbonation-calcination reactions of CaO such as its reversibility and kinetics. Subsequently, recent attempts to develop synthetic, CaO-based sorbents that possess high and cyclically stable CO2 uptakes are presented. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Mesoporous fluorocarbon-modified silica aerogel membranes enabling long-term continuous CO2 capture with large absorption flux enhancements.

PubMed

Lin, Yi-Feng; Chen, Chien-Hua; Tung, Kuo-Lun; Wei, Te-Yu; Lu, Shih-Yuan; Chang, Kai-Shiun

2013-03-01

The use of a membrane contactor combined with a hydrophobic porous membrane and an amine absorbent has attracted considerable attention for the capture of CO2 because of its extensive use, low operational costs, and low energy consumption. The hydrophobic porous membrane interface prevents the passage of the amine absorbent but allows the penetration of CO2 molecules that are captured by the amine absorbent. Herein, highly porous SiO2 aerogels modified with hydrophobic fluorocarbon functional groups (CF3 ) were successfully coated onto a macroporous Al2 O3 membrane; their performance in a membrane contactor for CO2 absorption is discussed. The SiO2 aerogel membrane modified with CF3 functional groups exhibits the highest CO2 absorption flux and can be continuously operated for CO2 absorption for extended periods of time. This study suggests that a SiO2 aerogel membrane modified with CF3 functional groups could potentially be used in a membrane contactor for CO2 absorption. Also, the resulting hydrophobic SiO2 aerogel membrane contactor is a promising technology for large-scale CO2 absorption during the post-combustion process in power plants. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

An adsorption of carbon dioxide on activated carbon controlled by temperature swing adsorption

NASA Astrophysics Data System (ADS)

Tomas, Korinek; Karel, Frana

2017-09-01

This work deals with a method of capturing carbon dioxide (CO2) in indoor air. Temperature Swing Adsorption (TSA) on solid adsorbent was chosen for CO2 capture. Commercial activated carbon (AC) in form of extruded pellets was used as a solid adsorbent. There was constructed a simple device to testing effectiveness of CO2 capture in a fixed bed with AC. The TSA cycle was also simulated using the open-source software OpenFOAM. There was a good agreement between results obtained from numerical simulations and experimental data for adsorption process.

ECONOMIC EVALUATION OF CO2 STORAGE AND SINK ENHANCEMENT OPTIONS

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bert Bock; Richard Rhudy; Howard Herzog

2003-02-01

This project developed life-cycle costs for the major technologies and practices under development for CO{sub 2} storage and sink enhancement. The technologies evaluated included options for storing captured CO{sub 2} in active oil reservoirs, depleted oil and gas reservoirs, deep aquifers, coal beds, and oceans, as well as the enhancement of carbon sequestration in forests and croplands. The capture costs for a nominal 500 MW{sub e} integrated gasification combined cycle plant from an earlier study were combined with the storage costs from this study to allow comparison among capture and storage approaches as well as sink enhancements.

Anion-activated, thermoreversible gelation system for the capture, release, and visual monitoring of CO2

NASA Astrophysics Data System (ADS)

Zhang, Xin; Lee, Songyi; Liu, Yifan; Lee, Minji; Yin, Jun; Sessler, Jonathan L.; Yoon, Juyoung

2014-04-01

Carbon dioxide (CO2) is an important green house gas. This is providing an incentive to develop new strategies to detect and capture CO2. Achieving both functions within a single molecular system represents an unmet challenge in terms of molecular design and could translate into enhanced ease of use. Here, we report an anion-activated chemosensor system, NAP-chol 1, that permits dissolved CO2 to be detected in organic media via simple color changes or through ratiometric differences in fluorescence intensity. NAP-chol 1 also acts as a super gelator for DMSO. The resulting gel is transformed into a homogeneous solution upon exposure to fluoride anions. Bubbling with CO2 regenerates the gel. Subsequent flushing with N2 or heating serves to release the CO2 and reform the sol form. This series of transformations is reversible and can be followed by easy-to-discern color changes. Thus, NAP-chol 1 allows for the capture and release of CO2 gas while acting as a three mode sensing system. In particular, it permits CO2 to be detected through reversible sol-gel transitions, simple changes in color, or ratiometric monitoring of the differences in the fluorescence features.

Intercalation and retention of carbon dioxide in a smectite clay promoted by interlayer cations.

PubMed

Michels, L; Fossum, J O; Rozynek, Z; Hemmen, H; Rustenberg, K; Sobas, P A; Kalantzopoulos, G N; Knudsen, K D; Janek, M; Plivelic, T S; da Silva, G J

2015-03-05

A good material for CO2 capture should possess some specific properties: (i) a large effective surface area with good adsorption capacity, (ii) selectivity for CO2, (iii) regeneration capacity with minimum energy input, allowing reutilization of the material for CO2 adsorption, and (iv) low cost and high environmental friendliness. Smectite clays are layered nanoporous materials that may be good candidates in this context. Here we report experiments which show that gaseous CO2 intercalates into the interlayer nano-space of smectite clay (synthetic fluorohectorite) at conditions close to ambient. The rate of intercalation, as well as the retention ability of CO2 was found to be strongly dependent on the type of the interlayer cation, which in the present case is Li(+), Na(+) or Ni(2+). Interestingly, we observe that the smectite Li-fluorohectorite is able to retain CO2 up to a temperature of 35°C at ambient pressure, and that the captured CO2 can be released by heating above this temperature. Our estimates indicate that smectite clays, even with the standard cations analyzed here, can capture an amount of CO2 comparable to other materials studied in this context.

Intercalation and Retention of Carbon Dioxide in a Smectite Clay promoted by Interlayer Cations

PubMed Central

Michels, L.; Fossum, J. O.; Rozynek, Z.; Hemmen, H.; Rustenberg, K.; Sobas, P. A.; Kalantzopoulos, G. N.; Knudsen, K. D.; Janek, M.; Plivelic, T. S.; da Silva, G. J.

2015-01-01

A good material for CO2 capture should possess some specific properties: (i) a large effective surface area with good adsorption capacity, (ii) selectivity for CO2, (iii) regeneration capacity with minimum energy input, allowing reutilization of the material for CO2 adsorption, and (iv) low cost and high environmental friendliness. Smectite clays are layered nanoporous materials that may be good candidates in this context. Here we report experiments which show that gaseous CO2 intercalates into the interlayer nano-space of smectite clay (synthetic fluorohectorite) at conditions close to ambient. The rate of intercalation, as well as the retention ability of CO2 was found to be strongly dependent on the type of the interlayer cation, which in the present case is Li+, Na+ or Ni2+. Interestingly, we observe that the smectite Li-fluorohectorite is able to retain CO2 up to a temperature of 35°C at ambient pressure, and that the captured CO2 can be released by heating above this temperature. Our estimates indicate that smectite clays, even with the standard cations analyzed here, can capture an amount of CO2 comparable to other materials studied in this context. PMID:25739522

Advanced wastewater treatment using microalgae: effect of temperature on removal of nutrients and organic carbon

NASA Astrophysics Data System (ADS)

Mohamad, Shurair; Fares, Almomani; Judd, Simon; Bhosale, Rahul; Kumar, Anand; Gosh, Ujjal; Khreisheh, Majeda

2017-05-01

This study evaluated the use of mixed indigenous microalgae (MIMA) as a treatment process for wastewaters and CO2 capturing technology at different temperatures. The study follows the growth rate of MIMA, CO2 Capturing from flue gas, removals of organic matter and nutrients from three types of wastewater (primary effluent, secondary effluent and septic effluent). A noticeable difference between the growth patterns of MIMA was observed at different CO2 and different operational temperatures. MIMA showed the highest growth grate when injected with CO2 dosage of 10% compared to the growth for the systems injected with 5% and 15 % of CO2. Ammonia and phosphorus removals for Spirulina were 69%, 75%, and 83%, and 20%, 45% and 75 % for the media injected with 0, 5 and 10% CO2. The results of this study show that simple and cost-effective microalgae-based wastewater treatment systems can be successfully employed at different temperatures as a successful CO2 capturing technology even with the small probability of inhibition at high temperatures.

Mineral Carbonation Feasibility, an Economic Approach.

NASA Astrophysics Data System (ADS)

Pasquier, L. C.; Kemache, N.; Cecchi, E.; Mercier, G.; Blais, J. F.; Kentish, S.

2016-12-01

Mineral Carbonation (MC) is one of the ways proposed to mitigate Carbon dioxide (CO2) emissions. Although it intends to transform CO2 into a stable and inert carbonate by reacting it with any divalent containing material, MC is still globally seen as an unrealistic methodology to reduce CO2, mostly because carbonation was seen as a sequestration technique only (after CO2 capture). Nevertheless, recent studies considered and showed the feasibility of an integrated capture/storage approach. Thus, MC can be adapted to flue gas or other industrial gas streams more or less concentrated in CO2. Furthermore, carbonation can be applied to various problematics and offers the advantage to be feasible with a broad range of feedstock such as alkaline industrial or mining residues. Using an economic approach where by-product valorization is favored, interesting approaches were identified. More specifically, the particular case of the Québec province shows that different synergies between wastes and industries can be elaborated. The results indicate that MC can be seen as a practical approach to both reduce CO2 emissions and enhance waste remediation. For instance, the feasibility to export significant amounts of serpentinite mining residue to distant industrial sites using the St Lawrence maritime route was demonstrated. Here the applicability stands on the high value of the generated by-products. On the other hand, steel slags or waste concrete need more local applications due to their limited reaction efficiencies and the lower price of calcium carbonates. While transportation is a major factor for the OPEX cost, the profitability relies on the by-products potential sale. Indeed, the production of low carbon footprint materials from the reaction product will also expand the offer of CO2 utilization avenues. The presentation highlights the results of research made in the lab and using economic modeling to draw a portrait of the opportunities and challenges identified with this regional approach that can apply to a wider range worldwide.

Influence of methane in CO2 transport and storage for CCS technology.

PubMed

Blanco, Sofía T; Rivas, Clara; Fernández, Javier; Artal, Manuela; Velasco, Inmaculada

2012-12-04

CO(2) Capture and Storage (CCS) is a good strategy to mitigate levels of atmospheric greenhouse gases. The type and quantity of impurities influence the properties and behavior of the anthropogenic CO(2), and so must be considered in the design and operation of CCS technology facilities. Their study is necessary for CO(2) transport and storage, and to develop theoretical models for specific engineering applications to CCS technology. In this work we determined the influence of CH(4), an important impurity of anthropogenic CO(2), within different steps of CCS technology: transport, injection, and geological storage. For this, we obtained new pressure-density-temperature (PρT) and vapor-liquid equilibrium (VLE) experimental data for six CO(2) + CH(4) mixtures at compositions which represent emissions from the main sources in the European Union and United States. The P and T ranges studied are within those estimated for CO(2) pipelines and geological storage sites. From these data we evaluated the minimal pressures for transport, regarding the density and pipeline's capacity requirements, and values for the solubility parameter of the mixtures, a factor which governs the solubility of substances present in the reservoir before injection. We concluded that the presence of CH(4) reduces the storage capacity and increases the buoyancy of the CO(2) plume, which diminishes the efficiency of solubility and residual trapping of CO(2), and reduces the injectivity into geological formations.

Carbon Capture and Utilization in the Industrial Sector.

PubMed

Psarras, Peter C; Comello, Stephen; Bains, Praveen; Charoensawadpong, Panunya; Reichelstein, Stefan; Wilcox, Jennifer

2017-10-03

The fabrication and manufacturing processes of industrial commodities such as iron, glass, and cement are carbon-intensive, accounting for 23% of global CO 2 emissions. As a climate mitigation strategy, CO 2 capture from flue gases of industrial processes-much like that of the power sector-has not experienced wide adoption given its high associated costs. However, some industrial processes with relatively high CO 2 flue concentration may be viable candidates to cost-competitively supply CO 2 for utilization purposes (e.g., polymer manufacturing, etc.). This work develops a methodology that determines the levelized cost ($/tCO 2 ) of separating, compressing, and transporting carbon dioxide. A top-down model determines the cost of separating and compressing CO 2 across 18 industrial processes. Further, the study calculates the cost of transporting CO 2 via pipeline and tanker truck to appropriately paired sinks using a bottom-up cost model and geo-referencing approach. The results show that truck transportation is generally the low-cost alternative given the relatively small volumes (ca. 100 kt CO 2 /a). We apply our methodology to a regional case study in Pennsylvania, which shows steel and cement manufacturing paired to suitable sinks as having the lowest levelized cost of capture, compression, and transportation.

Lithium-functionalized germanene: A promising media for CO2 capture

NASA Astrophysics Data System (ADS)

Mehdi Aghaei, S.; Monshi, M. M.; Torres, I.; Banakermani, M.; Calizo, I.

2018-02-01

Density functional theory (DFT) is employed to investigate the interactions of CO2 gas molecules with pristine and lithium-functionalized germanene. It is discovered that although a single CO2 molecule is weakly physisorbed on pristine germanene, a significant improvement on its adsorption energy is found by utilizing Li-functionalized germanene as the adsorbent. Excitingly, the moderate adsorption energy at high CO2 coverage secures an easy release step. Moreover, the structure of Li-functionalized germanene can be fully recovered after removal of CO2 gas molecules. Our results suggest that Li-functionalized germanene show promise for CO2 sensing and capture with a storage capacity of 12.57 mol/kg.

Microstructural Response of Variably Hydrated Ca-Rich Montmorillonite to Supercritical CO2

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lee, Mal Soon; McGrail, B. Peter; Glezakou, Vassiliki Alexandra

2014-08-05

We report on ab initio molecular dynamics simulations of Ca-rich montmorillonite systems, in different hydration states in the presence of supercritical CO2. Analysis of the molecular trajectories provides estimates of the relative H2O:CO2 ratio per interspatial cation. The vibrational density of states in direct comparison with dipole moment derived IR spectra for these systems provide unique signatures that can used to follow molecular transformation. In a co-sequestration scenario, these signatures could be used to identify the chemical state and fate of Sulfur compounds. Interpretation of CO2 asymmetric stretch shift is given based on a detailed analysis of scCO2 structure andmore » intermolecular interactions of the intercalated species. Based on our simulations, smectites with higher charge interlayer cations at sub-single to single hydration states should be more efficient in capturing CO2, while maintaining caprock integrity. This research would not have been possible without the support of the office of Fossil Energy, Department of Energy. The computational resources were made available through a user proposal of the EMSL User facility, a national scientific user facility sponsored by the Department of Energy's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory.« less

A first-principles density functional theory study of the electronic structural and thermodynamic properties of M2ZrO3 and M2CO3 (M=Na, K) and their capabilities for CO2 capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yuhua Duan

2012-01-01

Alkali metal zirconates could be used as solid sorbents for CO{sub 2} capture. The structural, electronic, and phonon properties of Na{sub 2}ZrO{sub 3}, K{sub 2}ZrO{sub 3}, Na{sub 2}CO{sub 3}, and K{sub 2}CO{sub 3} are investigated by combining the density functional theory with lattice phonon dynamics. The thermodynamics of CO{sub 2} absorption/desorption reactions of these two zirconates are analyzed. The calculated results show that their optimized structures are in a good agreement with experimental measurements. The calculated band gaps are 4.339 eV (indirect), 3.641 eV (direct), 3.935 eV (indirect), and 3.697 eV (direct) for Na{sub 2}ZrO{sub 3}, K{sub 2}ZrO{sub 3}, Na{submore » 2}CO{sub 3}, and K{sub 2}CO{sub 3}, respectively.The calculated phonon dispersions and phonon density of states for M{sub 2}ZrO{sub 3} and M{sub 2}CO{sub 3} (M = K, Na, Li) revealed that from K to Na to Li, their frequency peaks are shifted to high frequencies due to the molecular weight decreased from K to Li. From the calculated reaction heats and relationships of free energy change versus temperatures and CO{sub 2} pressures of the M{sub 2}ZrO{sub 3} (M = K, Na, Li) reacting with CO{sub 2}, we found that the performance of Na{sub 2}ZrO{sub 3} capturing CO{sub 2} is similar to that of Li{sub 2}ZrO{sub 3} and is better than that of K{sub 2}ZrO{sub 3}. Therefore, Na{sub 2}ZrO{sub 3} and Li{sub 2}ZrO{sub 3} are good candidates of high temperature CO{sub 2} sorbents and could be used for post combustion CO{sub 2} capture technologies.« less

Inorganic membranes for carbon capture and power generation

NASA Astrophysics Data System (ADS)

Snider, Matthew T.

Inorganic membranes are under consideration for cost-effective reductions of carbon emissions from coal-fired power plants, both in the capture of pollutants post-firing and in the direct electrochemical conversion of coal-derived fuels for improved plant efficiency. The suitability of inorganic membrane materials for these purposes stems as much from thermal and chemical stability in coal plant operating conditions as from high performance in gas separations and power generation. Hydrophilic, micro-porous zeolite membrane structures are attractive for separating CO2 from N2 in gaseous waste streams due to the attraction of CO2 to the membrane surface and micropore walls that gives the advantage to CO2 transport. Recent studies have indicated that retention of the templating agent used in zeolite synthesis can further block N2 from the micropore interior and significantly improve CO2/N2 selectivity. However, the role of the templating agent in micro-porous transport has not been well investigated. In this work, gas sorption studies were conducted by high-pressure thermo-gravimetric analysis on Zeolite Y membrane materials to quantify the effect of the templating agent on CO2, N2, and H2O adsorption/desorption, as well as to examine the effect of humidification on overall membrane performance. In equilibrium conditions, the N2 sorption enthalpy was nearly unchanged by the presence of the templating agent, but the N2 pore occupation was reduced ˜1000x. Thus, the steric nature of the blocking of N2 from the micropores by the templating agent was confirmed. CO2 and H2O sorption enthalpies were similarly unaffected by the templating agent, and the micropore occupations were only reduced as much as the void volume taken up by the templating agent. Thus, the steric blocking effect did not occur for molecules more strongly attracted to the micropore walls. Additionally, in time-transient measurements the CO 2 and H2O mobilities were significantly enhanced by the presence of the templating agent. This meant that small restrictions in the micropores were beneficial to the transport of molecules with some attraction to the micropore walls. Further evidence of this effect were discovered in transport studies on Zeolite Y membranes, in which small amounts of residual water were observed to enhance the CO2 permeance in a similar way as the templating agent in the powder. However, the effect was only observed for dry CO 2 streams and previously humidified membranes. H2O affinity for the zeolite framework was so high and mobility in the micropores was so low that even 0.8 mol% H2O included in the gas stream was enough to reduce CO2 transport by 100x. This poses a serious concern for carbon capture by zeolite Y membrane in coal-fired power plants: the waste stream must be dehumidified first. In the long-term, raising the efficiencies of fossil-fuel power plants is preferable to post-combustion capture for cost- and resource-effective carbon emissions reduction. Supplementing combustion of the fuel with electrochemical conversion by solid oxide fuel cell (SOFC) shows promise in this effort. Thin-film (<1microm thick) SOFCs have recently exhibited power densities at low temperature (LT) that rival those of thick-film, high-temperature designs, with improved stability and quick ramp times. Low operating temperatures also provide the potential for fast, high-volume production, but so far high-performing LT-SOFCs have all been made by micro-fabrication methods. In this work, thin-film LT-SOFC modules were fabricated by colloidal processing and their performance was demonstrated. Nano-particulate colloid syntheses, dip-coating, and rapid thermal processing methods yielded fine-particle membrane microstructures, with high porosity and conductivity in the platinum/gadolinium-doped ceria (GDC) composite electrodes and density in the yttria-stabilized zirconia (YSZ) electrolytes. Power densities of >1000 W/m2 at 450°C and ˜5000 W/m2 at 600°C were achieved, and the modules ran >100hrs at peak power after 8 thermal cycles. Thus it was demonstrated that high performing LT-SOFCs can be produced with large-scale methods.

Chemical and Biological Catalytic Enhancement of Weathering of Silicate Minerals and industrial wastes as a Novel Carbon Capture and Storage Technology

NASA Astrophysics Data System (ADS)

Park, A. H. A.

2014-12-01

Increasing concentration of CO2 in the atmosphere is attributed to rising consumption of fossil fuels around the world. The development of solutions to reduce CO2 emissions to the atmosphere is one of the most urgent needs of today's society. One of the most stable and long-term solutions for storing CO2 is via carbon mineralization, where minerals containing metal oxides of Ca or Mg are reacted with CO2 to produce thermodynamically stable Ca- and Mg-carbonates that are insoluble in water. Carbon mineralization can be carried out in-situ or ex-situ. In the case of in-situ mineralization, the degree of carbonation is thought to be limited by both mineral dissolution and carbonate precipitation reaction kinetics, and must be well understood to predict the ultimate fate of CO2 within geological reservoirs. While the kinetics of in-situ mineral trapping via carbonation is naturally slow, it can be enhanced at high temperature and high partial pressure of CO2. The addition of weak organic acids produced from food waste has also been shown to enhance mineral weathering kinetics. In the case of the ex-situ carbon mineralization, the role of these ligand-bearing organic acids can be further amplified for silicate mineral dissolution. Unfortunately, high mineral dissolution rates often lead to the formation of a silica-rich passivation layer on the surface of silicate minerals. Thus, the use of novel solvent mixture that allows chemically catalyzed removal of this passivation layer during enhanced Mg-leaching surface reaction has been proposed and demonstrated. Furthermore, an engineered biological catalyst, carbonic anhydrase, has been developed and evaluated to accelerate the hydration of CO2, which is another potentially rate-limiting step of the carbonation reaction. The development of these novel catalytic reaction schemes has significantly improved the overall efficiency and sustainability of in-situ and ex-situ mineral carbonation technologies and allowed direct capture and storage of CO2 from mixture gas streams eliminating the energy-intensive solvent regeneration and CO2 compression steps.

Tilted pillar array fabrication by the combination of proton beam writing and soft lithography for microfluidic cell capture Part 2: Image sequence analysis based evaluation and biological application.

PubMed

Járvás, Gábor; Varga, Tamás; Szigeti, Márton; Hajba, László; Fürjes, Péter; Rajta, István; Guttman, András

2018-02-01

As a continuation of our previously published work, this paper presents a detailed evaluation of a microfabricated cell capture device utilizing a doubly tilted micropillar array. The device was fabricated using a novel hybrid technology based on the combination of proton beam writing and conventional lithography techniques. Tilted pillars offer unique flow characteristics and support enhanced fluidic interaction for improved immunoaffinity based cell capture. The performance of the microdevice was evaluated by an image sequence analysis based in-house developed single-cell tracking system. Individual cell tracking allowed in-depth analysis of the cell-chip surface interaction mechanism from hydrodynamic point of view. Simulation results were validated by using the hybrid device and the optimized surface functionalization procedure. Finally, the cell capture capability of this new generation microdevice was demonstrated by efficiently arresting cells from a HT29 cell-line suspension. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Carbon Dioxide Separation from Flue Gases: A Technological Review Emphasizing Reduction in Greenhouse Gas Emissions

PubMed Central

Songolzadeh, Mohammad; Soleimani, Mansooreh; Takht Ravanchi, Maryam; Songolzadeh, Reza

2014-01-01

Increasing concentrations of greenhouse gases (GHGs) such as CO2 in the atmosphere is a global warming. Human activities are a major cause of increased CO2 concentration in atmosphere, as in recent decade, two-third of greenhouse effect was caused by human activities. Carbon capture and storage (CCS) is a major strategy that can be used to reduce GHGs emission. There are three methods for CCS: pre-combustion capture, oxy-fuel process, and post-combustion capture. Among them, post-combustion capture is the most important one because it offers flexibility and it can be easily added to the operational units. Various technologies are used for CO2 capture, some of them include: absorption, adsorption, cryogenic distillation, and membrane separation. In this paper, various technologies for post-combustion are compared and the best condition for using each technology is identified. PMID:24696663

Carbon dioxide separation from flue gases: a technological review emphasizing reduction in greenhouse gas emissions.

PubMed

Songolzadeh, Mohammad; Soleimani, Mansooreh; Takht Ravanchi, Maryam; Songolzadeh, Reza

2014-01-01

Increasing concentrations of greenhouse gases (GHGs) such as CO2 in the atmosphere is a global warming. Human activities are a major cause of increased CO2 concentration in atmosphere, as in recent decade, two-third of greenhouse effect was caused by human activities. Carbon capture and storage (CCS) is a major strategy that can be used to reduce GHGs emission. There are three methods for CCS: pre-combustion capture, oxy-fuel process, and post-combustion capture. Among them, post-combustion capture is the most important one because it offers flexibility and it can be easily added to the operational units. Various technologies are used for CO2 capture, some of them include: absorption, adsorption, cryogenic distillation, and membrane separation. In this paper, various technologies for post-combustion are compared and the best condition for using each technology is identified.

Efficient SO2 capture by amine functionalized PEG.

PubMed

Yang, Dezhong; Hou, Minqiang; Ning, Hui; Zhang, Jianling; Ma, Jun; Han, Buxing

2013-11-07

Polyethylene glycols (PEGs) are a class of non-toxic, non-volatile, biocompatible, and widely available polymers. In this work, we synthesized N-ethyl-N-(2-(2-(2-methoxyethoxy)ethoxy)ethyl)-2-aminoethanol (EE3AE) that combines the properties of PEG and amines, and N-decyl-N-ethyl-2-aminoethanol (DEAE). Their performances to capture SO2 were studied at different temperatures, pressures, and absorption times. The interaction between the absorbents and SO2 were characterized by NMR and FTIR techniques. It was demonstrated that both EE3AE and DEAE could absorb SO2 efficiently, and there existed chemical and physical interactions between the absorbents and SO2. In particular, the absorption capacity of EE3AE could be as high as 1.09 g SO2 per g EE3AE at 1 atm. The absorption capacity of EE3AE was much larger than that of DEAE because the ether group in the EE3AE interacted with SO2 more strongly than the alkyl group in the DEAE. The SO2 absorbed by EE3AE could be stripped out by bubbling N2 or by applying a vacuum and the EE3AE could be reused. Moreover, both absorbents exhibited a high SO2-CO2 selectivity.

High capacity immobilized amine sorbents

DOEpatents

Gray, McMahan L [Pittsburgh, PA; Champagne, Kenneth J [Fredericktown, PA; Soong, Yee [Monroeville, PA; Filburn, Thomas [Granby, CT

2007-10-30

A method is provided for making low-cost CO.sub.2 sorbents that can be used in large-scale gas-solid processes. The improved method entails treating an amine to increase the number of secondary amine groups and impregnating the amine in a porous solid support. The method increases the CO.sub.2 capture capacity and decreases the cost of utilizing an amine-enriched solid sorbent in CO.sub.2 capture systems.

Absorber modeling for NGCC carbon capture with aqueous piperazine.

PubMed

Zhang, Yue; Freeman, Brice; Hao, Pingjiao; Rochelle, Gary T

2016-10-20

A hybrid system combining amine scrubbing with membrane technology for carbon capture from natural gas combined cycle (NGCC) power plants is proposed in this paper. In this process, the CO 2 in the flue gas can be enriched from 4% to 18% by the membrane, and the amine scrubbing system will have lower capture costs. Aqueous piperazine (PZ) is chosen as the solvent. Different direct contact cooler (DCC) options, multiple absorber operating conditions, optimal intercooling designs, and different cooling options have been evaluated across a wide range of inlet CO 2 . Amine scrubbing without DCC is a superior design for NGCC carbon capture. Pump-around cooling at the bottom of the absorber can effectively manage the temperature of the hot flue gas, and still be effective for CO 2 absorption. The absorber gas inlet must be designed to avoid excessive localized temperature and solvent evaporation. When the inlet CO 2 increases from 4% to 18%, total absorber CAPEX decreases by 60%; another 10% of the total absorber CAPEX can be saved by eliminating the DCC. In-and-out intercooling works well for high CO 2 , while pump-around intercooling is more effective for low CO 2 . Dry cooling requires more packing and energy but appears to be technically and economically feasible if cooling water availability is limited.

Hybrid Encapsulated Ionic Liquids for Post-Combustion Carbon Dioxide (CO 2) Capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Brennecke, Joan F; Degnan, Jr, Thomas Francis; McCready, Mark J.

Ionic liquids (ILs) and Phase Change Ionic Liquids (PCILs) are excellent materials for selective removal of carbon dioxide from dilute post-combustion streams. However, they are typically characterized as having high viscosities, which impairs their effectiveness due to mass transfer limitations, caused by the high viscosities. In this project, we are examining the benefits of encapsulating ILs and PCILs in thin polymeric shells to produce particles of approximately 100 to 600 µm in diameter that can be used in a fluidized bed absorber. The particles are produced by microencapsulation of the ILs and PCILs in CO 2-permeable polymer shells. Here wemore » report on the encapsulation of the IL and PCIL materials, thermodynamic testing of the encapsulated materials, mass transfer measurements in both a fluidized bed and a packed bed, determination of the effect of impurities (SO 2, NO x and water) on the free and encapsulated IL and PCIL, recyclability of the CO 2 uptake, selection and synthesis of kg quantities of the IL and PCIL, identification of scale-up methods for encapsulation and production of a kg quantity of the PCIL, construction and shakedown of the laboratory scale unit to test the encapsulated particles for CO 2 capture ability and efficiency, use of our mass transfer model to predict mass transfer and identify optimal properties of the encapsulated particles, and initial testing of the encapsulated particles in the laboratory scale unit. We also show our attempts at developing shell materials that are resistant to water permeation. Overall, we have shown that the selected IL and PCIL can be successfully encapsulated in polymer shells and the methods scaled up to production levels. The IL/PCIL and encapsulated IL/PCIL react irreversibly with SO 2 and NO x so the CO 2 capture unit would need to be placed after the flue gas desulfurization and NO x reduction units. However, the reaction with CO 2 in the presence of water is completely reversible. Therefore, it is not necessary to exclude water from the capsules. Mass transfer in the fluidized and packed beds confirm that the fluidized bed arrangement is preferred and that the mass transfer can be predicted accurately by the rate based model that we have developed. Absorption and desorption experiments in the laboratory scale unit show good uptake and recyclability.« less

Analysing Trends in Light-Use Efficiency and Their Influence on Seasonal CO2 Amplitude Using a Simple Land Ecosystem Model

NASA Astrophysics Data System (ADS)

Thomas, R.; Prentice, I. C. C.; Graven, H. D.

2016-12-01

A simple model for gross primary production (GPP), the P-model, is used to analyse the recent increase in the amplitude of the seasonal cycle of CO2 (ASC) at high northern latitudes. Current terrestrial biosphere models and Earth System Models generally underestimate the observed increase in ASC since 1960. The increased ASC is primarily driven by an increase in net primary productivity (NPP), rather than respiration, so models are likely underestimating increases in NPP. In a recent study of process-based terrestrial biosphere models from the Multi-scale Synthesis and Terrestrial Model Intercomparison Project (MsTMIP), we showed that the concept of light-use efficiency can be used to separate modelled NPP changes into structural and physiological components (Thomas et al, 2016). The structural component (leaf area) can be tested against observations of greening, while the physiological component (light-use efficiency) is an emergent model property. The analysis suggests that current models are capturing the increases in vegetation greenness, but underestimating the increases in light-use efficiency and NPP. We test this hypothesis using the P-model, which explicitly uses greenness data and includes the effects of rising CO2 and climate change. In the P-model, GPP is calculated using only a few equations, which are based on a strong empirical and theoretical framework, and vegetation is not separated into plant functional types. The model is driven by observed greenness, CO2, temperature and vapour pressure, and modelled photosynthetically active radiation at a monthly time-step. Photosynthetic assimilation is based on two key assumptions: the co-limitation hypothesis (electron transport- and Rubisco-limited photosynthetic rates are equal), and the least-cost hypothesis (optimal ci:ca ratio), and is limited by modelled soil moisture. We present simulated changes in GPP over the satellite period (1982-2011) in the P-model, and assess the associated changes in light-use efficiency and ASC. Our results have implications for the attribution of drivers of ecosystem change and the formulation of prognostic and diagnostic biosphere models. Thomas, R. T. et al. 2016, CO2 and greening observations indicate increasing light-use efficiency in Northern terrestrial ecosystems, Geophys Res Lett, in review.

Integrating Reverse-Electrodialysis Stacks with Flow Batteries for Improved Energy Recovery from Salinity Gradients and Energy Storage.

PubMed

Zhu, Xiuping; Kim, Taeyoung; Rahimi, Mohammad; Gorski, Christopher A; Logan, Bruce E

2017-02-22

Salinity gradient energy can be directly converted into electrical power by using reverse electrodialysis (RED) and other technologies, but reported power densities have been too low for practical applications. Herein, the RED stack performance was improved by using 2,6-dihydroxyanthraquinone and ferrocyanide as redox couples. These electrolytes were then used in a flow battery to produce an integrated RED stack and flow battery (RED-FB) system capable of capturing, storing, and discharging salinity gradient energy. Energy captured from the RED stack was discharged in the flow battery at a maximum power density of 3.0 kW m -2 -anode, which was similar to the flow batteries charged by electrical power and could be used for practical applications. Salinity gradient energy captured from the RED stack was recovered from the electrolytes as electricity with 30 % efficiency, and the maximum energy density of the system was 2.4 kWh m -3 -anolyte. The combined RED-FB system overcomes many limitations of previous approaches to capture, store, and use salinity gradient energy from natural or engineered sources. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Review of Membrane Oxygen Enrichment for Efficient Combustion

NASA Astrophysics Data System (ADS)

Ariono, Danu; Kusuma Wardani, Anita

2017-07-01

Oxygen enrichment from air is a simple way of increasing the efficiency of combustion process, as in oxy-combustion. Oxy-combustion has become one of the most attracting combustion technologies because of its potential to address both pollutant reduction and CO2 capture. In oxy-combustion, the fuel and recycled flue gas are combusted with oxygen enriched air (OEA). By using OEA, many benefits can be obtained, such as increasing available heat, improving ignition characteristics, flue gas reduction, increasing productivity, energy efficiency, turndown ratio, and flame stability. Membrane-based gas separation for OEA production becomes an attractive technology over the conventional technology due to the some advantages, including low capital cost, low energy consumption, compact size, and modularity. A single pass through membrane usually can enrich O2 concentration in the air up to 35% and a 50% concentration can be achieved with a double pass of membrane. The use of OEA in the combustion process eliminates the presence of nitrogen in the flue gas. Hence, the flue gas is mainly composed of CO2 and condensable water that can be easily separated. This paper gives an overview of oxy-combustion with membrane technology for oxygen enrichment process. Special attention is given to OEA production and the effect of OEA to the efficiency of combustion.

The Description and Validation of a Computationally-Efficient CH4-CO-OH (ECCOH) Module for 3D Model Applications

NASA Technical Reports Server (NTRS)

Elshorbany, Yasin F.; Duncan, Bryan N.; Strode, Sarah A.; Wang, James S.; Kouatchou, Jules

2015-01-01

We present the Efficient CH4-CO-OH Module (ECCOH) that allows for the simulation of the methane, carbon monoxide and hydroxyl radical (CH4-CO-OH cycle, within a chemistry climate model, carbon cycle model, or earth system model. The computational efficiency of the module allows many multi-decadal, sensitivity simulations of the CH4-CO-OH cycle, which primarily determines the global tropospheric oxidizing capacity. This capability is important for capturing the nonlinear feedbacks of the CH4-CO-OH system and understanding the perturbations to relatively long-lived methane and the concomitant impacts on climate. We implemented the ECCOH module into the NASA GEOS-5 Atmospheric Global Circulation Model (AGCM), performed multiple sensitivity simulations of the CH4-CO-OH system over two decades, and evaluated the model output with surface and satellite datasets of methane and CO. The favorable comparison of output from the ECCOH module (as configured in the GEOS-5 AGCM) with observations demonstrates the fidelity of the module for use in scientific research.

CFD Simulations of a Regenerative Process for Carbon Dioxide Capture in Advanced Gasification Based Power Systems

DOE Office of Scientific and Technical Information (OSTI.GOV)

Arastoopour, Hamid; Abbasian, Javad

2014-07-31

This project describes the work carried out to prepare a highly reactive and mechanically strong MgO based sorbents and to develop a Population Balance Equations (PBE) approach to describe the evolution of the particle porosity distribution that is linked with Computational Fluid Dynamics (CFD) to perform simulations of the CO2 capture and sorbent regeneration. A large number of MgO-based regenerable sorbents were prepared using low cost and abundant dolomite as the base material. Among various preparation parameters investigated the potassium/magnesium (K/Mg) ratio was identified as the key variable affecting the reactivity and CO2 capacity of the sorbent. The optimum K/Mgmore » ratio is about 0.15. The sorbent formulation HD52-P2 was identified as the “best” sorbent formulation and a large batch (one kg) of the sorbent was prepared for the detailed study. The results of parametric study indicate the optimum carbonation and regeneration temperatures are 360° and 500°C, respectively. The results also indicate that steam has a beneficial effect on the rate of carbonation and regeneration of the sorbent and that the reactivity and capacity of the sorbent decreases in the cycling process (sorbent deactivation). The results indicate that to achieve a high CO2 removal efficiency, the bed of sorbent should be operated at a temperature range of 370-410°C which also favors production of hydrogen through the WGS reaction. To describe the carbonation reaction kinetics of the MgO, the Variable Diffusivity shrinking core Model (VDM) was developed in this project, which was shown to accurately fit the experimental data. An important advantage of this model is that the changes in the sorbent conversion with time can be expressed in an explicit manner, which will significantly reduce the CFD computation time. A Computational Fluid Dynamic/Population Balance Equations (CFD/PBE) model was developed that accounts for the particle (sorbent) porosity distribution and a new version of the method of moments, called Finite size domain Complete set of trial functions Method Of Moments (FCMOM) was used to solve the population balance equations. The PBE model was implemented in a commercial CFD code, Ansys Fluent 13.0. The code was used to test the model in some simple cases and the results were verified against available analytical solution in the literature. Furthermore, the code was used to simulate CO2 capture in a packed-bed and the results were in excellent agreement with the experimental data obtained in the packed bed. The National Energy Laboratory (NETL) Carbon Capture Unit (C2U) design was used in simulate of the hydrodynamics of the cold flow gas/solid system (Clark et al.58). The results indicate that the pressure drop predicted by the model is in good agreement with the experimental data. Furthermore, the model was shown to be able to predict chugging behavior, which was observed during the experiment. The model was used as a base-case for simulations of reactive flow at elevated pressure and temperatures. The results indicate that by controlling the solid circulation rate, up to 70% CO2 removal can be achieved and that the solid hold up in the riser is one of the main factors controlling the extent of CO2 removal. The CFD/PBE simulation model indicates that by using a simulated syngas with a composition of 20% CO2, 20% H2O, 30% CO, and 30% H2, the composition (wet basis) in the reactor outlet corresponded to about 60% CO2 capture with and exit gas containing 65% H2. A preliminary base-case-design was developed for a regenerative MgO-based pre-combustion carbon capture process for a 500 MW IGCC power plant. To minimize the external energy requirement, an extensive heat integration network was developed in Aspen/HYSYS® to produce the steam required in the regenerator and heat integration. In this process, liquid CO2 produced at 50 atm can easily be pumped and sequestered or stored. The preliminary economic analyses indicate that the estimated cost of carbon v capture is in the range of $31-$44/ton, suggesting that a regenerative MgO-Based process can be a viable option for pre-combustion carbon dioxide capture in advanced gasification based power systems.« less

Hopewell Beneficial CO2 Capture for Production of Fuels, Fertilizer and Energy

DOE Office of Scientific and Technical Information (OSTI.GOV)

UOP; Honeywell Resins & Chemicals; Honeywell Process Solutions

2010-09-30

For Phase 1 of this project, the Hopewell team developed a detailed design for the Small Scale Pilot-Scale Algal CO2 Sequestration System. This pilot consisted of six (6) x 135 gallon cultivation tanks including systems for CO2 delivery and control, algal cultivation, and algal harvesting. A feed tank supplied Hopewell wastewater to the tanks and a receiver tank collected the effluent from the algal cultivation system. The effect of environmental parameters and nutrient loading on CO2 uptake and sequestration into biomass were determined. Additionally the cost of capturing CO2 from an industrial stack emission at both pilot and full-scale wasmore » determined. The engineering estimate evaluated Amine Guard technology for capture of pure CO2 and direct stack gas capture and compression. The study concluded that Amine Guard technology has lower lifecycle cost at commercial scale, although the cost of direct stack gas capture is lower at the pilot scale. Experiments conducted under high concentrations of dissolved CO2 did not demonstrate enhanced algae growth rate. This result suggests that the dissolved CO2 concentration at neutral pH was already above the limiting value. Even though dissolved CO2 did not show a positive effect on biomass growth, controlling its value at a constant set-point during daylight hours can be beneficial in an algae cultivation stage with high algae biomass concentration to maximize the rate of CO2 uptake. The limited enhancement of algal growth by CO2 addition to Hopewell wastewater was due at least in part to the high endogenous CO2 evolution from bacterial degradation of dissolved organic carbon present at high levels in the wastewater. It was found that the high level of bacterial activity was somewhat inhibitory to algal growth in the Hopewell wastewater. The project demonstrated that the Honeywell automation and control system, in combination with the accuracy of the online pH, dissolved O2, dissolved CO2, turbidity, Chlorophyll A and conductivity sensors is suitable for process control of algae cultivation in an open pond systems. This project concluded that the Hopewell wastewater is very suitable for algal cultivation but the potential for significant CO2 sequestration from the plant stack gas emissions was minimal due to the high endogenous CO2 generation in the wastewater from the organic wastewater content. Algae cultivation was found to be promising, however, for nitrogen remediation in the Hopewell wastewater.« less

Environmental potential of the use of CO2 from alcoholic fermentation processes. The CO2-AFP strategy.

PubMed

Alonso-Moreno, Carlos; García-Yuste, Santiago

2016-10-15

A novel Carbon Dioxide Utilization (CDU) approach from a relatively minor CO2 emission source, i.e., alcoholic fermentation processes (AFP), is presented. The CO2 produced as a by-product from the AFP is estimated by examining the EtOH consumed per year reported by the World Health Organization in 2014. It is proposed that the extremely pure CO2 from the AFP is captured in NaOH solutions to produce one of the Top 10 commodities in the chemical industry, Na2CO3, as a good example of an atomic economy process. The novel CDU strategy could yield over 30.6Mt of Na2CO3 in oversaturated aqueous solution on using ca. 12.7Mt of captured CO2 and this process would consume less energy than the synthetic methodology (Solvay ammonia soda process) and would not produce low-value by-products. The quantity of Na2CO3 obtained by this strategy could represent ca. 50% of the world Na2CO3 production in one year. In terms of the green economy, the viability of the strategy is discussed according to the recommendations of the CO2Chem network, and an estimation of the CO2negative emission achieved suggests a capture of around 280.0Mt of CO2 from now to 2020 or ca. 1.9Gt from now to 2050. Finally, the results obtained for this new CDU proposal are discussed by considering different scenarios; the CO2 production in a typical winemaking corporation, the CO2 released in the most relevant wine-producing countries, and the use of CO2 from AFP as an alternative for the top Na2CO3-producing countries. Copyright © 2016 Elsevier B.V. All rights reserved.

Synthesis of sintering-resistant sorbents for CO2 capture.

PubMed

Liu, Wenqiang; Feng, Bo; Wu, Yueqin; Wang, Guoxiong; Barry, John; da Costa, João C Diniz

2010-04-15

Sorbents for high temperature CO2 capture are under intensive development owing to their potential applications in advanced zero emission power, sorption-enhanced steam methane reforming for hydrogen production and energy storage systems in chemical heat pumps. One of the challenges in the development is the prevention of sintering of the sorbent (normally a calcium oxide derivative) which causes the CO2 capture capacity of the material to deteriorate rapidly after a few cycles of utilization. Here we show that a simple wet mixing method can produce sintering-resistant sorbents from calcium and magnesium salts of d-gluconic acid. It was found that calcium oxide was well distributed in the sorbents with metal oxide nanoparticles on the surface acting as physical barriers, and the CO2 capture capacity of the sorbents was largely maintained over multiple cycles of utilization. This method was also applied to other organometallic salts of calcium and magnesium/aluminum and the produced sorbents showed similarly high reversibility.

Integrated CO2 capture-fixation chemistry via interfacial ionic liquid catalyst in laminar gas/liquid flow

NASA Astrophysics Data System (ADS)

Vishwakarma, Niraj K.; Singh, Ajay K.; Hwang, Yoon-Ho; Ko, Dong-Hyeon; Kim, Jin-Oh; Babu, A. Giridhar; Kim, Dong-Pyo

2017-03-01

Simultaneous capture of carbon dioxide (CO2) and its utilization with subsequent work-up would significantly enhance the competitiveness of CO2-based sustainable chemistry over petroleum-based chemistry. Here we report an interfacial catalytic reaction platform for an integrated autonomous process of simultaneously capturing/fixing CO2 in gas-liquid laminar flow with subsequently providing a work-up step. The continuous-flow microreactor has built-in silicon nanowires (SiNWs) with immobilized ionic liquid catalysts on tips of cone-shaped nanowire bundles. Because of the superamphiphobic SiNWs, a stable gas-liquid interface maintains between liquid flow of organoamines in upper part and gas flow of CO2 in bottom part of channel. The intimate and direct contact of the binary reagents leads to enhanced mass transfer and facilitating reactions. The autonomous integrated platform produces and isolates 2-oxazolidinones and quinazolines-2,4(1H,3H)-diones with 81-97% yields under mild conditions. The platform would enable direct CO2 utilization to produce high-valued specialty chemicals from flue gases without pre-separation and work-up steps.

Integrated CO2 capture-fixation chemistry via interfacial ionic liquid catalyst in laminar gas/liquid flow.

PubMed

Vishwakarma, Niraj K; Singh, Ajay K; Hwang, Yoon-Ho; Ko, Dong-Hyeon; Kim, Jin-Oh; Babu, A Giridhar; Kim, Dong-Pyo

2017-03-06

Simultaneous capture of carbon dioxide (CO 2 ) and its utilization with subsequent work-up would significantly enhance the competitiveness of CO 2 -based sustainable chemistry over petroleum-based chemistry. Here we report an interfacial catalytic reaction platform for an integrated autonomous process of simultaneously capturing/fixing CO 2 in gas-liquid laminar flow with subsequently providing a work-up step. The continuous-flow microreactor has built-in silicon nanowires (SiNWs) with immobilized ionic liquid catalysts on tips of cone-shaped nanowire bundles. Because of the superamphiphobic SiNWs, a stable gas-liquid interface maintains between liquid flow of organoamines in upper part and gas flow of CO 2 in bottom part of channel. The intimate and direct contact of the binary reagents leads to enhanced mass transfer and facilitating reactions. The autonomous integrated platform produces and isolates 2-oxazolidinones and quinazolines-2,4(1H,3H)-diones with 81-97% yields under mild conditions. The platform would enable direct CO 2 utilization to produce high-valued specialty chemicals from flue gases without pre-separation and work-up steps.

Integrated CO2 capture-fixation chemistry via interfacial ionic liquid catalyst in laminar gas/liquid flow

PubMed Central

Vishwakarma, Niraj K.; Singh, Ajay K.; Hwang, Yoon-Ho; Ko, Dong-Hyeon; Kim, Jin-Oh; Babu, A. Giridhar; Kim, Dong-Pyo

2017-01-01

Simultaneous capture of carbon dioxide (CO2) and its utilization with subsequent work-up would significantly enhance the competitiveness of CO2-based sustainable chemistry over petroleum-based chemistry. Here we report an interfacial catalytic reaction platform for an integrated autonomous process of simultaneously capturing/fixing CO2 in gas–liquid laminar flow with subsequently providing a work-up step. The continuous-flow microreactor has built-in silicon nanowires (SiNWs) with immobilized ionic liquid catalysts on tips of cone-shaped nanowire bundles. Because of the superamphiphobic SiNWs, a stable gas–liquid interface maintains between liquid flow of organoamines in upper part and gas flow of CO2 in bottom part of channel. The intimate and direct contact of the binary reagents leads to enhanced mass transfer and facilitating reactions. The autonomous integrated platform produces and isolates 2-oxazolidinones and quinazolines-2,4(1H,3H)-diones with 81–97% yields under mild conditions. The platform would enable direct CO2 utilization to produce high-valued specialty chemicals from flue gases without pre-separation and work-up steps. PMID:28262667

Development of a carbonate absorption-based process for post-combustion CO2 capture: The role of biocatalyst to promote CO2 absorption rate

USGS Publications Warehouse

Lu, Y.; Ye, X.; Zhang, Z.; Khodayari, A.; Djukadi, T.

2011-01-01

An Integrated Vacuum Carbonate Absorption Process (IVCAP) for post-combustion carbon dioxide (CO2) capture is described. IVCAP employs potassium carbonate (PC) as a solvent, uses waste or low quality steam from the power plant for CO2 stripping, and employs a biocatalyst, carbonic anhydrase (CA) enzyme, for promoting the CO2 absorption into PC solution. A series of experiments were performed to evaluate the activity of CA enzyme mixed in PC solutions in a stirred tank reactor system under various temperatures, CA dosages, CO2 loadings, CO2 partial pressures, and the presence of major flue gas contaminants. It was demonstrated that CA enzyme is an effective biocatalyst for CO2 absorption under IVCAP conditions. ?? 2011 Published by Elsevier Ltd.

Multiphase, multicomponent simulations and experiments of reactive flow, relevant for combining geologic CO2 sequestration with geothermal energy capture

NASA Astrophysics Data System (ADS)

Saar, Martin O.

2011-11-01

Understanding the fluid dynamics of supercritical carbon dioxide (CO2) in brine- filled porous media is important for predictions of CO2 flow and brine displacement during geologic CO2 sequestration and during geothermal energy capture using sequestered CO2 as the subsurface heat extraction fluid. We investigate multiphase fluid flow in porous media employing particle image velocimetry experiments and lattice-Boltzmann fluid flow simulations at the pore scale. In particular, we are interested in the motion of a drop (representing a CO2 bubble) through an orifice in a plate, representing a simplified porous medium. In addition, we study single-phase/multicomponent reactive transport experimentally by injecting water with dissolved CO2 into rocks/sediments typically considered for CO2 sequestration to investigate how resultant fluid-mineral reactions modify permeability fields. Finally, we investigate numerically subsurface CO2 and heat transport at the geologic formation scale.

Coal-fuelled systems for peaking power with 100% CO2 capture through integration of solid oxide fuel cells with compressed air energy storage

NASA Astrophysics Data System (ADS)

Nease, Jake; Adams, Thomas A.

2014-04-01

In this study, a coal-fuelled integrated solid oxide fuel cell (SOFC) and compressed air energy storage (CAES) system in a load-following power production scenario is discussed. Sixteen SOFC-based plants with optional carbon capture and sequestration (CCS) and syngas shifting steps are simulated and compared to a state-of-the-art supercritical pulverised coal (SCPC) plant. Simulations are performed using a combination of MATLAB and Aspen Plus v7.3. It was found that adding CAES to a SOFC-based plant can provide load-following capabilities with relatively small effects on efficiencies (1-2% HHV depending on the system configuration) and levelized costs of electricity (∼0.35 ¢ kW-1 h-1). The load-following capabilities, as measured by least-squares metrics, show that this system may utilize coal and achieve excellent load-tracking that is not adversely affected by the inclusion of CCS. Adding CCS to the SOFC/CAES system reduces measurable direct CO2 emission to zero. A seasonal partial plant shutdown schedule is found to reduce fuel consumption by 9.5% while allowing for cleaning and maintenance windows for the SOFC stacks without significantly affecting the performance of the system (∼1% HHV reduction in efficiency). The SOFC-based systems with CCS are found to become economically attractive relative to SCPC above carbon taxes of 22 ton-1.

CO2 Capture and Storage in Coal Gasification Projects

NASA Astrophysics Data System (ADS)

Rao, Anand B.; Phadke, Pranav C.

2017-07-01

In response to the global climate change problem, the world community today is in search for an effective means of carbon mitigation. India is a major developing economy and the economic growth is driven by ever-increasing consumption of energy. Coal is the only fossil fuel that is available in abundance in India and contributes to the major share of the total primary energy supply (TPES) in the country. Owing to the large unmet demand for affordable energy, primarily driven by the need for infrastructure development and increasing incomes and aspirations of people, as well as the energy security concerns, India is expected to have continued dependence on coal. Coal is not only the backbone of the electric power generation, but many major industries like cement, iron and steel, bricks, fertilizers also consume large quantities of coal. India has very low carbon emissions (˜ 1.5 tCO2 per capita) as compared to the world average (4.7 tCO2 per capita) and the developed world (11.2 tCO2 per capita). Although the aggregate emissions of the country are increasing with the rising population and fossil energy use, India has a very little contribution to the historical GHG accumulation in the atmosphere linked to the climate change problem. However, a large fraction of the Indian society is vulnerable to the impacts of climate change - due to its geographical location, large dependence on monsoon-based agriculture and limited technical, financial and institutional capacity. Today, India holds a large potential to offer cost-effective carbon mitigation to tackle the climate change problem. Carbon Capture and Storage (CCS) is the process of extraction of Carbon Dioxide (CO2) from industrial and energy related sources, transport to storage locations and long-term isolation from the atmosphere. It is a technology that has been developed in recent times and is considered as a bridging technology as we move towards carbon-neutral energy sources in response to the growing concerns about climate change problem. Carbon Capture and Storage (CCS) is being considered as a promising carbon mitigation technology, especially for large point sources such as coal power plants. Gasification of coal helps in better utilization of this resource offering multiple advantages such as pollution prevention, product flexibility (syngas and hydrogen) and higher efficiency (combined cycle). It also enables the capture of CO2 prior to the combustion, from the fuel gas mixture, at relatively lesser cost as compared to the post-combustion CO2 capture. CCS in gasification projects is considered as a promising technology for cost-effective carbon mitigation. Although many projects (power and non-power) have been announced internationally, very few large-scale projects have actually come up. This paper looks at the various aspects of CCS applications in gasification projects, including the technical feasibility and economic viability and discusses an Indian perspective. Impacts of including CCS in gasification projects (e.g. IGCC plants) have been assessed using a simulation tool. Integrated Environmental Control Model (IECM) - a modelling framework to simulate power plants - has been used to estimate the implications of adding CCS units in IGCC plants, on their performance and costs.

Enrichment of rare earth metal ions by the highly selective adsorption of phytate intercalated layered double hydroxide.

PubMed

Jin, Cheng; Liu, Huimin; Kong, Xianggui; Yan, Hong; Lei, Xiaodong

2018-02-27

Phytate intercalated MgAl layered double hydroxide (MgAl-LDH) was prepared by an anion exchange method with the precursor NO 3 - containing MgAl-LDH. The final as-synthesized product [Mg 0.69 Al 0.31 (OH) 2 ] (phytateNa 6 ) 0.05 (NO 3 ) 0.01 ·mH 2 O (phytate-LDH) has highly selective adsorption ability for some metal ions and can be used to enrich rare earth metal ions in mixed solution, such as Pr 3+ and Ce 3+ from a mixed solution of them with Pb 2+ and Co 2+ . At first, phytate-LDH has good adsorption performance for these ions in single metal ion solutions. At low concentration (below 10 mg L -1 ), all the capture rates of the four metal ions were more than 97%, for highly toxic Pb 2+ it was even up to nearly 100%, and a high capture rate (99.87%) was maintained for Pb 2+ at a high concentration (100 mg L -1 ). When all the four metal ions are co-existing in aqueous solution, the selectivity order is Pb 2+ ≫ Pr 3+ ≈ Ce 3+ > Co 2+ . In a solution containing mixtures of the three metal ions of Pr 3+ , Ce 3+ , and Co 2+ , the selectivity order is Pr 3+ ≈ Ce 3+ ≫ Co 2+ , and in a solution containing mixtures of Pr 3+ with Co 2+ and Ce 3+ with Co 2+ , the selectivity orders are Pr 3+ ≫ Co 2+ and Ce 3+ ≫ Co 2+ , respectively. The high selectivity and adsorption capacities for Pb 2+ , Co 2+ , Pr 3+ , and Ce 3+ result in the efficient removal of Pb 2+ and enrichment of the rare earth metal ions Pr 3+ and Ce 3+ by phytate-LDH. Based on the elemental analysis, it is found that the difference of the adsorption capacities is mainly due to the different coordination number of them with phytate-LDH. With molecular simulation, we believe that the adsorption selectivity is due to the difference of the binding energy between the metal ion and phytate-LDH. Therefore, the phytate-LDH is promising for the enrichment and/or purification of the rare earth metal ions and removal of toxic metal ions from waste water.

NRG CO 2NCEPT - Confirmation Of Novel Cost-effective Emerging Post-combustion Technology

DOE Office of Scientific and Technical Information (OSTI.GOV)

Stevenson, Matthew; Armpriester, Anthony

Under DOE's solicitation DE-FOA-0001190, NRG and Inventys conceptualized a Large-Scale pilot (>10MWe) post-combustion CO 2 capture project using Inventys' VeloxoThermTM carbon capture technology. The technology is comprised of an intensified thermal swing adsorption (TSA) process that uses a patented architecture of structured adsorbent and a novel process design and embodiment to capture CO 2 from industrial flue gas streams. The result of this work concluded that the retrofit of this technology is economically and technically viable, but that the sorbent material selected for the program would need improving to meet the techno-economic performance requirements of the solicitation.

The thiocyanate anion is a primary driver of carbon dioxide capture by ionic liquids

NASA Astrophysics Data System (ADS)

Chaban, Vitaly

2015-01-01

Carbon dioxide, CO2, capture by room-temperature ionic liquids (RTILs) is a vivid research area featuring both accomplishments and frustrations. This work employs the PM7-MD method to simulate adsorption of CO2 by 1,3-dimethylimidazolium thiocyanate at 300 K. The obtained result evidences that the thiocyanate anion plays a key role in gas capture, whereas the impact of the 1,3-dimethylimidazolium cation is mediocre. Decomposition of the computed wave function on the individual molecular orbitals confirms that CO2-SCN binding extends beyond just expected electrostatic interactions in the ion-molecular system and involves partial sharing of valence orbitals.

Inhibiting polysulfides diffusion of lithium-sulfur batteries using an acetylene black-CoS2 modified separator: Mechanism research and performance improvement

NASA Astrophysics Data System (ADS)

Zeng, Pan; Huang, Liwu; Zhang, Xinling; Han, Yamiao; Chen, Yungui

2018-01-01

Lithium-sulfur (Li-S) batteries are considered as one of the most promising chemistries in secondary energy storage field owing to their high energy density. However, the poor electrochemical performance mainly associated with the polysulfides shuttle has greatly hampered their practical application. Herein, a simple acetylene black (AB)-CoS2 coated separator is first designed to suppress the migration of polysulfides. The AB-CoS2 modified separator can not only efficiently capture the polysulfides by forming strong chemical bonding but also guarantee the rapid lithium ions diffusion. Moreover, the AB-CoS2 coating could serve as an upper current collector to accelerate electron transport for reinforcing the utilization of sulfur and ensuring the reactivation of the trapped active material. Consequently, the Li-S cell using AB-CoS2 modified separator shows a long-term cycling stability with an extremely low decay rate (0.09% per cycle) up to 450 cycles at a high rate of 2 C (3350 mA g-1). It also exhibits excellent rate capabilities, which maintains a capacity of 475 mAh g-1 even at 4.0 C rate.

Pilot-Scale Silicone Process for Low-Cost Carbon Dioxide Capture Preliminary Techno-Economic Analysis

DOE Office of Scientific and Technical Information (OSTI.GOV)

Singh, Surinder; Spiry, Irina; Wood, Benjamin

This report presents system and economic analysis for a carbon-capture unit which uses an aminosilicone-based solvent for CO{sub 2} capture in a pulverized coal (PC) boiler. The aminosilicone solvent is a 60/40 wt/wt mixture of 3-aminopropyl end-capped polydimethylsiloxane (GAP-1m) with tri-ethylene glycol (TEG) as a co-solvent. For comparison purposes, the report also shows results for a carbon-capture unit based on a conventional approach using mono-ethanol amine (MEA). The first year removal cost of CO{sub 2} for the aminosilicone-based carbon-capture process ismore » $46.04/ton of CO2 as compared to $$60.25/ton of CO{sub 2} when MEA is used. The aminosilicone-based process has <77% of the CAPEX of a system using MEA solvent. The lower CAPEX is due to several factors, including the higher working capacity of the aminosilicone solvent compared the MEA, which reduces the solvent flow rate required, reducing equipment sizes. If it is determined that carbon steel can be used in the rich-lean heat exchanger in the carbon capture unit, the first year removal cost of CO{sub 2} decreases to $$44.12/ton. The aminosilicone-based solvent has a higher thermal stability than MEA, allowing desorption to be conducted at higher temperatures and pressures, decreasing the number of compressor stages needed. The aminosilicone-based solvent also has a lower vapor pressure, allowing the desorption to be conducted in a continuous-stirred tank reactor versus a more expensive packed column. The aminosilicone-based solvent has a lower heat capacity, which decreases the heat load on the desorber. In summary, the amino-silicone solvent has significant advantages over conventional systems using MEA.« less

Process for CO.sub.2 capture using a regenerable magnesium hydroxide sorbent

DOEpatents

Siriwardane, Ranjani V; Stevens, Jr., Robert W

2013-06-25

A process for CO.sub.2 separation using a regenerable Mg(OH).sub.2 sorbent. The process absorbs CO.sub.2 through the formation of MgCO.sub.3 and releases water product H.sub.2O. The MgCO.sub.3 is partially regenerated through direct contact with steam, which acts to heat the magnesium carbonate to a higher temperature, provide heat duty required to decompose the magnesium carbonate to yield MgO and CO.sub.2, provide an H.sub.2O environment over the magnesium carbonate thereby shifting the equilibrium and increasing the potential for CO.sub.2 desorption, and supply H.sub.2O for rehydroxylation of a portion of the MgO. The mixture is polished in the absence of CO.sub.2 using water product H.sub.2O produced during the CO.sub.2 absorption to maintain sorbent capture capacity. The sorbent now comprised substantially of Mg(OH).sub.2 is then available for further CO.sub.2 absorption duty in a cyclic process.

Energy and economic analysis of the carbon dioxide capture installation with the use of monoethanolamine and ammonia

NASA Astrophysics Data System (ADS)

Bochon, Krzysztof; Chmielniak, Tadeusz

2015-03-01

In the study an accurate energy and economic analysis of the carbon capture installation was carried out. Chemical absorption with the use of monoethanolamine (MEA) and ammonia was adopted as the technology of carbon dioxide (CO2) capture from flue gases. The energy analysis was performed using a commercial software package to analyze the chemical processes. In the case of MEA, the demand for regeneration heat was about 3.5 MJ/kg of CO2, whereas for ammonia it totalled 2 MJ/kg CO2. The economic analysis was based on the net present value (NPV) method. The limit price for CO2 emissions allowances at which the investment project becomes profitable (NPV = 0) was more than 160 PLN/Mg for MEA and less than 150 PLN/Mg for ammonia. A sensitivity analysis was also carried out to determine the limit price of CO2 emissions allowances depending on electricity generation costs at different values of investment expenditures.

Bench-Scale Testing and Process Performance Projections of CO2 Capture by CO2–Binding Organic Liquids (CO2BOLs) With and Without Polarity-Swing-Assisted Regeneration

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zheng, Feng; Heldebrant, David J.; Mathias, Paul M.

This manuscript provides a detailed analysis of a continuous flow, bench scale study of the CO2BOL solvent platform with and without its Polarity Swing Assisted Regeneration (PSAR). This study encompassed four months of continuous flow testing of a candidate CO2BOL with a thermal regeneration and PSAR regeneration using decane antisolvent. In both regeneration schemes, steady state capture of >90 %CO2 was achieved using simulated flue gas at acceptable L/G ratios. Aspen Plus™ modeling was performed to assess process performance compared to previous equilibrium performance projections. This paper also includes net power projections, and comparisons to DOE’s Case 10 amine baseline.

Optimization of ELISA Conditions to Quantify Colorectal Cancer Antigen-Antibody Complex Protein (GA733-FcK) Expressed in Transgenic Plant

PubMed Central

Ahn, Junsik; Lee, Kyung Jin

2014-01-01

The purpose of this study is to optimize ELISA conditions to quantify the colorectal cancer antigen GA733 linked to the Fc antibody fragment fused to KDEL, an ER retention motif (GA733-FcK) expressed in transgenic plant. Variable conditions of capture antibody, blocking buffer, and detection antibody for ELISA were optimized with application of leaf extracts from transgenic plant expressing GA733-FcK. In detection antibody, anti-EpCAM/CD362 IgG recognizing the GA733 did not detect any GA733-FcK whereas anti-human Fc IgG recognizing the human Fc existed in plant leaf extracts. For blocking buffer conditions, 3% BSA buffer clearly blocked the plate, compared to the 5% skim-milk buffer. For capture antibody, monoclonal antibody (MAb) CO17-1A was applied to coat the plate with different amounts (1, 0.5, and 0.25 μg/well). Among the amounts of the capture antibody, 1 and 0.5 μg/well (capture antibody) showed similar absorbance, whereas 0.25 μg/well of the capture antibody showed significantly less absorbance. Taken together, the optimized conditions to quantify plant-derived GA733-FcK were 0.5 μg/well of MAb CO17-1A per well for the capture antibody, 3% BSA for blocking buffer, and anti-human Fc conjugated HRP. To confirm the optimized ELISA conditions, correlation analysis was conducted between the quantified amount of GA733-FcK in ELISA and its protein density values of different leaf samples in Western blot. The co-efficient value R2 between the ELISA quantified value and protein density was 0.85 (p<0.01), which indicates that the optimized ELISA conditions feasibly provides quantitative information of GA733-FcK expression in transgenic plant. PMID:24555929

Anion-activated, thermoreversible gelation system for the capture, release, and visual monitoring of CO2

PubMed Central

Zhang, Xin; Lee, Songyi; Liu, Yifan; Lee, Minji; Yin, Jun; Sessler, Jonathan L.; Yoon, Juyoung

2014-01-01

Carbon dioxide (CO2) is an important green house gas. This is providing an incentive to develop new strategies to detect and capture CO2. Achieving both functions within a single molecular system represents an unmet challenge in terms of molecular design and could translate into enhanced ease of use. Here, we report an anion-activated chemosensor system, NAP-chol 1, that permits dissolved CO2 to be detected in organic media via simple color changes or through ratiometric differences in fluorescence intensity. NAP-chol 1 also acts as a super gelator for DMSO. The resulting gel is transformed into a homogeneous solution upon exposure to fluoride anions. Bubbling with CO2 regenerates the gel. Subsequent flushing with N2 or heating serves to release the CO2 and reform the sol form. This series of transformations is reversible and can be followed by easy-to-discern color changes. Thus, NAP-chol 1 allows for the capture and release of CO2 gas while acting as a three mode sensing system. In particular, it permits CO2 to be detected through reversible sol-gel transitions, simple changes in color, or ratiometric monitoring of the differences in the fluorescence features. PMID:24699626

Monitoring Shallow Subsurface CO2 Migration using Electrical Imaging Technique, Pilot Site in Brazil

NASA Astrophysics Data System (ADS)

Oliva, A.; Chang, H. K.; Moreira, A.

2013-12-01

Carbon Capture and Geological Sequestration (CCGS or CCS) is one of the main technological strategies targeting Greenhouse Gases (GHG) emissions reduction, with special emphasis on carbon dioxide (CO2) coming from industrial sources. CCGS integrates the so called Carbon Management Strategies, as indicated by the Intergovernmental Panel on Climate Change (IPCC), and is the basis of main technical route likely to enable substantial emission reduction in a safe, quick and cost-effective way. Currently one of the main challenges in the area of CO2 storage research is to grant the development, testing and validation of accurate and efficient measuring, monitoring and verification (MMV) techniques to be deployed at the final storage site, targeting maximum storage efficiency at the minimal leakage risk levels. The implementation of the first CO2 MMV field lab in Brazil, located in Florianópolis, Santa Catarina state, offered an excellent opportunity for running controlled release experiments in a real open air environment. The purpose of this work is to present the results of a time lapse monitoring experiment of CO2 migration in both saturated and unsaturated sand-rich sediments, using electrical imaging technique. The experiment covered an area of approximately 6300 m2 and CO2 was continuously injected at depth of 8 m, during 12 days, at an average rate of 90 g/ day, totalizing 1080 g of injected CO2. 2D and 3D electrical images using Wenner array were acquired daily during 13 consecutive days. Comparison of post injection electrical imaging results with pre injection images shows change in resistivity values consistent with migration pathways of CO2. A pronounced increase in resistivity values (up to ~ 500 ohm.m) with respect to the pre-injection values occurs in the vicinity of the injection well. Background values of 530 ohm.m have changed to 1118 ohm.m, right after injection. Changes in resistivity values progressively diminish outward of the well, following groundwater flow path.

Molecular simulation study of the competitive adsorption of H2O and CO2 in zeolite 13X.

PubMed

Joos, Lennart; Swisher, Joseph A; Smit, Berend

2013-12-23

The presence of H2O in postcombustion gas streams is an important technical issue for deploying CO2-selective adsorbents. Because of its permanent dipole, H2O can interact strongly with materials where the selectivity for CO2 is a consequence of its quadrupole interacting with charges in the material. We performed molecular simulations to model the adsorption of pure H2O and CO2 as well as H2O/CO2 mixtures in 13X, a popular zeolite for CO2 capture processes that is commercially available. The simulations show that H2O reduces the capacity of these materials for adsorbing CO2 by an order of magnitude and that at the partial pressures of H2O relevant for postcombustion capture, 13X will be essentially saturated with H2O .

Energy requirements for CO2 capture from ambient air (DAC) competitive with capture from flue-gas (PCC)

NASA Astrophysics Data System (ADS)

Meinrenken, Christoph

2015-03-01

Capture of CO2, whether from a flue gas source (PCC) or from distributed sources via ambient air (DAC), is a key enabling technology to provide carbon for sustainable synthetic energy carriers such as solar fuels. Based on thermodynamic minimum considerations, DAC is often expected to require about 3 times more energy (per ton CO2 captured) than PCC because CO2 in ambient air is more dilute. Here, we calculate the energy required for a humidity swing-based DAC installation that uses an anionic exchange resin as sorbent. The calculation uses recently measured equilibrium CO2 loadings of the sorbent as function of partial CO2 pressure, temperature, and humidity. We calculate the installation's electricity consumption to be about 45 kJ per mole of pure CO2 at 1 bar (scenario-dependent). Furthermore, we estimate the amount of heat provided by ambient air and thus provide context of the overall energy and entropy balance and thermodynamic minimum views. The electricity consumption is competitive with typical parasitic loads of PCC-equipped coal-fired power plants (40-50 kJ per mole at same pressure) and significantly lower than predicted for other DAC installations such as Na(OH) sorbent-based systems. Our analyses elucidate why DAC is not always more energy-intensive that PCC, thus alleviating often cited concerns of significant cost impediments. Financial support by ABB for research presented herein is gratefully acknowledged.

Adherence of amino acids functionalized iron oxide nanoparticles on bacterial models E. Coli and B. subtilis

NASA Astrophysics Data System (ADS)

Trujillo, W.; Zarria, J.; Pino, J.; Menacho, L.; Coca, M.; Bustamante, A.

2018-03-01

Magnetic iron oxides nanoparticles (NPs) functionalized with lysine (Lys) and arginine (Arg) was obtained by following chemical co-precipitation route in basic medium. The synthesis was performed by mixing ferrous chloride (FeCl2•4H2O), ferric chloride (FeCl3•6H2O) and the specific amino acid in a molar ratio of 1: 2: 0.5, respectively. High pH sample was washed several times with distilled water to reach a pH similar to distilled water (Ph=7) after the synthesis process, part of the NPs obtained was dried. Of the measurements of XRD and MS was obtained that the samples are magnetic nanoparticles of maghemite of about 9 nm in diameter. Of the FTIR and zeta potential measures was obtained that the amino acids Lys and Arg were correctly functionalized at magnetic nanoparticles, referred to herein as M@Lys and M@Arg. In order to demonstrate the capture and adhesion of the nanoparticles to the bacteria, scanning electron microscopy (SEM) was performed. The obtained visualization of both bacteria shows that they are coated by the magnetic particles. In addition, M@Lys (B. sutilis) were cultured to verify the inhibition of growth measured by colony forming units (CFU), the concentrations of M@Lys were 1.75x102 g/mL and 0.875x102 g/mL. After the confrontation obtained efficiencies of 75.63% and 98.75% respectively for the third dilution. While for the fourth dilution were 90% and 98.57% respectively were obtained for each concentration of nanoparticles. Hinting that a high efficiency of bacterial capture at very low concentrations of NPs, which gives us a tool to capture nanobiotechnology bacteria in liquid cultures with application to capture them in wastewater. Based on our results we concluded that NPS functionalized with the amino acids Lys and Arg adhere to the bacteria efficiently in low concentrations.

Ionic-Liquid-Based CO2 Capture Systems: Structure, Interaction and Process.

PubMed

Zeng, Shaojuan; Zhang, Xiangping; Bai, Lu; Zhang, Xiaochun; Wang, Hui; Wang, Jianji; Bao, Di; Li, Mengdie; Liu, Xinyan; Zhang, Suojiang

2017-07-26

The inherent structure tunability, good affinity with CO 2 , and nonvolatility of ionic liquids (ILs) drive their exploration and exploitation in CO 2 separation field, and has attracted remarkable interest from both industries and academia. The aim of this Review is to give a detailed overview on the recent advances on IL-based materials, including pure ILs, IL-based solvents, and IL-based membranes for CO 2 capture and separation from the viewpoint of molecule to engineering. The effects of anions, cations and functional groups on CO 2 solubility and selectivity of ILs, as well as the studies on degradability of ILs are reviewed, and the recent developments on functionalized ILs, IL-based solvents, and IL-based membranes are also discussed. CO 2 separation mechanism with IL-based solvents and IL-based membranes are explained by combining molecular simulation and experimental characterization. Taking into consideration of the applications and industrialization, the recent achievements and developments on the transport properties of IL fluids and the process design of IL-based processes are highlighted. Finally, the future research challenges and perspectives of the commercialization of CO 2 capture and separation with IL-based materials are posed.

A new dawn for industrial photosynthesis.

PubMed

Robertson, Dan E; Jacobson, Stuart A; Morgan, Frederick; Berry, David; Church, George M; Afeyan, Noubar B

2011-03-01

Several emerging technologies are aiming to meet renewable fuel standards, mitigate greenhouse gas emissions, and provide viable alternatives to fossil fuels. Direct conversion of solar energy into fungible liquid fuel is a particularly attractive option, though conversion of that energy on an industrial scale depends on the efficiency of its capture and conversion. Large-scale programs have been undertaken in the recent past that used solar energy to grow innately oil-producing algae for biomass processing to biodiesel fuel. These efforts were ultimately deemed to be uneconomical because the costs of culturing, harvesting, and processing of algal biomass were not balanced by the process efficiencies for solar photon capture and conversion. This analysis addresses solar capture and conversion efficiencies and introduces a unique systems approach, enabled by advances in strain engineering, photobioreactor design, and a process that contradicts prejudicial opinions about the viability of industrial photosynthesis. We calculate efficiencies for this direct, continuous solar process based on common boundary conditions, empirical measurements and validated assumptions wherein genetically engineered cyanobacteria convert industrially sourced, high-concentration CO(2) into secreted, fungible hydrocarbon products in a continuous process. These innovations are projected to operate at areal productivities far exceeding those based on accumulation and refining of plant or algal biomass or on prior assumptions of photosynthetic productivity. This concept, currently enabled for production of ethanol and alkane diesel fuel molecules, and operating at pilot scale, establishes a new paradigm for high productivity manufacturing of nonfossil-derived fuels and chemicals.

Intro to Carbon Sequestration

ScienceCinema

None

2017-12-09

NETL's Carbon Sequestration Program is helping to develop technologies to capture, purify, and store carbon dioxide (CO2) in order to reduce greenhouse gas emissions without adversely influencing energy use or hindering economic growth. Carbon sequestration technologies capture and store CO2 that would otherwise reside in the atmosphere for long periods of time.

Pore-scale simulation of CO2-water-rock interactions

NASA Astrophysics Data System (ADS)

Deng, H.; Molins, S.; Steefel, C. I.; DePaolo, D. J.

2017-12-01

In Geologic Carbon Storage (GCS) systems, the migration of scCO2 versus CO2-acidifed brine ultimately determines the extent of mineral trapping and caprock integrity, i.e. the long-term storage efficiency and security. While continuum scale multiphase reactive transport models are valuable for large scale investigations, they typically (over-)simplify pore-scale dynamics and cannot capture local heterogeneities that may be important. Therefore, pore-scale models are needed in order to provide mechanistic understanding of how fine scale structural variations and heterogeneous processes influence the transport and geochemistry in the context of multiphase flow, and to inform parameterization of continuum scale modeling. In this study, we investigate the interplay of different processes at pore scale (e.g. diffusion, reactions, and multiphase flow) through the coupling of a well-developed multiphase flow simulator with a sophisticated reactive transport code. The objectives are to understand where brine displaced by scCO2 will reside in a rough pore/fracture, and how the CO2-water-rock interactions may affect the redistribution of different phases. In addition, the coupled code will provide a platform for model testing in pore-scale multiphase reactive transport problems.

Off-shore enhanced oil recovery in the north sea: matching CO_2 demand and supply given uncertain market conditions

NASA Astrophysics Data System (ADS)

Compernolle, Tine; Welkenhuysen, Kris; Huisman, Kuno; Piessens, Kris; Kort, Peter

2015-04-01

Introduction CO2 enhanced oil recovery (CO2-EOR) entails the injection of CO2 in mature oil fields in order to mobilize the oil. In particular, the injected CO2 reduces the oil's viscosity and acts as a propellant, resulting in an increased oil extraction rate (Leach et al., 2011). Given uncertainty in both oil price and CO2 price under the EU ETS system, aim of this study is to analyze under which economic conditions a CO2 exchange can be established between a CO2 supplier (an electricity producer for whom CO2 is a by-product) and a CO2 user (an offshore oil company that exploits oil fields in the North Sea and needs CO2 for enhanced oil recovery). Methodology A techno-economic simulation tool, PSS IV, was developed to provide investment decision support on integrated CO2-EOR projects (Welkenhuysen et al., 2014). Until now, a fixed onshore supply of CO2 was presumed. An economic optimization model is now developed for both the CO2 producer and the CO2 user. Because net present value and discounted cash flow methods are inadequate to deal with issues like uncertainty and the irreversibility of an investment decision, the real options theory is applied (Dixit and Pindyck, 1994). The way in which cooperation between the companies can take place, will be studied using game theoretical concepts (Lukas and Welling, 2014). Economic and technical data on CO2 capture are available from the PSS database (Piessens et al., 2012). Data on EOR performance, CO2 requirements and various costs are taken from literature (BERR, 2007; Klokk et al., 2010; Pershad et al., 2012). Results/Findings It will be shown what the impact of price uncertainty is on the investment decision of the electricity producer to capture and sell CO2, and on the decision of the oil producer to make the necessary investments to inject CO2 for enhanced oil recovery. Based on these results, it will be determined under which economic conditions a CO2 exchange and transport can take place. Furthermore, also the role of the ETS system will be discussed. In an initial stage, only the CO2-price and oil price market uncertainties are considered. In a further stage, uncertainties from the supply side (technology) and EOR (geological) will be added. References BERR. 2007. Development of a CO2 transport and storage network in the North Sea: report to the North Sea Basin Task Force. Dixit A, Pindyck R (1994). Investment under Uncertainty. In, Princeton University Press. Klokk Ø, Schreiner PF, Pagès-Bernaus A, Tomasgard A (2010). Optimizing a CO2 value chain for the Norwegian Continental Shelf. Energy Policy 38(11): 6604-6614 Leach A, Mason CF, Veld Kvt (2011). Co-optimization of enhanced oil recovery and carbon sequestration. Resource Energy Econ 33(4): 893-912 Lukas E, Welling A (2014). Timing and eco(nomic) efficiency of climate-friendly investments in supply chains. Eur J Oper Res 233(2): 448-457 Pershad, H., Durusut, E., Crerar, A., Black, D., Mackay, E. & Oldern, P., 2012. Economic Impacts of CO2-enhanced oil recovery for Scotland, Final report for Scottish Enterprise. Element energy, London. Piessens, K., Welkenhuysen K., Laenen, B., Ferket, H., Nijs, W., Duerinck, J., Cochez, E., Mathieu, Ph., Valentiny, D., Baele, J.-M., Dupont, N. & Hendriks, Ch., 2012. Policy Support System for Carbon Capture and Storage and Collaboration between Belgium-the Netherlands "PSS-CCS", Final report. Belgian Science Policy Office, Research Programme Science for a Sustainable Development contracts SD/CP/04a,b & SD/CP/803, 335p. Welkenhuysen, K., Compernolle, T., Piessens, K., Ramírez, A., Rupert, J. & Swennen, R., 2014. Geological uncertainty and investment risk in CO2-enhanced oil recovery. 12th International Conference on Greenhouse Gas Control Technologies (GHGT-12), Austin, Texas, 05-09/10/2014.

Flue-gas and direct-air capture of CO2 by porous metal–organic materials

PubMed Central

2017-01-01

Sequestration of CO2, either from gas mixtures or directly from air (direct air capture), is a technological goal important to large-scale industrial processes such as gas purification and the mitigation of carbon emissions. Previously, we investigated five porous materials, three porous metal–organic materials (MOMs), a benchmark inorganic material, Zeolite 13X and a chemisorbent, TEPA-SBA-15, for their ability to adsorb CO2 directly from air and from simulated flue-gas. In this contribution, a further 10 physisorbent materials that exhibit strong interactions with CO2 have been evaluated by temperature-programmed desorption for their potential utility in carbon capture applications: four hybrid ultramicroporous materials, SIFSIX-3-Cu, DICRO-3-Ni-i, SIFSIX-2-Cu-i and MOOFOUR-1-Ni; five microporous MOMs, DMOF-1, ZIF-8, MIL-101, UiO-66 and UiO-66-NH2; an ultramicroporous MOM, Ni-4-PyC. The performance of these MOMs was found to be negatively impacted by moisture. Overall, we demonstrate that the incorporation of strong electrostatics from inorganic moieties combined with ultramicropores offers improved CO2 capture performance from even moist gas mixtures but not enough to compete with chemisorbents. This article is part of the themed issue ‘Coordination polymers and metal–organic frameworks: materials by design’. PMID:27895255

Sequential Design of Experiments

DOE Office of Scientific and Technical Information (OSTI.GOV)

Anderson-Cook, Christine Michaela

2017-06-30

A sequential design of experiments strategy is being developed and implemented that allows for adaptive learning based on incoming results as the experiment is being run. The plan is to incorporate these strategies for the NCCC and TCM experimental campaigns to be run in the coming months. This strategy for experimentation has the advantages of allowing new data collected during the experiment to inform future experimental runs based on their projected utility for a particular goal. For example, the current effort for the MEA capture system at NCCC plans to focus on maximally improving the quality of prediction of COmore » 2 capture efficiency as measured by the width of the confidence interval for the underlying response surface that is modeled as a function of 1) Flue Gas Flowrate [1000-3000] kg/hr; 2) CO 2 weight fraction [0.125-0.175]; 3) Lean solvent loading [0.1-0.3], and; 4) Lean solvent flowrate [3000-12000] kg/hr.« less