Xu, Junyuan; Kan, Yuhe; Huang, Rui; Zhang, Bingsen; Wang, Bolun; Wu, Kuang-Hsu; Lin, Yangming; Sun, Xiaoyan; Li, Qingfeng; Centi, Gabriele; Su, Dangsheng
2016-05-23
Carbon nanotubes (CNTs) are functionalized with nitrogen atoms for reduction of carbon dioxide (CO2 ). The investigation explores the origin of the catalyst's activity and the role of nitrogen chemical states therein. The catalysts show excellent performances, with about 90 % current efficiency for CO formation and stability over 60 hours. The Tafel analyses and density functional theory calculations suggest that the reduction of CO2 proceeds through an initial rate-determining transfer of one electron to CO2 , which leads to the formation of carbon dioxide radical anion (CO2 (.-) ). The initial reduction barrier is too high on pristine CNTs, resulting in a very high overpotentials at which the hydrogen evolution reaction dominates over CO2 reduction. The doped nitrogen atoms stabilize the radical anion, thereby lowering the initial reduction barrier and improving the intrinsic activity. The most efficient nitrogen chemical state for this reaction is quaternary nitrogen, followed by pyridinic and pyrrolic nitrogen. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
NASA Technical Reports Server (NTRS)
Jeng, Frank F.; Lewis, John F.; Graf, John; LaFuse, Sharon; Nicholson, Leonard S. (Technical Monitor)
1999-01-01
This paper describes the analysis on integration requirements, CO2 compressor in particular, for integration of Carbon Dioxide Removal Assembly (CDRA) and CO2 Reduction Assembly (CRA) as a part of the Node 3 project previously conducted at JSC/NASA. A system analysis on the volume and operation pressure range of the CO2 accumulator was conducted. The hardware and operational configurations of the CO2 compressor were developed. The performance and interface requirements of the compressor were specified. An existing Four-Bed Molecular Sieve CO2 removal computer model was modified into a CDRA model and used in analyzing the requirements of the CDRA CO2 compressor. This CDRA model was also used in analyzing CDRA operation parameters that dictate CO2 pump sizing. Strategy for the pump activation was also analyzed.
Reduced graphene oxide supported gold nanoparticles for electrocatalytic reduction of carbon dioxide
NASA Astrophysics Data System (ADS)
Saquib, Mohammad; Halder, Aditi
2018-02-01
Electrochemical reduction of carbon dioxide is one of the methods which have the capability to recycle CO2 into valuable products for energy and industrial applications. This research article describes about a new electrocatalyst "reduced graphene oxide supported gold nanoparticles" for selective electrochemical conversion of carbon dioxide to carbon monoxide. The main aim for conversion of CO2 to CO lies in the fact that the latter is an important component of syn gas (a mixture of hydrogen and carbon monoxide), which is then converted into liquid fuel via well-known industrial process called Fischer-Tropsch process. In this work, we have synthesized different composites of the gold nanoparticles supported on defective reduced graphene oxide to evaluate the catalytic activity of reduced graphene oxide (RGO)-supported gold nanoparticles and the role of defective RGO support towards the electrochemical reduction of CO2. Electrochemical and impedance measurements demonstrate that higher concentration of gold nanoparticles on the graphene support led to remarkable decrease in the onset potential of 240 mV and increase in the current density for CO2 reduction. Lower impedance and Tafel slope values also clearly support our findings for the better performance of RGOAu than bare Au for CO2 reduction.
Investigation of industrial-scale carbon dioxide reduction using pulsed electron beams
DOE Office of Scientific and Technical Information (OSTI.GOV)
Petrov, G. M.; Apruzese, J. P.; Petrova, Tz. B.
Carbon dioxide is the most important greenhouse gas contributing to global warming. To help mitigate increasing CO{sub 2} concentrations, we investigate a method of carbon dioxide reduction using high-power electron beams, which can be used on an industrial scale. A series of experiments are conducted in which the reduction of CO{sub 2} is measured for different gas compositions and power deposition rates. An electron beam deposition model is applied to compute reduction rates of CO{sub 2} and energy cost for breaking a CO{sub 2} molecule in flue gas and pure carbon dioxide at atmospheric pressure. For flue gas consisting ofmore » 82% N{sub 2}, 6% O{sub 2}, and 12% CO{sub 2}, the calculated energy cost is 85 eV per molecule. In order to dissociate 50% of the CO{sub 2} molecules, beam energy density deposition on the order of 20 J/cm{sup 3} is required. Electron beam irradiation of 12.6 liter gas volume containing 90% CO{sub 2} and 10% CH{sub 4} at beam energy density deposition of 4.2 J/cm{sup 3}, accumulated over 43 shots in a 20 min interval, reduced the CO{sub 2} concentration to 78%. Analogous experiments with a gas mixture containing 11.5% CO{sub 2}, 11.5% CH{sub 4}, and balance of Ar, reduced the CO{sub 2} concentration to below 11% with energy deposition 0.71 J/cm{sup 3}, accumulated over 10 shots in a 5 min interval. The experimental data and the theoretical predictions of CO{sub 2} reduction using pulsed electron beams are in agreement within the experimental error. Other techniques to enhance the removal of CO{sub 2} with pulsed electron beams are also explored, yielding new possible avenues of research.« less
NASA Technical Reports Server (NTRS)
Swickrath, Michael J.; Anderson, Molly
2012-01-01
Through the respiration process, humans consume oxygen (O2) while producing carbon dioxide (CO2) and water (H2O) as byproducts. For long term space exploration, CO2 concentration in the atmosphere must be managed to prevent hypercapnia. Moreover, CO2 can be used as a source of oxygen through chemical reduction serving to minimize the amount of oxygen required at launch. Reduction can be achieved through a number of techniques. NASA is currently exploring the Sabatier reaction, the Bosch reaction, and co- electrolysis of CO2 and H2O for this process. Proof-of-concept experiments and prototype units for all three processes have proven capable of returning useful commodities for space exploration. All three techniques have demonstrated the capacity to reduce CO2 in the laboratory, yet there is interest in understanding how all three techniques would perform at a system level within a spacecraft. Consequently, there is an impetus to develop predictive models for these processes that can be readily rescaled and integrated into larger system models. Such analysis tools provide the ability to evaluate each technique on a comparable basis with respect to processing rates. This manuscript describes the current models for the carbon dioxide reduction processes under parallel developmental efforts. Comparison to experimental data is provided were available for verification purposes.
Electrocatalytic reduction of carbon dioxide on electrodeposited tin-based surfaces
NASA Astrophysics Data System (ADS)
Alba, Bianca Christina S.; Camayang, John Carl A.; Mopon, Marlon L.; del Rosario, Julie Anne D.
2017-08-01
The electrocatalytic reduction of carbon dioxide to small organic molecular compounds provides a means of generating alternative fuel source while suppressing climate change. Suitable catalysts, however, are necessary to optimize its reaction kinetics towards more valuable products. Consequently, in this study, electrodeposited Sn electrodes have been developed as catalysts for CO2 electroreduction. Deposition potential was varied to produce different Sn catalysts. SEM showed varying morphologies and increasing amount as the applied potential becomes more negative. Cyclic voltammetry and chronoamperometry showed that the activity and stability of the catalysts towards CO2 reduction depend on the morphology and presence of tin oxides. These results provide a better understanding on the performance of electrodeposited Sn-based surfaces as catalysts for CO2 reduction.
NASA Technical Reports Server (NTRS)
Swickrath, Michael J.; Anderson, Molly
2011-01-01
Through the respiration process, humans consume oxygen (O2) while producing carbon dioxide (CO2) and water (H2O) as byproducts. For long term space exploration, CO2 concentration in the atmosphere must be managed to prevent hypercapnia. Moreover, CO2 can be used as a source of oxygen through chemical reduction serving to minimize the amount of oxygen required at launch. Reduction can be achieved through a number of techniques. The National Aeronautics and Space Administration (NASA) is currently exploring the Sabatier reaction, the Bosch reaction, and co-electrolysis of CO2 and H2O for this process. Proof-of-concept experiments and prototype units for all three processes have proven capable of returning useful commodities for space exploration. While all three techniques have demonstrated the capacity to reduce CO2 in the laboratory, there is interest in understanding how all three techniques would perform at a system-level within a spacecraft. Consequently, there is an impetus to develop predictive models for these processes that can be readily re-scaled and integrated into larger system models. Such analysis tools provide the ability to evaluate each technique on a comparable basis with respect to processing rates. This manuscript describes the current models for the carbon dioxide reduction processes under parallel developmental e orts. Comparison to experimental data is provided were available for veri cation purposes.
Shimoda, Tomoe; Morishima, Takeshi; Kodama, Koichi; ...
2018-04-26
Trigonal-bipyramidal Co(II) complexes are used for photochemical carbon dioxide (CO 2) reduction with Ru(bpy) 3 2+ as a photosensitizer, tri-p-tolylamine (TTA) as a reversible quencher, and triethylamine (TEA) as a sacrificial electron donor to produce carbon monoxide and dihydrogen. Here, the CO 2 reduction is slow because of the large structural changes, spin flipping in the cobalt catalytic intermediates, and an uphill reaction for reduction to catalytically active Co(0) by the photoproduced [Ru(bpy) 3] +.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Shimoda, Tomoe; Morishima, Takeshi; Kodama, Koichi
Trigonal-bipyramidal Co(II) complexes are used for photochemical carbon dioxide (CO 2) reduction with Ru(bpy) 3 2+ as a photosensitizer, tri-p-tolylamine (TTA) as a reversible quencher, and triethylamine (TEA) as a sacrificial electron donor to produce carbon monoxide and dihydrogen. Here, the CO 2 reduction is slow because of the large structural changes, spin flipping in the cobalt catalytic intermediates, and an uphill reaction for reduction to catalytically active Co(0) by the photoproduced [Ru(bpy) 3] +.
Bajón Fernández, Y; Soares, A; Villa, R; Vale, P; Cartmell, E
2014-05-01
The increasing concentration of carbon dioxide (CO2) in the atmosphere and the stringent greenhouse gases (GHG) reduction targets, require the development of CO2 sequestration technologies applicable for the waste and wastewater sector. This study addressed the reduction of CO2 emissions and enhancement of biogas production associated with CO2 enrichment of anaerobic digesters (ADs). The benefits of CO2 enrichment were examined by injecting CO2 at 0, 0.3, 0.6 and 0.9 M fractions into batch ADs treating food waste or sewage sludge. Daily specific methane (CH4) production increased 11-16% for food waste and 96-138% for sewage sludge over the first 24h. Potential CO2 reductions of 8-34% for sewage sludge and 3-11% for food waste were estimated. The capacity of ADs to utilise additional CO2 was demonstrated, which could provide a potential solution for onsite sequestration of CO2 streams while enhancing renewable energy production. Copyright © 2014 Elsevier Ltd. All rights reserved.
NASA Astrophysics Data System (ADS)
Suryati, Isra; Turmuzi Lubis, Muhammad; Mawaddah, Nurul
2018-03-01
Carbon Dioxide (CO2) is one of the greenhouse gases. One source of greenhouse gases comes from the use of fossil fuels from the transport sector. The transportation sector is one of the dominant sectors in contributing to the greenhouse effect. This study aims to calculate the amount of CO2 from transportation activities by using mobile six equations in Gatot Subroto Street, Medan City. A sampling of CO2 concentration was done using Carbon Dioxide Monitor with Non-Dispersive Infra Red (NDIR) Analyzer method. Also, a simulation of the reduction of the number of private vehicles to mass transportation such as BRT gas-fired. The results showed CO2 emissions calculations with mobile six ranged from 47.2 kg CO2 - 978.2 kg CO2. Meanwhile, measurements range from 3,004 ppm - 3,405 ppm. Implementation of the concept of environmentally friendly transportation such as BRT in Gatot Subroto Street, Medan City will be able to reduce the average emissions load CO2 by 42.75% -78.80%. Based on the calculation simulation in this study is estimated the number of BRT required approximately 71 units.
Short run effects of a price on carbon dioxide emissions from U.S. electric generators.
Newcomer, Adam; Blumsack, Seth A; Apt, Jay; Lave, Lester B; Morgan, M Granger
2008-05-01
The price of delivered electricity will rise if generators have to pay for carbon dioxide emissions through an implicit or explicit mechanism. There are two main effects that a substantial price on CO2 emissions would have in the short run (before the generation fleet changes significantly). First, consumers would react to increased price by buying less, described by their price elasticity of demand. Second, a price on CO2 emissions would change the order in which existing generators are economically dispatched, depending on their carbon dioxide emissions and marginal fuel prices. Both the price increase and dispatch changes depend on the mix of generation technologies and fuels in the region available for dispatch, although the consumer response to higher prices is the dominant effect. We estimate that the instantaneous imposition of a price of $35 per metric ton on CO2 emissions would lead to a 10% reduction in CO2 emissions in PJM and MISO at a price elasticity of -0.1. Reductions in ERCOT would be about one-third as large. Thus, a price on CO2 emissions that has been shown in earlier workto stimulate investment in new generation technology also provides significant CO2 reductions before new technology is deployed at large scale.
USDA-ARS?s Scientific Manuscript database
Farming practices can have a large impact on the soil carbon cycle and the resulting net emission of greenhouse gases including carbon dioxide (CO**2), methane and nitrous oxide. Primary sources of CO**2 emission on dairy farms are soil, plant, and animal respiration with smaller contributions from ...
NASA Astrophysics Data System (ADS)
Bajracharya, Suman; Srikanth, Sandipam; Mohanakrishna, Gunda; Zacharia, Renju; Strik, David PBTB; Pant, Deepak
2017-07-01
Carbon dioxide (CO2) utilization/recycling for the production of chemicals and gaseous/liquid energy-carriers is a way to moderate the rising CO2 in the atmosphere. One of the possible solutions for the CO2 sequestration is the electrochemical reduction of this stable molecule to useful fuel/products. Nevertheless, the surface chemistry of CO2 reduction is a challenge due to the presence of large energy barriers, requiring noticeable catalysis. The recent approach of microbial electrocatalysis of CO2 reduction has promising prospects to reduce the carbon level sustainably, taking full advantage of CO2-derived chemical commodities. We review the currently investigated bioelectrochemical approaches that could possibly be implemented to enable the handling of CO2 emissions. This review covers the most recent advances in the bioelectrochemical approaches of CO2 transformations in terms of biocatalysts development and process design. Furthermore, the extensive research on carbon fixation and conversion to different value added chemicals is reviewed. The review concludes by detailing the key challenges and future prospects that could enable economically feasible microbial electrosynthesis technology.
Homogeneous Reduction of Carbon Dioxide with Hydrogen.
Dong, Kaiwu; Razzaq, Rauf; Hu, Yuya; Ding, Kuiling
2017-04-01
Carbon dioxide (CO 2 ), a key greenhouse gas produced from both anthropogenic and natural sources, has been recently considered to be an important C1 building-block for the synthesis of many industrial fuels and chemicals. Catalytic hydrogenation of CO 2 using a homogeneous system is regarded as an efficient process for CO 2 valorization. This approach leads to the direct products including formic acid (HCOOH), carbon monoxide (CO), methanol (MeOH), and methane (CH 4 ). The hydrogenation of CO 2 to CO followed by alkene carbonylation provides value-added compounds, which also avoids the tedious separation and transportation of toxic CO. Moreover, the reduction of CO 2 with H 2 in the presence of amines is of significance to attain fine chemicals through catalytic formylation and methylation reactions. The synthesis of higher alcohols and dialkoxymethane from CO 2 and H 2 has been demonstrated recently, which opens access to new molecular structures using CO 2 as an important C1 source.
Microfluidic platform for studying the electrochemical reduction of carbon dioxide
NASA Astrophysics Data System (ADS)
Whipple, Devin Talmage
Diminishing supplies of conventional energy sources and growing concern over greenhouse gas emissions present significant challenges to supplying the world's rapidly increasing demand for energy. The electrochemical reduction of carbon dioxide has the potential to address many of these issues by providing a means of storing electricity in chemical form. Storing electrical energy as chemicals is beneficial for leveling the output of clean, but intermittent renewable energy sources such as wind and solar. Electrical energy stored as chemicals can also be used as carbon neutral fuels for portable applications allowing petroleum derived fuels in the transportation sector to be replaced by more environmentally friendly energy sources. However, to be a viable technology, the electrochemical reduction of carbon dioxide needs to have both high current densities and energetic efficiencies (Chapter 1). Although many researchers have studied the electrochemical reduction of CO2 including parameters such as catalysts, electrolytes and temperature, further investigation is needed to improve the understanding of this process and optimize the performance (Chapter 2). This dissertation reports the development and validation of a microfluidic reactor for the electrochemical reduction of CO2 (Chapter 3). The design uses a flowing liquid electrolyte instead of the typical polymer electrolyte membrane. In addition to other benefits, this flowing electrolyte gives the reactor great flexibility, allowing independent analysis of each electrode and the testing of a wide variety of conditions. In this work, the microfluidic reactor has been used in the following areas: • Comparison of different metal catalysts for the reduction of CO2 to formic acid and carbon monoxide (Chapter 4). • Investigation of the effects of the electrolyte pH on the reduction of CO2 to formic acid and carbon monoxide (Chapter 5). • Study of amine based electrolytes for lowering the overpotentials for CO2 reduction and suppressing undesirable hydrogen evolution (Chapter 6). • Investigation of the effects of reaction temperature on the Faradaic efficiency and current density for CO2 reduction on several catalysts (Chapter 7). These studies demonstrate the utility of this flexible reactor design and provide increased understanding of the electrochemical reduction of CO2 and the critical parameters for optimization of this process.
Application of gas diffusion biocathode in microbial electrosynthesis from carbon dioxide.
Bajracharya, Suman; Vanbroekhoven, Karolien; Buisman, Cees J N; Pant, Deepak; Strik, David P B T B
2016-11-01
Microbial catalysis of carbon dioxide (CO 2 ) reduction to multi-carbon compounds at the cathode is a highly attractive application of microbial electrosynthesis (MES). The microbes reduce CO 2 by either taking the electrons or reducing the equivalents produced at the cathode. While using gaseous CO 2 as the carbon source, the biological reduction process depends on the dissolution and mass transfer of CO 2 in the electrolyte. In order to deal with this issue, a gas diffusion electrode (GDE) was investigated by feeding CO 2 through the GDE into the MES reactor for its reduction at the biocathode. A combination of the catalyst layer (porous activated carbon and Teflon binder) and the hydrophobic gas diffusion layer (GDL) creates a three-phase interface at the electrode. So, CO 2 and reducing equivalents will be available to the biocatalyst on the cathode surface. An enriched inoculum consisting of acetogenic bacteria, prepared from an anaerobic sludge, was used as a biocatalyst. The cathode potential was maintained at -1.1 V vs Ag/AgCl to facilitate direct and/or hydrogen-mediated CO 2 reduction. Bioelectrochemical CO 2 reduction mainly produced acetate but also extended the products to ethanol and butyrate. Average acetate production rates of 32 and 61 mg/L/day, respectively, with 20 and 80 % CO 2 gas mixture feed were achieved with 10 cm 2 of GDE. The maximum acetate production rate remained 238 mg/L/day for 20 % CO 2 gas mixture. In conclusion, a gas diffusion biocathode supported bioelectrochemical CO 2 reduction with enhanced mass transfer rate at continuous supply of gaseous CO 2 . Graphical abstract ᅟ.
Reduction of CO2 using a Rhenium Bipyridine Complex Containing Ancillary BODIPY Redox Reservoirs
DOE Office of Scientific and Technical Information (OSTI.GOV)
Teesdale, Justin; Pistner, Allen; Yapp, Glenn P. A.
2014-01-01
The reduction of carbon dioxide to chemical fuels such as carbon monoxide is an important challenge in the field of renewable energy conversion. Given the thermodynamic stability of carbon dioxide, it is difficult to efficiently activate this substrate in a selective fashion and the development of new electrocatalysts for CO2 reduction is of prime importance. To this end, we have prepared and studied a new fac-ReI(CO)3 complex supported by a bipyridine ligand containing ancillary BODIPY moieties ([Re(BB2)(CO)3Cl]). Voltammetry experiments revealed that this system displays a rich redox chemistry under N2, as [Re(BB2)(CO)3Cl] can be reduced by up to four electronsmore » at modest potentials. These redox events have been characterized as the ReI/0 couple, and three ligand based reductions two of which are localized on the BODIPY units. The ability of the BB2 ligand to serve as a noninnocent redox reservoir is manifest in an enhanced electrocatalysis with CO2 as compared to an unsubstituted Re-bipyridine complex lacking BODIPY units ([Re(bpy)(CO)3Cl]). The second order rate constant for reduction of CO2 by [Re(BB2)(CO)3Cl] was measured to be k = 3400 M 1s 1 at an applied potential of 2.0 V versus SCE, which is roughly three times greater than the corresponding unsubstituted Re-bipyridine homologue. Photophysical and photochemical studies were also carried out to determine if [Re(BB2)(CO)3Cl] was a competent platform for CO2 reduction using visible light. These experiments showed that this complex supports unusual excited state dynamics that are not typically observed for fac- ReI(CO)3 complexes.« less
Wang, Zhijiang; Wu, Lina; Sun, Kun; Chen, Ting; Jiang, Zhaohua; Cheng, Tao; Goddard, William A
2018-05-23
We have explored functionalizing metal catalysts with surface ligands as an approach to facilitate electrochemical carbon dioxide reduction reaction (CO 2 RR). To provide a molecular level understanding of the mechanism by which this enhancement occurs, we combine in situ spectroscopy analysis with an interpretation based on quantum mechanics (QM) calculations. We find that a surface ligand can play a critical role in stabilizing the chemisorbed CO 2 , which facilitates CO 2 activation and leads to a 0.3 V decrease in the overpotential for carbon monoxide (CO) formation. Moreover, the presence of the surface ligand leads to nearly exclusive CO production. At -0.6 V (versus reversible hydrogen electrode, RHE), CO is the only significant product with a faradic efficiency of 93% and a current density of 1.9 mA cm -2 . This improvement corresponds to 53-fold enhancement in turnover frequency compared with the Ag nanoparticles (NPs) without surface ligands.
NASA Technical Reports Server (NTRS)
Jeng, Frank F.; Lafuse, Sharon; Smith, Frederick D.; Lu, Sao-Dung; Knox, James C.; Campbell, Mellssa L.; Scull, Timothy D.; Green Steve
2010-01-01
A tool has been developed by the Sabatier Team for analyzing/optimizing CO2 removal assembly, CO2 compressor size, its operation logic, water generation from Sabatier, utilization of CO2 from crew metabolic output, and Hz from oxygen generation assembly. Tests had been conducted using CDRA/Simulation compressor set-up at MSFC in 2003. Analysis of test data has validated CO2 desorption rate profile, CO2 compressor performance, CO2 recovery and CO2 vacuum vent in CDRA desorption. Optimizing the compressor size and compressor operation logic for an integrated closed air revitalization system Is being conducted by the Sabatier Team.
Electrocatalytic Reduction of Carbon Dioxide with a Well-Defined PN 3 -Ru Pincer Complex
Min, Shixiong; Rasul, Shahid; Li, Huaifeng; ...
2015-11-13
We established a well-defined PN 3-Ru pincer complex (5) bearing a redox-active bipyridine ligand with an aminophosphine arm as an effective and stable molecular electrocatalyst for CO 2 reduction to CO and HCOOH with negligible formation of H 2 in a H 2O/MeCN mixture.
Light-driven carbon dioxide reduction to methane by nitrogenase in a photosynthetic bacterium
Fixen, Kathryn R.; Zheng, Yanning; Harris, Derek F.; Shaw, Sudipta; Yang, Zhi-Yong; Dean, Dennis R.; Seefeldt, Lance C.
2016-01-01
Nitrogenase is an ATP-requiring enzyme capable of carrying out multielectron reductions of inert molecules. A purified remodeled nitrogenase containing two amino acid substitutions near the site of its FeMo cofactor was recently described as having the capacity to reduce carbon dioxide (CO2) to methane (CH4). Here, we developed the anoxygenic phototroph, Rhodopseudomonas palustris, as a biocatalyst capable of light-driven CO2 reduction to CH4 in vivo using this remodeled nitrogenase. Conversion of CO2 to CH4 by R. palustris required constitutive expression of nitrogenase, which was achieved by using a variant of the transcription factor NifA that is able to activate expression of nitrogenase under all growth conditions. Also, light was required for generation of ATP by cyclic photophosphorylation. CH4 production by R. palustris could be controlled by manipulating the distribution of electrons and energy available to nitrogenase. This work shows the feasibility of using microbes to generate hydrocarbons from CO2 in one enzymatic step using light energy. PMID:27551090
Efficient Hydrogen-Dependent Carbon Dioxide Reduction by Escherichia coli.
Roger, Magali; Brown, Fraser; Gabrielli, William; Sargent, Frank
2018-01-08
Hydrogen-dependent reduction of carbon dioxide to formic acid offers a promising route to greenhouse gas sequestration, carbon abatement technologies, hydrogen transport and storage, and the sustainable generation of renewable chemical feedstocks [1]. The most common approach to performing direct hydrogenation of CO 2 to formate is to use chemical catalysts in homogeneous or heterogeneous reactions [2]. An alternative approach is to use the ability of living organisms to perform this reaction biologically. However, although CO 2 fixation pathways are widely distributed in nature, only a few enzymes have been described that have the ability to perform the direct hydrogenation of CO 2 [3-5]. The formate hydrogenlyase (FHL) enzyme from Escherichia coli normally oxidizes formic acid to carbon dioxide and couples that reaction directly to the reduction of protons to molecular hydrogen [6]. In this work, the reverse reaction of FHL is unlocked. It is established that FHL can operate as a highly efficient hydrogen-dependent carbon dioxide reductase when gaseous CO 2 and H 2 are placed under pressure (up to 10 bar). Using intact whole cells, the pressurized system was observed to rapidly convert 100% of gaseous CO 2 to formic acid, and >500 mM formate was observed to accumulate in solution. Harnessing the reverse reaction has the potential to allow the versatile E. coli system to be employed as an exciting new carbon capture technology or as a cell factory dedicated to formic acid production, which is a commodity in itself as well as a feedstock for the synthesis of other valued chemicals. Copyright © 2017 The Author(s). Published by Elsevier Ltd.. All rights reserved.
Yang, Piaoping; Zhao, Zhi-Jian; Chang, Xiaoxia; Mu, Rentao; Zha, Shenjun; Zhang, Gong; Gong, Jinlong
2018-06-25
Carbon dioxide (CO 2 ) reduction in aqueous solutions is an attractive strategy for carbon capture and utilization. Cuprous oxide (Cu 2 O) is a promising catalyst for CO 2 reduction as it can convert CO 2 into valuable hydrocarbons and suppress the side hydrogen evolution reaction (HER). However, the nature of the active sites in Cu 2 O remains under debate because of the complex surface structure of Cu 2 O under reducing conditions, leading to limited guidance in designing improved Cu 2 O catalysts. This paper describes the functionality of surface-bonded hydroxy groups on partially reduced Cu 2 O(111) for the CO 2 reduction reaction (CO 2 RR) by combined density functional theory (DFT) calculations and experimental studies. We find that the surface hydroxy groups play a crucial role in the CO 2 RR and HER, and a moderate coverage of hydroxy groups is optimal for promotion of the CO 2 RR and suppression of the HER simultaneously. Electronic structure analysis indicates that the charge transfer from hydroxy groups to coordination-unsaturated Cu (Cu CUS ) sites stabilizes surface-adsorbed COOH*, which is a key intermediate during the CO 2 RR. Moreover, the CO 2 RR was evaluated over Cu 2 O octahedral catalysts with {111} facets and different surface coverages of hydroxy groups, which demonstrates that Cu 2 O octahedra with moderate coverage of hydroxy groups can indeed enhance the CO 2 RR and suppress the HER. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.
Iodide-Photocatalyzed Reduction of Carbon Dioxide to Formic Acid with Thiols and Hydrogen Sulfide.
Berton, Mateo; Mello, Rossella; González-Núñez, María Elena
2016-12-20
The photolysis of iodide anions promotes the reaction of carbon dioxide with hydrogen sulfide or thiols to quantitatively yield formic acid and sulfur or disulfides. The reaction proceeds in acetonitrile and aqueous solutions, at atmospheric pressure and room temperature by irradiation using a low-pressure mercury lamp. This transition-metal-free photocatalytic process for CO 2 capture coupled with H 2 S removal may have been relevant as a prebiotic carbon dioxide fixation. © 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.
Characterization of amine-functionalized electrode for aqueous carbon dioxide (CO2) direct detection
NASA Astrophysics Data System (ADS)
Sato, Hiroshi
2017-03-01
In this study, fabrication of amino groups and ferrocenes co-modified sensor electrode and electrochemical detection of carbon dioxide (CO2) in the saline solution is reported. Electrochemical detection of CO2 was carried out using cyclic voltammetry in saline solution containing sodium bicarbonate as CO2 source. Oxidation and reduction peak current intensities computed from cyclic voltammograms varied as a function of concentration of CO2 molecules. The calibration curve was obtained by plotting oxidation peak current intensities as a function of CO2 concentration. The sensor electrode prepared in this study can estimate the differences between concentrations of CO2 in normal seawater up to 10 times higher. Furthermore, the surface analysis was performed to clarify the CO2 detection mechanism.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Thoi, VanSara; Kornienko, Nick; Margarit, C
2013-06-07
The solar-driven reduction of carbon dioxide to value-added chemical fuels is a longstanding challenge in the fields of catalysis, energy science, and green chemistry. In order to develop effective CO2 fixation, several key considerations must be balanced, including (1) catalyst selectivity for promoting CO2 reduction over competing hydrogen generation from proton reduction, (2) visible-light harvesting that matches the solar spectrum, and (3) the use of cheap and earth-abundant catalytic components. In this report, we present the synthesis and characterization of a new family of earth-abundant nickel complexes supported by N-heterocyclic carbene amine ligands that exhibit high selectivity and activity formore » the electrocatalytic and photocatalytic conversion of CO2 to CO. Systematic changes in the carbene and amine donors of the ligand have been surveyed, and [Ni(Prbimiq1)]2+ (1c, where Prbimiq1 = bis(3-(imidazolyl)isoquinolinyl)propane) emerges as a catalyst for electrochemical reduction of CO2 with the lowest cathodic onset potential (Ecat = 1.2 V vs SCE). Using this earth-abundant catalyst with Ir(ppy)3 (where ppy = 2-phenylpyridine) and an electron donor, we have developed a visible-light photoredox system for the catalytic conversion of CO2 to CO that proceeds with high selectivity and activity and achieves turnover numbers and turnover frequencies reaching 98,000 and 3.9 s1, respectively. Further studies reveal that the overall efficiency of this solar-to-fuel cycle may be limited by the formation of the active Ni catalyst and/or the chemical reduction of CO2 to CO at the reduced nickel center and provide a starting point for improved photoredox systems for sustainable carbon-neutral energy conversion.« less
Reversible interconversion of carbon dioxide and formate by an electroactive enzyme
Reda, Torsten; Plugge, Caroline M.; Abram, Nerilie J.; Hirst, Judy
2008-01-01
Carbon dioxide (CO2) is a kinetically and thermodynamically stable molecule. It is easily formed by the oxidation of organic molecules, during combustion or respiration, but is difficult to reduce. The production of reduced carbon compounds from CO2 is an attractive proposition, because carbon-neutral energy sources could be used to generate fuel resources and sequester CO2 from the atmosphere. However, available methods for the electrochemical reduction of CO2 require excessive overpotentials (are energetically wasteful) and produce mixtures of products. Here, we show that a tungsten-containing formate dehydrogenase enzyme (FDH1) adsorbed to an electrode surface catalyzes the efficient electrochemical reduction of CO2 to formate. Electrocatalysis by FDH1 is thermodynamically reversible—only small overpotentials are required, and the point of zero net catalytic current defines the reduction potential. It occurs under thoroughly mild conditions, and formate is the only product. Both as a homogeneous catalyst and on the electrode, FDH1 catalyzes CO2 reduction with a rate more than two orders of magnitude faster than that of any known catalyst for the same reaction. Formate oxidation is more than five times faster than CO2 reduction. Thermodynamically, formate and hydrogen are oxidized at similar potentials, so formate is a viable energy source in its own right as well as an industrially important feedstock and a stable intermediate in the conversion of CO2 to methanol and methane. FDH1 demonstrates the feasibility of interconverting CO2 and formate electrochemically, and it is a template for the development of robust synthetic catalysts suitable for practical applications. PMID:18667702
Carbon Dioxide Reduction Technology Trade Study
NASA Technical Reports Server (NTRS)
Jeng, Frank F.; Anderson, Molly S.; Abney, Morgan B.
2011-01-01
For long-term human missions, a closed-loop atmosphere revitalization system (ARS) is essential to minimize consumables. A carbon dioxide (CO2) reduction technology is used to reclaim oxygen (O2) from metabolic CO2 and is vital to reduce the delivery mass of metabolic O2. A key step in closing the loop for ARS will include a proper CO2 reduction subsystem that is reliable and with low equivalent system mass (ESM). Sabatier and Bosch CO2 reduction are two traditional CO2 reduction subsystems (CRS). Although a Sabatier CRS has been delivered to International Space Station (ISS) and is an important step toward closing the ISS ARS loop, it recovers only 50% of the available O2 in CO2. A Bosch CRS is able to reclaim all O2 in CO2. However, due to continuous carbon deposition on the catalyst surface, the penalties of replacing spent catalysts and reactors and crew time in a Bosch CRS are significant. Recently, technologies have been developed for recovering hydrogen (H2) from Sabatier-product methane (CH4). These include methane pyrolysis using a microwave plasma, catalytic thermal pyrolysis of CH4 and thermal pyrolysis of CH4. Further, development in Sabatier reactor designs based on microchannel and microlith technology could open up opportunities in reducing system mass and enhancing system control. Improvements in Bosch CRS conversion have also been reported. In addition, co-electrolysis of steam and CO2 is a new technology that integrates oxygen generation and CO2 reduction functions in a single system. A co-electrolysis unit followed by either a Sabatier or a carbon formation reactor based on Bosch chemistry could improve the overall competitiveness of an integrated O2 generation and CO2 reduction subsystem. This study evaluates all these CO2 reduction technologies, conducts water mass balances for required external supply of water for 1-, 5- and 10-yr missions, evaluates mass, volume, power, cooling and resupply requirements of various technologies. A system analysis and comparison among the technologies was made based on ESM, technology readiness level and reliability. Those technologies with potential were recommended for development.
NASA Astrophysics Data System (ADS)
Lv, Weixin; Zhou, Jing; Bei, Jingjing; Zhang, Rui; Wang, Lei; Xu, Qi; Wang, Wei
2017-01-01
Electrochemical reduction of carbon dioxide (CO2) to formate is energetically inefficient because high overpotential is required for reduction of CO2 to formate on most traditional catalysts. In this paper, a novel nano-sized Bi-based electrocatalyst deposited on a Cu foil has been synthesized, which can be used as a cathode for electrochemical reduction of CO2 to formate with a low overpotential (0.69 V) and a high selectivity (91.3%). The electrocatalyst can show excellent catalytic performance toward reduction of CO2 which can probably be attributed to the nano-sized structure and the surface oxide layer. The energy efficiency for reduction of CO2 to formate can reach to 50% when an IrxSnyRuzO2/Ti electrode is used as anode, it is one of the highest values found in the literatures and very practicable for sustainable fuel synthesis.
John R. Butnor; Kurt H. Johnsen; Ram Oren; Gabriel G. Katul
2003-01-01
Elevated atmospheric carbon dioxide (CO2e) increases soil respiration rates in forest, grassland, agricultural and wetland systems as a result of increased growth, root biomass and enhanced biological activity of soil microorganisms. Less is known about how forest floor fluxes respond to the combined effects of elevated CO...
Oxygenates from Electrochemical Reduction of CO2.
Feng, Guanghui; Chen, Wei; Wang, Baiyin; Song, Yanfang; Li, Guihua; Fang, Jianhui; Wei, Wei; Sun, Yuhan
2018-05-29
Electrochemical reduction of carbon dioxide (CO2) driven by renewable electricity to chemicals and fuels is considered as an ideal approach that can alleviate both carbon emission and energy tension stresses. High-value chemicals such as oxygenates can be effectively produced from CO2 electroreduction, which is highly attractive for the great promotion of the economy and applicability of CO2 utilization. This review focuses the recent advancements on the CO2 electrochemical reduction to formic acid, methanol, ethanol, acetic acid, and other oxygenates. The related principles, influence factors, and typical catalysts are summarized. On the basis of the aforementioned discussions, we present the future prospects for further development of CO2 electroreduction to oxygenates. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Study of carbon dioxide gas treatment based on equations of kinetics in plasma discharge reactor
NASA Astrophysics Data System (ADS)
Abedi-Varaki, Mehdi
2017-08-01
Carbon dioxide (CO2) as the primary greenhouse gas, is the main pollutant that is warming earth. CO2 is widely emitted through the cars, planes, power plants and other human activities that involve the burning of fossil fuels (coal, natural gas and oil). Thus, there is a need to develop some method to reduce CO2 emission. To this end, this study investigates the behavior of CO2 in dielectric barrier discharge (DBD) plasma reactor. The behavior of different species and their reaction rates are studied using a zero-dimensional model based on equations of kinetics inside plasma reactor. The results show that the plasma reactor has an effective reduction on the CO2 density inside the reactor. As a result of reduction in the temporal variations of reaction rate, the speed of chemical reactions for CO2 decreases and very low concentration of CO2 molecules inside the plasma reactor is generated. The obtained results are compared with the existing experimental and simulation findings in the literature.
Oxygen Generation from Carbon Dioxide for Advanced Life Support
NASA Technical Reports Server (NTRS)
Bishop, Sean; Duncan, Keith; Hagelin-Weaver, Helena; Neal, Luke; Sanchez, Jose; Paul, Heather L.; Wachsman, Eric
2007-01-01
The partial electrochemical reduction of carbon dioxide (CO2) using ceramic oxygen generators (COGs) is well known and widely studied. However, complete reduction of metabolically produced CO2 (into carbon and oxygen) has the potential of reducing oxygen storage weight for life support if the oxygen can be recovered. Recently, the University of Florida devel- oped novel ceramic oxygen generators employing a bilayer elec- trolyte of gadolinia-doped ceria and erbia-stabilized bismuth ox- ide (ESB) for NASA's future exploration of Mars. The results showed that oxygen could be reliably produced from CO2 at temperatures as low as 400 C. The strategy discussed here for advanced life support systems employs a catalytic layer com- bined with a COG cell so that CO2 is reduced all the way to solid carbon and oxygen without carbon buildup on the COG cell and subsequent deactivation.
Sonochemical reduction of carbon dioxide.
Harada, H
1998-06-01
Sonolysis of carbon dioxide dissolved in water was performed from a standpoint of reducing this material in atmosphere. During one hour of sonication, the amount of CO2 decreased to about half at 5 degrees C under CO2-Ar atmosphere. The decreasing rate for CO2 followed the order Ar > He > H2 > N2 and it was down with increasing temperature in the range of 5-45 degrees C. The most favorable concentration for reducing CO2 was 0.03 (mole fraction of CO2 in gas phase). This concentration in gas phase means an equal mixture of CO2 and Ar in water, because CO2 is more soluble than Ar. Since carbon dioxide dissolved in water would be partly ionized, the roles of ions on the sonolysis were also examined. Gaseous reaction products were CO, H2 and a small amount of O2. Carbon monoxide and hydrogen might be obtained from CO2 and H2O by sonolysis, respectively. Both gases are fuel and react each other to C1 compounds such as methanol, and so on. Therefore, irradiation of ultrasonic waves should be an important technique for reducing CO2.
CO2 to methanol conversion using hydride terminated porous silicon nanoparticles.
Dasog, M; Kraus, S; Sinelnikov, R; Veinot, J G C; Rieger, B
2017-03-09
Porous silicon nanoparticles (Si-NPs) prepared via magnesiothermic reduction were used to convert carbon dioxide (CO 2 ) into methanol. The hydride surface of the silicon nanoparticles acted as a CO 2 reducing reagent without any catalyst at temperatures above 100 °C. The Si nanoparticles were reused up to four times without significant loss in methanol yields. The reduction process was monitored using in situ FT-IR and the materials were characterized using SEM, TEM, NMR, XPS, and powder XRD techniques. The influence of reaction temperature, pressure, and Si-NP concentration on CO 2 reduction were also investigated. Finally, Si particles produced directly from sand were used to convert CO 2 to methanol.
This evaluation, part of the Pollution Prevention Clean Technology Demonstration (CTD) Program, addresses the product quality, waste reduction, and economic issues of spray paint application using supercritical carbon dioxide (CO2). Anion Carbide has developed this technology and...
Subsurface Oxygen in Oxide-Derived Copper Electrocatalysts for Carbon Dioxide Reduction
Eilert, Andre; Cavalca, Filippo; Roberts, F. Sloan; ...
2016-12-16
Copper electrocatalysts derived from an oxide have shown extraordinary electrochemical properties for the carbon dioxide reduction reaction (CO 2RR). Using in situ ambient pressure X-ray photoelectron spectroscopy and quasi in situ electron energy-loss spectroscopy in a transmission electron microscope, we show that there is a substantial amount of residual oxygen in nanostructured, oxide-derived copper electrocatalysts but no residual copper oxide. On the basis of these findings in combination with density functional theory simulations, we propose that residual subsurface oxygen changes the electronic structure of the catalyst and creates sites with higher carbon monoxide binding energy. If such sites are stablemore » under the strongly reducing conditions found in CO 2RR, these findings would explain the high efficiencies of oxide-derived copper in reducing carbon dioxide to multicarbon compounds such as ethylene.« less
USDA-ARS?s Scientific Manuscript database
Effect of frame size and season on enteric methane (CH4) and carbon dioxide (CO2) emissions in Angus brood cows grazing native tall-grass prairie in central Oklahoma, USA J.P.S. Neel USDA ARS, El Reno, OK A reduction in enteric CH4 production in ruminants is associated with improved production effic...
Options for lowering U.S. carbon dioxide emissions
NASA Astrophysics Data System (ADS)
Bierbaum, Rosina M.; Friedman, Robert M.; Levenson, Howard; Rapoport, Richard D.; Sundt, Nick
1992-03-01
The United States can decrease its emissions of carbon dioxide (CO2) to as much as 35 percent below 1987 levels within the next 25 years by adopting an aggressive package of policies crossing all sectors of the economy. Such emissions reductions will be difficult to achieve and may be costly, but no major technological breakthroughs are needed. In this paper, we identify a ``Tough'' package of energy conservation, energy supply, and forest managment practices to accomplish this level of emissions reductions. We also present a package of cost-effective, ``Moderate'' technical options, which if adopted, would hold CO2 emissions to about 15-percent increase over 1987 levels by 2015. In constrast, if the United State takes not new actions to curb energy use, CO2 emissions will likely rise 50 percent during that time. A variety of Federal policy initiatives will be required to achieve large reductions in U.S. CO2 emissions. Such policy actions will have to include both regulatory ``push'' and market ``pull'' mechanisms--including performance standards, tax incentive programs, carbon-emission or energy taxes, labeling and efficiency ratings, and research, development, and demostration activities.
Light-driven carbon dioxide reduction to methane by nitrogenase in a photosynthetic bacterium
Fixen, Kathryn R.; Zheng, Yanning; Harris, Derek F.; ...
2016-08-22
Nitrogenase is an ATP-requiring enzyme capable of carrying out multielectron reductions of inert molecules. A purified remodeled nitrogenase containing two amino acid substitutions near the site of its FeMo cofactor was recently described as having the capacity to reduce carbon dioxide (CO 2) to methane (CH 4). Here, we developed the anoxygenic phototroph, Rhodopseudomonas palustris, as a biocatalyst capable of light-driven CO 2 reduction to CH 4 in vivo using this remodeled nitrogenase. Conversion of CO 2 to CH 4 by R. palustris required constitutive expression of nitrogenase, which was achieved by using a variant of the transcription factor NifAmore » that is able to activate expression of nitrogenase under all growth conditions. Also, light was required for generation of ATP by cyclic photophosphorylation. CH 4 production by R. palustris could be controlled by manipulating the distribution of electrons and energy available to nitrogenase. Furthermore, this work shows the feasibility of using microbes to generate hydrocarbons from CO 2 in one enzymatic step using light energy.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Bobik, T.A.; Wolfe, R.S.
1988-01-01
The heterodisulfide of the two coenzymes 2-mercaptoethanesulfonic acid (coenzyme M, HS-CoM) and N-(7-mercaptoheptanoyl)threonine O/sup 3/-phosphate (HS-HTP) increased the rate of CO/sub 2/ reduction to methane by cell extracts 42-fold. The stimulation resulted from activation of the initial step of methanogenesis, the production of formylmethanofuran from methanofuran and CO/sub 2/. These results establish a role for this heterodisulfide (CoM-S-S-HTP) in the reduction of CO/sub 2/ to formylmethanofuran. Evidence indicates that CoM-S-S-HTP is the labile intermediate that accounts for the coupling of the reduction of 2-(methylthio)ethanesulfonic acid by the methylreductase to formylmethanofuran biosynthesis, the RPG effect. The heterodisulfide was found to bemore » labile in cell extracts due to enzyme-catalyzed reduction and possibly thiol-disulfide exchange.« less
Analysis of Emission Reduction Strategies for Power Boilers in the US Pulp and Paper Industry.
The U.S. pulp and paper industry utilizes a variety of fuels to provide energy for process needs. Energy production results in air emissions of sulfur dioxide (SO2), nitrogen oxides (NOX), particulate matter (PM), and greenhouse gases such as carbon dioxide (CO2). Air emissions f...
Exclusive Ni-N4 Sites Realize Near-Unity CO Selectivity for Electrochemical CO2 Reduction.
Li, Xiaogang; Bi, Wentuan; Chen, Minglong; Sun, Yuexiang; Ju, Huanxin; Yan, Wensheng; Zhu, Junfa; Wu, Xiaojun; Chu, Wangsheng; Wu, Changzheng; Xie, Yi
2017-10-25
Electrochemical reduction of carbon dioxide (CO 2 ) to value-added carbon products is a promising approach to reduce CO 2 levels and mitigate the energy crisis. However, poor product selectivity is still a major obstacle to the development of CO 2 reduction. Here we demonstrate exclusive Ni-N 4 sites through a topo-chemical transformation strategy, bringing unprecedentedly high activity and selectivity for CO 2 reduction. Topo-chemical transformation by carbon layer coating successfully ensures preservation of the Ni-N 4 structure to a maximum extent and avoids the agglomeration of Ni atoms to particles, providing abundant active sites for the catalytic reaction. The Ni-N 4 structure exhibits excellent activity for electrochemical reduction of CO 2 with particularly high selectivity, achieving high faradaic efficiency over 90% for CO in the potential range from -0.5 to -0.9 V and gives a maximum faradaic efficiency of 99% at -0.81 V with a current density of 28.6 mA cm -2 . We anticipate exclusive catalytic sites will shed new light on the design of high-efficiency electrocatalysts for CO 2 reduction.
Portenkirchner, Engelbert; Kianfar, Elham; Sariciftci, Niyazi Serdar; Knör, Günther
2014-01-01
Rhenium(I) carbonyl complexes carrying substituted bis(arylimino)acenaphthene ligands (BIAN-R) have been tested as potential catalysts for the two-electron reduction of carbon dioxide. Cyclic voltammetric studies as well as controlled potential electrolysis experiments were performed using CO2-saturated solutions of the complexes in acetonitrile and acetonitrile–water mixtures. Faradaic efficiencies of more than 30 % have been determined for the electrocatalytic production of CO. The effects of ligand substitution patterns and water content of the reaction medium on the catalytic performance of the new catalysts are discussed. PMID:24737649
Fischer-Tropsch synthesis in supercritical phase carbon dioxide: Recycle rates
NASA Astrophysics Data System (ADS)
Soti, Madhav
With increasing oil prices and attention towards the reduction of anthropogenic CO2, the use of supercritical carbon dioxide for Fischer Tropsch Synthesis (FTS) is showing promise in fulfilling the demand of clean liquid fuels. The evidence of consumption of carbon dioxide means that it need not to be removed from the syngas feed to the Fischer Tropsch reactor after the gasification process. Over the last five years, research at SIUC have shown that FTS in supercritical CO2reduces the selectivities for methane, enhances conversion, reduces the net CO2produces in the coal to liquid fuels process and increase the life of the catalyst. The research has already evaluated the impact of various operating and feed conditions on the FTS for the once through process. We believe that the integration of unreacted feed recycle would enhance conversion, increase the yield and throughput of liquid fuels for the same reactor size. The proposed research aims at evaluating the impact of recycle of the unreacted feed gas along with associated product gases on the performance of supercritical CO2FTS. The previously identified conditions will be utilized and various recycle ratios will be evaluated in this research once the recycle pump and associated fittings have been integrated to the supercritical CO2FTS. In this research two different catalysts (Fe-Zn-K, Fe-Co-Zn-K) were analyzed under SC-FTS in different recycle rate at 350oC and 1200 psi. The use of recycle was found to improve conversion from 80% to close to 100% with both catalysts. The experiment recycle rate at 4.32 and 4.91 was clearly surpassing theoretical recycle curve. The steady state reaction rate constant was increased to 0.65 and 0.8 min-1 for recycle rate of 4.32 and 4.91 respectively. Carbon dioxide selectivity was decreased for both catalyst as it was converting to carbon monoxide. Carbon dioxide consumption was increased from 0.014 to 0.034 mole fraction. This concluded that CO2is being used in the system and converting which created the concentration of the feed gas higher inside the reactor. The research has provided the best conditions for the enhanced conversion while minimizing CO2formation. Though this research was not able to provide the optimal recycle rate it have created the path for the future research to proceed in the right direction. This reduction and utilization of CO2will help to reduce the cost of carbon dioxide removal and saves the environment from carbon dioxide emission.
Light-Driven Heterogeneous Reduction of Carbon Dioxide: Photocatalysts and Photoelectrodes
White, James L.; Baruch, Maor F.; Pander, III, James E.; ...
2015-10-07
A thorough review article on work to publication date on the photocatalysis and photoelectrochemistry of CO 2 reduction chemistry. This work also contains an up to date tutorial on photoelectrochemistry in general.
Li, Yu Hang; Cheng, Ling; Liu, Peng Fei; Zhang, Le; Zu, Meng Yang; Wang, Chong Wu; Jin, Yan Huan; Cao, Xiao Ming; Yang, Hua Gui; Li, Chunzhong
2018-05-09
A simple cadmium sulfide nanomaterial is found to be an efficient and stable electrocatalyst for CO 2 reduction in aqueous medium for more than 40 h with a steady CO faradaic efficiency of approximately 95 %. Moreover, it can realize a current density of -10 mA cm -2 at an overpotential of -0.55 V on a porous substrate with similar selectivity. Theoretical and experimental results confirm that the high selectivity for CO 2 reduction is due to its (0 0 0 2) face with sulfur vacancies that prefers CO 2 molecule reduction in aqueous medium. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Abbasi, Pedram; Asadi, Mohammad; Liu, Cong
2017-01-24
Electrocatalytic conversion of carbon dioxide (CO2) into energy-rich fuels is considered to be the most efficient approach to achieve a carbon neutral cycle. Transition-metal dichalcogenides (TMDCs) have recently shown a very promising catalytic performance for CO2 reduction reaction in an ionic liquid electrolyte. Here, we report that the catalytic performance of molybdenum disulfide (MoS2), a member of TMDCs, can be significantly improved by using an appropriate dopant. Our electrochemical results indicate that 5% niobium (Nb)-doped vertically aligned MoS2 in ionic liquid exhibits 1 order of magnitude higher CO formation turnover frequency (TOF) than pristine MoS2 at an overpotential range ofmore » 50-150 mV. The TOF of this catalyst is also 2 orders of magnitude higher than that of Ag nanoparticles over the entire range of studied overpotentials (100-650 mV). Moreover, the in situ differential electrochemical mass spectrometry experiment shows the onset overpotential of 31 mV for this catalyst, which is the lowest onset potential for CO2 reduction reaction reported so far. Our density functional theory calculations reveal that low concentrations of Nb near the Mo edge atoms can enhance the TOF of CO formation by modifying the binding energies of intermediates to MoS2 edge atoms.« less
The Gelation of CO(2): A Sustainable Route to the Creation of Microcellular Materials.
Shi; Huang; Kilic; Xu; Enick; Beckman; Carr; Melendez; Hamilton
1999-11-19
Compounds with strong thermodynamic affinity for carbon dioxide (CO(2)) have been designed and synthesized that dissolve in CO(2), then associate to form gels. Upon removal of the CO(2), these gels produced free-standing foams with cells with an average diameter smaller than 1 micrometer and a bulk density reduction of 97 percent relative to the parent material.
An audit of the use of the CO2 laser in oral and maxillofacial surgery
NASA Astrophysics Data System (ADS)
Pinheiro, Antonio L. B.; Santos de Almeida, Darcy
2004-09-01
The use of the Carbon dioxide Laser to perform surgical procedures in the oral cavity has been described as a successful method for the treatment of several conditions affecting the maxillofacial region. Several benefits of the use of the CO2 Laser have been reported and includes reduction of postoperative pain and edema, local hemosthasis, reduction of scaring and wound contraction and infection. The aim of this work is to present our clinical experience in performing several surgical procedures using the CO2 Laser to treat soft tissue pathologies of both benign and malign origin as well as on performing pre-prosthetic surgery, apical surgery and on the treatment of pre-malignancies. Our experience demonstrate that the use of the Carbon dioxide Laser in treating oral soft-tissue pathology presents advantages over conventional techniques and local discomfort and pain are the most common complaints after Laser surgery. The Carbon dioxide Laser does not offer any enhanced cure-rate for oral pathology, but rather it is a precise means of removing soft tissue lesions with little upset afterwards.
Carbon dioxide hydrogenation catalysed by well-defined Mn(i) PNP pincer hydride complexes.
Bertini, Federica; Glatz, Mathias; Gorgas, Nikolaus; Stöger, Berthold; Peruzzini, Maurizio; Veiros, Luis F; Kirchner, Karl; Gonsalvi, Luca
2017-07-01
The catalytic reduction of carbon dioxide is of great interest for its potential as a hydrogen storage method and to use carbon dioxide as C-1 feedstock. In an effort to replace expensive noble metal-based catalysts with efficient and cheap earth-abundant counterparts, we report the first example of Mn(i)-catalysed hydrogenation of CO 2 to HCOOH. The hydride Mn(i) catalyst [Mn(PNP NH - i Pr)(H)(CO) 2 ] showed higher stability and activity than its Fe(ii) analogue. TONs up to 10 000 and quantitative yields were obtained after 24 h using DBU as the base at 80 °C and 80 bar total pressure. At catalyst loadings as low as 0.002 mol%, TONs greater than 30 000 could be achieved in the presence of LiOTf as the co-catalyst, which are among the highest activities reported for base-metal catalysed CO 2 hydrogenations to date.
Nichols, Eva M.; Derrick, Jeffrey S.; Nistanaki, Sepand K.; ...
2018-01-01
The development of catalysts for electrochemical reduction of carbon dioxide offers an attractive approach to transforming this greenhouse gas into value-added carbon products with sustainable energy input.
Metallic nanocatalysts for electrochemical CO2 reduction in aqueous solutions.
Wang, Yuanxing; Niu, Cailing; Wang, Dunwei
2018-05-16
How to effectively and efficiently reduce carbon dioxide (CO 2 ) to value-added chemicals represent a frontier in catalysis research. Due to the high activation energy needs and the endothermic nature of CO 2 reduction, the reactions are difficult to carry out. When H 2 O is present, hydrogen evolution reactions (HER) often compete favorably with CO 2 reduction reactions. For these reactions, catalysts are of critical importance to CO 2 reduction. In this article, we review the various metal nanocatalysts for electrochemical CO 2 reduction (ECR) reactions. In recognition of the importance of H 2 O to CO 2 reduction, we focus our discussions on systems in aqueous solutions. Nanostructured metal catalysts are chosen for the discussions because they represent the most effective catalysts for ECR. After a brief introduction of the fundamental principles of ECR, we devote the rest of the article on the discussions of various types of nanostructured metallic catalysts, which are categorized by their compositions and working mechanisms. Lastly, strategies for improving reaction efficiency and selectivity are discussed. Copyright © 2018 Elsevier Inc. All rights reserved.
Electrochemical reduction of CO2 to CO over Zn in propylene carbonate/tetrabutylammonium perchlorate
NASA Astrophysics Data System (ADS)
Shen, Feng-xia; Shi, Jin; Chen, Tian-you; Shi, Feng; Li, Qing-yuan; Zhen, Jian-zheng; Li, Yun-fei; Dai, Yong-nian; Yang, Bin; Qu, Tao
2018-02-01
Developing low cost and high efficient electrode for carbon dioxide (CO2) reduction in organic media is essential for practical application. Zn is a cheap metal and has high catalytic effects on CO2 reduction to carbon monoxide (CO) in aqueous solution. However, little attention has been given to investigate the performance of Zn in organic media for CO2 reduction. In present work, we have conducted CO2 reduction in propylene carbonate/tetrabutylammonium perchlorate on Zn due to that propylene carbonate is a widely used industrial absorber, and tetrabutylammonium perchlorate is a commonly used organic supporting electrolyte. In addition, because electrochemical reduction of CO2 to CO naturally produces H2O, we have discussed water effects on CO2 reduction in propylene carbonate/tetrabutylammonium perchlorate+6.8 wt % H2O. Our experiment results reveal that the faradaic efficiency for CO formation reaches to 83%, and the current density remains stable at 6.72 mA/cm2 at voltage -2.3 V for 4 h. Interestingly, Zn presents higher catalytic activity than Ag, and slightly lower than Au. X-ray photoelectron spectroscopy results confirm that no poisonous species is formed and absorbed on the cathode, which is an important advantage in practical application.
Reducing U.S. residential energy use and CO2 emissions: how much, how soon, and at what cost?
Lima Azevedo, Inês; Morgan, M Granger; Palmer, Karen; Lave, Lester B
2013-03-19
There is growing interest in reducing energy use and emissions of carbon dioxide from the residential sector by deploying cost-effectiveness energy efficiency measures. However, there is still large uncertainty about the magnitude of the reductions that could be achieved by pursuing different energy efficiency measures across the nation. Using detailed estimates of the current inventory and performance of major appliances in U.S. homes, we model the cost, energy, and CO2 emissions reduction if they were replaced with alternatives that consume less energy or emit less CO2. We explore trade-offs between reducing CO2, reducing primary or final energy, or electricity consumption. We explore switching between electricity and direct fuel use, and among fuels. The trade-offs between different energy efficiency policy goals, as well as the environmental metrics used, are important but have been largely unexplored by previous energy modelers and policy-makers. We find that overnight replacement of the full stock of major residential appliances sets an upper bound of just over 710 × 10(6) tonnes/year of CO2 or a 56% reduction from baseline residential emissions. However, a policy designed instead to minimize primary energy consumption instead of CO2 emissions will achieve a 48% reduction in annual carbon dioxide emissions from the nine largest energy consuming residential end-uses. Thus, we explore the uncertainty regarding the main assumptions and different policy goals in a detailed sensitivity analysis.
Study on Introduction of CO2 Free Energy to Japan with Liquid Hydrogen
NASA Astrophysics Data System (ADS)
Kamiya, Shoji; Nishimura, Motohiko; Harada, Eichi
In Japan, both CO2(Carbon dioxide) emission reduction and energy security are the very important social issues after Fukushima Daiichi accident. On the other hand, FCV (Fuel Cell Vehicle)using hydrogen will be on the market in 2015. Introducing large mass hydrogen energy is being expected as expanding hydrogen applications, or solution to energy issues of Japan.And then,the Japanese government announced the road map for introducing hydrogen energy supply chain in this June,2014. Under these circumstances, imported CO2 free hydrogen will be one of the solutions for energy security and CO2 reduction, if the hydrogen price is affordable. To achieve this, Kawasaki Heavy Industries, Ltd. (KHI) performed a feasibility studyon CO2-free hydrogen energy supply chainfrom Australian brown coal linked with CCS (Carbon dioxide Capture and Storage) to Japan. In the study, hydrogen production systems utilizing brown coal gasificationandLH2 (liquid hydrogen)systems as storing and transporting hydrogen are examined.This paper shows the possibilityof realizingthe CO2 free hydrogen supply chain, the cost breakdown of imported hydrogen cost, its cost competitiveness with conventionalfossil, andLH2systems as key technologies of the hydrogen energy chain.
Ferrentino, Giovanna; Balzan, Sara; Dorigato, Andrea; Pegoretti, Alessandro; Spilimbergo, Sara
2012-05-01
The objective of the present study was the evaluation of the effectiveness of supercritical carbon dioxide (SC-CO(2)) as a nonthermal technology for the pasteurization of fresh-cut coconut, as an example of ready-to-eat and minimally processed food. First, the inactivation kinetics of microbiota on coconut were determined using SC-CO(2) treatments (pressures at 8 and 12 MPa, temperatures from 24 to 45 °C, treatment times from 5 to 60 min). Second, the effects of SC-CO(2) on the hardness and microstructure of fresh-cut coconut processed at the optimal conditions for microbial reduction were investigated. SC-CO(2) treatment of 15 min at 45 °C and 12 MPa induced 4 log CFU/g reductions of mesophilic microorganisms, lactic acid bacteria, total coliforms, and yeasts and molds. The hardness of coconut was not affected by the treatment but the samples developed an irregular and disorderly microstructure. Results suggested the potential of SC-CO(2) in preserving fresh-cut fruits and ready-to-eat products. © 2012 Institute of Food Technologists®
U.S. sulfur dioxide emission reductions: Shifting factors and a carbon dioxide penalty
Brown, Marilyn Ann; Li, Yufei; Massetti, Emanuele; ...
2017-01-18
For more than 20 years, the large-scale application of flue gas desulfurization technology has been a dominant cause of SO 2 emission reductions. From 1994–2004, electricity generation from coal increased, but the shift to low-sulfur coal eclipsed this. From 2004–2014, electricity generation from coal decreased, but a shift to higher-sulfur subbituminous and lignite coal overshadowed this. Here, the shift in coal quality has also created a CO 2 emissions penalty, representing 2% of the sector’s total emissions in 2014.
NASA Technical Reports Server (NTRS)
Abney, Morgan; Miller, Lee; Greenwood, Zach; Iannantuono, Michelle; Jones, Kenny
2013-01-01
State-of-the-art life support carbon dioxide (CO2) reduction technology, based on the Sabatier reaction, is theoretically capable of 50% recovery of oxygen from metabolic CO2. This recovery is constrained by the limited availability of reactant hydrogen. Post-processing of the methane byproduct from the Sabatier reactor results in hydrogen recycle and a subsequent increase in oxygen recovery. For this purpose, a Methane Post-Processor Assembly containing three sub-systems has been developed and tested. The assembly includes a Methane Purification Assembly (MePA) to remove residual CO2 and water vapor from the Sabatier product stream, a Plasma Pyrolysis Assembly (PPA) to partially pyrolyze methane into hydrogen and acetylene, and an Acetylene Separation Assembly (ASepA) to purify the hydrogen product for recycle. The results of partially integrated testing of the sub-systems are reported.
NASA Technical Reports Server (NTRS)
Abney, Morgan B.; Greenwood, Zachary; Miller, Lee A.; Alvarez, Giraldo; Iannantuono, Michelle; Jones, Kenny
2013-01-01
State-of-the-art life support carbon dioxide (CO2) reduction technology, based on the Sabatier reaction, is theoretically capable of 50% recovery of oxygen from metabolic CO2. This recovery is constrained by the limited availability of reactant hydrogen. Post-processing of the methane byproduct from the Sabatier reactor results in hydrogen recycle and a subsequent increase in oxygen recovery. For this purpose, a Methane Post-Processor Assembly containing three sub-systems has been developed and tested. The assembly includes a Methane Purification Assembly (MePA) to remove residual CO2 and water vapor from the Sabatier product stream, a Plasma Pyrolysis Assembly (PPA) to partially pyrolyze methane into hydrogen and acetylene, and an Acetylene Separation Assembly (ASepA) to purify the hydrogen product for recycle. The results of partially integrated testing of the sub-systems are reported
Zhang, Xing; Wu, Zishan; Zhang, Xiao; Li, Liewu; Li, Yanyan; Xu, Haomin; Li, Xiaoxiao; Yu, Xiaolu; Zhang, Zisheng; Liang, Yongye; Wang, Hailiang
2017-01-01
Electrochemical reduction of carbon dioxide with renewable energy is a sustainable way of producing carbon-neutral fuels. However, developing active, selective and stable electrocatalysts is challenging and entails material structure design and tailoring across a range of length scales. Here we report a cobalt-phthalocyanine-based high-performance carbon dioxide reduction electrocatalyst material developed with a combined nanoscale and molecular approach. On the nanoscale, cobalt phthalocyanine (CoPc) molecules are uniformly anchored on carbon nanotubes to afford substantially increased current density, improved selectivity for carbon monoxide, and enhanced durability. On the molecular level, the catalytic performance is further enhanced by introducing cyano groups to the CoPc molecule. The resulting hybrid catalyst exhibits >95% Faradaic efficiency for carbon monoxide production in a wide potential range and extraordinary catalytic activity with a current density of 15.0 mA cm−2 and a turnover frequency of 4.1 s−1 at the overpotential of 0.52 V in a near-neutral aqueous solution. PMID:28272403
2017-01-01
Developing efficient methods for capture and controlled release of carbon dioxide is crucial to any carbon capture and utilization technology. Herein we present an approach using an organic semiconductor electrode to electrochemically capture dissolved CO2 in aqueous electrolytes. The process relies on electrochemical reduction of a thin film of a naphthalene bisimide derivative, 2,7-bis(4-(2-(2-ethylhexyl)thiazol-4-yl)phenyl)benzo[lmn][3,8]phenanthroline-1,3,6,8(2H,7H)-tetraone (NBIT). This molecule is specifically tailored to afford one-electron reversible and one-electron quasi-reversible reduction in aqueous conditions while not dissolving or degrading. The reduced NBIT reacts with CO2 to form a stable semicarbonate salt, which can be subsequently oxidized electrochemically to release CO2. The semicarbonate structure is confirmed by in situ IR spectroelectrochemistry. This process of capturing and releasing carbon dioxide can be realized in an oxygen-free environment under ambient pressure and temperature, with uptake efficiency for CO2 capture of ∼2.3 mmol g–1. This is on par with the best solution-phase amine chemical capture technologies available today. PMID:28378994
Structural change as a key component for agricultural non-CO2 mitigation efforts.
Frank, Stefan; Beach, Robert; Havlík, Petr; Valin, Hugo; Herrero, Mario; Mosnier, Aline; Hasegawa, Tomoko; Creason, Jared; Ragnauth, Shaun; Obersteiner, Michael
2018-03-13
Agriculture is the single largest source of anthropogenic non-carbon dioxide (non-CO 2 ) emissions. Reaching the climate target of the Paris Agreement will require significant emission reductions across sectors by 2030 and continued efforts thereafter. Here we show that the economic potential of non-CO 2 emissions reductions from agriculture is up to four times as high as previously estimated. In fact, we find that agriculture could achieve already at a carbon price of 25 $/tCO 2 eq non-CO 2 reductions of around 1 GtCO 2 eq/year by 2030 mainly through the adoption of technical and structural mitigation options. At 100 $/tCO 2 eq agriculture could even provide non-CO 2 reductions of 2.6 GtCO 2 eq/year in 2050 including demand side efforts. Immediate action to favor the widespread adoption of technical options in developed countries together with productivity increases through structural changes in developing countries is needed to move agriculture on track with a 2 °C climate stabilization pathway.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Alfonso, Dominic R., E-mail: alfonso@netl.doe.gov; Kauffman, Douglas; Matranga, Christopher
2016-05-14
Recent experimental studies have reported the electrochemical reduction of carbon dioxide (CO{sub 2}) into CO at atomically precise negatively charged Au{sub 25}{sup −} nanoclusters. The studies showed CO{sub 2} conversion at remarkably low overpotentials, but the exact mechanisms and nature of the active sites remain unclear. We used first-principles density functional theory and continuum solvation models to examine the role of the cluster during electrochemical CO{sub 2} reduction and analyze the free energies of proposed intermediate species. Contrary to previous assumptions, our results show that the fully ligand protected cluster is not an active CO{sub 2} reduction catalyst because formationmore » of the crucial carboxyl intermediate required very high electrochemical potentials. Instead, our calculations suggest that the reduction process likely occurs on a dethiolated gold site, and adsorbed carboxyl intermediate formation was significantly stabilized at dethiolated gold sites. These findings point to the crucial role of exposed metal sites during electrochemical CO{sub 2} reduction at gold nanocluster catalysts.« less
Inactivation of Bacillus spores by the supercritical carbon dioxide micro-bubble method.
Ishikawa, H; Shimoda, M; Tamaya, K; Yonekura, A; Kawano, T; Osajima, Y
1997-06-01
Bacillus spores were effectively inactivated by the supercritical (SC) CO2 micro-bubble method. The micro-bubble SC CO2 treatment of B. cereus, B. subtilis, B. megaterium, B. polymyxa, and B. coagulans at 40 degrees C and 30 MPa for 30 min produced greater reduction (about 3 log cycles of reduction) than a similar treatment without a filter. The SC CO2 treatment of B. polymyxa, B. cereus, and B. subtilis spores at 45 degrees C, 50 degrees C, respectively, and 30 MPa for 60 min resulted in a 6-log cycle reduction of survival. The SC CO2 treatment under the foregoing conditions should offer higher efficiency than that of heat treatment at 100 degrees C for 60 min. In addition, the SC CO2 treatment (30 MPa, 60 degrees C, 30 min) of B. polymyxa and B. cereus spores also produced a 6-log cycle reduction.
A TECHNOLOGY FOR REDUCTION OF CO2 EMISSIONS FROM THE TRANSPORTATION SECTOR
The paper gives results of a preliminary assessment of the Hydrocarb Process which indicates that substantially more fuel energy can be produced--and at lower cost--than other current options for mitigating carbon dioxide (CO2) from mobile sources. The incremental cost...
Effects of recent energy system changes on CO2 projections for the United States
Recent projections of United States carbon dioxide (CO2) emissions are considerably lower than those made just a decade ago. A myriad of factors have contributed to lower forecasts, including reductions in end-use energy service demands, improvements in energy efficiency, techno...
Electrochemical Reduction of Protic Supercritical CO2 on Copper Electrodes.
Melchaeva, Olga; Voyame, Patrick; Bassetto, Victor Costa; Prokein, Michael; Renner, Manfred; Weidner, Eckhard; Petermann, Marcus; Battistel, Alberto
2017-09-22
The electrochemical reduction of carbon dioxide is usually studied in aqueous solutions under ambient conditions. However, the main disadvantages of this method are high hydrogen evolution and low faradaic efficiencies of carbon-based products. Supercritical CO 2 (scCO 2 ) can be used as a solvent itself to suppresses hydrogen evolution and tune the carbon-based product yield; however, it has received little attention for this purpose. Therefore, the focus of this study was on the electrochemical reduction of scCO 2 . The conductivity of scCO 2 was increased through the addition of supporting electrolyte and a cosolvent (acetonitrile). Furthermore, the addition of protic solutions of different pH to scCO 2 was investigated. 1 m H 2 SO 4 , trifluoroethanol, H 2 O, KOH, and CsHCO 3 solutions were used to determine the effect on current density, faradaic efficiency, and selectivity of the scCO 2 reduction. The reduction of scCO 2 to methanol and ethanol are reported for the first time. However, methane and ethylene were not observed. Additionally, corrosion of the Cu electrode was noticed. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Zhang, Sheng; Kang, Peng; Bakir, Mohammed
2015-12-14
Developing sustainable energy strategies based on CO2 reduction is an increasingly important issue given the world’s continued reliance on hydrocarbon fuels and the rise in CO2 concentrations in the atmosphere. An important option is electrochemical or photoelectrochemical CO2 reduction to carbon fuels. We describe here an electrodeposition strategy for preparing highly dispersed, ultrafine metal nanoparticle catalysts on an electroactive polymeric film including nanoalloys of Cu and Pd. Compared with nanoCu catalysts, which are state-of-the-art catalysts for CO2 reduction to hydrocarbons, the bimetallic CuPd nanoalloy catalyst exhibits a greater than twofold enhancement in Faradaic efficiency for CO2 reduction to methane. Themore » origin of the enhancement is suggested to arise from a synergistic reactivity interplay between Pd–H sites and Cu–CO sites during electrochemical CO2 reduction. The polymer substrate also appears to provide a basis for the local concentration of CO2 resulting in the enhancement of catalytic current densities by threefold. The procedure for preparation of the nanoalloy catalyst is straightforward and appears to be generally applicable to the preparation of catalytic electrodes for incorporation into electrolysis devices.« less
Zhang, Sheng; Kang, Peng; Bakir, Mohammed; Lapides, Alexander M.; Dares, Christopher J.; Meyer, Thomas J.
2015-01-01
Developing sustainable energy strategies based on CO2 reduction is an increasingly important issue given the world’s continued reliance on hydrocarbon fuels and the rise in CO2 concentrations in the atmosphere. An important option is electrochemical or photoelectrochemical CO2 reduction to carbon fuels. We describe here an electrodeposition strategy for preparing highly dispersed, ultrafine metal nanoparticle catalysts on an electroactive polymeric film including nanoalloys of Cu and Pd. Compared with nanoCu catalysts, which are state-of-the-art catalysts for CO2 reduction to hydrocarbons, the bimetallic CuPd nanoalloy catalyst exhibits a greater than twofold enhancement in Faradaic efficiency for CO2 reduction to methane. The origin of the enhancement is suggested to arise from a synergistic reactivity interplay between Pd–H sites and Cu–CO sites during electrochemical CO2 reduction. The polymer substrate also appears to provide a basis for the local concentration of CO2 resulting in the enhancement of catalytic current densities by threefold. The procedure for preparation of the nanoalloy catalyst is straightforward and appears to be generally applicable to the preparation of catalytic electrodes for incorporation into electrolysis devices. PMID:26668386
Chen, Manhua; Sui, Xiao; Ma, Xixiu; Feng, Xiaomei; Han, Yuqian
2015-03-30
Supercritical carbon dioxide (SC-CO2 ) has been shown to have a good pasteurising effect on food. However, very few research papers have investigated the possibility to exploit this treatment for solid foods, particularly for seafood. Considering the microbial safety of raw seafood consumption, the study aimed to explore the feasibility of microbial inactivation of shrimp (Metapenaeus ensis) and conch (Rapana venosa) by SC-CO2 treatment. Response surface methodology (RSM) models were established to predict and analyse the SC-CO2 process. A 3.69-log reduction in the total aerobic plate count (TPC) of shrimp was observed by SC-CO2 treatment at 53°C, 15 MPa for 40 min, and the logarithmic reduction in TPC of conch was 3.31 at 55°C, 14 MPa for 42 min. Sensory scores of the products achieved approximately 8 (desirable). The optimal parameters for microbial inactivation of shrimp and conch by SC-CO2 might be 55°C, 15 MPa and 40 min. SC-CO2 exerted a strong bactericidal effect on the TPC of shrimp and conch, and the products maintained good organoleptic properties. This study verified the feasibility of microbial inactivation of shrimp and conch by SC-CO2 treatment. © 2014 Society of Chemical Industry.
Favaro, Marco; Xiao, Hai; Cheng, Tao; Goddard, William A; Yano, Junko; Crumlin, Ethan J
2017-06-27
A national priority is to convert CO 2 into high-value chemical products such as liquid fuels. Because current electrocatalysts are not adequate, we aim to discover new catalysts by obtaining a detailed understanding of the initial steps of CO 2 electroreduction on copper surfaces, the best current catalysts. Using ambient pressure X-ray photoelectron spectroscopy interpreted with quantum mechanical prediction of the structures and free energies, we show that the presence of a thin suboxide structure below the copper surface is essential to bind the CO 2 in the physisorbed configuration at 298 K, and we show that this suboxide is essential for converting to the chemisorbed CO 2 in the presence of water as the first step toward CO 2 reduction products such as formate and CO. This optimum suboxide leads to both neutral and charged Cu surface sites, providing fresh insights into how to design improved carbon dioxide reduction catalysts.
Favaro, Marco; Yano, Junko; Crumlin, Ethan J.
2017-01-01
A national priority is to convert CO2 into high-value chemical products such as liquid fuels. Because current electrocatalysts are not adequate, we aim to discover new catalysts by obtaining a detailed understanding of the initial steps of CO2 electroreduction on copper surfaces, the best current catalysts. Using ambient pressure X-ray photoelectron spectroscopy interpreted with quantum mechanical prediction of the structures and free energies, we show that the presence of a thin suboxide structure below the copper surface is essential to bind the CO2 in the physisorbed configuration at 298 K, and we show that this suboxide is essential for converting to the chemisorbed CO2 in the presence of water as the first step toward CO2 reduction products such as formate and CO. This optimum suboxide leads to both neutral and charged Cu surface sites, providing fresh insights into how to design improved carbon dioxide reduction catalysts. PMID:28607092
Neaţu, Ştefan; Maciá-Agulló, Juan Antonio; Garcia, Hermenegildo
2014-01-01
The reduction of carbon dioxide to useful chemicals has received a great deal of attention as an alternative to the depletion of fossil resources without altering the atmospheric CO2 balance. As the chemical reduction of CO2 is energetically uphill due to its remarkable thermodynamic stability, this process requires a significant transfer of energy. Achievements in the fields of photocatalysis during the last decade sparked increased interest in the possibility of using sunlight to reduce CO2. In this review we discuss some general features associated with the photocatalytic reduction of CO2 for the production of solar fuels, with considerations to be taken into account of the photocatalyst design, of the limitations arising from the lack of visible light response of titania, of the use of co-catalysts to overcome this shortcoming, together with several strategies that have been applied to enhance the photocatalytic efficiency of CO2 reduction. The aim is not to provide an exhaustive review of the area, but to present general aspects to be considered, and then to outline which are currently the most efficient photocatalytic systems. PMID:24670477
Neațu, Stefan; Maciá-Agulló, Juan Antonio; Garcia, Hermenegildo
2014-03-25
The reduction of carbon dioxide to useful chemicals has received a great deal of attention as an alternative to the depletion of fossil resources without altering the atmospheric CO2 balance. As the chemical reduction of CO2 is energetically uphill due to its remarkable thermodynamic stability, this process requires a significant transfer of energy. Achievements in the fields of photocatalysis during the last decade sparked increased interest in the possibility of using sunlight to reduce CO2. In this review we discuss some general features associated with the photocatalytic reduction of CO2 for the production of solar fuels, with considerations to be taken into account of the photocatalyst design, of the limitations arising from the lack of visible light response of titania, of the use of co-catalysts to overcome this shortcoming, together with several strategies that have been applied to enhance the photocatalytic efficiency of CO2 reduction. The aim is not to provide an exhaustive review of the area, but to present general aspects to be considered, and then to outline which are currently the most efficient photocatalytic systems.
An investigation of the reduction of carbon dioxide in a silent electric discharge
NASA Technical Reports Server (NTRS)
Luce, R. S.; Greenough, B. (Editor)
1978-01-01
The reduction of CO2 to O2 and CO in a silent electric discharge was studied. It was found that current alone (in the ionized plasma induced by the silent electric discharge) was reponsible for the CO2 reduction process. Voltage and frequency were important only in so far as they induced current in the plasma. Pressure and temperature were of minimum influence in the process. The large power consumption in the process was recognized as resulting from the low power factor of the reactor vessel which electrically behaved like a capacitor. The power factor was subsequently improved by adding an inductive element to make the reactor vessel capacitance part of a resonant circuit. It was found that the CO2 reduction process was most efficient in terms of power vs reduction rate when a voltage was employed that was only slightly higher than that needed to induce the plasma.
Evaluation of Carbon Dioxide Laser in the Treatment of Epidermal Nevi.
Bhat, Yasmeen Jabeen; Hassan, Iffat; Sajad, Peerzada; Yaseen, Atiya; Mubashir, Syed; Akhter, Saniya; Wani, Roohi
2016-01-01
Epidermal naevi are benign hamartomatous growths of the skin which are generally asymptomatic with a benign course but are cosmetically disagreeable. Topical treatments such as steroids, calcipotriol, 5 fluorouracil, podophyllin, retinoids and cryotherapy are ineffective and surgical excision results in scar formation. Therapy is often challenging. To study the response of carbon dioxide (CO 2 ) laser in the management of epidermal naevi. We conducted a study of CO 2 laser treatment on 15 patients of epidermal naevi, eight with verrucous epidermal naevi and seven with sebaceous naevi. A thorough history and examination was done to rule out any epidermal naevus syndrome. The diagnosis was confirmed by histopathology. The number of treatment sessions varied from 1 to 8. Response was excellent (>90% reduction in lesion size) in three patients, very good (>75% reduction) in five, good (>50% reduction in lesion size) in five and poor (<50% reduction in lesion size) in two patients. The side effects were hyperpigmentation and scarring. Long-term follow-up over a period of 10 months showed a recurrence rate of 20%. We conclude that CO 2 laser treatment might be an effective option with long-term safety, minimal discomfort and rapid recovery.
Analyzing and forecasting CO2 emission reduction in China's steel industry
NASA Astrophysics Data System (ADS)
Gao, Chengkang; Wang, Dan; Zhao, Baohua; Chen, Shan; Qin, Wei
2015-03-01
Recent measures of carbon dioxide emissions from the steel industry of China have indicated a high rate of total CO2 emissions from the industry, even compared to the rest of the world. So, CO2 emission reduction in China's steel industry was analyzed, coupling the whole process and scenarios analysis. First, assuming that all available advanced technologies are almost adopted, this study puts forward some key potential-sectors and explores an optimal technical route for reducing CO2 emissions from the Chinese steel industry based on whole process analysis. The results show that in the stages of coking, sintering, and iron making, greater potential for reducing emissions would be fulfilled by taking some technological measures. If only would above well-developed technologies be fulfill, the CO2 emissions from 5 industry production stages would be reduced substantially, and CO2 emissions per ton of steel could be decreased to 1.24 (ton/ton-steel) by 2020. At the same time, the scenarios analysis indicates that if mature carbon-reducing technologies are adopted, and if the difference between steel output growth rate and the GDP growth rate could be controlled below 3%, CO2 emissions from China's steel industry would approach the goal of reducing CO2 emissions per GDP unit by 40%-45% of the 2005 level by 2020. This indicates that the focus of carbon dioxide emissions reduction in China lies in policy adjustments in order to enhance technological application, and lies in reasonably controlling the pace of growth of GDP and steel output.
The World Bank’s Clean Technology Fund (CTF)
2008-11-24
economies such as China and India. The incremental carbon dioxide (CO2) emissions from China and India alone have accounted for an estimated 62% of new...gas reductions. Carbon dioxide emissions from power plants are directly proportional to efficiency, so a plant going with an 18% absolute increase in...efficiency would produce 18% less carbon dioxide . These are the higher heating value (HHV) thermal efficiency rates, not be confused with lower heating
Solvent-driven reductive activation of carbon dioxide by gold anions.
Knurr, Benjamin J; Weber, J Mathias
2012-11-14
Catalytic activation and electrochemical reduction of CO(2) for the formation of chemically usable feedstock and fuel are central goals for establishing a carbon neutral fuel cycle. The role of solvent molecules in catalytic processes is little understood, although solvent-solute interactions can strongly influence activated intermediate species. We use vibrational spectroscopy of mass-selected Au(CO(2))(n)(-) cluster ions to probe the solvation of AuCO(2)(-) as a model for a reactive intermediate in the reductive activation of a CO(2) ligand by a single-atom catalyst. For the first few solvent molecules, solvation of the complex preferentially occurs at the CO(2) moiety, enhancing reductive activation through polarization of the excess charge onto the partially reduced ligand. At higher levels of solvation, direct interaction of additional solvent molecules with the Au atom diminishes reduction. The results show how the solvation environment can enhance or diminish the effects of a catalyst, offering design criteria for single-atom catalyst engineering.
Pang, Hong; Masuda, Takuya; Ye, Jinhua
2018-01-18
The photoelectrochemical (PEC) carbon dioxide reduction process stands out as a promising avenue for the conversion of solar energy into chemical feedstocks, among various methods available for carbon dioxide mitigation. Semiconductors derived from cheap and abundant elements are interesting candidates for catalysis. Whether employed as intrinsic semiconductors or hybridized with metallic cocatalysts, biocatalysts, and metal molecular complexes, semiconductor photocathodes exhibit good performance and low overpotential during carbon dioxide reduction. Apart from focusing on carbon dioxide reduction materials and chemistry, PEC cells towards standalone devices that use photohybrid electrodes or solar cells have also been a hot topic in recent research. An overview of the state-of-the-art progress in PEC carbon dioxide reduction is presented and a deep understanding of the catalysts of carbon dioxide reduction is also given. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.
Electrochemical processing of carbon dioxide.
Oloman, Colin; Li, Hui
2008-01-01
With respect to the negative role of carbon dioxide on our climate, it is clear that the time is ripe for the development of processes that convert CO(2) into useful products. The electroreduction of CO(2) is a prime candidate here, as the reaction at near-ambient conditions can yield organics such as formic acid, methanol, and methane. Recent laboratory work on the 100 A scale has shown that reduction of CO(2) to formate (HCO(2)(-)) may be carried out in a trickle-bed continuous electrochemical reactor under industrially viable conditions. Presuming the problems of cathode stability and formate crossover can be overcome, this type of reactor is proposed as the basis for a commercial operation. The viability of corresponding processes for electrosynthesis of formate salts and/or formic acid from CO(2) is examined here through conceptual flowsheets for two process options, each converting CO(2) at the rate of 100 tonnes per day.
For Frank Princiotta’s book, Global Climate Change—The Technology Challenge Carbon dioxide (CO2) accounts for more than 90% of worldwide CO2-eq green-house gas (GHG) emissions from industrial sectors other than power generation. Amongst these sectors, the cement industry is one ...
NEMETH, BALAZS; KISS, ISTVAN; JENCSIK, TIMEA; PETER, IVAN; KRESKA, ZITA; KOSZEGI, TAMAS; MISETA, ATTILA; KUSTAN, PETER; BONCZ, IMRE; LACZO, ANDREA; AJTAY, ZENO
2017-01-01
Aim: To study the effect of carbon dioxide (CO2) therapy on the nitric oxide (NO) pathway by monitoring plasma asymmetric dimethylarginine (ADMA) concentrations. Patients and Methods: Forty-seven hypertensive patients who underwent transcutaneous CO2 therapy were enrolled. Thirty healthy individuals were recruited for the control group. Blood samples were taken one hour before, as well as one hour, 24 hours and 3 weeks after the first CO2 treatment. Controls did not undergo CO2 treatment. Plasma ADMA levels were measured by ELISA. Results: ADMA levels decreased significantly one hour after the first CO2 treatment compared to the baseline concentrations (p=0.003). Significantly greater reduction was found among patients in whom angiotensin converting enzyme inhibitors (ACEIs) were administered (p=0.019). Conclusion: The short- and long-term decrease of ADMA levels suggests that CO2 is not only a vasodilator, but also has a beneficial effect on the NO pathway. ACE inhibition seems to enhance the effect of CO2 treatment. PMID:28438873
Photoredox activation of carbon dioxide for amino acid synthesis in continuous flow
NASA Astrophysics Data System (ADS)
Seo, Hyowon; Katcher, Matthew H.; Jamison, Timothy F.
2017-05-01
Although carbon dioxide (CO2) is highly abundant, its low reactivity has limited its use in chemical synthesis. In particular, methods for carbon-carbon bond formation generally rely on two-electron mechanisms for CO2 activation and require highly activated reaction partners. Alternatively, radical pathways accessed via photoredox catalysis could provide new reactivity under milder conditions. Here we demonstrate the direct coupling of CO2 and amines via the single-electron reduction of CO2 for the photoredox-catalysed continuous flow synthesis of α-amino acids. By leveraging the advantages of utilizing gases and photochemistry in flow, a commercially available organic photoredox catalyst effects the selective α-carboxylation of amines that bear various functional groups and heterocycles. The preliminary mechanistic studies support CO2 activation and carbon-carbon bond formation via single-electron pathways, and we expect that this strategy will inspire new perspectives on using this feedstock chemical in organic synthesis.
Zhao, Zhi; Kong, Xiangtao; Yang, Dong; Yuan, Qinqin; Xie, Hua; Fan, Hongjun; Zhao, Jijun; Jiang, Ling
2017-05-04
The reaction of copper and silver cations with carbon dioxide was studied by mass-selected infrared photodissociation spectroscopy. Quantum chemical calculations were performed on these products, which aided the experimental assignments of the infrared spectra and helped to elucidate the geometrical and electronic structures. The Cu + and Ag + cations bind to an oxygen atom of CO 2 in an end-on configuration via a charge-quadrupole electrostatic interaction in the [M(CO 2 ) n ] + complexes. The formation of oxide-carbonyl and carbonyl-carbonate structures is not favored for the interaction of CO 2 with Cu + and Ag + . For n = 3 and 4, the n + 0 structure is preferred. [Note on the nomenclature: Using i + j, i denotes the number of CO 2 molecules in the first coordination shell, and j denotes the number of CO 2 molecules in the second coordination shell.] The two nearly energy-identical n + 0 and (n - 1) + 1 structures coexist in n = 5 and 6. While the six-coordinated structure is favored for [Cu(CO 2 ) n=7,8 ] + , the n + 0 configuration is dominated in [Ag(CO 2 ) n=7,8 ] + . The reaction of CO 2 with the cationic metal atoms has been compared to that with the neutral and anionic metal atoms, which would have important implications for understanding the interaction of CO 2 with reduction catalysts and rationally designing catalysts for CO 2 reduction based on cost-effective transition metals.
Catholyte-Free Electrocatalytic CO2 Reduction to Formate.
Lee, Wonhee; Kim, Young Eun; Youn, Min Hye; Jeong, Soon Kwan; Park, Ki Tae
2018-04-16
Electrochemical reduction of carbon dioxide (CO 2 ) into value-added chemicals is a promising strategy to reduce CO 2 emission and mitigate climate change. One of the most serious problems in electrocatalytic CO 2 reduction (CO 2 R) is the low solubility of CO 2 in an aqueous electrolyte, which significantly limits the cathodic reaction rate. This paper proposes a facile method of catholyte-free electrocatalytic CO 2 reduction to avoid the solubility limitation using commercial tin nanoparticles as a cathode catalyst. Interestingly, as the reaction temperature rises from 303 K to 363 K, the partial current density (PCD) of formate improves more than two times with 52.9 mA cm -2 , despite the decrease in CO 2 solubility. Furthermore, a significantly high formate concentration of 41.5 g L -1 is obtained as a one-path product at 343 K with high PCD (51.7 mA cm -2 ) and high Faradaic efficiency (93.3 %) via continuous operation in a full flow cell at a low cell voltage of 2.2 V. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.
Molecular approaches to the photocatalytic reduction of carbon dioxide for solar fuels.
Morris, Amanda J; Meyer, Gerald J; Fujita, Etsuko
2009-12-21
The scientific community now agrees that the rise in atmospheric CO(2), the most abundant green house gas, comes from anthropogenic sources such as the burning of fossil fuels. This atmospheric rise in CO(2) results in global climate change. Therefore methods for photochemically transforming CO(2) into a source of fuel could offer an attractive way to decrease atmospheric concentrations. One way to accomplish this conversion is through the light-driven reduction of carbon dioxide to methane (CH(4(g))) or methanol (CH(3)OH((l))) with electrons and protons derived from water. Existing infrastructure already supports the delivery of natural gas and liquid fuels, which makes these possible CO(2) reduction products particularly appealing. This Account focuses on molecular approaches to photochemical CO(2) reduction in homogeneous solution. The reduction of CO(2) by one electron to form CO(2)(*-) is highly unfavorable, having a formal reduction potential of -2.14 V vs SCE. Rapid reduction requires an overpotential of up to 0.6 V, due at least in part to the kinetic restrictions imposed by the structural difference between linear CO(2) and bent CO(2)(*-). An alternative and more favorable pathway is to reduce CO(2) though proton-assisted multiple-electron transfer. The development of catalysts, redox mediators, or both that efficiently drive these reactions remains an important and active area of research. We divide these reactions into two class types. In Type I photocatalysis, a molecular light absorber and a transition metal catalyst work in concert. We also consider a special case of Type 1 photocatalysis, where a saturated hydrocarbon links the catalyst and the light absorber in a supramolecular compound. In Type II photocatalysis, the light absorber and the catalyst are the same molecule. In these reactions, transition-metal coordination compounds often serve as catalysts because they can absorb a significant portion of the solar spectrum and can promote activation of small molecules. This Account discusses four classes of transition-metal catalysts: (A) metal tetraaza-macrocyclic compounds; (B) supramolecular complexes; (C) metalloporphyrins and related metallomacrocycles; (D) Re(CO)(3)(bpy)X-based compounds where bpy = 2,2'-bipyridine. Carbon monoxide and formate are the primary CO(2) reduction products, and we also propose bicarbonate/carbonate production. For comprehensiveness, we briefly discuss hydrogen formation, a common side reaction that occurs concurrently with CO(2) reduction, though the details of that process are beyond the scope of this Account. It is our hope that drawing attention both to current mechanistic hypotheses and to the areas that are poorly understood will stimulate research that could one day provide an efficient solution to this global problem.
A 3-hydroxypropionate/4-hydroxybutyrate autotrophic carbon dioxide assimilation pathway in Archaea.
Berg, Ivan A; Kockelkorn, Daniel; Buckel, Wolfgang; Fuchs, Georg
2007-12-14
The assimilation of carbon dioxide (CO2) into organic material is quantitatively the most important biosynthetic process. We discovered that an autotrophic member of the archaeal order Sulfolobales, Metallosphaera sedula, fixed CO2 with acetyl-coenzyme A (acetyl-CoA)/propionyl-CoA carboxylase as the key carboxylating enzyme. In this system, one acetyl-CoA and two bicarbonate molecules were reductively converted via 3-hydroxypropionate to succinyl-CoA. This intermediate was reduced to 4-hydroxybutyrate and converted into two acetyl-CoA molecules via 4-hydroxybutyryl-CoA dehydratase. The key genes of this pathway were found not only in Metallosphaera but also in Sulfolobus, Archaeoglobus, and Cenarchaeum species. Moreover, the Global Ocean Sampling database contains half as many 4-hydroxybutyryl-CoA dehydratase sequences as compared with those found for another key photosynthetic CO2-fixing enzyme, ribulose-1,5-bisphosphate carboxylase-oxygenase. This indicates the importance of this enzyme in global carbon cycling.
Lyu, Lingyun; Zeng, Xu; Yun, Jun; Wei, Feng; Jin, Fangming
2014-05-20
The "greenhouse effect" caused by the increasing atmospheric CO2 level is becoming extremely serious, and thus, the reduction of CO2 emissions has become an extensive, urgent, and long-term task. The dissociation of water for CO2 reduction with solar energy is regarded as one of the most promising methods for the sustainable development of the environment and energy. However, a high solar-to-fuel efficiency keeps a great challenge. In this work, the first observation of a highly effective, highly selective, and robust system of dissociating water for the reduction of carbon dioxide (CO2) into formic acid with metallic manganese (Mn) is reported. A considerably high formic acid yield of more than 75% on a carbon basis from NaHCO3 was achieved with 98% selectivity in the presence of simple commercially available Mn powder without the addition of any catalyst, and the proposed process is exothermic. Thus, this study may provide a promising method for the highly efficient dissociation of water for CO2 reduction by combining solar-driven thermochemistry with the reduction of MnO into Mn.
Portenkirchner, Engelbert; Kianfar, Elham; Sariciftci, Niyazi Serdar; Knör, Günther
2014-05-01
Rhenium(I) carbonyl complexes carrying substituted bis(arylimino)acenaphthene ligands (BIAN-R) have been tested as potential catalysts for the two-electron reduction of carbon dioxide. Cyclic voltammetric studies as well as controlled potential electrolysis experiments were performed using CO2-saturated solutions of the complexes in acetonitrile and acetonitrile-water mixtures. Faradaic efficiencies of more than 30 % have been determined for the electrocatalytic production of CO. The effects of ligand substitution patterns and water content of the reaction medium on the catalytic performance of the new catalysts are discussed. © 2014 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA. This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.
Yan, Yibo; Li, Kaixin; Chen, Xiaoping; Yang, Yanhui; Lee, Jong-Min
2017-12-01
Expedition of electron transfer efficiency and optimization of surface reactant adsorption products desorption processes are two main challenges for developing non-noble catalysts in the oxygen reduction reaction (ORR) and CO 2 reduction reaction (CRR). A heterojunction prototype on Co 3 S 4 @Co 3 O 4 core-shell octahedron structure is established via hydrothermal lattice anion exchange protocol to implement the electroreduction of oxygen and carbon dioxide with high performance. The synergistic bifunctional catalyst consists of p-type Co 3 O 4 core and n-type Co 3 S 4 shell, which afford high surface electron density along with high capacitance without sacrificing mechanical robustness. A four electron ORR process, identical to the Pt catalyzed ORR, is validated using the core-shell octahedron catalyst. The synergistic interaction between cobalt sulfide and cobalt oxide bicatalyst reduces the activation energy to convert CO 2 into adsorbed intermediates and hereby enables CRR to run at a low overpotential, with formate as the highly selective main product at a high faraday efficiency of 85.3%. The remarkable performance can be ascribed to the synergistic coupling effect of the structured co-catalysts; heterojunction structure expedites the electron transfer efficiency and optimizes surface reactant adsorption product desorption processes, which also provide theoretical and pragmatic guideline for catalyst development and mechanism explorations. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Using the adsorption chillers for waste heat utilisation from the CCS installation
NASA Astrophysics Data System (ADS)
Sztekler, Karol; Kalawa, Wojciech; Nowak, Wojciech; Stefański, Sebastian; Krzywański, Jarosław; Grabowska, Karolina
2018-06-01
Worldwide tendencies in the scope of environmental protection demonstrate the requirement for the limited carbon dioxide emission, that influences on the development of greenhouse effect. As a result of coal as a basic fuel used in the professional power industry, this industry sector is the greatest CO2 polluter and it means that works on the reduction of carbon dioxide in such industry are completely justified. In the IPSEpro programming environment, a reference block model for a conventional coal power station was elaborated, including the CO2 separation unit basing on the adsorption methods with the CO2 preparation installation to liquid state. Simulation researches were conducted with means of numeric techniques, that enabled the system analysis for the CO2 separation unit with the CO2 preparation system to the liquid state, as well as analysis was made for the use of chiller systems, basing on the adsorption technology for waste heat use originating from the compression of CO2 in a cascade system, as well as for potential opportunities for further exploitation of the produced chilled water in the CCS cycle. We analysed in these papers the opportunities for chiller systems application, based on the adsorption chillers in the CCS installation used for the reduction of CO2 emission in the coal power station and its influence on the operation of a power station cycle.
ABSORPTION OF CO2 AND SUBSEQUENT VISCOSITY REDUCTION OF AN ACRYLONITRILE COPOLYMER. (R829555)
Acrylonitrile (AN) copolymers (AN content greater than about 85 mol%) are traditionally solution processed to avoid a cyclization and crosslinking reaction that takes place at temperatures where melt processing would be feasible. It is well known that carbon dioxide (CO
NASA Astrophysics Data System (ADS)
Sidorin, D. I.
2015-12-01
The carbon dioxide (CO2) production intensity by a secondary school student is studied using a nondispersive infrared CO2 logger for different conditions: relaxation, mental stress, and physical stress. CO2 production measured for mental stress is 24% higher than that for relaxation, while CO2 production for physical stress is more than 2.5 times higher than relaxation levels. Dynamics of CO2 concentration in the classroom air is measured for a typical school building. It is shown that even when the classroom is ventilated between classes, CO2 concentration exceeds 2100 parts per million (ppm), which is significantly higher than the recommended limits defined in developed countries. The ability of seventh-grade school students to perform tasks requiring mental concentration is tested under different CO2 concentration conditions (below 1000 ppm and above 2000 ppm). Five-letter word anagrams are used as test tasks. Statistical analysis of the test results revealed a significant reduction in the number of provided correct answers and an increase in the number of errors when CO2 levels exceeded 2000 ppm.
Thakur, Indu Shekhar; Kumar, Manish; Varjani, Sunita J; Wu, Yonghong; Gnansounou, Edgard; Ravindran, Sindhu
2018-05-01
To meet the CO 2 emission reduction targets, carbon dioxide capture and utilization (CCU) comes as an evolve technology. CCU concept is turning into a feedstock and technologies have been developed for transformation of CO 2 into useful organic products. At industrial scale, utilization of CO 2 as raw material is not much significant as compare to its abundance. Mechanisms in nature have evolved for carbon concentration, fixation and utilization. Assimilation and subsequent conversion of CO 2 into complex molecules are performed by the photosynthetic and chemolithotrophic organisms. In the last three decades, substantial research is carry out to discover chemical and biological conversion of CO 2 in various synthetic and biological materials, such as carboxylic acids, esters, lactones, polymer biodiesel, bio-plastics, bio-alcohols, exopolysaccharides. This review presents an over view of catalytic transformation of CO 2 into biofuels and biomaterials by chemical and biological methods. Copyright © 2018 Elsevier Ltd. All rights reserved.
Global warming: is weight loss a solution?
Gryka, A; Broom, J; Rolland, C
2012-03-01
The current climate change has been most likely caused by the increased greenhouse gas emissions. We have looked at the major greenhouse gas, carbon dioxide (CO(2)), and estimated the reduction in the CO(2) emissions that would occur with the theoretical global weight loss. The calculations were based on our previous weight loss study, investigating the effects of a low-carbohydrate diet on body weight, body composition and resting metabolic rate of obese volunteers with type 2 diabetes. At 6 months, we observed decreases in weight, fat mass, fat free mass and CO(2) production. We estimated that a 10 kg weight loss of all obese and overweight people would result in a decrease of 49.560 Mt of CO(2) per year, which would equal to 0.2% of the CO(2) emitted globally in 2007. This reduction could help meet the CO(2) emission reduction targets and unquestionably would be of a great benefit to the global health.
Tsai, Chia-Hua; Chirdon, Danielle N; Kagalwala, Husain N; Maurer, Andrew B; Kaur, Aman; Pintauer, Tomislav; Bernhard, Stefan; Noonan, Kevin J T
2015-08-03
The synthesis and characterization of electron-poor thiophene 1,1-dioxides bearing cyanated phenyl groups are reported. The electron-accepting nature of these compounds was evaluated by cyclic voltammetry, and highly reversible and facile reductions were observed for several derivatives. Moreover, some of the reduced thiophene dioxides form colorful anions, which were investigated spectroelectrochemically. Photoluminescence spectra of the electron-deficient sulfones were measured in CH2 Cl2, and they emit in the blue-green region with significant variation in the quantum yield depending on the aryl substituents. By expanding the degree of substitution on the phenyl rings, quantum yields up to 34 % were obtained. X-ray diffraction data are reported for two of the thiophene 1,1-dioxides, and the electronic structure was probed for all synthesized derivatives through DFT calculations. The dioxides were also examined as electron relays in a photocatalytic water reduction reaction, and they showed potential to boost the efficiency. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Carbon dioxide fluxes from an urban area in Beijing
NASA Astrophysics Data System (ADS)
Song, Tao; Wang, Yuesi
2012-03-01
A better understanding of urban carbon dioxide (CO 2) emissions is important for quantifying urban contributions to the global carbon budget. From January to December 2008, CO 2 fluxes were measured, by eddy covariance at 47 m above ground on a meteorological tower in a high-density residential area in Beijing. The results showed that the urban surface was a net source of CO 2 in the atmosphere. Diurnal flux patterns were similar to those previously observed in other cities and were largely influenced by traffic volume. Carbon uptake by both urban vegetation during the growing season and the reduction of fuel consumption for domestic heating resulted in less-positive daily fluxes in the summer. The average daily flux measured in the summer was 0.48 mg m - 2 s - 1 , which was 82%, 35% and 36% lower than those in the winter, spring and autumn, respectively. The reduction of vehicles on the road during the 29th Olympic and Paralympic Games had a significant impact on CO 2 flux. The flux of 0.40 mg m - 2 s - 1 for September 2008 was approximately 0.17 mg m - 2 s - 1 lower than the flux for September 2007. Annual CO 2 emissions from the study site were estimated at 20.6 kg CO 2 m - 2 y - 1 , considerably higher than yearly emissions obtained from other urban and suburban landscapes.
Favaro, Marco; Xiao, Hai; Cheng, Tao; ...
2017-06-12
A national priority is to convert CO 2 into high-value chemical products such as liquid fuels. Because current electrocatalysts are not adequate, we aim to discover new catalysts by obtaining a detailed understanding of the initial steps of CO 2 electroreduction on copper surfaces, the best current catalysts. Using ambient pressure X-ray photoelectron spectroscopy interpreted with quantum mechanical prediction of the structures and free energies, we show that the presence of a thin suboxide structure below the copper surface is essential to bind the CO 2 in the physisorbed configuration at 298 K, and we show that this suboxide ismore » essential for converting to the chemisorbed CO 2 in the presence of water as the first step toward CO 2 reduction products such as formate and CO. This optimum suboxide leads to both neutral and charged Cu surface sites, providing fresh insights into how to design improved carbon dioxide reduction catalysts.« less
Recent Advances in Inorganic Heterogeneous Electrocatalysts for Reduction of Carbon Dioxide.
Zhu, Dong Dong; Liu, Jin Long; Qiao, Shi Zhang
2016-05-01
In view of the climate changes caused by the continuously rising levels of atmospheric CO2 , advanced technologies associated with CO2 conversion are highly desirable. In recent decades, electrochemical reduction of CO2 has been extensively studied since it can reduce CO2 to value-added chemicals and fuels. Considering the sluggish reaction kinetics of the CO2 molecule, efficient and robust electrocatalysts are required to promote this conversion reaction. Here, recent progress and opportunities in inorganic heterogeneous electrocatalysts for CO2 reduction are discussed, from the viewpoint of both experimental and computational aspects. Based on elemental composition, the inorganic catalysts presented here are classified into four groups: metals, transition-metal oxides, transition-metal chalcogenides, and carbon-based materials. However, despite encouraging accomplishments made in this area, substantial advances in CO2 electrolysis are still needed to meet the criteria for practical applications. Therefore, in the last part, several promising strategies, including surface engineering, chemical modification, nanostructured catalysts, and composite materials, are proposed to facilitate the future development of CO2 electroreduction. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Quantified, Localized Health Benefits of Accelerated Carbon Dioxide Emissions Reductions.
Shindell, Drew; Faluvegi, Greg; Seltzer, Karl; Shindell, Cary
2018-01-01
Societal risks increase as Earth warms, but also for emissions trajectories accepting relatively high levels of near-term emissions while assuming future negative emissions will compensate even if they lead to identical warming [1]. Accelerating carbon dioxide (CO 2 ) emissions reductions, including as a substitute for negative emissions, hence reduces long-term risks but requires dramatic near-term societal transformations [2]. A major barrier to emissions reductions is the difficulty of reconciling immediate, localized costs with global, long-term benefits [3, 4]. However, 2°C trajectories not relying on negative emissions or 1.5°C trajectories require elimination of most fossil fuel related emissions. This generally reduces co-emissions that cause ambient air pollution, resulting in near-term, localized health benefits. We therefore examine the human health benefits of increasing ambition of 21 st century CO 2 reductions by 180 GtC; an amount that would shift a 'standard' 2°C scenario to 1.5°C or could achieve 2°C without negative emissions. The decreased air pollution leads to 153±43 million fewer premature deaths worldwide, with ~40% occurring during the next 40 years, and minimal climate disbenefits. More than a million premature deaths would be prevented in many metropolitan areas in Asia and Africa, and >200,000 in individual urban areas on every inhabited continent except Australia.
Quantified, localized health benefits of accelerated carbon dioxide emissions reductions
NASA Astrophysics Data System (ADS)
Shindell, Drew; Faluvegi, Greg; Seltzer, Karl; Shindell, Cary
2018-04-01
Societal risks increase as Earth warms, and increase further for emissions trajectories accepting relatively high levels of near-term emissions while assuming future negative emissions will compensate, even if they lead to identical warming as trajectories with reduced near-term emissions1. Accelerating carbon dioxide (CO2) emissions reductions, including as a substitute for negative emissions, hence reduces long-term risks but requires dramatic near-term societal transformations2. A major barrier to emissions reductions is the difficulty of reconciling immediate, localized costs with global, long-term benefits3,4. However, 2 °C trajectories not relying on negative emissions or 1.5 °C trajectories require elimination of most fossil-fuel-related emissions. This generally reduces co-emissions that cause ambient air pollution, resulting in near-term, localized health benefits. We therefore examine the human health benefits of increasing 21st-century CO2 reductions by 180 GtC, an amount that would shift a `standard' 2 °C scenario to 1.5 °C or could achieve 2 °C without negative emissions. The decreased air pollution leads to 153 ± 43 million fewer premature deaths worldwide, with 40% occurring during the next 40 years, and minimal climate disbenefits. More than a million premature deaths would be prevented in many metropolitan areas in Asia and Africa, and >200,000 in individual urban areas on every inhabited continent except Australia.
Evaluation of Carbon Dioxide Laser in the Treatment of Epidermal Nevi
Bhat, Yasmeen Jabeen; Hassan, Iffat; Sajad, Peerzada; Yaseen, Atiya; Mubashir, Syed; Akhter, Saniya; Wani, Roohi
2016-01-01
Background: Epidermal naevi are benign hamartomatous growths of the skin which are generally asymptomatic with a benign course but are cosmetically disagreeable. Topical treatments such as steroids, calcipotriol, 5 fluorouracil, podophyllin, retinoids and cryotherapy are ineffective and surgical excision results in scar formation. Therapy is often challenging. Aim of the Study: To study the response of carbon dioxide (CO2) laser in the management of epidermal naevi. Subjects and Methods: We conducted a study of CO2 laser treatment on 15 patients of epidermal naevi, eight with verrucous epidermal naevi and seven with sebaceous naevi. A thorough history and examination was done to rule out any epidermal naevus syndrome. The diagnosis was confirmed by histopathology. The number of treatment sessions varied from 1 to 8. Results: Response was excellent (>90% reduction in lesion size) in three patients, very good (>75% reduction) in five, good (>50% reduction in lesion size) in five and poor (<50% reduction in lesion size) in two patients. The side effects were hyperpigmentation and scarring. Long-term follow-up over a period of 10 months showed a recurrence rate of 20%. Conclusion: We conclude that CO2 laser treatment might be an effective option with long-term safety, minimal discomfort and rapid recovery. PMID:27761089
Lim, Mihee; Han, Gi-Chun; Ahn, Ji-Whan; You, Kwang-Suk
2010-01-01
This paper reviews the application of carbonation technology to the environmental industry as a way of reducing carbon dioxide (CO2), a green house gas, including the presentation of related projects of our research group. An alternative technology to very slow natural carbonation is the co-called ‘accelerated carbonation’, which completes its fast reaction within few hours by using pure CO2. Carbonation technology is widely applied to solidify or stabilize solid combustion residues from municipal solid wastes, paper mill wastes, etc. and contaminated soils, and to manufacture precipitated calcium carbonate (PCC). Carbonated products can be utilized as aggregates in the concrete industry and as alkaline fillers in the paper (or recycled paper) making industry. The quantity of captured CO2 in carbonated products can be evaluated by measuring mass loss of heated samples by thermo-gravimetric (TG) analysis. The industrial carbonation technology could contribute to both reduction of CO2 emissions and environmental remediation. PMID:20195442
Role of water and carbonates in photocatalytic transformation of CO{sub 2} to CH{sub 4} on titania.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Dimitrijevic, N. M.; Vijayan, B. K.; Poluektov, O. G.
Using the electron paramagnetic resonance technique, we have elucidated the multiple roles of water and carbonates in the overall photocatalytic reduction of carbon dioxide to methane over titania nanoparticles. The formation of H atoms (reduction product) and {center_dot}OH radicals (oxidation product) from water, and CO{sub 3}{sup -} radical anions (oxidation product) from carbonates, was detected in CO{sub 2}-saturated titania aqueous dispersion under UV illumination. Additionally, methoxyl, {center_dot}OCH{sub 3}, and methyl, {center_dot}CH{sub 3}, radicals were identified as reaction intermediates. The two-electron, one-proton reaction proposed as an initial step in the reduction of CO{sub 2} on the surface of TiO{sub 2} ismore » supported by the results of first-principles calculations.« less
Role of Water and Carbonates in Photocatalytic Transformation of CO2 to CH4 on Titania
DOE Office of Scientific and Technical Information (OSTI.GOV)
Dimitrijevic, Nada; Vijayan, Baiju K.; Poluektov, Oleg G.
Using the electron paramagnetic resonance technique, we have elucidated the multiple roles of water and carbonates in the overall photocatalytic reduction of carbon dioxide to methane over titania nanoparticles. The formation of H atoms (reduction product) and {sm_bullet}OH radicals (oxidation product) from water, and CO{sub 3}{sup -} radical anions (oxidation product) from carbonates, was detected in CO{sub 2}-saturated titania aqueous dispersion under UV illumination. Additionally, methoxyl, {sm_bullet}OCH{sub 3}, and methyl, {sm_bullet}CH{sub 3}, radicals were identified as reaction intermediates. The two-electron, one-proton reaction proposed as an initial step in the reduction of CO{sub 2}, on the surface of TiO{sub 2}, ismore » supported by the results of first-principles calculations.« less
NASA Technical Reports Server (NTRS)
Schubert, F. H.; Wynveen, R. A.; Hallick, T. M.
1976-01-01
Regenerative processes for the revitalization of spacecraft atmospheres require an Oxygen Reclamation System (ORS) for the collection of carbon dioxide and water vapor and the recovery of oxygen from these metabolic products. Three life support subsystems uniquely qualified to form such an ORS are an Electrochemical CO2 Depolarized Concentrator (EDC), a CO2 Reduction Subsystem (BRS) and a Water Electrolysis Subsystem (WES). A program to develop and test the interface hardware and control concepts necessary for integrated operation of a four man capacity EDC with a four man capacity BRS was successfully completed. The control concept implemented proved successful in operating the EDC with the BRS for both constant CO2 loading as well as variable CO2 loading, based on a repetitive mission profile of the Space Station Prototype (SSP).
Waller, Diane L.; Bartsch, Michelle; Bartsch, Lynn; Jackson, Craig
2018-01-01
Levels of carbon dioxide (CO2) that have been proposed for aquatic invasive species (AIS) control [24 000 – 96 000 µatm partial pressure CO2 (PCO2); 1 atm = 101.325 kPa] were tested on juvenile mussels, the Fatmucket (Lampsilis siliquoidea) and the U.S. federally endangered Higgins Eye (L. higginsii). A suite of responses (survival, growth, behavior, and gene expression) were measured after 28-d exposure and 14-d postexposure to CO2. The 28-d LC20 (lethal concentration to 20%) was lower for L. higginsii (31 800 µatm PCO2, 95% confidence interval (CI) 15 000 – 42 800 µatm) than for L. siliquoidea (58 200 µatm PCO2, 95% CI 45 200 – 68 100 µatm). Treatment-related reductions occurred in all measures of growth and condition. Expression of chitin synthase, key for shell formation, was down-regulated at 28-d exposure. Carbon dioxide caused narcotization and unburial of mussels, behaviors that could increase mortality by predation and displacement. We conclude that survival and growth of juvenile mussels could be reduced by continuous exposure to elevated CO2, but recovery may be possible in shorter duration exposure.
Holck, Askild L; Pettersen, Marit K; Moen, Marie H; Sørheim, Oddvin
2014-07-01
Modified atmosphere packaging containing CO2 is widely used for extending the shelf life of chicken meat. Active packaging by adding CO2 emitter sachets to packages of meat is an alternative to traditional modified atmosphere packaging. The purpose of the study was to investigate the shelf life of chicken filets under different CO2 concentrations at 4°C storage. The inhibition of microbial growth was proportional to the CO2 concentration. Storage in 100% CO2 both with and without a CO2 emitter sachet gave a microbiological shelf-life extension of 7 days compared with 60% CO2. Carnobacterium divergens, Carnobacterium sp., and Lactococcus sp. were the dominating species at the end of the storage period. During storage in pure CO2, the carbon dioxide dissolved in the meat and caused the collapse of the packages. The resulting squeeze of the meat lead to a severe increase in drip loss. The drip loss was reduced profoundly by using the CO2 emitting sachet in the packages. The addition of CO2 emitters can easily be implemented at industrial packaging lines without reduction in production efficiency.
Ye, Lingting; Zhang, Minyi; Huang, Ping; Guo, Guocong; Hong, Maochun; Li, Chunsen; Irvine, John T. S.; Xie, Kui
2017-01-01
Sustainable future energy scenarios require significant efficiency improvements in both electricity generation and storage. High-temperature solid oxide cells, and in particular carbon dioxide electrolysers, afford chemical storage of available electricity that can both stabilize and extend the utilization of renewables. Here we present a double doping strategy to facilitate CO2 reduction at perovskite titanate cathode surfaces, promoting adsorption/activation by making use of redox active dopants such as Mn linked to oxygen vacancies and dopants such as Ni that afford metal nanoparticle exsolution. Combined experimental characterization and first-principle calculations reveal that the adsorbed and activated CO2 adopts an intermediate chemical state between a carbon dioxide molecule and a carbonate ion. The dual doping strategy provides optimal performance with no degradation being observed after 100 h of high-temperature operation and 10 redox cycles, suggesting a reliable cathode material for CO2 electrolysis. PMID:28300066
Analyzing the efficacy of subtropical urban forests in offsetting carbon emissions from cities
Francisco Escobedo; Sebastian Varela; Min Zhao; John E. Wagner; Wayne Zipperer
2010-01-01
Urban forest management and policies have been promoted as a tool to mitigate carbon dioxide (CO2) emissions. This study used existing CO2 reduction measures from subtropical Miami-Dade and Gainesville, USA and modeled carbon storage and sequestration by trees to analyze policies that use urban forests to offset carbon emissions. Field data were analyzed, modeled, and...
Nemeth, Balazs; Kiss, Istvan; Jencsik, Timea; Peter, Ivan; Kreska, Zita; Koszegi, Tamas; Miseta, Attila; Kustan, Peter; Boncz, Imre; Laczo, Andrea; Ajtay, Zeno
2017-01-01
To study the effect of carbon dioxide (CO 2 ) therapy on the nitric oxide (NO) pathway by monitoring plasma asymmetric dimethylarginine (ADMA) concentrations. Forty-seven hypertensive patients who underwent transcutaneous CO 2 therapy were enrolled. Thirty healthy individuals were recruited for the control group. Blood samples were taken one hour before, as well as one hour, 24 hours and 3 weeks after the first CO 2 treatment. Controls did not undergo CO 2 treatment. Plasma ADMA levels were measured by ELISA. ADMA levels decreased significantly one hour after the first CO2 treatment compared to the baseline concentrations (p=0.003). Significantly greater reduction was found among patients in whom angiotensin converting enzyme inhibitors (ACEIs) were administered (p=0.019). The short- and long-term decrease of ADMA levels suggests that CO 2 is not only a vasodilator, but also has a beneficial effect on the NO pathway. ACE inhibition seems to enhance the effect of CO 2 treatment. Copyright© 2017, International Institute of Anticancer Research (Dr. George J. Delinasios), All rights reserved.
2017-01-01
Conversion of carbon monoxide (CO), a major one-carbon product of carbon dioxide (CO2) reduction, into value-added multicarbon species is a challenge to addressing global energy demands and climate change. Here we report a modular synthetic approach for aqueous electrochemical CO reduction to carbon–carbon coupled products via self-assembly of supramolecular cages at molecular–materials interfaces. Heterobimetallic cavities formed by face-to-face coordination of thiol-terminated metalloporphyrins to copper electrodes through varying organic struts convert CO to C2 products with high faradaic efficiency (FE = 83% total with 57% to ethanol) and current density (1.34 mA/cm2) at a potential of −0.40 V vs RHE. The cage-functionalized electrodes offer an order of magnitude improvement in both selectivity and activity for electrocatalytic carbon fixation compared to parent copper surfaces or copper functionalized with porphyrins in an edge-on orientation. PMID:28979945
Gong, Ming; Cao, Zhi; Liu, Wei; ...
2017-09-13
Conversion of carbon monoxide (CO), a major one-carbon product of carbon dioxide (CO 2) reduction, into value-added multicarbon species is a challenge to addressing global energy demands and climate change. Here in this paper, we report a modular synthetic approach for aqueous electrochemical CO reduction to carbon-carbon coupled products via self-assembly of supramolecular cages at molecular-materials interfaces. Heterobimetallic cavities formed by face-to-face coordination of thiol-terminated metalloporphyrins to copper electrodes through varying organic struts convert CO to C2 products with high faradaic efficiency (FE = 83% total with 57% to ethanol) and current density (1.34 mA/cm 2) at a potential ofmore » -0.40 V vs RHE. The cage-functionalized electrodes offer an order of magnitude improvement in both selectivity and activity for electrocatalytic carbon fixation compared to parent copper surfaces or copper functionalized with porphyrins in an edge-on orientation.« less
Schlager, Stefanie; Dumitru, Liviu Mihai; Haberbauer, Marianne; Fuchsbauer, Anita; Neugebauer, Helmut; Hiemetsberger, Daniela; Wagner, Annika; Portenkirchner, Engelbert; Sariciftci, Niyazi Serdar
2016-03-21
We present results for direct bio-electrocatalytic reduction of CO2 to C1 products using electrodes with immobilized enzymes. Enzymatic reduction reactions are well known from biological systems where CO2 is selectively reduced to formate, formaldehyde, or methanol at room temperature and ambient pressure. In the past, the use of such enzymatic reductions for CO2 was limited due to the necessity of a sacrificial co-enzyme, such as nicotinamide adenine dinucleotide (NADH), to supply electrons and the hydrogen equivalent. The method reported here in this paper operates without the co-enzyme NADH by directly injecting electrons from electrodes into immobilized enzymes. We demonstrate the immobilization of formate, formaldehyde, and alcohol dehydrogenases on one-and-the-same electrode for direct CO2 reduction. Carbon felt is used as working electrode material. An alginate-silicate hybrid gel matrix is used for the immobilization of the enzymes on the electrode. Generation of methanol is observed for the six-electron reduction with Faradaic efficiencies of around 10%. This method of immobilization of enzymes on electrodes offers the opportunity for electrochemical application of enzymatic electrodes to many reactions in which a substitution of the expensive sacrificial co-enzyme NADH is desired. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
NASA Technical Reports Server (NTRS)
Mulloth, Lila M.; Rosen, Micha; Affleck, David; LeVan, M. Douglas; Wang, Yuan
2005-01-01
The air revitalization system of the International Space Station (ISS) operates in an open loop mode and relies on the resupply of oxygen and other consumables from earth for the life support of astronauts. A compressor is required for delivering the carbon dioxide from a removal assembly to a reduction unit to recover oxygen and thereby dosing the air-loop. We have developed a temperature-swing adsorption compressor (TSAC) that is energy efficient, quiet, and has no rapidly moving parts for performing these tasks. The TSAC is a solid-state compressor that has the capability to remove CO2 from a low- pressure source, and subsequently store, compress, and deliver at a higher pressure as required by a processor. The TSAC is an ideal interface device for CO2 removal and reduction units in the air revitalization loop of a spacecraft for oxygen recovery. This paper discusses the design and testing of a TSAC for carbon dioxide that has application in the ISS and future spacecraft for closing the air revitalization loop.
Coupling molecular catalysts with nanostructured surfaces for efficient solar fuel production
NASA Astrophysics Data System (ADS)
Jin, Tong
Solar fuel generation via carbon dioxide (CO2) reduction is a promising approach to meet the increasing global demand for energy and to minimize the impact of energy consumption on climate change. However, CO2 is thermodynamically stable; its activation often requires the use of appropriate catalysts. In particular, molecular catalysts with well-defined structures and tunability have shown excellent activity in photochemical CO2 reduction. These homogenous catalysts, however, suffer from poor stability under photochemical conditions and difficulty in recycling from the reaction media. Heterogenized molecular catalysts, particularly those prepared by coupling molecular catalysts with solid-state surfaces, have attracted more attention in recent years as potential solutions to address the issues associated with molecular catalysts. In this work, solar CO2 reduction is investigated using systems coupling molecular catalysts with robust nanostructured surfaces. In Chapter 2, heterogenization of macrocyclic cobalt(III) and nickel (II) complexes on mesoporous silica surface was achieved by different methods. Direct ligand derivatization significantly lowered the catalytic activity of Co(III) complex, while grafting the Co(III) complex onto silica surface through Si-O-Co linkage resulted in hybrid catalysts with excellent activity in CO2 reduction in the presence of p-terphenyl as a molecular photosensitizer. An interesting loading effect was observed, in which the optimal activity was achieved at a medium Co(III) surface density. Heterogenization of the Ni(II) complex on silica surface has also been implemented, the poor photocatalytic activity of the hybrid catalyst can be attributed to the intrinsic nature of the homogeneous analogue. This study highlighted the importance of appropriate linking strategies in preparing functional heterogenized molecular catalysts. Coupling molecular complexes with light-harvesting surfaces could avoid the use of expensive molecular photosensitizers. In Chapter 3, effective coupling of the macrocyclic Co(III) complex with titanium dioxide (TiO¬2) nanoparticles was achieved by two deposition methods. The synthesized hybrid photocatalysts were thoroughly characterized with a variety of techniques. Upon UV light irradiation, photoexcited electrons in TiO2 nanoparticles were transferred to the surface Co(III) catalyst for CO2 reduction. Production of carbon monoxide (CO) from CO2 was confirmed by isotope labeling combined with infrared spectroscopy. Deposition of the Co(III) catalyst through Ti-O-Co linkages was essential for the photo-induced electron transfer and CO2-reduction activity using the hybrid photocatalysts. In Chapter 4, molecular Re(I) and Co(II) catalysts were coupled with silicon-based photoelectrodes, including a silicon nanowire (SiNW) photoelectrode, to achieve photoelectrochemical CO2 reduction. Photovoltages between 300-600 mV were obtained using the molecular catalysts on the silicon photoelectrodes. SiNWs exhibited enhanced properties, including significantly higher photovoltages than a planar silicon photoelectrode, the ability to protect one of the molecular catalysts from photo-induced decomposition, and excellent selectivity towards CO production in CO2 reduction. Recent theoretical and experimental work have demonstrated low-energy, binuclear pathways for CO2-to-CO conversion using several molecular catalysts. In such binuclear pathways, two metal centers work cooperatively to achieve two-electron CO2 reduction. Chapter 5 describes our effort to promote the binuclear pathway by grafting the molecular Co(III) catalyst onto silica surfaces. Different linking strategies were attempted to achieve this goal by planting the surface Co(III) sites in close proximity.
Carbon dioxide from coal combustion: Variation with rank of US coal
Quick, J.C.; Glick, D.C.
2000-01-01
Carbon dioxide from combustion of US coal systematically varies with ASTM rank indices, allowing the amount of CO2 produced per net unit of energy to be predicted for individual coals. No single predictive equation is applicable to all coals. Accordingly, we provide one equation for coals above high volatile bituminous rank and another for lower rank coals. When applied to public data for commercial coals from western US mines these equations show a 15% variation of kg CO2 (net GJ)-1. This range of variation suggests reduction of US CO2 emissions is possible by prudent selection of coal for combustion. Maceral and mineral content are shown to slightly affect CO2 emissions from US coal. We also suggest that CO2 emissions increased between 6 and 8% in instances where Midwestern US power plants stopped burning local, high-sulfur bituminous coal and started burning low-sulfur, subbituminous C rank coal from the western US.
Eilert, André; Roberts, F. Sloan; Friebel, Daniel; ...
2016-04-04
Nanostructured copper cathodes are among the most efficient and selective catalysts to date for making multicarbon products from the electrochemical carbon dioxide reduction reaction (CO 2RR). We report an in situ X-ray absorption spectroscopy investigation of the formation of a copper nanocube CO 2RR catalyst with high activity that highly favors ethylene over methane production. The results show that the precursor for the copper nanocube formation is copper(I)-oxide, not copper(I)-chloride as previously assumed. A second route to an electrochemically similar material via a copper(II)–carbonate/hydroxide is also reported. In conclusion, this study highlights the importance of using oxidized copper precursors formore » constructing selective CO 2 reduction catalysts and shows the precursor oxidation state does not affect the electrocatalyst selectivity toward ethylene formation.« less
Regeneration of 2-amino-2-methyl-1-propanol used for carbon dioxide absorption.
Zhang, Pei; Shi, Yao; Wei, Jianwen; Zhao, Wei; Ye, Qing
2008-01-01
To improve the efficiency of the carbon dioxide cycling process and to reduce the regeneration energy consumption, a sterically hindered amine of 2-amino-2-methyl-1-propranol (AMP) was investigated to determine its regeneration behavior as a CO2 absorbent. The CO2 absorption and amine regeneration characteristics were experimentally examined under various operating conditions. The regeneration efficiency increased from 86.2% to 98.3% during the temperature range of 358 to 403 K. The most suitable regeneration temperature for AMP was 383 K, in this experiment condition, and the regeneration efficiency of absorption/regenerationruns descended from 98.3% to 94.0%. A number of heat-stable salts (HSS) could cause a reduction in CO2 absorption capacity and regeneration efficiency. The results indicated that aqueous AMP was easier to regenerate with less loss of absorption capacity than other amines, such as, monoethanolamine (MEA), diethanolamine (DEA), diethylenetriamine (DETA), and N-methyldiethanolamine (MDEA).
NASA Astrophysics Data System (ADS)
Shindell, D. T.
2014-12-01
How can society place a value on clean air? I present a multi-impact economic valuation framework called the Social Cost of Atmospheric Release (SCAR) that extends the Social Cost of Carbon (SCC) used previously for carbon dioxide (CO2) to a broader range of pollutants and impacts. Values consistently incorporate health impacts of air quality along with climate damages. The latter include damages associated with aerosol-induced hydrologic cycle changes that lead to net climate benefits when reducing cooling aerosols. Evaluating a 1% reduction in current global emissions, benefits with a high discount rate are greatest for reductions of co-emitted products of incomplete combustion (PIC), followed by sulfur dioxide (SO2), nitrogen oxides (NOx) and then CO2, ammonia and methane. With a low discount rate, benefits are greatest for CO2 reductions, though the sum of SO2, PIC and methane is substantially larger. These results suggest that efforts to mitigate atmosphere-related environmental damages should target a broad set of emissions including CO2, methane and aerosol/ozone precursors. Illustrative calculations indicate environmental damages are 410-1100 billion yr-1 for current US electricity generation ( 19-46¢ per kWh for coal, 4-24¢ for gas) and 3.80 (-1.80/+2.10) per gallon of gasoline ($4.80 (-3.10/+3.50) per gallon for diesel). These results suggest that total atmosphere-related environmental damages plus generation costs are much greater for coal-fired power than other types of electricity generation, and that damages associated with gasoline vehicles substantially exceed those for electric vehicles.
Chisholm, Jessica M; Pang, Daniel S J
2016-01-01
Exposure to carbon dioxide (CO2) gas as a killing method is aversive and exposure to high concentrations is likely to be painful. Bradycardia during exposure to CO2 is associated with nociception and pain. However, it is unclear if bradycardia occurs before loss of consciousness as definitions of loss of consciousness vary in the literature. The objectives of this study were to explore the relationship between recumbency, loss of righting reflex (LORR) and a quiescent electromyograph as measures of loss of consciousness, and identify the onset of bradycardia in relation to these measures. Our primary hypothesis was that CO2 exposure would result in bradycardia, which would precede LORR. Thirty-two adult, female Sprague-Dawley rats were instrumented with a telemetry device and randomly assigned to one of four killing methods (concentrations of 100% CO2, CO2 (70%)/O2 (30%), isoflurane (5%) and intraperitoneal pentobarbital (200 mg/kg). Time to achieve recumbency, LORR, quiescent electromyograph, isoelectric electrocorticograph, heart rate and apnea were recorded. The general order of progression was recumbency, LORR, quiescent electromyograph, isoelectric electrocorticograph and apnea. Recumbency preceded LORR in the majority of animals (CO2; 7/8, CO2/O2; 8/8, isoflurane; 5/8, pentobarbital; 4/8). Bradycardia occurred before recumbency in the CO2 (p = 0.0002) and CO2/O2 (p = 0.005) groups, with a 50% reduction in heart rate compared to baseline. The slowest (time to apnea) and least consistent killing methods were CO2/O2 (1180 ± 658.1s) and pentobarbital (875 [239 to 4680]s). Bradycardia, and consequently nociception and pain, occurs before loss of consciousness during CO2 exposure. Pentobarbital displayed an unexpected lack of consistency, questioning its classification as an acceptable euthanasia method in rats.
Activation of CO2 by supported Cu clusters.
Iyemperumal, Satish Kumar; Deskins, N Aaron
2017-11-01
Catalytic reduction of carbon dioxide to useful chemicals is a potent way to mitigate this greenhouse gas, but the challenge lies in finding active reduction catalysts. Using density functional theory we studied CO 2 activation over TiO 2 -supported Cu clusters of size 1-4 atoms. The linear to bent transformation of CO 2 is necessary for activation, and we found that all the clusters stabilized bent CO 2 , along with a significant gain of electrons on the CO 2 (indicative of activation). On all the TiO 2 supported Cu clusters, the interfacial sites were found to stabilize the bent CO 2 adsorption, where the active site of adsorption on Cu dimer, trimer and tetramer was on the Cu atom farthest away from the TiO 2 surface. Particularly, the Cu dimer stabilized bent CO 2 very strongly, although this species was found to be unstable on the surface. A synthesis technique that could stabilize the Cu dimer could therefore lead to a very active catalyst. Furthermore we found (using vibrational and charge analysis) that the active sites for the CO 2 activation predominantly had 0 and +1 oxidation states; the oxidation state of Cu is known to directly affect CO 2 reduction activity. Our study shows TiO 2 -supported small Cu clusters can be active catalysts for CO 2 reduction and also provides further motivation for theoretical and experimental studies of metal clusters.
Barton Cole, Emily E.; Baruch, Maor F.; L’Esperance, Robert P.; ...
2014-11-15
A series of substituted pyridiniums were examined for their catalytic ability to electrochemically reduce carbon dioxide to methanol. It is found that in general increased basicity of the nitrogen of the amine and higher LUMO energy of the pyridinium correlate with enhanced carbon dioxide reduction. The highest faradaic yield for methanol production at a platinum electrode was 39 ± 4 % for 4-aminopyridine compared to 22 ± 2 % for pyridine. However, 4-tertbutyl and 4-dimethylamino pyridine showed decreased catalytic behavior, contrary to the enhanced activity associated with the increased basicity and LUMO energy, and suggesting that steric effects also playmore » a significant role in the behavior of pyridinium electrocatalysts. As a result, mechanistic models for the the reaction of the pyridinium with carbon dioxide are considered.« less
NASA Astrophysics Data System (ADS)
Keller, David P.; Lenton, Andrew; Scott, Vivian; Vaughan, Naomi E.; Bauer, Nico; Ji, Duoying; Jones, Chris D.; Kravitz, Ben; Muri, Helene; Zickfeld, Kirsten
2018-03-01
The recent IPCC reports state that continued anthropogenic greenhouse gas emissions are changing the climate, threatening severe, pervasive and irreversible
impacts. Slow progress in emissions reduction to mitigate climate change is resulting in increased attention to what is called geoengineering, climate engineering, or climate intervention - deliberate interventions to counter climate change that seek to either modify the Earth's radiation budget or remove greenhouse gases such as CO2 from the atmosphere. When focused on CO2, the latter of these categories is called carbon dioxide removal (CDR). Future emission scenarios that stay well below 2 °C, and all emission scenarios that do not exceed 1.5 °C warming by the year 2100, require some form of CDR. At present, there is little consensus on the climate impacts and atmospheric CO2 reduction efficacy of the different types of proposed CDR. To address this need, the Carbon Dioxide Removal Model Intercomparison Project (or CDRMIP) was initiated. This project brings together models of the Earth system in a common framework to explore the potential, impacts, and challenges of CDR. Here, we describe the first set of CDRMIP experiments, which are formally part of the 6th Coupled Model Intercomparison Project (CMIP6). These experiments are designed to address questions concerning CDR-induced climate reversibility
, the response of the Earth system to direct atmospheric CO2 removal (direct air capture and storage), and the CDR potential and impacts of afforestation and reforestation, as well as ocean alkalinization.>
DOE Office of Scientific and Technical Information (OSTI.GOV)
Keller, David P.; Lenton, Andrew; Scott, Vivian
The recent IPCC reports state that continued anthropogenic greenhouse gas emissions are changing the climate, threatening severe, pervasive and irreversible impacts. Slow progress in emissions reduction to mitigate climate change is resulting in increased attention to what is called geoengineering, climate engineering, or climate intervention – deliberate interventions to counter climate change that seek to either modify the Earth's radiation budget or remove greenhouse gases such as CO 2 from the atmosphere. When focused on CO 2, the latter of these categories is called carbon dioxide removal (CDR). Future emission scenarios that stay well below 2 °C, and all emissionmore » scenarios that do not exceed 1.5 °C warming by the year 2100, require some form of CDR. At present, there is little consensus on the climate impacts and atmospheric CO 2 reduction efficacy of the different types of proposed CDR. To address this need, the Carbon Dioxide Removal Model Intercomparison Project (or CDRMIP) was initiated. This project brings together models of the Earth system in a common framework to explore the potential, impacts, and challenges of CDR. Here, we describe the first set of CDRMIP experiments, which are formally part of the 6th Coupled Model Intercomparison Project (CMIP6). These experiments are designed to address questions concerning CDR-induced climate reversibility, the response of the Earth system to direct atmospheric CO 2 removal (direct air capture and storage), and the CDR potential and impacts of afforestation and reforestation, as well as ocean alkalinization.>« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Favaro, Marco; Xiao, Hai; Cheng, Tao
A national priority is to convert CO 2 into high-value chemical products such as liquid fuels. Because current electrocatalysts are not adequate, we aim to discover new catalysts by obtaining a detailed understanding of the initial steps of CO 2 electroreduction on copper surfaces, the best current catalysts. Using ambient pressure X-ray photoelectron spectroscopy interpreted with quantum mechanical prediction of the structures and free energies, we show that the presence of a thin suboxide structure below the copper surface is essential to bind the CO 2 in the physisorbed configuration at 298 K, and we show that this suboxide ismore » essential for converting to the chemisorbed CO 2 in the presence of water as the first step toward CO 2 reduction products such as formate and CO. This optimum suboxide leads to both neutral and charged Cu surface sites, providing fresh insights into how to design improved carbon dioxide reduction catalysts.« less
Talhelm, Alan F; Pregitzer, Kurt S; Zak, Donald R
2009-11-01
We repeatedly sampled the surface mineral soil (0-20 cm depth) in three northern temperate forest communities over an 11-year experimental fumigation to understand the effects of elevated carbon dioxide (CO(2)) and/or elevated phyto-toxic ozone (O(3)) on soil carbon (C). After 11 years, there was no significant main effect of CO(2) or O(3) on soil C. However, within the community containing only aspen (Populus tremuloides Michx.), elevated CO(2) caused a significant decrease in soil C content. Together with the observations of increased litter inputs, this result strongly suggests accelerated decomposition under elevated CO(2.) In addition, an initial reduction in the formation of new (fumigation-derived) soil C by O(3) under elevated CO(2) proved to be only a temporary effect, mirroring trends in fine root biomass. Our results contradict predictions of increased soil C under elevated CO(2) and decreased soil C under elevated O(3) and should be considered in models simulating the effects of Earth's altered atmosphere.
21 CFR 868.2480 - Cutaneous carbon dioxide (PcCO 2) monitor.
Code of Federal Regulations, 2013 CFR
2013-04-01
... 21 Food and Drugs 8 2013-04-01 2013-04-01 false Cutaneous carbon dioxide (PcCO 2) monitor. 868... dioxide (PcCO 2) monitor. (a) Identification. A cutaneous carbon dioxide (PcCO2) monitor is a noninvasive... relative changes in a hemodynamically stable patient's cutaneous carbon dioxide tension as an adjunct to...
21 CFR 868.2480 - Cutaneous carbon dioxide (PcCO 2) monitor.
Code of Federal Regulations, 2014 CFR
2014-04-01
... 21 Food and Drugs 8 2014-04-01 2014-04-01 false Cutaneous carbon dioxide (PcCO 2) monitor. 868... dioxide (PcCO 2) monitor. (a) Identification. A cutaneous carbon dioxide (PcCO2) monitor is a noninvasive... relative changes in a hemodynamically stable patient's cutaneous carbon dioxide tension as an adjunct to...
Cho, Dong-Wan; Kwon, Gihoon; Ok, Yong Sik; Kwon, Eilhann E; Song, Hocheol
2017-04-19
In this study, pyrolysis of lignin impregnated with cobalt (Co) was conducted to fabricate a Co-biochar (i.e., Co/lignin biochar) for use as a catalyst for bromate (BrO 3 - ) reduction. Carbon dioxide (CO 2 ) was employed as a reaction medium in the pyrolysis to induce desired effects associated with CO 2 ; (1) the enhanced thermal cracking of volatile organic compounds (VOCs) evolved from the thermal degradation of biomass, and (2) the direct reaction between CO 2 and VOCs, which resulted in the enhanced generation of syngas (i.e., H 2 and CO). This study placed main emphases on three parts: (1) the role of impregnated Co in pyrolysis of lignin in the presence of CO 2 , (2) the characterization of Co/lignin biochar, and (3) evaluation of catalytic capability of Co-lignin biochar in BrO 3 - reduction. The findings from the pyrolysis experiments strongly evidenced that the desired CO 2 effects were strengthened due to catalytic effect of impregnated Co in lignin. For example, the enhanced generation of syngas from pyrolysis of Coimpregnated lignin in CO 2 was more significant than the case without Co impregnation. Moreover, pyrolysis of Coimpregnated lignin in CO 2 led to production of biochar of which surface area (599 m 2 g -1 ) is nearly 100 times greater than the biochar produced in N 2 (6.6 m 2 g -1 ). Co/lignin biochar produced in CO 2 also showed a great performance in catalyzing BrO 3 - reduction as compared to the biochar produced in N 2 .
Well-defined iron catalyst for improved hydrogenation of carbon dioxide and bicarbonate.
Ziebart, Carolin; Federsel, Christopher; Anbarasan, Pazhamalai; Jackstell, Ralf; Baumann, Wolfgang; Spannenberg, Anke; Beller, Matthias
2012-12-26
The most efficient, stable, and easy-to-synthesize non-noble metal catalyst system for the reduction of CO(2) and bicarbonates is presented. In the presence of the iron(II)-fluoro-tris(2-(diphenylphosphino)phenyl)phosphino]tetrafluoroborate complex 3, the hydrogenation of bicarbonates proceeds in good yields with high catalyst productivity and activity (TON > 7500, TOF > 750). High-pressure NMR studies of the hydrogenation of carbon dioxide demonstrate that the corresponding iron-hydridodihydrogen complex 4 is crucial in the catalytic cycle.
The report examines process alternatives for the optimal use of natural gas and biomass for production of fuel-cell vehicle fuel, emphasizing maximum displacement of petroleum and maximum reduction of overall fuel-cycle carbon dioxide (CO2) emissions at least cost. Three routes a...
NASA Astrophysics Data System (ADS)
Yang, Dongxu; Zhang, Huifang; Liu, Yi; Chen, Baozhang; Cai, Zhaonan; Lü, Daren
2017-08-01
Monitoring atmospheric carbon dioxide (CO2) from space-borne state-of-the-art hyperspectral instruments can provide a high precision global dataset to improve carbon flux estimation and reduce the uncertainty of climate projection. Here, we introduce a carbon flux inversion system for estimating carbon flux with satellite measurements under the support of "The Strategic Priority Research Program of the Chinese Academy of Sciences—Climate Change: Carbon Budget and Relevant Issues". The carbon flux inversion system is composed of two separate parts: the Institute of Atmospheric Physics Carbon Dioxide Retrieval Algorithm for Satellite Remote Sensing (IAPCAS), and CarbonTracker-China (CT-China), developed at the Chinese Academy of Sciences. The Greenhouse gases Observing SATellite (GOSAT) measurements are used in the carbon flux inversion experiment. To improve the quality of the IAPCAS-GOSAT retrieval, we have developed a post-screening and bias correction method, resulting in 25%-30% of the data remaining after quality control. Based on these data, the seasonal variation of XCO2 (column-averaged CO2 dry-air mole fraction) is studied, and a strong relation with vegetation cover and population is identified. Then, the IAPCAS-GOSAT XCO2 product is used in carbon flux estimation by CT-China. The net ecosystem CO2 exchange is -0.34 Pg C yr-1 (±0.08 Pg C yr-1), with a large error reduction of 84%, which is a significant improvement on the error reduction when compared with in situ-only inversion.
NASA Astrophysics Data System (ADS)
Ryan, Charles; Mead, Anna; Lakkaraju, Prasad; Kaczur, Jerry; Bennett, Christopher; Dobbins, Tabbetha
Research on conversion of carbon dioxide into chemicals and fuels has the potential to address three problems of global relevance. (a) By removing carbon dioxide from the atmosphere, we are able to reduce the amount of greenhouse gases in the atmosphere, (b) by converting carbon dioxide into fuels, we are providing pathways for renewable energy sources, (c) by converting carbon dioxide into C2 and higher order compounds, and we are able to generate valuable precursors for organic synthesis. Formate salts are formed by the electrochemical reduction of carbon dioxide in aqueous media. However, in order to increase the utilization of carbon dioxide, methods need to be developed for the conversion of formate into compounds containing two carbon atoms such as oxalate or oxalic acid. Recently, we examined the thermal conversion of sodium formate into sodium oxalate utilizing a hydride ion catalyst. The proposed mechanism for this reaction involves the carbon dioxide dianion. Currently at NASA Goddard Space Flight Center.
Forecasting carbon dioxide emissions.
Zhao, Xiaobing; Du, Ding
2015-09-01
This study extends the literature on forecasting carbon dioxide (CO2) emissions by applying the reduced-form econometrics approach of Schmalensee et al. (1998) to a more recent sample period, the post-1997 period. Using the post-1997 period is motivated by the observation that the strengthening pace of global climate policy may have been accelerated since 1997. Based on our parameter estimates, we project 25% reduction in CO2 emissions by 2050 according to an economic and population growth scenario that is more consistent with recent global trends. Our forecasts are conservative due to that we do not have sufficient data to fully take into account recent developments in the global economy. Copyright © 2015 Elsevier Ltd. All rights reserved.
NASA Technical Reports Server (NTRS)
Isenberg, Arnold O.; Cusick, Robert J.
1988-01-01
The direct electrochemical reduction of carbon dioxide (CO2) is achieved without catalysts and at sufficiently high temperatures to avoid carbon formation. The tubular electrolysis cell consists of thin layers of anode, electrolyte, cathode and cell interconnection. The electrolyte is made from yttria-stabilized zirconia which is an oxygen ion conductor at elevated temperatures. Anode and cell interconnection materials are complex oxides and are electronic conductors. The cathode material is a composite metal-ceramic structure. Cell performance characteristics have been determined using varying feed gas compositions and degrees of electrochemical decomposition. Cell test data are used to project the performance of a three-person CO2-electrolysis breadboard system.
Wang, Wan -Hui; Himeda, Yuichiro; Muckerman, James T.; ...
2015-09-03
In this study, carbon dioxide is one of the end products of combustion, and is not a benign component of the atmosphere. The concentration of CO 2 in the atmosphere has reached unprecedented levels and continues to increase owing to an escalating rate of fossil fuel combustion, causing concern about climate change and rising sea levels. In view of the inevitable depletion of fossil fuels, a possible solution to this problem is the recycling of carbon dioxide, possibly captured at its point of generation, to fuels. Researchers in this field are using solar energy for CO 2 activation and utilizationmore » in several ways: (i) so-called artificial photosynthesis using photo-induced electrons; (ii) bulk electrolysis of a CO 2 saturated solution using electricity produced by photovoltaics; (iii) CO 2 hydrogenation using solar-produced H 2; and (iv) the thermochemical reaction of metal oxides at extremely high temperature reached by solar collectors. Since the thermodynamics of CO 2 at high temperature (> 1000 ºC) are quite different from those near room temperature, only chemistry below 200 ºC is discussed in this review.« less
Zhang, Wenjun; Hu, Yi; Ma, Lianbo; Zhu, Guoyin; Wang, Yanrong; Xue, Xiaolan; Chen, Renpeng; Yang, Songyuan
2017-01-01
Abstract The worldwide unrestrained emission of carbon dioxide (CO2) has caused serious environmental pollution and climate change issues. For the sustainable development of human civilization, it is very desirable to convert CO2 to renewable fuels through clean and economical chemical processes. Recently, electrocatalytic CO2 conversion is regarded as a prospective pathway for the recycling of carbon resource and the generation of sustainable fuels. In this review, recent research advances in electrocatalytic CO2 reduction are summarized from both experimental and theoretical aspects. The referred electrocatalysts are divided into different classes, including metal–organic complexes, metals, metal alloys, inorganic metal compounds and carbon‐based metal‐free nanomaterials. Moreover, the selective formation processes of different reductive products, such as formic acid/formate (HCOOH/HCOO−), monoxide carbon (CO), formaldehyde (HCHO), methane (CH4), ethylene (C2H4), methanol (CH3OH), ethanol (CH3CH2OH), etc. are introduced in detail, respectively. Owing to the limited energy efficiency, unmanageable selectivity, low stability, and indeterminate mechanisms of electrocatalytic CO2 reduction, there are still many tough challenges need to be addressed. In view of this, the current research trends to overcome these obstacles in CO2 electroreduction field are summarized. We expect that this review will provide new insights into the further technique development and practical applications of CO2 electroreduction. PMID:29375961
Zhang, Wenjun; Hu, Yi; Ma, Lianbo; Zhu, Guoyin; Wang, Yanrong; Xue, Xiaolan; Chen, Renpeng; Yang, Songyuan; Jin, Zhong
2018-01-01
The worldwide unrestrained emission of carbon dioxide (CO 2 ) has caused serious environmental pollution and climate change issues. For the sustainable development of human civilization, it is very desirable to convert CO 2 to renewable fuels through clean and economical chemical processes. Recently, electrocatalytic CO 2 conversion is regarded as a prospective pathway for the recycling of carbon resource and the generation of sustainable fuels. In this review, recent research advances in electrocatalytic CO 2 reduction are summarized from both experimental and theoretical aspects. The referred electrocatalysts are divided into different classes, including metal-organic complexes, metals, metal alloys, inorganic metal compounds and carbon-based metal-free nanomaterials. Moreover, the selective formation processes of different reductive products, such as formic acid/formate (HCOOH/HCOO - ), monoxide carbon (CO), formaldehyde (HCHO), methane (CH 4 ), ethylene (C 2 H 4 ), methanol (CH 3 OH), ethanol (CH 3 CH 2 OH), etc. are introduced in detail, respectively. Owing to the limited energy efficiency, unmanageable selectivity, low stability, and indeterminate mechanisms of electrocatalytic CO 2 reduction, there are still many tough challenges need to be addressed. In view of this, the current research trends to overcome these obstacles in CO 2 electroreduction field are summarized. We expect that this review will provide new insights into the further technique development and practical applications of CO 2 electroreduction.
TES/Aura L2 Carbon Dioxide (CO2) Nadir V6 (TL2CO2N)
Atmospheric Science Data Center
2018-01-18
TES/Aura L2 Carbon Dioxide (CO2) Nadir (TL2CO2N) News: TES News ... Level: L2 Platform: TES/Aura L2 Carbon Dioxide Spatial Coverage: 5.2 x 8.5 km nadir ... Contact User Services Parameters: Carbon Dioxide Legacy: Retired data product , click here ...
TES/Aura L2 Carbon Dioxide (CO2) Nadir V6 (TL2CO2NS)
Atmospheric Science Data Center
2018-01-22
TES/Aura L2 Carbon Dioxide (CO2) Nadir (TL2CO2NS) News: TES News ... Level: L2 Platform: TES/Aura L2 Carbon Dioxide Spatial Coverage: 5.3 x 8.5 km nadir ... Contact ASDC User Services Parameters: Carbon Dioxide Legacy: Retired data product , click here ...
DOE Office of Scientific and Technical Information (OSTI.GOV)
Not Available
2008-10-01
The U.S. Department of Energy?s Wind Powering America Program is committed to educating state-level policymakers and other stakeholders about the economic, CO2 emissions, and water conservation impacts of wind power. This analysis highlights the expected impacts of 1000 MW of wind power in Maine. Although construction and operation of 1000 MW of wind power is a significant effort, six states have already reached the 1000-MW mark. We forecast the cumulative economic benefits from 1000 MW of development in Maine to be $1.3 billion, annual CO2 reductions are estimated at 2.8 million tons, and annual water savings are 1,387 million gallons.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Not Available
2008-10-01
The U.S. Department of Energy?s Wind Powering America Program is committed to educating state-level policymakers and other stakeholders about the economic, CO2 emissions, and water conservation impacts of wind power. This analysis highlights the expected impacts of 1000 MW of wind power in Wisconsin. Although construction and operation of 1000 MW of wind power is a significant effort, six states have already reached the 1000-MW mark. We forecast the cumulative economic benefits from 1000 MW of development in Wisconsin to be $1.1 billion, annual CO2 reductions are estimated at 3.2 million tons, and annual water savings are 1,476 million gallons.
Abiotic CO2 reduction during geologic carbon sequestration facilitated by Fe(II)-bearing minerals
NASA Astrophysics Data System (ADS)
Nielsen, L. C.; Maher, K.; Bird, D. K.; Brown, G. E.; Thomas, B.; Johnson, N. C.; Rosenbauer, R. J.
2012-12-01
Redox reactions involving subsurface minerals and fluids and can lead to the abiotic generation of hydrocarbons from CO2 under certain conditions. Depleted oil reservoirs and saline aquifers targeted for geologic carbon sequestration (GCS) can contain significant quantities of minerals such as ferrous chlorite, which could facilitate the abiotic reduction of carbon dioxide to n-carboxylic acids, hydrocarbons, and amorphous carbon (C0). If such reactions occur, the injection of supercritical CO2 (scCO2) could significantly alter the oxidation state of the reservoir and cause extensive reorganization of the stable mineral assemblage via dissolution and reprecipitation reactions. Naturally occurring iron oxide minerals such as magnetite are known to catalyze CO2 reduction, resulting in the synthesis of organic compounds. Magnetite is thermodynamically stable in Fe(II) chlorite-bearing mineral assemblages typical of some reservoir formations. Thermodynamic calculations demonstrate that GCS reservoirs buffered by the chlorite-kaolinite-carbonate(siderite/magnesite)-quartz assemblage favor the reduction of CO2 to n-carboxylic acids, hydrocarbons, and C0, although the extent of abiotic CO2 reduction may be kinetically limited. To investigate the rates of abiotic CO2 reduction in the presence of magnetite, we performed batch abiotic CO2 reduction experiments using a Dickson-type rocking hydrothermal apparatus at temperatures (373 K) and pressures (100 bar) within the range of conditions relevant to GCS. Blank experiments containing CO2 and H2 were used to rule out the possibility of catalytic activity of the experimental apparatus. Reaction of brine-suspended magnetite nanoparticles with scCO2 at H2 partial pressures typical of reservoir rocks - up to 100 and 0.1 bars respectively - was used to investigate the kinetics of magnetite-catalyzed abiotic CO2 reduction. Later experiments introducing ferrous chlorite (ripidolite) were carried out to determine the potential for heterogeneous catalysis in GCS systems.
21 CFR 868.2480 - Cutaneous carbon dioxide (PcCO2) monitor.
Code of Federal Regulations, 2011 CFR
2011-04-01
... 21 Food and Drugs 8 2011-04-01 2011-04-01 false Cutaneous carbon dioxide (PcCO2) monitor. 868.2480... (CONTINUED) MEDICAL DEVICES ANESTHESIOLOGY DEVICES Monitoring Devices § 868.2480 Cutaneous carbon dioxide (PcCO2) monitor. (a) Identification. A cutaneous carbon dioxide (PcCO2) monitor is a noninvasive heated...
[Ni III(OMe)]-mediated reductive activation of CO 2 affording a Ni(κ 1-OCO) complex
Chiou, Tzung -Wen; Tseng, Yen -Ming; Lu, Tsai -Te; ...
2016-02-24
Here, carbon dioxide is expected to be employed as an inexpensive and potential feedstock of C 1 sources for the mass production of valuable chemicals and fuel. Versatile chemical transformations of CO 2, i.e. insertion of CO 2 producing bicarbonate/acetate/formate, cleavage of CO 2 yielding μ-CO/μ-oxo transition-metal complexes, and electrocatalytic reduction of CO 2 affording CO/HCOOH/CH 3OH/CH 4/C 2H 4/oxalate were well documented. Herein, we report a novel pathway for the reductive activation of CO 2 by the [Ni III(OMe)(P(C 6H 3-3-SiMe 3-2-S) 3)] – complex, yielding the [Ni III(κ 1-OCO˙ –)(P(C 6H 3-3-SiMe 3-2-S) 3)] – complex. The formationmore » of this unusual Ni III(κ 1-OCO ˙–) complex was characterized by single-crystal X-ray diffraction, EPR, IR, SQUID, Ni/S K-edge X-ray absorption spectroscopy, and Ni valence-to-core X-ray emission spectroscopy. The inertness of the analogous complexes [Ni III(SPh)], [Ni II(CO)], and [Ni II(N 2H 4)] toward CO 2, in contrast, demonstrates that the ionic [Ni III(OMe)] core attracts the binding of weak σ-donor CO 2 and triggers the subsequent reduction of CO 2 by the nucleophilic [OMe] – in the immediate vicinity. This metal–ligand cooperative activation of CO 2 may open a novel pathway promoting the subsequent incorporation of CO 2 in the buildup of functionalized products.« less
NASA Technical Reports Server (NTRS)
James, John T.; Meyers, Valerie E.; Sipes, Walter; Scully, Robert R.; Matty, Christopher M.
2011-01-01
Carbon dioxide (CO2) removal is one of the primary functions of the International Space Station (ISS) atmosphere revitalization systems. Primary CO2 removal is via the ISS s two Carbon Dioxide Removal Assemblies (CDRAs) and the Russian carbon dioxide removal assembly (Vozdukh); both of these systems are regenerable, meaning that their CO2 removal capacity theoretically remains constant as long as the system is operating. Contingency CO2 removal capability is provided by lithium hydroxide (LiOH) canisters, which are consumable, meaning that their CO2 removal capability disappears once the resource is used. With the advent of 6 crew ISS operations, experience showing that CDRA failures are not uncommon, and anecdotal association of crew symptoms with CO2 values just above 4 mmHg, the question arises: How much lower do we keep CO2 levels to minimize the risk to crew health and performance, and what will the operational cost to the CDRAs be to do it? The primary crew health concerns center on the interaction of increased intracranial pressure from fluid shifts and the increased intracranial blood flow induced by CO2. Typical acute symptoms include headache, minor visual disturbances, and subtle behavioral changes. The historical database of CO2 exposures since the beginning of ISS operations has been compared to the incidence of crew symptoms reported in private medical conferences. We have used this database in an attempt to establish an association between the CO2 levels and the risk of crew symptoms. This comparison will answer the question of the level needed to protect the crew from acute effects. As for the second part of the question, operation of the ISS s regenerable CO2 removal capability reduces the limited life of constituent parts. It also consumes limited electrical power and thermal control resources. Operation of consumable CO2 removal capability (LiOH) uses finite consumable materials, which must be replenished in the long term. Therefore, increased CO2 removal means increased resource use, with increased logistical capability to maintain necessary resources on board ISS. We must strike a balance between sufficiently low CO2 levels to maintain crew health and CO2 levels which are operationally feasible for the ISS program
Electrochemical carbon dioxide concentrator advanced technology tasks
NASA Technical Reports Server (NTRS)
Schneider, J. J.; Schubert, F. H.; Hallick, T. M.; Woods, R. R.
1975-01-01
Technology advancement studies are reported on the basic electrochemical CO2 removal process to provide a basis for the design of the next generation cell, module and subsystem hardware. An Advanced Electrochemical Depolarized Concentrator Module (AEDCM) is developed that has the characteristics of low weight, low volume, high CO2, removal, good electrical performance and low process air pressure drop. Component weight and noise reduction for the hardware of a six man capacity CO2 collection subsystem was developed for the air revitalization group of the Space Station Prototype (SSP).
Bhowmik, Arghya; Vegge, Tejs; Hansen, Heine A
2016-11-23
A detailed understanding of the electrochemical reduction of CO 2 into liquid fuels on rutile metal oxide surfaces is developed by using DFT calculations. We consider oxide overlayer structures on RuO 2 (1 1 0) surfaces as model catalysts to elucidate the trends and limitations in the CO 2 reduction reaction (CO2RR) based on thermodynamic analysis. We aim to specify the requirements for CO2RR catalysts to establish adsorbate scaling relations and use these to derive activity volcanoes. Computational results show that the OH* binding free energy is a good descriptor of the thermodynamic limitations and it defines the left leg of the activity volcano for CO2RR. HCOOH* is a key intermediate for products formed through further reduction, for example, methanediol, methanol, and methane. The surfaces that do not bind HCOOH* are selective towards formic acid (HCOOH) production, but hydrogen evolution limits their suitability. We determine the ideal binding free energy for H* and OH* to facilitate selective CO2RR over H 2 /CO evolution to be ΔG B [H]>0.5 eV and -0.5 eV<ΔG B [OH]<0.1 eV. The Re-containing overlayers considered in this work display excellent promise for selectivity, although they are active at a highly reducing potential. © 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.
CO 2-scrubbing and methanation as purification system for PEFC
NASA Astrophysics Data System (ADS)
Ledjeff-Hey, K.; Roes, J.; Wolters, R.
Hydrogen is usually produced by steam reforming of natural gas in large-scale processes. The reformate consists of hydrogen, carbon dioxide, carbon monoxide, and residues of hydrocarbons. Since the anode catalyst of a polymer electrolyte membrane fuel cell (PEFC) is usually based on platinum, which is easily poisoned by carbon monoxide, the conditioned feed gas should contain less than 100 ppmv CO, and preferably, less than 10 ppmv. Depending on the design and operating conditions of the hydrogen production process, the CO content of a typical reformate gas, even after the CO shift reactor may be in the range of 0.2-1.0 vol.%; this is far higher than a PEFC can tolerate. A CO management system is required to lower the CO concentration to acceptable levels. In many cases, the CO purification system consists of a combination of physical or chemical processes to achieve the necessary reduction in CO content. A promising alternative for hydrogen purification is a combined process consisting of a carbon dioxide scrubber with subsequent methanation to reduce the carbon monoxide content to an acceptable level of less than 10 ppmv.
NASA Astrophysics Data System (ADS)
Zhang, Zhaoguo; Huang, Zhengfeng; Cheng, Xudong; Wang, Qingli; Chen, Yi; Dong, Peimei; Zhang, Xiwen
2015-11-01
The influence of nitrogen-source on the photocatalytic properties of nitrogen-doped titanium dioxide is herein first investigated from the perspective of the chemical bond form of the nitrogen element in the nitrogen-source. The definitive role of groups such as Nsbnd N from the nitrogen-source on the surface of as-prepared samples in the selectivity of the dominant product of photocatalytic reduction is demonstrated. Well-crystallized one-dimensional Nsbnd TiO2 nanorod arrays with a preferred orientation of the rutile (3 1 0) facet are manufactured via a hydrothermal treatment using hydrazine and ammonia variously as the source of nitrogen. Significant selectivity of the dominant reduced products has been exhibited for Nsbnd TiO2 prepared from different nitrogen-sources in carbon dioxide photocatalytic reduction under visible light illumination. CH4 is the main product with N2H4-doped Nsbnd TiO2, while CO is the main product with NH3-doped Nsbnd TiO2, which can be attributed to the existence of the reducing Nsbnd N groups in the N2H4-doped Nsbnd TiO2 surfaces after the hydrothermal treatment. Compared with the approaches previously reported, the facile one-step route utilized here accomplishes the fabrication of Nsbnd TiO2 possessing visible-light activity and attainment of selectivity of dominant photocatalytic reduction product simultaneously by choosing a nitrogen-source with appropriate chemical bond form, which provides a completely new approach to understanding the effects of doping treatment on photocatalytic properties.
Opitz, Alexander K; Nenning, Andreas; Rameshan, Christoph; Kubicek, Markus; Götsch, Thomas; Blume, Raoul; Hävecker, Michael; Knop-Gericke, Axel; Rupprechter, Günther; Klötzer, Bernhard; Fleig, Jürgen
2017-10-18
Any substantial move of energy sources from fossil fuels to renewable resources requires large scale storage of excess energy, for example, via power to fuel processes. In this respect electrochemical reduction of CO 2 may become very important, since it offers a method of sustainable CO production, which is a crucial prerequisite for synthesis of sustainable fuels. Carbon dioxide reduction in solid oxide electrolysis cells (SOECs) is particularly promising owing to the high operating temperature, which leads to both improved thermodynamics and fast kinetics. Additionally, compared to purely chemical CO formation on oxide catalysts, SOECs have the outstanding advantage that the catalytically active oxygen vacancies are continuously formed at the counter electrode, and move to the working electrode where they reactivate the oxide surface without the need of a preceding chemical (e.g., by H 2 ) or thermal reduction step. In the present work, the surface chemistry of (La,Sr)FeO 3-δ and (La,Sr)CrO 3-δ based perovskite-type electrodes was studied during electrochemical CO 2 reduction by means of near-ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) at SOEC operating temperatures. These measurements revealed the formation of a carbonate intermediate, which develops on the oxide surface only upon cathodic polarization (i.e., under sufficiently reducing conditions). The amount of this adsorbate increases with increasing oxygen vacancy concentration of the electrode material, thus suggesting vacant oxygen lattice sites as the predominant adsorption sites for carbon dioxide. The correlation of carbonate coverage and cathodic polarization indicates that an electron transfer is required to form the carbonate and thus to activate CO 2 on the oxide surface. The results also suggest that acceptor doped oxides with high electron concentration and high oxygen vacancy concentration may be particularly suited for CO 2 reduction. In contrast to water splitting, the CO 2 electrolysis reaction was not significantly affected by metallic particles, which were exsolved from the perovskite electrodes upon cathodic polarization. Carbon formation on the electrode surface was only observed under very strong cathodic conditions, and the carbon could be easily removed by retracting the applied voltage without damaging the electrode, which is particularly promising from an application point of view.
2017-01-01
Any substantial move of energy sources from fossil fuels to renewable resources requires large scale storage of excess energy, for example, via power to fuel processes. In this respect electrochemical reduction of CO2 may become very important, since it offers a method of sustainable CO production, which is a crucial prerequisite for synthesis of sustainable fuels. Carbon dioxide reduction in solid oxide electrolysis cells (SOECs) is particularly promising owing to the high operating temperature, which leads to both improved thermodynamics and fast kinetics. Additionally, compared to purely chemical CO formation on oxide catalysts, SOECs have the outstanding advantage that the catalytically active oxygen vacancies are continuously formed at the counter electrode, and move to the working electrode where they reactivate the oxide surface without the need of a preceding chemical (e.g., by H2) or thermal reduction step. In the present work, the surface chemistry of (La,Sr)FeO3−δ and (La,Sr)CrO3−δ based perovskite-type electrodes was studied during electrochemical CO2 reduction by means of near-ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) at SOEC operating temperatures. These measurements revealed the formation of a carbonate intermediate, which develops on the oxide surface only upon cathodic polarization (i.e., under sufficiently reducing conditions). The amount of this adsorbate increases with increasing oxygen vacancy concentration of the electrode material, thus suggesting vacant oxygen lattice sites as the predominant adsorption sites for carbon dioxide. The correlation of carbonate coverage and cathodic polarization indicates that an electron transfer is required to form the carbonate and thus to activate CO2 on the oxide surface. The results also suggest that acceptor doped oxides with high electron concentration and high oxygen vacancy concentration may be particularly suited for CO2 reduction. In contrast to water splitting, the CO2 electrolysis reaction was not significantly affected by metallic particles, which were exsolved from the perovskite electrodes upon cathodic polarization. Carbon formation on the electrode surface was only observed under very strong cathodic conditions, and the carbon could be easily removed by retracting the applied voltage without damaging the electrode, which is particularly promising from an application point of view. PMID:28933825
Bertini, Federica; Glatz, Mathias; Gorgas, Nikolaus; Stöger, Berthold; Peruzzini, Maurizio; Veiros, Luis F.
2017-01-01
The catalytic reduction of carbon dioxide is of great interest for its potential as a hydrogen storage method and to use carbon dioxide as C-1 feedstock. In an effort to replace expensive noble metal-based catalysts with efficient and cheap earth-abundant counterparts, we report the first example of Mn(i)-catalysed hydrogenation of CO2 to HCOOH. The hydride Mn(i) catalyst [Mn(PNPNH-iPr)(H)(CO)2] showed higher stability and activity than its Fe(ii) analogue. TONs up to 10 000 and quantitative yields were obtained after 24 h using DBU as the base at 80 °C and 80 bar total pressure. At catalyst loadings as low as 0.002 mol%, TONs greater than 30 000 could be achieved in the presence of LiOTf as the co-catalyst, which are among the highest activities reported for base-metal catalysed CO2 hydrogenations to date. PMID:28970889
DOE Office of Scientific and Technical Information (OSTI.GOV)
Bremer, D.J.; Ham, J.M.; Owensby, C.E.
1996-07-01
Increasing concentrations of atmospheric carbon dioxide (CO{sub 2}) may influence plant-water relations in natural and agricultural ecosystems. A tallgrass prairie near Manhattan, KS, was exposed to elevated atmospheric CO{sub 2} using open-top chambers (OTCs). Heat balance sap flow gauges were used to measure transpiration in ironweed [Vernonia baldwini var. interior (Small) Schub.], aC{sub 3}forb, and on individual grass culms of big bluestem (Andropogan geradii Vitman) and indiangrass [Sorghastrum nutans (L>) Nash], both C{sub 4} grasses, in each of three treatments: (1) CE (chamber enriched, 2x ambient CO{sub 2}); (2) CA (chamber ambient, no CO{sub 2} enrichment); and (3) NC (nomore » chamber, no CO{sub 2} enrichment). Sap flow data were coupled with measurements of stomatal conductance, plant/canopy resistance, and whole-chamber evapotranspiration (ET) to determine the effect of elevated CO{sub 2} on water use at different scales. Because of frequent rainfall during the study, all data were collected under well-watered conditions. Comparisons of CE and CA showed that sap flow was reduced by 33% in ironweed, 18% in big bluestem, and 22% in indiangrass under CO{sub 2} enrichment. Whole-chamber ET was reduced by 23 to 27% under CO{sub 2} enrichment. Comparisons of CA and NC showed that the environmental effect of the OTCs caused a 21 to 24% reduction in transpiration. Stomatal conductance decreased from 7.9 to 3.6 mm s{sup {minus}1} in big bluestem and from 5.3 to 3.2 mm s{sup {minus}1} in indiangrass under CO{sub 2} enrichment. Soil water was consistently highest under elevated CO{sub 2}, reflecting the large reductions in transpiration. During sap flow measurements, whole-plant stomatal resistance to water vapor flux in big bluestem increased from 103 to 194 s m{sup {minus}1} under elevated CO{sub 2}. 23 refs., 7 figs., 4 tabs.« less
Duan, Yan-Xin; Meng, Fan-Lu; Liu, Kai-Hua; Yi, Sha-Sha; Li, Si-Jia; Yan, Jun-Min; Jiang, Qing
2018-04-01
Conversion of carbon dioxide (CO 2 ) into valuable chemicals, especially liquid fuels, through electrochemical reduction driven by sustainable energy sources, is a promising way to get rid of dependence on fossil fuels, wherein developing of highly efficient catalyst is still of paramount importance. In this study, as a proof-of-concept experiment, first a facile while very effective protocol is proposed to synthesize amorphous Cu NPs. Unexpectedly, superior electrochemical performances, including high catalytic activity and selectivity of CO 2 reduction to liquid fuels are achieved, that is, a total Faradaic efficiency of liquid fuels can sum up to the maximum value of 59% at -1.4 V, with formic acid (HCOOH) and ethanol (C 2 H 6 O) account for 37% and 22%, respectively, as well as a desirable long-term stability even up to 12 h. More importantly, this work opens a new avenue for improved electroreduction of CO 2 based on amorphous metal catalysts. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Fractional capacity electrolyzer development for CO2 and H2O electrolysis
NASA Technical Reports Server (NTRS)
Wynveen, R. A.
1980-01-01
The electrolyzer module was designed to produce 0.24 kg/d (0.53 lb/d) of breathable oxygen from the electrolysis of metabolic carbon dioxide and water vapor. The fractional capacity electrolyzer module is constructed from three electrochemical tube cells and contains only three critical seals. The module design illustrated an 84 percent reduction in the total number of seals for a one person capacity oxygen generating system based on the solid electrolyte carbon dioxide and water vapor electrolysis concept. The electrolyzer module was successfully endurance tested for 71 days.
NASA Astrophysics Data System (ADS)
Holz, Christian; Siegel, Lori S.; Johnston, Eleanor; Jones, Andrew P.; Sterman, John
2018-06-01
Mitigation scenarios to limit global warming to 1.5 °C or less in 2100 often rely on large amounts of carbon dioxide removal (CDR), which carry significant potential social, environmental, political and economic risks. A precautionary approach to scenario creation is therefore indicated. This letter presents the results of such a precautionary modelling exercise in which the models C-ROADS and En-ROADS were used to generate a series of 1.5 °C mitigation scenarios that apply increasingly stringent constraints on the scale and type of CDR available. This allows us to explore the trade-offs between near-term stringency of emission reductions and assumptions about future availability of CDR. In particular, we find that regardless of CDR assumptions, near-term ambition increase (‘ratcheting’) is required for any 1.5 °C pathway, making this letter timely for the facilitative, or Talanoa, dialogue to be conducted by the UNFCCC in 2018. By highlighting the difference between net and gross reduction rates, often obscured in scenarios, we find that mid-term gross CO2 emission reduction rates in scenarios with CDR constraints increase to levels without historical precedence. This in turn highlights, in addition to the need to substantially increase CO2 reduction rates, the need to improve emission reductions for non-CO2 greenhouse gases. Further, scenarios in which all or part of the CDR is implemented as non-permanent storage exhibit storage loss emissions, which partly offset CDR, highlighting the importance of differentiating between net and gross CDR in scenarios. We find in some scenarios storage loss trending to similar values as gross CDR, indicating that gross CDR would have to be maintained simply to offset the storage losses of CO2 sequestered earlier, without any additional net climate benefit.
Carbon Dioxide Emissions Effects of Grid-Scale Electricity Storage in a Decarbonizing Power System
Craig, Michael T.; Jaramillo, Paulina; Hodge, Bri-Mathias
2018-01-03
While grid-scale electricity storage (hereafter 'storage') could be crucial for deeply decarbonizing the electric power system, it would increase carbon dioxide (CO 2) emissions in current systems across the United States. To better understand how storage transitions from increasing to decreasing system CO 2 emissions, we quantify the effect of storage on operational CO 2 emissions as a power system decarbonizes under a moderate and strong CO 2 emission reduction target through 2045. Under each target, we compare the effect of storage on CO 2 emissions when storage participates in only energy, only reserve, and energy and reserve markets. Wemore » conduct our study in the Electricity Reliability Council of Texas (ERCOT) system and use a capacity expansion model to forecast generator fleet changes and a unit commitment and economic dispatch model to quantify system CO 2 emissions with and without storage. We find that storage would increase CO 2 emissions in the current ERCOT system, but would decrease CO 2 emissions in 2025 through 2045 under both decarbonization targets. Storage reduces CO 2 emissions primarily by enabling gas-fired generation to displace coal-fired generation, but also by reducing wind and solar curtailment. We further find that the market in which storage participates drives large differences in the magnitude, but not the direction, of the effect of storage on CO 2 emissions.« less
Carbon Dioxide Emissions Effects of Grid-Scale Electricity Storage in a Decarbonizing Power System
DOE Office of Scientific and Technical Information (OSTI.GOV)
Craig, Michael T.; Jaramillo, Paulina; Hodge, Bri-Mathias
While grid-scale electricity storage (hereafter 'storage') could be crucial for deeply decarbonizing the electric power system, it would increase carbon dioxide (CO 2) emissions in current systems across the United States. To better understand how storage transitions from increasing to decreasing system CO 2 emissions, we quantify the effect of storage on operational CO 2 emissions as a power system decarbonizes under a moderate and strong CO 2 emission reduction target through 2045. Under each target, we compare the effect of storage on CO 2 emissions when storage participates in only energy, only reserve, and energy and reserve markets. Wemore » conduct our study in the Electricity Reliability Council of Texas (ERCOT) system and use a capacity expansion model to forecast generator fleet changes and a unit commitment and economic dispatch model to quantify system CO 2 emissions with and without storage. We find that storage would increase CO 2 emissions in the current ERCOT system, but would decrease CO 2 emissions in 2025 through 2045 under both decarbonization targets. Storage reduces CO 2 emissions primarily by enabling gas-fired generation to displace coal-fired generation, but also by reducing wind and solar curtailment. We further find that the market in which storage participates drives large differences in the magnitude, but not the direction, of the effect of storage on CO 2 emissions.« less
Carbon dioxide emissions effects of grid-scale electricity storage in a decarbonizing power system
NASA Astrophysics Data System (ADS)
Craig, Michael T.; Jaramillo, Paulina; Hodge, Bri-Mathias
2018-01-01
While grid-scale electricity storage (hereafter ‘storage’) could be crucial for deeply decarbonizing the electric power system, it would increase carbon dioxide (CO2) emissions in current systems across the United States. To better understand how storage transitions from increasing to decreasing system CO2 emissions, we quantify the effect of storage on operational CO2 emissions as a power system decarbonizes under a moderate and strong CO2 emission reduction target through 2045. Under each target, we compare the effect of storage on CO2 emissions when storage participates in only energy, only reserve, and energy and reserve markets. We conduct our study in the Electricity Reliability Council of Texas (ERCOT) system and use a capacity expansion model to forecast generator fleet changes and a unit commitment and economic dispatch model to quantify system CO2 emissions with and without storage. We find that storage would increase CO2 emissions in the current ERCOT system, but would decrease CO2 emissions in 2025 through 2045 under both decarbonization targets. Storage reduces CO2 emissions primarily by enabling gas-fired generation to displace coal-fired generation, but also by reducing wind and solar curtailment. We further find that the market in which storage participates drives large differences in the magnitude, but not the direction, of the effect of storage on CO2 emissions.
Modeling of sonochemistry in water in the presence of dissolved carbon dioxide.
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.
Intramolecular B/N frustrated Lewis pairs and the hydrogenation of carbon dioxide.
Courtemanche, Marc-André; Pulis, Alexander P; Rochette, Étienne; Légaré, Marc-André; Stephan, Douglas W; Fontaine, Frédéric-Georges
2015-06-18
The FLP species 1-BR2-2-NMe2-C6H4 (R = 2,4,6-Me3C6H2, 2,4,5-Me3C6H2) reacts with H2 in sequential hydrogen activation and protodeborylation reactions to give (1-BH2-2-NMe2-C6H4)2. While reacts with H2/CO2 to give formyl, acetal and methoxy-derivatives, reacts with H2/CO2 to give C6H4(NMe2)(B(2,4,5-Me3C6H2)O)2CH2. The mechanism of CO2 reduction is considered.
Multi-stage catalyst systems and uses thereof
Ozkan, Umit S [Worthington, OH; Holmgreen, Erik M [Columbus, OH; Yung, Matthew M [Columbus, OH
2009-02-10
Catalyst systems and methods provide benefits in reducing the content of nitrogen oxides in a gaseous stream containing nitric oxide (NO), hydrocarbons, carbon monoxide (CO), and oxygen (O.sub.2). The catalyst system comprises an oxidation catalyst comprising a first metal supported on a first inorganic oxide for catalyzing the oxidation of NO to nitrogen dioxide (NO.sub.2), and a reduction catalyst comprising a second metal supported on a second inorganic oxide for catalyzing the reduction of NO.sub.2 to nitrogen (N.sub.2).
Carbon Dioxide Reduction Post-Processing Sub-System Development
NASA Technical Reports Server (NTRS)
Abney, Morgan B.; Miller, Lee A.; Greenwood, Zachary; Barton, Katherine
2012-01-01
The state-of-the-art Carbon Dioxide (CO2) Reduction Assembly (CRA) on the International Space Station (ISS) facilitates the recovery of oxygen from metabolic CO2. The CRA utilizes the Sabatier process to produce water with methane as a byproduct. The methane is currently vented overboard as a waste product. Because the CRA relies on hydrogen for oxygen recovery, the loss of methane ultimately results in a loss of oxygen. For missions beyond low earth orbit, it will prove essential to maximize oxygen recovery. For this purpose, NASA is exploring an integrated post-processor system to recover hydrogen from CRA methane. The post-processor, called a Plasma Pyrolysis Assembly (PPA) partially pyrolyzes methane to recover hydrogen with acetylene as a byproduct. In-flight operation of post-processor will require a Methane Purification Assembly (MePA) and an Acetylene Separation Assembly (ASepA). Recent efforts have focused on the design, fabrication, and testing of these components. The results and conclusions of these efforts will be discussed as well as future plans.
Taxing pollution instead of labor: Is it a prudent CO[sub 2] reduction policy
DOE Office of Scientific and Technical Information (OSTI.GOV)
Sanghi, A.K.; Joseph, A.L.
Any serious attempt to reduce carbon dioxide emissions will require reductions from all sectors of the economy. The authors believe that top-down approaches to a carbon tax will generate heavy excess revenues, thus causing administrative and equity problems. They suggest that a better approach, which was espoused by Vice President Gore, could come through a targeted trust fund approach.
Push or Pull? Proton Responsive Ligand Effects in Rhenium Tricarbonyl CO 2 Reduction Catalysts
Manbeck, Gerald F.; Muckerman, James T.; Szalda, David J.; ...
2015-02-19
Proton responsive ligands offer control of catalytic reactions through modulation of pH-dependent properties, second coordination sphere stabilization of transition states, or by providing a local proton source for multi-proton, multi-electron reactions. Two fac-[ReI(α-diimine)(CO)₃Cl] complexes with α-diimine = 4,4'- (or 6,6'-) dihydroxy-2,2'-bipyridine (4DHBP and 6DHBP) have been prepared and analyzed as electrocatalysts for reduction of carbon dioxide. Consecutive electrochemical reduction of these complexes yields species identical to those obtained by chemical deprotonation. An energetically feasible mechanism for reductive deprotonation is proposed in which the bpy anion is protonated followed by loss of H₂ and 2H⁺. Cyclic voltammetry reveals a two-electron, three-wavemore » system owing to competing EEC and ECE pathways. The chemical step of the ECE pathway might be attributed to the reductive deprotonation. but cannot be distinguished from chloride dissociation. The rate obtained by digital simulation is approximately 8 s⁻¹. Under CO₂, these competing reactions generate a two-slope catalytic waveform with onset potential of –1.65 V vs Ag/AgCl. Reduction of CO₂ to CO by the [ReI (4DHBP–2H⁺)(CO)₃]⁻ suggests the interaction of CO₂ with the deprotonated species or a third reduction followed by catalysis. Conversely, the reduced form of [Re(6DHBP)(CO)₃Cl] converts CO₂ to CO with a single turnover.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hossain, Md. Sohrab; Nik Ab Rahman, Nik Norulaini; Balakrishnan, Venugopal
2015-04-15
Highlights: • Supercritical carbon dioxide sterilization of clinical solid waste. • Inactivation of bacteria in clinical solid waste using supercritical carbon dioxide. • Reduction of the hazardous exposure of clinical solid waste. • Optimization of the supercritical carbon dioxide experimental conditions. - Abstract: Clinical solid waste (CSW) poses a challenge to health care facilities because of the presence of pathogenic microorganisms, leading to concerns in the effective sterilization of the CSW for safe handling and elimination of infectious disease transmission. In the present study, supercritical carbon dioxide (SC-CO{sub 2}) was applied to inactivate gram-positive Staphylococcus aureus, Enterococcus faecalis, Bacillus subtilis,more » and gram-negative Escherichia coli in CSW. The effects of SC-CO{sub 2} sterilization parameters such as pressure, temperature, and time were investigated and optimized by response surface methodology (RSM). Results showed that the data were adequately fitted into the second-order polynomial model. The linear quadratic terms and interaction between pressure and temperature had significant effects on the inactivation of S. aureus, E. coli, E. faecalis, and B. subtilis in CSW. Optimum conditions for the complete inactivation of bacteria within the experimental range of the studied variables were 20 MPa, 60 °C, and 60 min. The SC-CO{sub 2}-treated bacterial cells, observed under a scanning electron microscope, showed morphological changes, including cell breakage and dislodged cell walls, which could have caused the inactivation. This espouses the inference that SC-CO{sub 2} exerts strong inactivating effects on the bacteria present in CSW, and has the potential to be used in CSW management for the safe handling and recycling-reuse of CSW materials.« less
Methane Post-Processing for Oxygen Loop Closure
NASA Technical Reports Server (NTRS)
Greenwood, Zachary W.; Abney, Morgan B.; Miller, Lee
2016-01-01
State-of-the-art United States Atmospheric Revitalization carbon dioxide (CO2) reduction is based on the Sabatier reaction process, which recovers approximately 50% of the oxygen (O2) from crew metabolic CO2. Oxygen recovery from carbon dioxide is constrained by the limited availability of reactant hydrogen. Post-processing of methane to recover hydrogen with the Umpqua Research Company Plasma Pyrolysis Assembly (PPA) has the potential to further close the Atmospheric Revitalization oxygen loop. The PPA decomposes methane into hydrogen and hydrocarbons, predominantly acetylene, and a small amount of solid carbon. The hydrogen must then be purified before it can be recycled for additional oxygen recovery. Long duration testing and evaluation of a four crew-member sized PPA and a discussion of hydrogen recycling system architectures are presented.
Nitrous oxide emission reduction in temperate biochar-amended soils
NASA Astrophysics Data System (ADS)
Felber, R.; Hüppi, R.; Leifeld, J.; Neftel, A.
2012-01-01
Biochar, a pyrolysis product of organic residues, is an amendment for agricultural soils to improve soil fertility, sequester CO2 and reduce greenhouse gas (GHG) emissions. In highly weathered tropical soils laboratory incubations of soil-biochar mixtures revealed substantial reductions for nitrous oxide (N2O) and carbon dioxide (CO2). In contrast, evidence is scarce for temperate soils. In a three-factorial laboratory incubation experiment two different temperate agricultural soils were amended with green waste and coffee grounds biochar. N2O and CO2 emissions were measured at the beginning and end of a three month incubation. The experiments were conducted under three different conditions (no additional nutrients, glucose addition, and nitrate and glucose addition) representing different field conditions. We found mean N2O emission reductions of 60 % compared to soils without addition of biochar. The reduction depended on biochar type and soil type as well as on the age of the samples. CO2 emissions were slightly reduced, too. NO3- but not NH4+ concentrations were significantly reduced shortly after biochar incorporation. Despite the highly significant suppression of N2O emissions biochar effects should not be transferred one-to-one to field conditions but need to be tested accordingly.
Evaluation and characterization of the methane-carbon dioxide decomposition reaction
NASA Technical Reports Server (NTRS)
Davenport, R. J.; Schubert, F. H.; Shumar, J. W.; Steenson, T. S.
1975-01-01
A program was conducted to evaluate and characterize the carbon dioxide-methane (CO2-CH4) decomposition reaction, i.e., CO2 + CH4 = 2C + 2H2O. The primary objective was to determine the feasibility of applying this reaction at low temperatures as a technique for recovering the oxygen (O2) remaining in the CO2 which exits mixed with CH4 from a Sabatier CO2 reduction subsystem (as part of an air revitalization system of a manned spacecraft). A test unit was designed, fabricated, and assembled for characterizing the performance of various catalysts for the reaction and ultraviolet activation of the CH4 and CO2. The reactor included in the test unit was designed to have sufficient capacity to evaluate catalyst charges of up to 76 g (0.17 lb). The test stand contained the necessary instrumentation and controls to obtain the data required to characterize the performance of the catalysts and sensitizers tested: flow control and measurement, temperature control and measurement, product and inlet gas analysis, and pressure measurement. A product assurance program was performed implementing the concepts of quality control and safety into the program effort.
Thermal analysis, optimization and design of a Martian oxygen production plant
NASA Technical Reports Server (NTRS)
Iyer, Venkatesh A.; Sridhar, K. R.
1991-01-01
The objective is to optimally design the thermal components of a system that uses carbon dioxide (CO2) from the Martian atmosphere to produce oxygen (O2) for spacecraft propulsion and/or life-support. Carbon dioxide is thermally decomposed into carbon monoxide (CO) and O2 followed by the electrochemical separation of O2. The design of the overall system and its various individual components depends on, among other things, the fraction of the stoichiometric yield of O2 that can be realized in the system and the temperature of operation of the electrochemical separation membrane. The analysis indicates that a substantial reduction could be obtained in the mass and power requirements of the system if the unreacted CO2 were to be recycled. The concepts of an optimum temperature of the zirconia cell and impracticality of plant operation at low cell efficiencies are also discussed. The design of the thermal equipment is such that the mass and power requirements of the individual components and of the overall system are optimized.
Examining ruthenium chromophores for the photochemical reduction of CO2 to methanol
NASA Astrophysics Data System (ADS)
Boston, David J.
Our consumption of energy for transportation and electricity has been growing as quickly as our population. As this demand for energy increases we increase our production of carbon dioxide by the burning of fossil fuels to try and meet this increasing demand. A sustainable method to convert carbon dioxide (CO2) to a viable liquid fuel is one potential way in which both the increasing energy demand and increasing CO2 concentration issues can both be helped. Currently such methods being investigated include thermal, electrochemical, and photochemical processes. Because thermal conversion is not an ideal situation because of the requirement of strong reducing agents or extreme conditions such as steam reformation reactions, we need to find better alternatives such as electrochemical and photochemical methods. Both electrochemical and photochemical methods have the ability to be sustainable, however, the vast majority of these systems are limited to producing CO and/or formic acid, with only a few performing deeper reduction to products such formaldehyde, methanol and methane. All of the systems capable of reducing CO2 past two electrons involve either a heterogeneous catalyst (e.g. TiO2) or an electrode. In recent times Bocarsly and coworkers have shown that pyridine was capable of reducing CO2 to methanol through a sequential process of proton and electron transfers. This process seems to start with the formation of a CO2-pyridine adduct in solution that is reduced one more time to form formate/formic acid. The next reduction is a slow process and allows for a buildup of formate in solution leading to a higher formate concentration in solution. The subsequent reductions seem to occur very rapidly and form methanol at good efficiencies. Theoretical work done recently has argued for the necessity of the Pt, Pd, or GaP surface in the electrochemistry. Carter and coworkers have claimed that the surface of the electrode is a necessary part of the catalysis with the pyridinium being only a cocatalyst for the reduction of CO2. However, Musgrave and coworkers predict that the homogeneous reductions can take place with the aid of water molecules in solution. They allow for a PCET process to take place between the CO 2 and the pyridinium radical. This would allow for a second pathway for the catalytic reduction of CO2 to methanol. Work done during this dissertation has shown that the photochemical reduction of carbon dioxide to methanol is possible using pyridine in a similar manner to Bocarsly and coworkers in their electrochemical system. By replacing the electrode with Ru(phen)3Cl2 it is still possible to drive the reaction using excited states of the chromophore to provide the electrons with enough energy to reduce the pyridinium to the radical species. This system has been shown to produce up to 66 BM methanol after 6 hours of irradiation of 470 nm light. Production of formate is also observed, with ~27 mM being observed within the first hour of irradiation. This system was further investigated with the incorporation of the pyridine catalyst into a chromophore system using the complex [Ru(phen)2dppz](PF 6)2, [Ru(phen)2pbtpalpha](PF6) 2, and [Ru(phen)2pbtpbeta](PF6)2. Cyclic voltammetry experiments for these complexes show similar reduction potentials for with ~100 mV difference between them with [Ru(phen)2dppz](PF 6)2 being the most negative and [Ru(phen)2pbtpbeta](PF 6)2 being the most positive. When the electrolyte solution was saturated with CO2 only [Ru(phen)2pbtpalpha](PF 6)2 and [Ru(phen)2pbtpbeta](PF6) 2 showed a response signifying catalysis was taking place. Initial photochemical tests with these complexes showed that [Ru(phen)2pbtpalpha](PF 6)2 seemed to undergo dimer formation in the absence of CO 2 with [Ru(phen)2pbtpbeta](PF6)2 forming a singly reduced species that is oxidized upon introduction of additional CO2. Electrolysis of [Ru(phen)2pbtpbeta](PF6 )2 produces ~900 BM methanol with both CO and formate being produced as well. Photolysis of [Ru(phen)2pbtpbeta](PF6 )2 in DMF with 1 M H2O and 0.1M TEA, no CO formation observed, however, both methanol and formic acid were observed after 1 hours of irradiation with methanol reaching 45 BM, 285 microM formaldehyde and 650 microM formate.
Effects of recent energy system changes on CO2 projections for the United States.
Lenox, Carol S; Loughlin, Daniel H
2017-09-21
Recent projections of future United States carbon dioxide (CO 2 ) emissions are considerably lower than projections made just a decade ago. A myriad of factors have contributed to lower forecasts, including reductions in end-use energy service demands, improvements in energy efficiency, and technological innovations. Policies that have encouraged these changes include renewable portfolio standards, corporate vehicle efficiency standards, smart growth initiatives, revisions to building codes, and air and climate regulations. Understanding the effects of these and other factors can be advantageous as society evaluates opportunities for achieving additional CO 2 reductions. Energy system models provide a means to develop such insights. In this analysis, the MARKet ALlocation (MARKAL) model was applied to estimate the relative effects of various energy system changes that have happened since the year 2005 on CO 2 projections for the year 2025. The results indicate that transformations in the transportation and buildings sectors have played major roles in lowering projections. Particularly influential changes include improved vehicle efficiencies, reductions in projected travel demand, reductions in miscellaneous commercial electricity loads, and higher efficiency lighting. Electric sector changes have also contributed significantly to the lowered forecasts, driven by demand reductions, renewable portfolio standards, and air quality regulations.
NASA Technical Reports Server (NTRS)
Keefe, Anthony D.; Miller, Stanley L.; McDonald, Gene; Bada, Jeffrey
1995-01-01
An autotrophic theory of the origin of metabolism and life has been proposed in which carbon dioxide is reduced by ferrous sulfide and hydrogen sulfide by means of a reversed citric acid cycle, leading to the production of amino acids. Similar processes have been proposed for purine synthesis. Ferrous sulfide is a strong reducing agent in the presence of hydrogen sulfide and can produce hydrogen as well as reduce alkenes, alkynes, and thiols to saturated hydrocarbons and reduce ketones to thiols. However, the reduction of carbon dioxide has not been demonstrated. We show here that no amino acids, purities, or pyrimidines are produced from carbon dioxide with the ferrous sulfide and hydrogen sulfide system. Furthermore, this system does not produce amino acids from carboxylic acids by reductive amination and carboxylation. Thus, the proposed autotrophic theory, using carbon dioxide, ferrous sulfide, and hydrogen sulfide, lacks the robustness needed to be a geological process and is, therefore, unlikely to have played a role In the origin of metabolism or the origin of life.
NASA Technical Reports Server (NTRS)
Keefe, Anthony D.; Miller, Stanley L.; McDonald, Gene; Bada, Jeffrey
1995-01-01
An autotrophic theory of the origin of metabolism and life has been proposed in which carbon dioxide is reduced by ferrous sulfide and hydrogen sulfide by means of a reversed citric acid cycle, leading to the production of amino acids. Similar processes have been proposed for purine synthesis. Ferrous sulfide is a strong reducing agent in the presence of hydrogen sulfide and can produce hydrogen as well as reduce alkenes, alkynes, and thiols to saturated hydrocarbons and reduce ketones to thiols. However, the reduction of carbon dioxide has not been demonstrated. We show here that no amino acids, purines, or pyrimidines are produced from carbon dioxide with the ferrous sulfide and hydrogen sulfide system. Furthermore, this system does not produce amino acids from carboxylic acids by reductive amination and carboxylation. Thus, the proposed autotrophic theory, using carbon dioxide, ferrous sulfide, and hydrogen sulfide, lacks the robustness needed to be a geological process and is, therefore, unlikely to have played a role in the origin of metabolism or the origin of life.
Nichols, Eva M.; Derrick, Jeffrey S.; Nistanaki, Sepand K.; Smith, Peter T.
2018-01-01
The development of catalysts for electrochemical reduction of carbon dioxide offers an attractive approach to transforming this greenhouse gas into value-added carbon products with sustainable energy input. Inspired by natural bioinorganic systems that feature precisely positioned hydrogen-bond donors in the secondary coordination sphere to direct chemical transformations occurring at redox-active metal centers, we now report the design, synthesis, and characterization of a series of iron tetraphenylporphyrin (Fe-TPP) derivatives bearing amide pendants at various positions at the periphery of the metal core. Proper positioning of the amide pendants greatly affects the electrocatalytic activity for carbon dioxide reduction to carbon monoxide. In particular, derivatives bearing proximal and distal amide pendants on the ortho position of the phenyl ring exhibit significantly larger turnover frequencies (TOF) compared to the analogous para-functionalized amide isomers or unfunctionalized Fe-TPP. Analysis of TOF as a function of catalyst standard reduction potential enables first-sphere electronic effects to be disentangled from second-sphere through-space interactions, suggesting that the ortho-functionalized porphyrins can utilize the latter second-sphere property to promote CO2 reduction. Indeed, the distally-functionalized ortho-amide isomer shows a significantly larger through-space interaction than its proximal ortho-amide analogue. These data establish that proper positioning of secondary coordination sphere groups is an effective design element for breaking electronic scaling relationships that are often observed in electrochemical CO2 reduction. PMID:29732079
DOE Office of Scientific and Technical Information (OSTI.GOV)
Andrade, Gabriel; Pistner, Allen; Yapp, Glenn P. A.
2013-01-01
Harnessing of solar energy to drive the reduction of carbon dioxide to fuels requires the development of efficient catalysts that absorb sunlight. In this work, we detail the synthesis, electrochemistry and photophysical properties of a set of homologous fac-ReI(CO)3 complexes containing either an ancillary phenyl (8) or BODIPY (12) substituent. These studies demonstrate that both the electronic properties of the rhenium center and BODIPY chromophore are maintained for these systems. Photolysis studies demonstrate that both assemblies 8 and 12 are competent catalysts for the photochemical reduction of CO2 to CO in DMF using triethanolamine (TEOA) as a sacrificial reductant. Bothmore » these systems display TOFs for photocatalytic CO production upon irradiation with light ( ex 400 nm) of ~5 hr 1 with TON values of approximately 20. Although structural and photophysical measurements demonstrate that electronic coupling between the BODIPY and fac-ReI(CO)3 units is limited for complex 12, this work clearly shows that the photoactive BODIPY moiety is tolerated during catalysis and does not interfere with the observed photochemistry. When taken together, these results provide a clear roadmap for the development of advanced rhenium bipyridine complexes bearing ancillary BODIPY groups for the efficient photocatalytic reduction of CO2 using visible light.« less
NASA Technical Reports Server (NTRS)
Minh, N. Q.; Chung, B. W.; Doshi, R.; Lear, G. R.; Montgomery, K.; Ong, E. T.
1999-01-01
The use of the Martian atmosphere (95% CO2) to produce oxygen (for propellant and life support) can significantly lower the required launch mass and dramatically reduce the total cost for Mars missions. Zirconia electrolysis cells are one of the technologies being considered for oxygen generation from carbon dioxide in Mars In Situ Resource Utilization (ISRU) production plants. The attractive features of the zirconia cell for this application include simple operation and lightweight, low volume system.
Nanostructured transition metal dichalcogenide electrocatalysts for CO2 reduction in ionic liquid
DOE Office of Scientific and Technical Information (OSTI.GOV)
Asadi, M.; Kim, K.; Liu, C.
2016-07-28
Conversion of carbon dioxide (CO2) into fuels is an attractive solution to many energy and environmental challenges. However, the chemical inertness of CO2 renders many electrochemical and photochemical conversion processes inefficient. We report a transition metal dichalcogenide nanoarchitecture for catalytic electrochemical CO2 conversion to carbon monoxide (CO) in an ionic liquid. We found that tungsten diselenide nanoflakes show a current density of 18.95 milliamperes per square centimeter, CO faradaic efficiency of 24%, and CO formation turnover frequency of 0.28 per second at a low overpotential of 54 millivolts. We also applied this catalyst in a light-harvesting artificial leaf platform thatmore » concurrently oxidized water in the absence of any external potential.« less
Increases in desert shrub productivity under elevated carbon dioxide vary with water availability
Housman, D.C.; Naumburg, E.; Huxman, T. E.; Charlet, T.N.; Nowak, R.S.; Smith, S.D.
2006-01-01
Productivity of aridland plants is predicted to increase substantially with rising atmospheric carbon dioxide (CO2) concentrations due to enhancement in plant water-use efficiency (WUE). However, to date, there are few detailed analyses of how intact desert vegetation responds to elevated CO2. From 1998 to 2001, we examined aboveground production, photosynthesis, and water relations within three species exposed to ambient (around 38 Pa) or elevated (55 Pa) CO2 concentrations at the Nevada Desert Free-Air CO2 Enrichment (FACE) Facility in southern Nevada, USA. The functional types sampled - evergreen (Larrea tridentata), drought-deciduous (Ambrosia dumosa), and winter-deciduous shrubs (Krameria erecta) - represent potentially different responses to elevated CO2 in this ecosystem. We found elevated CO2 significantly increased aboveground production in all three species during an anomalously wet year (1998), with relative production ratios (elevated:ambient CO2) ranging from 1.59 (Krameria) to 2.31 (Larrea). In three below-average rainfall years (1999-2001), growth was much reduced in all species, with only Ambrosia in 2001 having significantly higher production under elevated CO2. Integrated photosynthesis (mol CO2 m-2 y-1) in the three species was 1.26-2.03-fold higher under elevated CO2 in the wet year (1998) and 1.32-1.43-fold higher after the third year of reduced rainfall (2001). Instantaneous WUE was also higher in shrubs grown under elevated CO2. The timing of peak canopy development did not change under elevated CO2; for example, there was no observed extension of leaf longevity into the dry season in the deciduous species. Similarly, seasonal patterns in CO2 assimilation did not change, except for Larrea. Therefore, phenological and physiological patterns that characterize Mojave Desert perennials - early-season lags in canopy development behind peak photosynthetic capacity, coupled with reductions in late-season photosynthetic capacity prior to reductions in leaf area - were not significantly affected by elevated CO2. Together, these findings suggest that elevated CO2 can enhance the productivity of Mojave Desert shrubs, but this effect is most pronounced during years with abundant rainfall when soil resources are most available. ?? 2006 Springer Science+Business Media, Inc.
Song, Yang; Peng, Rui; Hensley, Dale K.; ...
2016-09-28
Carbon dioxide is a pollutant, but also a potential carbon source provided an efficient means to convert it to useful products. Herein we report a nanostructured catalyst for the direct electrochemical reduction of dissolved CO 2 to ethanol with high Faradaic efficiency (63%) and high selectivity (84%). The catalyst is comprised of Cu nanoparticle on a highly textured, N-doped graphene film. Detailed electrochemical analysis and complementary DFT calculations indicate a novel mechanism in which multiple active sites, working sequentially, control the coupling of carbon monoxide radicals and mediate the subsequent electrochemical reduction to alcohol.
Understanding the contribution of non-carbon dioxide gases in deep mitigation scenarios
DOE Office of Scientific and Technical Information (OSTI.GOV)
Gernaat, David; Calvin, Katherine V.; Lucas, Paul
2015-07-01
The combined 2010 emissions of methane (CH4), nitrous oxide (N2O) and the fluorinated gasses (F-gas) account for about 20-30% of total emissions and about 30% of radiative forcing. At the moment, most studies looking at reaching ambitious climate targets project the emission of carbon dioxide (CO2) to be reduced to zero (or less) by the end of the century. As for non-CO2 gases, the mitigation potential seem to be more constrained, we find that by the end of the century in the current deep mitigation scenarios non-CO2 emissions could form the lion’s share of remaining greenhouse gas emissions. In ordermore » to support effective climate policy strategies, in this paper we provide a more in-depth look at the role of non-CO2¬ emission sources (CH4, N2O and F-gases) in achieving deep mitigation targets (radiative forcing target of 2.8 W/m2 in 2100). Specifically, we look at the sectorial mitigation potential and the remaining non-CO2 emissions. By including a set of different models, we provide some insights into the associated uncertainty. Most of the remaining methane emissions in 2100 in the climate mitigation scenario come from the livestock sector. Strong reductions are seen in the energy supply sector across all models. For N2O, less reduction potential is seen compared to methane and the sectoral differences are larger between the models. The paper shows that the assumptions on remaining non-CO2 emissions are critical for the feasibility of reaching ambitious climate targets and the associated costs.« less
Enhanced electrocatalytic CO2 reduction via field-induced reagent concentration
NASA Astrophysics Data System (ADS)
Liu, Min; Pang, Yuanjie; Zhang, Bo; de Luna, Phil; Voznyy, Oleksandr; Xu, Jixian; Zheng, Xueli; Dinh, Cao Thang; Fan, Fengjia; Cao, Changhong; de Arquer, F. Pelayo García; Safaei, Tina Saberi; Mepham, Adam; Klinkova, Anna; Kumacheva, Eugenia; Filleter, Tobin; Sinton, David; Kelley, Shana O.; Sargent, Edward H.
2016-09-01
Electrochemical reduction of carbon dioxide (CO2) to carbon monoxide (CO) is the first step in the synthesis of more complex carbon-based fuels and feedstocks using renewable electricity. Unfortunately, the reaction suffers from slow kinetics owing to the low local concentration of CO2 surrounding typical CO2 reduction reaction catalysts. Alkali metal cations are known to overcome this limitation through non-covalent interactions with adsorbed reagent species, but the effect is restricted by the solubility of relevant salts. Large applied electrode potentials can also enhance CO2 adsorption, but this comes at the cost of increased hydrogen (H2) evolution. Here we report that nanostructured electrodes produce, at low applied overpotentials, local high electric fields that concentrate electrolyte cations, which in turn leads to a high local concentration of CO2 close to the active CO2 reduction reaction surface. Simulations reveal tenfold higher electric fields associated with metallic nanometre-sized tips compared to quasi-planar electrode regions, and measurements using gold nanoneedles confirm a field-induced reagent concentration that enables the CO2 reduction reaction to proceed with a geometric current density for CO of 22 milliamperes per square centimetre at -0.35 volts (overpotential of 0.24 volts). This performance surpasses by an order of magnitude the performance of the best gold nanorods, nanoparticles and oxide-derived noble metal catalysts. Similarly designed palladium nanoneedle electrocatalysts produce formate with a Faradaic efficiency of more than 90 per cent and an unprecedented geometric current density for formate of 10 milliamperes per square centimetre at -0.2 volts, demonstrating the wider applicability of the field-induced reagent concentration concept.
NASA Astrophysics Data System (ADS)
Heimann, M.
2014-01-01
Becker et al. (2013) argue that an afforestation of 0.73 × 109 ha with Jatropha curcas plants would generate an additional terrestrial carbon sink of 4.3 PgC yr-1, enough to stabilise the atmospheric mixing ratio of carbon dioxide (CO2) at current levels. However, this is not consistent with the dynamics of the global carbon cycle. Using a well-established global carbon cycle model, the effect of adding such a hypothetical sink leads to a reduction of atmospheric CO2 levels in the year 2030 by 25 ppm compared to a reference scenario. However, the stabilisation of the atmospheric CO2 concentration requires a much larger additional sink or corresponding reduction of anthropogenic emissions.
NASA Astrophysics Data System (ADS)
Heimann, M.
2013-08-01
Becker et al. (2013) argue that an afforestation of 0.73 109 ha with Jatropha curcas plants would generate an additional terrestrial carbon sink of 4.3 PgC yr-1, enough to stabilise the atmospheric mixing ratio of carbon dioxide (CO2) at current levels. However, this is not consistent with the dynamics of the global carbon cycle. Using a well established global carbon cycle model, the effect of adding such a hypothetical sink leads to a reduction of atmospheric CO2 levels in the year 2030 by 25 ppm compared to a reference scenario. However, the stabilisation of the atmospheric CO2 concentration requires a much larger additional sink or corresponding reduction of anthropogenic emissions.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Eilert, André; Roberts, F. Sloan; Friebel, Daniel
Nanostructured copper cathodes are among the most efficient and selective catalysts to date for making multicarbon products from the electrochemical carbon dioxide reduction reaction (CO 2RR). We report an in situ X-ray absorption spectroscopy investigation of the formation of a copper nanocube CO 2RR catalyst with high activity that highly favors ethylene over methane production. The results show that the precursor for the copper nanocube formation is copper(I)-oxide, not copper(I)-chloride as previously assumed. A second route to an electrochemically similar material via a copper(II)–carbonate/hydroxide is also reported. In conclusion, this study highlights the importance of using oxidized copper precursors formore » constructing selective CO 2 reduction catalysts and shows the precursor oxidation state does not affect the electrocatalyst selectivity toward ethylene formation.« less
NASA Astrophysics Data System (ADS)
Norhana Selamat, Siti; Nor, Nik Hisyamudin Muhd; Rashid, Muhammad Hanif Abdul; Fauzi Ahmad, Mohd; Mohamad, Fariza; Ismail, Al Emran; Fahrul Hassan, Mohd; Turan, Faiz Mohd; Zain, Mohd Zamzuri Mohd; Abu Bakar, Elmi; Seiji, Yokoyama
2017-10-01
Climate change, greenhouse gas effect, and global warming is envisioning to turn more awful and more terrible by year. Since the leading cause of global warming is uncontrolled CO2 in atmosphere. The amount of unused steel slag is expected to increment later on, steel industries is one of the mechanical industries that contribute the CO2 emission. That because this businesses deliver carbon in light of powers reductant and substantial volume of steel. The changes of atmosphere these day is truly developing concern and that make steel creator are confronted with test of discovering methods for bringing down CO2 emission. Malaysia is working decidedly in the diminishment of CO2 gas. There are a few techniques in decreasing the amount of CO2 in the air as underlined by the Intergovernmental Panel of Climate Change (IPCC), an organization under the United Country however CCS is an extremely encouraging innovation to moderate CO2 emission in air. Mineral carbonation is another technique to store carbon dioxide permanently, long term stability and vast capacity.
Hwang, Hyojin; Yeon, Young Joo; Lee, Sumi; Choe, Hyunjun; Jang, Min Gee; Cho, Dae Haeng; Park, Sehkyu; Kim, Yong Hwan
2015-06-01
The use of biocatalysts to convert CO2 into useful chemicals is a promising alternative to chemical conversion. In this study, the electro-biocatalytic conversion of CO2 to formate was attempted with a whole cell biocatalyst. Eight species of Methylobacteria were tested for CO2 reduction, and one of them, Methylobacterium extorquens AM1, exhibited an exceptionally higher capability to synthesize formate from CO2 by supplying electrons with electrodes, which produced formate concentrations of up to 60mM. The oxygen stability of the biocatalyst was investigated, and the results indicated that the whole cell catalyst still exhibited CO2 reduction activity even after being exposed to oxygen gas. From the results, we could demonstrate the electro-biocatalytic conversion of CO2 to formate using an obligate aerobe, M. extorquens AM1, as a whole cell biocatalyst without providing extra cofactors or hydrogen gas. This electro-biocatalytic process suggests a promising approach toward feasible way of CO2 conversion to formate. Copyright © 2015 Elsevier Ltd. All rights reserved.
Nitrogenase Reduction of Carbon-Containing Compounds
Seefeldt, Lance C.; Yang, Zhi-Yong; Duval, Simon; Dean, Dennis R.
2013-01-01
Nitrogenase is an enzyme found in many bacteria and archaea that catalyzes biological dinitrogen fixation, the reduction of N2 to NH3, accounting for the major input of fixed nitrogen into the biogeochemical N cycle. In addition to reducing N2 and protons, nitrogenase can reduce a number of small, non-physiological substrates. Among these alternative substrates are included a wide array of carbon containing compounds. These compounds have provided unique insights into aspects of the nitrogenase mechanism. Recently, it was shown that carbon monoxide (CO) and carbon dioxide (CO2) can also be reduced by nitrogenase to yield hydrocarbons, opening new insights into the mechanism of small molecule activation and reduction by this complex enzyme as well as providing clues for the design of novel molecular catalysts. PMID:23597875
Kai, Tianhan; Zhou, Min; Duan, Zhiyao; Henkelman, Graeme A; Bard, Allen J
2017-12-27
The electrocatalytic reduction of CO 2 has been studied extensively and produces a number of products. The initial reaction in the CO 2 reduction is often taken to be the 1e formation of the radical anion, CO 2 •- . However, the electrochemical detection and characterization of CO 2 •- is challenging because of the short lifetime of CO 2 •- , which can dimerize and react with proton donors and even mild oxidants. Here, we report the generation and quantitative determination of CO 2 •- in N,N-dimethylformamide (DMF) with the tip generation/substrate collection (TG/SC) mode of scanning electrochemical microscopy (SECM). CO 2 was reduced at a hemisphere-shaped Hg/Pt ultramicroelectrode (UME) or a Hg/Au film UME, which were utilized as the SECM tips. The CO 2 •- produced can either dimerize to form oxalate within the nanogap between SECM tip and substrate or collected at SECM substrate (e.g., an Au UME). The collection efficiency (CE) for CO 2 •- depends on the distance (d) between the tip and substrate. The dimerization rate (6.0 × 10 8 M -1 s -1 ) and half-life (10 ns) of CO 2 •- can be evaluated by fitting the collection efficiency vs distance curve. The dimerized species of CO 2 •- , oxalate, can also be determined quantitatively. Furthermore, the formal potential (E 0 ') and heterogeneous rate constant (k 0 ) for CO 2 reduction were determined with different quaternary ammonium electrolytes. The significant difference in k 0 is due to a tunneling effect caused by the adsorption of the electrolytes on the electrode surface at negative potentials.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Michael G. McKellar; Manohar S. Sohal; Lila Mulloth
2010-03-01
NASA has been evaluating two closed-loop atmosphere revitalization architectures based on Sabatier and Bosch carbon dioxide, CO2, reduction technologies. The CO2 and steam, H2O, co-electrolysis process is another option that NASA has investigated. Utilizing recent advances in the fuel cell technology sector, the Idaho National Laboratory, INL, has developed a CO2 and H2O co-electrolysis process to produce oxygen and syngas (carbon monoxide, CO and hydrogen, H2 mixture) for terrestrial (energy production) application. The technology is a combined process that involves steam electrolysis, CO2 electrolysis, and the reverse water gas shift (RWGS) reaction. A number of process models have been developedmore » and analyzed to determine the theoretical power required to recover oxygen, O2, in each case. These models include the current Sabatier and Bosch technologies and combinations of those processes with high-temperature co-electrolysis. The cases of constant CO2 supply and constant O2 production were evaluated. In addition, a process model of the hydrogenation process with co-electrolysis was developed and compared. Sabatier processes require the least amount of energy input per kg of oxygen produced. If co-electrolysis replaces solid polymer electrolyte (SPE) electrolysis within the Sabatier architecture, the power requirement is reduced by over 10%, but only if heat recuperation is used. Sabatier processes, however, require external water to achieve the lower power results. Under conditions of constant incoming carbon dioxide flow, the Sabatier architectures require more power than the other architectures. The Bosch, Boudouard with co-electrolysis, and the hydrogenation with co-electrolysis processes require little or no external water. The Bosch and hydrogenation processes produce water within their reactors, which aids in reducing the power requirement for electrolysis. The Boudouard with co-electrolysis process has a higher electrolysis power requirement because carbon dioxide is split instead of water, which has a lower heat of formation. Hydrogenation with co-electrolysis offers the best overall power performance for two reasons: it requires no external water, and it produces its own water, which reduces the power requirement for co-electrolysis.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hsieh, Yu-Chi; Senanayake, Sanjaya D.; Zhang, Yu
2015-09-04
Metallic silver (Ag) is known as an efficient electrocatalyst for the conversion of carbon dioxide (CO 2) to carbon monoxide (CO) in aqueous or nonaqueous electrolytes. However, polycrystalline silver electrocatalysts require significant overpotentials in order to achieve high selectivity toward CO 2 reduction, as compared to the side reaction of hydrogen evolution. Here we report a high-surface-area Ag nanocoral catalyst, fabricated by an oxidation–reduction method in the presence of chloride anions in an aqueous medium, for the electro-reduction of CO 2 to CO with a current efficiency of 95% at the low overpotential of 0.37 V and the current densitymore » of 2 mA cm –2. A lower limit of TOF of 0.4 s –1 and TON > 8.8 × 10 4 (over 72 h) was estimated for the Ag nanocoral catalyst at an overpotential of 0.49 V. The Ag nanocoral catalyst demonstrated a 32-fold enhancement in surface-area-normalized activity, at an overpotential of 0.49 V, as compared to Ag foil. We found that, in addition to the effect on nanomorphology, the adsorbed chloride anions play a critical role in the observed enhanced activity and selectivity of the Ag nanocoral electrocatalyst toward CO 2 reduction. Synchrotron X-ray photoelectron spectroscopy (XPS) studies along with a series of control experiments suggest that the chloride anions, remaining adsorbed on the catalyst surface under electrocatalytic conditions, can effectively inhibit the side reaction of hydrogen evolution and enhance the catalytic performance for CO 2 reduction.« less
Diffusivity of Carbon Dioxide in Aqueous Solutions under Geologic Carbon Sequestration Conditions.
Perera, Pradeep N; Deng, Hang; Schuck, P James; Gilbert, Benjamin
2018-04-26
Accurate assessment of the long-term security of geologic carbon sequestration requires knowledge of the mobility of carbon dioxide in brines under pressure and temperature conditions that prevail in subsurface aquifers. Here, we report Raman spectroscopic measurements of the rate of CO 2 diffusion in water and brines as a function of pressure, salinity, and concentration of CO 2 . In pure water at 50 ± 2 °C and 90 ± 2 bar, we find the diffusion coefficient, D, to be (3.08 ± 0.03) × 10 -9 m 2 /s, a value that is consistent with a recent microfluidic study but lower than earlier PVT measurements. Under reservoir conditions, salinity affects the mobility of CO 2 significantly and D decreased by 45% for a 4 M solution of NaCl. We find significant differences of diffusivity of CO 2 in brines (0-4 M NaCl), in both the absolute values and the trend compared to the Stokes-Einstein prediction under our experimental conditions. We observe that D decreases significantly at the high CO 2 concentrations expected in subsurface aquifers (∼15% reduction at 0.55 mol/kg of CO 2 ) and provides an empirical correction to the commonly reported D values that assume a tracer concentration dependence on diffusivity.
Park, Taehyung; Joo, Hyun-Woo; Kim, Gyeong-Yeong; Kim, Seunghee; Yoon, Sukhwan; Kwon, Tae-Hyuk
2017-01-01
Injecting and storing of carbon dioxide (CO 2 ) in deep geologic formations is considered as one of the promising approaches for geologic carbon storage. Microbial wettability alteration of injected CO 2 is expected to occur naturally by microorganisms indigenous to the geologic formation or microorganisms intentionally introduced to increase CO 2 storage capacity in the target reservoirs. The question as to the extent of microbial CO 2 wettability alteration under reservoir conditions still warrants further investigation. This study investigated the effect of a lipopeptide biosurfactant-surfactin, on interfacial tension (IFT) reduction and contact angle alteration in CO 2 /water/quartz systems under a laboratory setup simulating in situ reservoir conditions. The temporal shifts in the IFT and the contact angle among CO 2 , brine, and quartz were monitored for different CO 2 phases (3 MPa, 30°C for gaseous CO 2 ; 10 MPa, 28°C for liquid CO 2 ; 10 MPa, 37°C for supercritical CO 2 ) upon cultivation of Bacillus subtilis strain ATCC6633 with induced surfactin secretion activity. Due to the secreted surfactin, the IFT between CO 2 and brine decreased: from 49.5 to 30 mN/m, by ∼39% for gaseous CO 2 ; from 28.5 to 13 mN/m, by 54% for liquid CO 2 ; and from 32.5 to 18.5 mN/m, by ∼43% for supercritical CO 2 , respectively. The contact angle of a CO 2 droplet on a quartz disk in brine increased: from 20.5° to 23.2°, by 1.16 times for gaseous CO 2 ; from 18.4° to 61.8°, by 3.36 times for liquid CO 2 ; and from 35.5° to 47.7°, by 1.34 times for supercritical CO 2 , respectively. With the microbially altered CO 2 wettability, improvement in sweep efficiency of injected and displaced CO 2 was evaluated using 2-D pore network model simulations; again the increment in sweep efficiency was the greatest in liquid CO 2 phase due to the largest reduction in capillary factor. This result provides novel insights as to the role of naturally occurring biosurfactants in CO 2 storage and suggests that biostimulation of biosurfactant production may be a feasible technique for enhancement of CO 2 storage capacity.
Park, Taehyung; Joo, Hyun-Woo; Kim, Gyeong-Yeong; Kim, Seunghee; Yoon, Sukhwan; Kwon, Tae-Hyuk
2017-01-01
Injecting and storing of carbon dioxide (CO2) in deep geologic formations is considered as one of the promising approaches for geologic carbon storage. Microbial wettability alteration of injected CO2 is expected to occur naturally by microorganisms indigenous to the geologic formation or microorganisms intentionally introduced to increase CO2 storage capacity in the target reservoirs. The question as to the extent of microbial CO2 wettability alteration under reservoir conditions still warrants further investigation. This study investigated the effect of a lipopeptide biosurfactant—surfactin, on interfacial tension (IFT) reduction and contact angle alteration in CO2/water/quartz systems under a laboratory setup simulating in situ reservoir conditions. The temporal shifts in the IFT and the contact angle among CO2, brine, and quartz were monitored for different CO2 phases (3 MPa, 30°C for gaseous CO2; 10 MPa, 28°C for liquid CO2; 10 MPa, 37°C for supercritical CO2) upon cultivation of Bacillus subtilis strain ATCC6633 with induced surfactin secretion activity. Due to the secreted surfactin, the IFT between CO2 and brine decreased: from 49.5 to 30 mN/m, by ∼39% for gaseous CO2; from 28.5 to 13 mN/m, by 54% for liquid CO2; and from 32.5 to 18.5 mN/m, by ∼43% for supercritical CO2, respectively. The contact angle of a CO2 droplet on a quartz disk in brine increased: from 20.5° to 23.2°, by 1.16 times for gaseous CO2; from 18.4° to 61.8°, by 3.36 times for liquid CO2; and from 35.5° to 47.7°, by 1.34 times for supercritical CO2, respectively. With the microbially altered CO2 wettability, improvement in sweep efficiency of injected and displaced CO2 was evaluated using 2-D pore network model simulations; again the increment in sweep efficiency was the greatest in liquid CO2 phase due to the largest reduction in capillary factor. This result provides novel insights as to the role of naturally occurring biosurfactants in CO2 storage and suggests that biostimulation of biosurfactant production may be a feasible technique for enhancement of CO2 storage capacity. PMID:28744272
Hydrogen storage and delivery: the carbon dioxide - formic acid couple.
Laurenczy, Gábor
2011-01-01
Carbon dioxide and the carbonates, the available natural C1 sources, can be easily hydrogenated into formic acid and formates in water; the rate of this reduction strongly depends on the pH of the solution. This reaction is catalysed by ruthenium(II) pre-catalyst complexes with a large variety of water-soluble phosphine ligands; high conversions and turnover numbers have been realised. Although ruthenium(II) is predominant in these reactions, the iron(II) - tris[(2-diphenylphosphino)-ethyl]phosphine (PP3) complex is also active, showing a new perspective to use abundant and inexpensive iron-based compounds in the CO2 reduction. In the catalytic hydrogenation cycles the in situ formed metal hydride complexes play a key role, their structures with several other intermediates have been proven by multinuclear NMR spectroscopy. In the other hand safe and convenient hydrogen storage and supply is the fundamental question for the further development of the hydrogen economy; and carbon dioxide has been recognised to be a viable H2 vector. Formic acid--containing 4.4 weight % of H2, that is 53 g hydrogen per litre--is suitable for H2 storage; we have shown that in aqueous solutions it can be selectively decomposed into CO-free (CO < 10 ppm) CO2 and H2. The reaction takes place under mild experimental conditions and it is able to generate high pressure H2 (up to 600 bar). The cleavage of HCOOH is catalysed by several hydrophilic Ru(II) phosphine complexes (meta-trisulfonated triphenylphosphine, mTPPTS, being the most efficient one), either in homogeneous systems or as immobilised catalysts. We have also shown that the iron(II)--hydrido tris[(2-diphenylphosphino)ethyl]phosphine complex catalyses with an exceptionally high rate and efficiency (turnover frequency, TOF = 9425 h(-1)mol(-1); turnover number, TON = 92400) the formic acid cleavage, in environmentally friendly propylene carbonate solution, opening the way to use cheap, non-noble metal based catalysts for this reaction, too.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Cook, W.J.; Brown, W.R.; Siwajek, L.
1998-09-01
The project is a landfill gas to energy project rated at about 4 megawatts (electric) at startup, increasing to 8 megawatts over time. The project site is Boului Landfill, near Bucharest, Romania. The project improves regional air quality, reduces emission of greenhouse gases, controls and utilizes landfill methane, and supplies electric power to the local grid. The technical and economic feasibility of pre-treating Boului landfill gas with Acrion`s new landfill gas cleanup technology prior to combustion for power production us attractive. Acrion`s gas treatment provides several benefits to the currently structured electric generation project: (1) increase energy density of landfillmore » gas from about 500 Btu/ft{sup 3} to about 750 Btu/ft{sup 3}; (2) remove contaminants from landfill gas to prolong engine life and reduce maintenance;; (3) recover carbon dioxide from landfill gas for Romanian markets; and (4) reduce emission of greenhouse gases methane and carbon dioxide. Greenhouse gas emissions reduction attributable to successful implementation of the landfill gas to electric project, with commercial liquid CO{sub 2} recovery, is estimated to be 53 million metric tons of CO{sub 2} equivalent of its 15 year life.« less
Meric, Pascal; Yu, Kai Man K; Tsang, Shik Chi
2004-09-28
A new approach of employing metal particles in micelles for the hydrogenation of organic molecules in the presence of fluorinated surfactant and water in supercritical carbon dioxide has very recently been introduced. This is allegedly to deliver many advantages for carrying out catalysis including the use of supercritical carbon dioxide (scCO2) as a greener solvent. Following this preliminary account, the present work aims to provide direct visual evidence on the formation of metal microemulsions and to investigate whether metal located in the soft micellar assemblies could affect reaction selectivity. Synthesis of Pd nanoparticles in perfluorohydrocarboxylate anionic micelles in scCO2 is therefore carried out in a stainless steel batch reactor at 40 degrees C and in a 150 bar CO2/H2 mixture. Homogeneous dispersion of the microemulsion containing Pd nanoparticles in scCO2 is observed through a sapphire window reactor at W0 ratios (molar water-to-surfactant ratios) ranging from 2 to 30. It is also evidenced that the use of micelle assemblies as new metal catalyst nanocarriers could indeed exert a great influence on product selectivity. The hydrogenation of a citral molecule that contains three reducible groups (aldehyde, double bonds at the 2,3-position and the 6,7-position) is studied. An unusually high selectivity toward citronellal (a high regioselectivity toward the reduction of the 2,3-unsaturation) is observed in supercritical carbon dioxide. On the other hand, when the catalysis is carried out in the conventional liquid or vapor phase over the same reaction time, total hydrogenation of the two double bonds is achieved. It is thought that the high kinetic reluctance for double bond hydrogenation of the citral molecule at the hydrophobic end (the 6,7-position) is due to the unique micelle environment that is in close proximity to the metal surface in supercritical carbon dioxide that guides a head-on attack of the molecule toward the core metal particle.
Electrochemical carbon dioxide concentrator subsystem development
NASA Technical Reports Server (NTRS)
Koszenski, E. P.; Heppner, D. B.; Bunnell, C. T.
1986-01-01
The most promising concept for a regenerative CO2 removal system for long duration manned space flight is the Electrochemical CO2 Concentrator (EDC), which allows for the continuous, efficient removal of CO2 from the spacecraft cabin. This study addresses the advancement of the EDC system by generating subsystem and ancillary component reliability data through extensive endurance testing and developing related hardware components such as electrochemical module lightweight end plates, electrochemical module improved isolation valves, an improved air/liquid heat exchanger and a triple redundant relative humidity sensor. Efforts included fabrication and testing the EDC with a Sabatier CO2 Reduction Reactor and generation of data necessary for integration of the EDC into a space station air revitalization system. The results verified the high level of performance, reliability and durability of the EDC subsystem and ancillary hardware, verified the high efficiency of the Sabatier CO2 Reduction Reactor, and increased the overall EDC technology engineering data base. The study concluded that the EDC system is approaching the hardware maturity levels required for space station deployment.
Discovery of a new metal and NAD+-dependent formate dehydrogenase from Clostridium ljungdahlii.
Çakar, M Mervan; Mangas-Sanchez, Juan; Birmingham, William R; Turner, Nicholas J; Binay, Barış
2018-04-21
Over the next decades, with the growing concern of rising atmospheric carbon dioxide (CO 2 ) levels, the importance of investigating new approaches for its reduction becomes crucial. Reclamation of CO 2 for conversion into biofuels represents an alternative and attractive production method that has been studied in recent years, now with enzymatic methods gaining more attention. Formate dehydrogenases (FDHs) are NAD(P)H-dependent oxidoreductases that catalyze the conversion of formate into CO 2 and have been extensively used for cofactor recycling in chemoenzymatic processes. A new FDH from Clostridium ljungdahlii (ClFDH) has been recently shown to possess activity in the reverse reaction: the mineralization of CO 2 into formate. In this study, we show the successful homologous expression of ClFDH in Escherichia coli. Biochemical and kinetic characterization of the enzyme revealed that this homologue also demonstrates activity toward CO 2 reduction. Structural analysis of the enzyme through homology modeling is also presented.
Niu, Dong-jie; Huang, Hui; Dai, Xiao-hu; Zhao, You-cai
2013-01-01
About 20 million tonnes of sludge (with 80% moisture content) is discharged by the sewage treatment plants per year in China, which, if not treated properly, can be a significant source of greenhouse gases (GHGs) emissions. Anaerobic digestion is a conventional sewage sludge treatment method and will continue to be one of the main technologies in the following years. This research has taken into consideration GHGs emissions from typical processes of sludge thickening+anaerobic digestion+dewatering+residue land application in China. Fossil CO(2), biogenic CO(2), CH(4,) and avoided CO(2) as the main objects is discussed respectively. The results show that the total CO(2)-eq is about 1133 kg/t DM (including the biogenic CO(2)), while the net CO(2)-eq is about 372 kg/t DM (excluding the biogenic CO(2)). An anaerobic digestion unit as the main GHGs emission source occupies more than 91% CO(2)-eq of the whole process. The use of biogas is important for achieving carbon dioxide emission reductions, which could reach about 24% of the total CO(2)-eq reduction. Copyright © 2012 Elsevier Ltd. All rights reserved.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Li, Jingtian; Luo, Deliang; Yang, Chengju
2013-07-15
Three copper(II) imidazolate frameworks were synthesized by a hydrothermal (or precipitation) reaction. The catalysts were characterized by X-ray diffraction (XRD), nitrogen adsorption, transmission electron microscopy (TEM), ultraviolet–visible spectroscopy (UV–vis), Fourier transform infrared spectra (FTIR), thermogravimetry (TG). Meanwhile, the photocatalytic activities of the samples for reduction of CO{sub 2} into methanol and degradation of methylene blue (MB) under visible light irradiation were also investigated. The results show that the as-prepared samples exhibit better photocatalytic activities for the reduction of carbon dioxide into methanol with water and degradation of MB under visible light irradiation. The orthorhombic copper(II) imidazolate frameworks with a bandmore » gap of 2.49 eV and green (G) color has the best photocatalytic activity for reduction of CO{sub 2} into methanol, 1712.7 μmol/g over 5 h, which is about three times as large as that of monoclinic copper(II) imidazolate frameworks with a band gap 2.70 eV and blue (J) color. The degradation kinetics of MB over three photocatalysts fitted well to the apparent first-order rate equation and the apparent rate constants for the degradation of MB over G, J and P (with pink color) are 0.0038, 0.0013 and 0.0016 min{sup −1}, respectively. The synergistic effects of smallest band gap and orthorhombic crystal phase structure are the critical factors for the better photocatalytic activities of G. Moreover, three frameworks can also be stable up to 250 °C. The investigation of Cu-based zeolitic imidazolate frameworks maybe provide a design strategy for a new class of photocatalysts applied in degradation of contaminations, reduction of CO{sub 2}, and even water splitting into hydrogen and oxygen under visible light. - Graphical abstract: Carbon dioxide was reduced into methanol with water over copper(II) imidazolate frameworks under visible light irradiation. - Highlights: • Three copper(II) imidazolate frameworks were first applied in the photo-reduction of CO{sub 2}. • The photocatalytic activities of the frameworks depend on their band gap and phase structures. • The photocatalytic activity of orthorhombic frameworks is 3 times that of monoclinic frameworks. • The degradation kinetics of MB over three photocatalysts followed the first-order rate equation. • The largest yield for reduction of CO{sub 2} into methanol on green framworks was 1712.7 μmol/g over 5 h.« less
NASA Technical Reports Server (NTRS)
Rosen, Micha; Mulloth, Lila; Varghese, Mini
2005-01-01
This paper describes the results of long-duration testing of a temperature-swing adsorption compressor that has application in the International Space Station (ISS) and future spacecraft for closing the air revitalization loop. The air revitalization system of the ISS operates in an open loop mode and relies on the resupply of oxygen and other consumables from Earth for the life support of astronauts. A compressor is required for delivering the carbon dioxide from a removal assembly to a reduction unit to recover oxygen and thereby closing the air-loop. The TSAC is a solid-state compressor that has the capability to remove CO2 from a low-pressure source, and subsequently store, compress, and deliver at a higher pressure as required by a processor. The TSAC is an ideal interface device for CO2 removal and reduction units in the air revitalization loop of a spacecraft for oxygen recovery. The TSAC was developed and its operation was successfully verified in integration tests with the flight-like Carbon Dioxide Removal Assembly (CDRA) at Marshall Space Flight Center prior to the long-duration tests. Long-duration tests reveal the impacts of repeated thermal cycling on the compressor components and the adsorbent material.
Dutta, Prabir K [Worthington, OH; Lee, Inhee [Columbus, OH; Akbar, Sheikh A [Hilliard, OH
2011-11-15
The present invention generally relates to carbon dioxide (CO.sub.2) sensors. In one embodiment, the present invention relates to a carbon dioxide (CO.sub.2) sensor that incorporates lithium phosphate (Li.sub.3PO.sub.4) as an electrolyte and sensing electrode comprising a combination of lithium carbonate (Li.sub.2CO.sub.3) and barium carbonate (BaCO.sub.3). In another embodiment, the present invention relates to a carbon dioxide (CO.sub.2) sensor has a reduced sensitivity to humidity due to a sensing electrode with a layered structure of lithium carbonate and barium carbonate. In still another embodiment, the present invention relates to a method of producing carbon dioxide (CO.sub.2) sensors having lithium phosphate (Li.sub.3PO.sub.4) as an electrolyte and sensing electrode comprising a combination of lithium carbonate (Li.sub.2CO.sub.3) and barium carbonate (BaCO.sub.3).
Assessment of the Incentives, Disincentives, and Alternatives for Steel Industry CO2 Reduction
DOE Office of Scientific and Technical Information (OSTI.GOV)
Paul T. Leuchte; DR. John Stubbles; Professor Fruehan
This report presents the results of the third element of a trilogy of studies sponsored by the U.S. Department of Energy's Office of Industrial Technologies on the consumption of energy and the emissions of carbon dioxide in the U.S. steel industry
Morales Quinteros, Luis; Bringué Roque, Josep; Kaufman, David; Artigas Raventós, Antonio
2018-02-24
Important recent insights have emerged regarding the cellular and molecular role of carbon dioxide (CO 2 ) and the effects of hypercapnia. The latter may have beneficial effects in patients with acute lung injury, affording reductions in pulmonary inflammation, lessened oxidative alveolar damage, and the regulation of innate immunity and host defenses by inhibiting the expression of inflammatory cytokines. However, other studies suggest that CO 2 can have deleterious effects upon the lung, reducing alveolar wound repair in lung injury, decreasing the rate of reabsorption of alveolar fluid, and inhibiting alveolar cell proliferation. Clearly, hypercapnia has both beneficial and harmful consequences, and it is important to determine the net effect under specific conditions. The purpose of this review is to describe the immunological and physiological effects of carbon dioxide, considering their potential consequences in patients with acute respiratory failure. Copyright © 2018 Elsevier España, S.L.U. y SEMICYUC. All rights reserved.
Shi, Guodong; Yu, Luo; Ba, Xin; Zhang, Xiaoshu; Zhou, Jianqing; Yu, Ying
2017-08-15
Electrocatalytic conversion of carbon dioxide (CO 2 ) has been considered as an ideal method to simultaneously solve the energy crisis and environmental issue around the world. In this work, ultrasmall Cu nanoparticle interspersed flower-like MoS 2 was successfully fabricated via a facile microwave hydrothermal method. The designed optimal hierarchical Cu/MoS 2 composite not only exhibited remarkably enhanced electronic conductivity and specific surface area but also possessed improved CO 2 adsorption capacity, resulting in a significant increase in overall faradaic efficiency and a 7-fold augmentation of the faradaic efficiency of CH 4 in comparison with bare MoS 2 . In addition, the Cu/MoS 2 composite had superior stability with high efficiency retained for 48 h in the electrochemical process. It is anticipated that the designed Cu/MoS 2 composite electrocatalyst may provide new insights for transition metal sulfides and non-noble particles applied to CO 2 reduction.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Eilert, Andre; Cavalca, Filippo; Roberts, F. Sloan
Copper electrocatalysts derived from an oxide have shown extraordinary electrochemical properties for the carbon dioxide reduction reaction (CO 2RR). Using in situ ambient pressure X-ray photoelectron spectroscopy and quasi in situ electron energy-loss spectroscopy in a transmission electron microscope, we show that there is a substantial amount of residual oxygen in nanostructured, oxide-derived copper electrocatalysts but no residual copper oxide. On the basis of these findings in combination with density functional theory simulations, we propose that residual subsurface oxygen changes the electronic structure of the catalyst and creates sites with higher carbon monoxide binding energy. If such sites are stablemore » under the strongly reducing conditions found in CO 2RR, these findings would explain the high efficiencies of oxide-derived copper in reducing carbon dioxide to multicarbon compounds such as ethylene.« less
Homogeneous Electrocatalytic Reduction of Carbon Dioxide to Carbon Monoxide by Ni(cyclam)
NASA Astrophysics Data System (ADS)
Froehlich, Jesse Dan
The homogeneous electrochemical reduction of CO2 by the molecular catalyst [Ni(cyclam)]2+ was studied by electrochemistry and infrared spectroelectrochemistry. This catalyst has been previously shown to have increased CO2 reduction activity when adsorbed on a mercury electrode. The homogeneous reactivity, without a mercury electrode, was often ignored in the literature. Ni(cyclam) was found to efficiently and selectively produce CO at moderate overpotentials in both aqueous and mixed organic solvent systems in a homogenous fashion at an inert glassy carbon electrode. Methylated analogs of Ni(cyclam) were also studied and observed to have more positive reduction potentials and attenuated CO2 reduction activity. The electrochemical kinetics were probed by varying CO2 substrate and proton concentrations. Products of CO2 reduction are observed in infrared spectra obtained from spectroelectrochemical experiments. The two major species observed were a Ni(I) carbonyl, [Ni(cyclam)(CO)]+, and a Ni(II) coordinated bicarbonate, [Ni(cyclam)(CO2OH)] +. The rate-limiting step during electrocatalysis was determined to be CO loss from the deactivated species, [Ni(cyclam)(CO)]+, to produce the active catalyst, [Ni(cyclam)]+. Another macrocyclic complex, [Ni(TMC)]+, was deployed as a CO scavenger in order to inhibit the deactivation of [Ni(cyclam)] + by CO. Addition of the CO scavenger was shown to dramatically increase the catalytic current observed for CO2 reduction by [Ni(cyclam)] +. Evidence for the [Ni(TMC)]+ acting as a CO scavenger includes the observation of [Ni(TMC)(CO)]+ by IR. Density functional theory calculations, probing the optimized geometry of the [Ni(cyclam)(CO)] + species, are also presented. These findings have implications on the increased activity for CO2 reduction when [Ni(cyclam)] + is adsorbed on a mercury electrode. The [Ni(cyclam)(CO)] + structure has significant distortion of the Ni center out of the plane of the cyclam nitrogens. This distortion strengthens the Ni-CO interaction by increasing back-bonding interactions. This leads to the hypothesis that the mercury surface, through Hg-Ni interactions, prevents the distorted geometry seen in solution leading to a more planar geometry. This helps to destabilize the carbonyl adduct which inhibits the extent of CO poisoning of the catalyst when adsorbed on a mercury electrode. Alternative approaches to prevent CO poisoning without using such a toxic substance as mercury are critical to improving this unique catalytic system.
A Ashour, Eman; Kulkarni, Vijay; Almutairy, Bjad; Park, Jun-Bom; Shah, Sejal P; Majumdar, Soumyajit; Lian, Zhuoyang; Pinto, Elanor; Bi, Vivian; Durig, Thomas; Martin, Scott T; Repka, Michael A
2016-01-01
The aim of the current research project was to investigate the effect of pressurized carbon dioxide (P-CO 2 ) on the physico-mechanical properties of ketoprofen (KTP)-incorporated hydroxypropylcellulose (HPC) (Klucel™ ELF, EF, and LF) produced using hot-melt extrusion (HME) techniques and to assess the plasticization effect of P-CO 2 on the various polymers tested. The physico-mechanical properties of extrudates with and without injection of P-CO 2 were examined and compared with extrudates with the addition of 5% liquid plasticizer of propylene glycol (PG). The extrudates were milled and compressed into tablets. Tablet characteristics of the extrudates with and without injection of P-CO 2 were evaluated. P-CO 2 acted as a plasticizer for tested polymers, which allowed for the reduction in extrusion processing temperature. The microscopic morphology of the extrudates was changed to a foam-like structure due to the expansion of the CO 2 at the extrusion die. The foamy extrudates demonstrated enhanced KTP release compared with the extrudates processed without P-CO 2 due to the increase of porosity and surface area of those extrudates. Furthermore, the hardness of the tablets prepared by foamy extrudates was increased and the percent friability was decreased. Thus, the good binding properties and compressibility of the extrudates were positively influenced by utilizing P-CO 2 processing.
Ashour, Eman A.; Kulkarni, Vijay; Almutairy, Bjad; Park, Jun-Bom; Shah, Sejal; Majumdar, Soumyajit; Lian, Zhuoyang; Pinto, Elanor; Bi, Yunxia; Durig, Thomas; Martin, Scott T.; Repka, Michael A.
2017-01-01
Objectives The aim of the current research project was to investigate the effect of pressurized carbon dioxide (P-CO2) on the physico-mechanical properties of Ketoprofen (KTP)-incorporated hydroxypropylcellulose (HPC) (Klucel™ ELF, EF and LF) produced using hot melt extrusion (HME) techniques and to assess the plasticization effect of P-CO2 on the various polymers tested. Methods The physico-mechanical properties of extrudates with and without injection of P-CO2 were examined and compared to extrudates with the addition of 5% liquid plasticizer of propylene glycol (PG). The extrudates were milled and compressed into tablets. Tablet characteristics of the extrudates with and without injection of P-CO2 were evaluated. Results & conclusion P-CO2 acted as a plasticizer for tested polymers, which allowed for the reduction in extrusion processing temperature. The microscopic morphology of the extrudates were changed to a foam-like structure due to expansion of the CO2 at the extrusion die. The foamy extrudates demonstrated enhanced KTP release compared to the extrudates processed without P-CO2 due to the increase of porosity and surface area of those extrudates. Furthermore, the hardness of the tablets prepared by foamy extrudates was increased and the percent friability was decreased. Thus, the good binding properties and compressibility of the extrudates were positively influenced by utilizing P-CO2 processing. PMID:25997363
Rodríguez-Hernández, María del Carmen; Moreno, Diego A; Carvajal, Micaela; Martínez-Ballesta, María del Carmen
2014-12-01
Climatic change predicts elevated salinity in soils as well as increased carbon dioxide dioxide [CO2] in the atmosphere. The present study aims to determine the effect of combined salinity and elevated [CO2] on sulfur (S) metabolism and S-derived phytochemicals in green and purple broccoli (cv. Naxos and cv. Viola, respectively). Elevated [CO2] involved the amelioration of salt stress, especially in cv. Viola, where a lower biomass reduction by salinity was accompanied by higher sodium (Na(+)) and chloride (Cl(-)) compartmentation in the vacuole. Moreover, salinity and elevated [CO2] affected the mineral and glucosinolate contents and the activity of biosynthetic enzymes of S-derived compounds and the degradative enzyme of glucosinolate metabolism, myrosinase, as well as the related amino acids and the antioxidant glutathione (GSH). In cv. Naxos, elevated [CO2] may trigger the antioxidant response to saline stress by means of increased GSH concentration. Also, in cv. Naxos, indolic glucosinolates were more influenced by the NaCl×CO2 interaction whereas in cv. Viola the aliphatic glucosinolates were significantly increased by these conditions. Salinity and elevated [CO2] enhanced the S cellular partitioning and metabolism affecting the myrosinase-glucosinolate system. © The Author 2014. Published by Oxford University Press on behalf of Japanese Society of Plant Physiologists. All rights reserved. For permissions, please email: journals.permissions@oup.com.
Development of a three-man preprototype CO2 collection subsystem for spacecraft application
NASA Technical Reports Server (NTRS)
Schubert, F. H.; Wynveen, R. A.; Quattrone, P. D.; Marshall, R. D.
1977-01-01
Future long-duration manned space missions will require regenerable carbon dioxide (CO2) collection concepts such as the Electrochemical Depolarized CO2 Concentrator (EDC). A three-man-capacity preprototype CO2 Collection Subsystem (CS-3) is being developed for eventual flight demonstration as part of the Air Revitalization System (ARS) of the Regenerative Life Support Evaluation (RLSE) experiment. The CS-3 employs an EDC to concentrate CO2 from the low partial-pressure levels required of spacecraft atmospheres to high partial-pressure levels needed for oxygen (O2) recovery through CO2 reduction processes. The CS-3 is sized to remove a nominal 3.0 kg/day (6.6 lb/day) of the CO2 to maintain the CO2 partial pressure (pCO2) of the cabin atmosphere at 400 Pa (3 mm Hg) or less. This paper presents the preprototype design, configuration, operation, and projected performance characteristics.
Carbon Dioxide Fixation in Isolated Kalanchoe Chloroplasts 1
Levi, Carolyn; Gibbs, Martin
1975-01-01
Chloroplasts isolated from Kalanchoe diagremontiana leaves were capable of photosynthesizing at a rate of 5.4 μmoles of CO2 per milligram of chlorophyll per hour. The dark rate of fixation was about 1% of the light rate. A high photosynthetic rate was associated with low starch content of the leaves. Ribose 5-phosphate, fructose 1,6-diphosphate, and dithiothreitol stimulated fixation, whereas phosphoenolpyruvate and azide were inhibitors. The products of CO2 fixation were primarily those of the photosynthetic carbon reduction cycle. PMID:16659249
Promoter Effects of Alkali Metal Cations on the Electrochemical Reduction of Carbon Dioxide
Resasco, Joaquin; Chen, Leanne D.; Clark, Ezra; ...
2017-07-24
The electrochemical reduction of CO 2 is known to be influenced by the identity of the alkali metal cation in the electrolyte; however, a satisfactory explanation for this phenomenon has not been developed. Here we present the results of experimental and theoretical studies aimed at elucidating the effects of electrolyte cation size on the intrinsic activity and selectivity of metal catalysts for the reduction of CO 2. Experiments were conducted under conditions where the influence of electrolyte polarization is minimal in order to show that cation size affects the intrinsic rates of formation of certain reaction products, most notably formore » HCOO –, C 2H 4, and C 2H 5OH over Cu(100)- and Cu(111)-oriented thin films, and for CO and HCOO– over polycrystalline Ag and Sn. Interpretation of the findings for CO 2 reduction was informed by studies of the reduction of glyoxal and CO, key intermediates along the reaction pathway to final products. Density functional theory calculations show that the alkali metal cations influence the distribution of products formed as a consequence of electrostatic interactions between solvated cations present at the outer Helmholtz plane and adsorbed species having large dipole moments. As a result, the observed trends in activity with cation size are attributed to an increase in the concentration of cations at the outer Helmholtz plane with increasing cation size.« less
Promoter Effects of Alkali Metal Cations on the Electrochemical Reduction of Carbon Dioxide
DOE Office of Scientific and Technical Information (OSTI.GOV)
Resasco, Joaquin; Chen, Leanne D.; Clark, Ezra
The electrochemical reduction of CO 2 is known to be influenced by the identity of the alkali metal cation in the electrolyte; however, a satisfactory explanation for this phenomenon has not been developed. Here we present the results of experimental and theoretical studies aimed at elucidating the effects of electrolyte cation size on the intrinsic activity and selectivity of metal catalysts for the reduction of CO 2. Experiments were conducted under conditions where the influence of electrolyte polarization is minimal in order to show that cation size affects the intrinsic rates of formation of certain reaction products, most notably formore » HCOO –, C 2H 4, and C 2H 5OH over Cu(100)- and Cu(111)-oriented thin films, and for CO and HCOO– over polycrystalline Ag and Sn. Interpretation of the findings for CO 2 reduction was informed by studies of the reduction of glyoxal and CO, key intermediates along the reaction pathway to final products. Density functional theory calculations show that the alkali metal cations influence the distribution of products formed as a consequence of electrostatic interactions between solvated cations present at the outer Helmholtz plane and adsorbed species having large dipole moments. As a result, the observed trends in activity with cation size are attributed to an increase in the concentration of cations at the outer Helmholtz plane with increasing cation size.« less
Nanostructured transition metal dichalcogenide electrocatalysts for CO2 reduction in ionic liquid.
Asadi, Mohammad; Kim, Kibum; Liu, Cong; Addepalli, Aditya Venkata; Abbasi, Pedram; Yasaei, Poya; Phillips, Patrick; Behranginia, Amirhossein; Cerrato, José M; Haasch, Richard; Zapol, Peter; Kumar, Bijandra; Klie, Robert F; Abiade, Jeremiah; Curtiss, Larry A; Salehi-Khojin, Amin
2016-07-29
Conversion of carbon dioxide (CO2) into fuels is an attractive solution to many energy and environmental challenges. However, the chemical inertness of CO2 renders many electrochemical and photochemical conversion processes inefficient. We report a transition metal dichalcogenide nanoarchitecture for catalytic electrochemical CO2 conversion to carbon monoxide (CO) in an ionic liquid. We found that tungsten diselenide nanoflakes show a current density of 18.95 milliamperes per square centimeter, CO faradaic efficiency of 24%, and CO formation turnover frequency of 0.28 per second at a low overpotential of 54 millivolts. We also applied this catalyst in a light-harvesting artificial leaf platform that concurrently oxidized water in the absence of any external potential. Copyright © 2016, American Association for the Advancement of Science.
Cade, W Todd; Nabar, Sharmila R; Keyser, Randall E
2004-05-01
The purpose of this study was to determine the reproducibility of the indirect Fick method for the measurement of mixed venous carbon dioxide partial pressure (P(v)CO(2)) and venous carbon dioxide content (C(v)CO(2)) for estimation of cardiac output (Q(c)), using the exponential rise method of carbon dioxide rebreathing, during non-steady-state treadmill exercise. Ten healthy participants (eight female and two male) performed three incremental, maximal exercise treadmill tests to exhaustion within 1 week. Non-invasive Q(c) measurements were evaluated at rest, during each 3-min stage, and at peak exercise, across three identical treadmill tests, using the exponential rise technique for measuring mixed venous PCO(2) and CCO(2) and estimating venous-arterio carbon dioxide content difference (C(v-a)CO(2)). Measurements were divided into measured or estimated variables [heart rate (HR), oxygen consumption (VO(2)), volume of expired carbon dioxide (VCO(2)), end-tidal carbon dioxide (P(ET)CO(2)), arterial carbon dioxide partial pressure (P(a)CO(2)), venous carbon dioxide partial pressure ( P(v)CO(2)), and C(v-a)CO(2)] and cardiorespiratory variables derived from the measured variables [Q(c), stroke volume (V(s)), and arteriovenous oxygen difference ( C(a-v)O(2))]. In general, the derived cardiorespiratory variables demonstrated acceptable (R=0.61) to high (R>0.80) reproducibility, especially at higher intensities and peak exercise. Measured variables, excluding P(a)CO(2) and C(v-a)CO(2), also demonstrated acceptable (R=0.6 to 0.79) to high reliability. The current study demonstrated acceptable to high reproducibility of the exponential rise indirect Fick method in measurement of mixed venous PCO(2) and CCO(2) for estimation of Q(c) during incremental treadmill exercise testing, especially at high-intensity and peak exercise.
Sedimentary reservoir oxidation during geologic CO2 sequestration
NASA Astrophysics Data System (ADS)
Lammers, Laura N.; Brown, Gordon E.; Bird, Dennis K.; Thomas, Randal B.; Johnson, Natalie C.; Rosenbauer, Robert J.; Maher, Katharine
2015-04-01
Injection of carbon dioxide into subsurface geologic reservoirs during geologic carbon sequestration (GCS) introduces an oxidizing supercritical CO2 phase into a subsurface geologic environment that is typically reducing. The resulting redox disequilibrium provides the chemical potential for the reduction of CO2 to lower free energy organic species. However, redox reactions involving carbon typically require the presence of a catalyst. Iron oxide minerals, including magnetite, are known to catalyze oxidation and reduction reactions of C-bearing species. If the redox conditions in the reservoir are modified by redox transformations involving CO2, such changes could also affect mineral stability, leading to dissolution and precipitation reactions and alteration of the long-term fate of CO2 in GCS reservoirs. We present experimental evidence that reservoirs with reducing redox conditions are favorable environments for the relatively rapid abiotic reduction of CO2 to organic molecules. In these experiments, an aqueous suspension of magnetite nanoparticles was reacted with supercritical CO2 under pressure and temperature conditions relevant to GCS in sedimentary reservoirs (95-210 °C and ∼100 bars of CO2). Hydrogen production was observed in several experiments, likely caused by Fe(II) oxidation either at the surface of magnetite or in the aqueous phase. Heating of the Fe(II)-rich system resulted in elevated PH2 and conditions favorable for the reduction of CO2 to acetic acid. Implications of these results for the long-term fate of CO2 in field-scale systems were explored using reaction path modeling of CO2 injection into reservoirs containing Fe(II)-bearing primary silicate minerals, with kinetic parameters for CO2 reduction obtained experimentally. The results of these calculations suggest that the reaction of CO2 with reservoir constituents will occur in two primary stages (1) equilibration of CO2 with organic acids resulting in mineral-fluid disequilibrium, and (2) gradual dissolution of primary minerals promoting significant CO2 reduction through the release of Fe(II). The reduction of CO2 is identified as a new trapping mechanism that could significantly enhance the long-term stability of GCS reservoirs. Identification of reservoir characteristics that promote CO2 redox transformations could be used as an additional factor in screening geologic reservoirs for GCS.
Das, Santu; Kumar, Saurabh; Garai, Somenath; Pochamoni, Ramudu; Paul, Shounik; Roy, Soumyajit
2017-10-11
An immediate challenge for chemists is to devise different methods to trap chemical energy using light by reduction of carbon dioxide to a transportable fuel. To reach this goal the major obstacle lies in finding a suitable material that is abundant and possesses catalytic power to effect such reduction reaction and perform this reduction reaction without using any external photosensitizer. Here we report for the first time a softoxometalate based on a {[K 6.5 Cu(OH) 8.5 (H 2 O) 7.5 ] 0.5 [K 3 PW 12 O 40 ]} metal oxide framework which is stable in reaction conditions that effectively performs photochemical CO 2 reduction reaction in water with a very high turnover number of 613 and TOF of 47.15 h -1 . We observe that during this reaction water gets oxidized to oxygen, while the electrons released directly go to CO 2 reducing it to formic acid. A detailed account of the characterization of the catalyst along with that of products of this reaction is reported.
Barriers and Prospects of Carbon Sequestration in India.
Gupta, Anjali; Nema, Arvind K
2014-04-01
Carbon sequestration is considered a leading technology for reducing carbon dioxide (CO2) emissions from fossil-fuel based electricity generating power plants and could permit the continued use of coal and gas whilst meeting greenhouse gas targets. India will become the world's third largest emitter of CO2 by 2015. Considering the dependence of health of the Indian global economy, there is an imperative need to develop a global approach which could address the capturing and securely storing carbon dioxide emitted from an array of energy. Therefore technology such as carbon sequestration will deliver significant CO2 reductions in a timely fashion. Considerable energy is required for the capture, compression, transport and storage steps. With the availability of potential technical storage methods for carbon sequestration like forest, mineral and geological storage options with India, it would facilitate achieving stabilization goal in the near future. This paper examines the potential carbon sequestration options available in India and evaluates them with respect to their strengths, weakness, threats and future prospects.
Ocean acidification in a geoengineering context
Williamson, Phillip; Turley, Carol
2012-01-01
Fundamental changes to marine chemistry are occurring because of increasing carbon dioxide (CO2) in the atmosphere. Ocean acidity (H+ concentration) and bicarbonate ion concentrations are increasing, whereas carbonate ion concentrations are decreasing. There has already been an average pH decrease of 0.1 in the upper ocean, and continued unconstrained carbon emissions would further reduce average upper ocean pH by approximately 0.3 by 2100. Laboratory experiments, observations and projections indicate that such ocean acidification may have ecological and biogeochemical impacts that last for many thousands of years. The future magnitude of such effects will be very closely linked to atmospheric CO2; they will, therefore, depend on the success of emission reduction, and could also be constrained by geoengineering based on most carbon dioxide removal (CDR) techniques. However, some ocean-based CDR approaches would (if deployed on a climatically significant scale) re-locate acidification from the upper ocean to the seafloor or elsewhere in the ocean interior. If solar radiation management were to be the main policy response to counteract global warming, ocean acidification would continue to be driven by increases in atmospheric CO2, although with additional temperature-related effects on CO2 and CaCO3 solubility and terrestrial carbon sequestration. PMID:22869801
NASA Astrophysics Data System (ADS)
Choens, R. C., II; Dewers, T. A.; Ilgen, A.; Espinoza, N.; Aman, M.
2016-12-01
Experimental rock deformation was used to quantify the relationship between supercritical carbon dioxide (scCO2), water vapor, and failure strength in an analog for Tertiary sandstone saline formation reservoirs. Storing large volumes of carbon dioxide in depleted petroleum reservoirs and deep saline aquifers over geologic time is an important tool in mitigating effects of climate change. Carbon dioxide is injected as a supercritical phase, where it forms a buoyant plume. At brine-plume interfaces, scCO2 dissolves over time into the brine, lowering pH and perturbing the local chemical environment. Previous work has shown that the resulting geochemical changes at mineral-fluid interfaces can alter rock mechanical properties, generally causing a decrease in strength. Additionally, water from the native brine can dissolve into the scCO2 plume where it is present as humidity. This study investigates the effect of hydrous scCO2 and CO2-saturated brine on shear failure of Boise sandstone. Samples are held in a hydrostatic pressure vessel at 2250 PSI confining pressure (PC) and 70 C, and scCO2 at specific humidity is circulated through the core for 24 hours at 2000 PSI and 70 C. Experiments are conducted at relative humidity levels of 0, 14, 28, 42, 56, 70, 84, 98, and 100% relative humidity. After the scCO2 core flood is finished, triaxial compression experiments are conducted on the samples at room temperature and an axial strain rate of 10-5 sec-1. Experiments are conducted at 500, 1000, and 1500 PSI PC. The results demonstrate that water present as humidity in scCO2 can reduce failure strength and lower slopes of the Mohr-Coulomb failure envelope. These effects increase with increasing humidity, as dry scCO2 does not affect rock strength, and may be influenced by capillary condensation of water films from humid scCO2. The reductions in failure strength seen in this study could be important in predicting reservoir response to injection, reservoir caprock integrity, and borehole stability of injection wells. Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Security Administration under contract DE-AC04-94AL85000. SAND2016-7552A
Chen, Lingjing; Guo, Zhenguo; Wei, Xi-Guang; Gallenkamp, Charlotte; Bonin, Julien; Anxolabéhère-Mallart, Elodie; Lau, Kai-Chung; Lau, Tai-Chu; Robert, Marc
2015-09-02
Molecular catalysis of carbon dioxide reduction using earth-abundant metal complexes as catalysts is a key challenge related to the production of useful products--the "solar fuels"--in which solar energy would be stored. A direct approach using sunlight energy as well as an indirect approach where sunlight is first converted into electricity could be used. A Co(II) complex and a Fe(III) complex, both bearing the same pentadentate N5 ligand (2,13-dimethyl-3,6,9,12,18-pentaazabicyclo[12.3.1]octadeca-1(18),2,12,14,16-pentaene), were synthesized, and their catalytic activity toward CO2 reduction was investigated. Carbon monoxide was formed with the cobalt complex, while formic acid was obtained with the iron-based catalyst, thus showing that the catalysis product can be switched by changing the metal center. Selective CO2 reduction occurs under electrochemical conditions as well as photochemical conditions when using a photosensitizer under visible light excitation (λ > 460 nm, solvent acetonitrile) with the Co catalyst. In the case of the Fe catalyst, selective HCOOH production occurs at low overpotential. Sustained catalytic activity over long periods of time and high turnover numbers were observed in both cases. A catalytic mechanism is suggested on the basis of experimental results and preliminary quantum chemistry calculations.
Arterial-to-end-tidal carbon dioxide tension difference in children with congenital heart disease.
Choudhury, Minati; Kiran, Usha; Choudhary, Shiv Kumar; Airan, Balram
2006-04-01
This study estimated the arterial-to-end-tidal carbon dioxide tension difference (deltaPaCO2-PE'CO2) in children with congenital heart disease; evaluated whether hyperventilation can reduce this difference; and analyzed the relationship between the difference and the oxygen saturation (SaO2) and hemoglobin level. Prospective clinical study. Tertiary health care center. One hundred patients scheduled for correction of their underlying cardiac defect with either right-to-left or left-to-right intracardiac shunts were divided into 4 groups (n = 25 each): (1) N1, cyanotic with severe pulmonary artery hypertension; (2) N2, cyanotic with normal or decreased pulmonary artery pressure (PAP); (3) N3, acyanotic with normal or mild increases in PAP and severe increases in pulmonary blood flow (PBF); and (4) N4, acyanotic with normal PAP and normal or mild increase in PBF. All the patients received the same anesthetic regimen. The initial settings for tidal volume, respiratory rate, and inspiratory-to-expiratory (I:E) ratio were 10 mL/kg, 15 to 30 breath/min, and inspired time 40% of the total respiratory period with a 10% end-inspiratory pause. After the measurement of oxygen saturation, PO2, Hb, and deltaPaCO2-PE'CO2, all the children were hyperventilated (tidal volume: 14-15 mL/kg, respiratory rate: 5-6 breaths/min more than the initial rate, I:E ratio: same) to observe its effects on the deltaPaCO2-PE'CO2. The deltaPaCO2-PE'CO2, when predicted from the oxygen saturation, hemoglobin concentration, and PaO2, was found to be greater than the observed value in the first 3 groups (p < 0.001); whereas in group N4 these 2 values were comparable. It was also found that the gradient was higher when there was a decrease in SaO2 and an increase in the hemoglobin level. After hyperventilation, in groups N1 and N3, deltaPaCO2-PE'CO2 was decreased when compared with their baseline values; this reduction was not as much as predicted (p = 0.363 and 0.236, respectively). However, in groups N2 and N4 posthyperventilation, the deltaPaCO2-PE'27 CO2 was decreased significantly below their baseline measurements. These decreases were as much predicted. The deltaPaCO2-end-tidal carbon dioxide (PE'CO2) can be increased both in cyanotic and acyanotic children. Increased PAP is as important as increased PBF or right-to-left shunting in producing disorders in carbon dioxide homeostasis. Hyperventilation is of little use in reducing deltaPaCO2-PE'CO2 in children with high PAPs and pulmonary hyperperfusion.
Carbon Dioxide and Acetate-Free Biofiltration: A Relationship to be Investigated.
Marano, Marco; D'Amato, Anna; Patriarca, Alessandro; Di Nuzzi, Luigi Michele; Giordano, Gelsomina; Iulianiello, Giuseppe
2015-11-01
As the name reveals, acetate-free biofiltration (AFB) is featured by lack of acetate and this would seem to allow better hemodynamic stability. However, AFB also has a unique characteristic of carbon dioxide (CO2 )-free dialysate, whereas all other modern dialysis techniques imply an overload of CO2 from dialysate to the patient. This notwithstanding the role of CO2 in tolerance to dialysis treatment, both AFB and all other dialysis techniques seem not investigated in due depth. Specifically, the amount of CO2 coming back to the patient's bloodstream during AFB and bicarbonate dialysis (BD) is unknown. We measured partial pressure of CO2 (pCO2 ) in blood samples withdrawn from the venous line of the extracorporeal circuit during BD and subsequently during AFB in 22 stable chronic hemodialysis outpatients. The amount of CO2 coming back to the patient's bloodstream is higher in BD (59.1 ± 4.0 mmol/L) than in AFB (42.8 ± 4.5 mmol/L, P < 0.0001). Such difference exceeds 30%. Moreover, shifting from BD to AFB shows, notably for each patient, the reduction of pCO2 toward physiological values. BD implies CO2 overload from dialysate, whereas AFB does not. Further studies are required to evaluate if AFB would be the most appropriate dialysis technique in patients affected by chronic, but especially acute, lung diseases. Copyright © 2015 International Center for Artificial Organs and Transplantation and Wiley Periodicals, Inc.
Dreyse, Paulina; Honores, Jessica; Quezada, Diego; Isaacs, Mauricio
2015-11-01
The electrochemical reduction of carbon dioxide is studied herein by using conducting polymers based on metallotetraruthenated porphyrins (MTRPs). The polymers on glassy carbon electrodes were obtained by electropolymerization processes of the monomeric MTRP. The linear sweep voltammetry technique resulted in polymeric films that showed electrocatalytic activity toward carbon dioxide reduction with an onset potential of -0.70 V. The reduction products obtained were hydrogen, formic acid, formaldehyde, and methanol, with a tendency for a high production of methanol with a maximum value of turnover frequency equal to 15.07 when using a zinc(II) polymeric surface. Studies of the morphology (AFM) and electrochemical impedance spectroscopy results provide an adequate background to explain that the electrochemical reduction is governed by the roughness of the polymer, for which the possible mechanism involves a series of one-electron reduction reactions. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Videmsek, Urska; Hagn, Alexandra; Suhadolc, Marjetka; Radl, Viviane; Knicker, Heike; Schloter, Michael; Vodnik, Dominik
2009-07-01
Gaseous conditions at natural CO2 springs (mofettes) affect many processes in these unique ecosystems. While the response of plants to extreme and fluctuating CO2 concentrations ([CO2]) is relatively well documented, little is known on microbial life in mofette soil. Therefore, it was the aim of this study to investigate the abundance and diversity of CO2-fixing bacteria in grassland soils in different distances to a natural carbon dioxide spring. Samples of the same soil type were collected from the Stavesinci mofette, a natural CO2 spring which is known for very pure CO2 emissions, at different distances from the CO2 releasing vents, at locations that clearly differed in soil CO2 efflux (from 12.5 to over 200 micromol CO2 m(-2) s(-1) yearly average). Bulk and rhizospheric soil samples were included into analyses. The microbial response was followed by a molecular analysis of cbbL genes, encoding for the large subunit of RubisCO, a carboxylase which is of crucial importance for C assimilation in chemolitoautotrophic microbes. In all samples analyzed, the "red-like" type of cbbL genes could be detected. In contrast, the "green-like" type of cbbL could not be measured by the applied technique. Surprisingly, a reduction of "red-like" cbbL genes copies was observed in bulk soil and rhizosphere samples from the sites with the highest CO2 concentrations. Furthermore, the diversity pattern of "red-like" cbbL genes changed depending on the CO(2) regime. This indicates that only a part of the autotrophic CO2-fixing microbes could adapt to the very high CO2 concentrations and adverse life conditions that are governed by mofette gaseous regime.
Mg-Doped CuFeO 2 Photocathodes for Photoelectrochemical Reduction of Carbon Dioxide
DOE Office of Scientific and Technical Information (OSTI.GOV)
Gu, Jing; Wuttig, Anna; Krizan, Jason W.
2013-05-22
Mg-doped CuFeO 2 delafossite is reported to be photoelectrochemically active for CO 2 reduction. The material was prepared via conventional solid-state methods, and subsequently assembled into an electrode as a pressed pellet. Addition of a Mg 2+ dopant is found to substantially improve the conductivity of the material, with 0.05% Mg-doped CuFeO 2 electrodes displaying photocathodic currents under visible irradiation. Photocurrent is found to onset at irradiation wavelengths of ~800 nm with the incident photon-to-current efficiency reaching a value of 14% at 340 nm using an applied electrode potential of –0.4 V vs SCE. Photoelectrodes were determined to have amore » –1.1 V vs SCE conduction band edge and were found capable of the reduction of CO 2 to formate at 400 mV of underpotential. The conversion efficiency is maximized at –0.9 V vs SCE, with H 2 production contributing as a considerable side reaction. Lastly, these results highlight the potential to produce Mg-doped p-type metal oxide photocathodes with a band structure tuned to optimize CO 2 reduction.« less
Exploring the impact of determining factors behind CO2 emissions in China: A CGE appraisal.
Xiao, Bowen; Niu, Dongxiao; Wu, Han
2017-03-01
Along with the arrival of the post-Kyoto Protocol era, the Chinese government faces ever greater pressure to reduce greenhouse gases (GHGs). Hence, this paper aims to discuss the drivers of carbon dioxide (CO 2 ) emissions and their impact on society as a whole. First, we analyzed the background and overall situations of CO 2 emissions in China. Then, we reviewed previous studies to explore the determinants behind China's CO 2 emissions. It is widely acknowledged that energy efficiency, energy mix, and economy structure are three key factors contributing to CO 2 emissions. To explore the impacts of those three factors on the economy and CO 2 emissions, we established a computable general equilibrium (CGE) model. The following results were found: (1) The decline of a secondary industry can cause an emission reduction effect, but this is at the expense of the gross domestic product (GDP), whereas the development of a tertiary industry can boost the economy and help to reduce CO 2 emissions. (2) Cutting coal consumption can contribute significantly to emission reduction, which is accompanied by a great loss in the whole economy. (3) Although the energy efficiency improvement plays a positive role in promoting economic development, a backfire effect can weaken the effects of emission reduction and energy savings. Copyright © 2016 Elsevier B.V. All rights reserved.
NASA Astrophysics Data System (ADS)
Kumar, Bhupendra
Light assisted or driven fuel generation by carbon dioxide and proton reduction can be achieved by a p-type semiconductor/liquid junction. There are four different types of schemes which are typically used for carbon dioxide and proton reduction for fuel generation applications. In these systems, the semiconductor can serve the dual role of a catalyst and a light absorber. Specific electrocatalysts (heterogeneous and homogeneous) can be driven by p-type semiconductor where it works only as light absorber in order to achieve better selectivity and faster rates of catalysis. The p-type semiconductor/molecular catalyst junction is primarily explored in this dissertation for CO2 and proton photoelectrochemical reduction. A general principle for the operation of p-type semiconductor/molecular junctions is proposed and validated for several molecular catalysts in contact with p-Si photocathode. It is also shown that the light assisted homogeneous and heterogeneous catalysis can coexist. This principle is extended to achieve direct conversion of CO 2 to methanol on Platinum nanoparticles decorated p-Si in aqueous medium through pyridine/pyridinium system for CO2 reduction. An open circuit voltage higher than 600 mV is achieved for p-Si/Re(bipy-tBu)(CO) 3Cl [where bipy-tBu = 4,4'- tert-butyl-2,2'-bipyridine] (Re-catalyst) junction. The photoelectrochemical conversion of CO2 to CO using a p-Si/Re-catalyst junction is obtained at 100 % Faradaic efficiency. The homogeneous catalytic current density for CO2 by p-Si/Re-catalyst junction under illumination scales linearly with illumination intensity (both polychromatic and monochromatic). This indicates that the homogeneous catalysis is light driven for the p-Si/Re-catalyst junction system up to light intensities approaching one sun. The photoelectrochemical reduction of other active members of Re(bipyridyl)(CO)3Cl molecular catalyst family is also observed on illuminated p-Si photocathode. Effects of surface modification and nanowire morphology of the p-Si photocathode on the homogeneous catalytic reduction of CO2 by using p-Si/Re-catalyst junction are also described in this dissertation. For phenyl ethyl modified p-Si photocathode, the rate of homogeneous catalysis for CO2 reduction by Re-catalyst is three times greater than glassy carbon electrode and six times greater than the hexyl modified and the hydrogen terminated p-Si photocathodes. When hexyl modified p-Si nanowires are used as photocathode, the homogeneous catalytic current density increased by a factor of two compared to planar p-Si (both freshly etched and hexyl modified) photocathode. A successful light assisted generation of syngas (H2:CO = 2:1) from CO2 and water is achieved by using p-Si/Re-catalyst. In this system, water is reduced heterogeneously on p-Si surface and CO2 is reduced homogeneously by Re-catalyst. The same principle is extended to the homogeneous proton reduction by using p-Si/[FeFe] complex junction where [FeFe] complex [Fe2(micro-bdt)(CO) 6] (bdt = benzene-1,2-dithiolate)] is a proton reduction molecular catalyst. A short circuit quantum efficiency of 79 % with 100 % Faradaic efficiency and 600 mV open circuit are achieved by using p-Si/[FeFe] complex for proton reduction with 300 mM perchloric acid as a proton source. Cobalt difluororyl-diglyoximate (Co-catalyst) is a proton reduction catalyst with only 200 mV of overpotential for the hydrogen evolution reaction (HRE). The Co-catalyst is photoelectrochemically reduced with a photovoltage of 470 mV on illuminated p-Si photocathode. For p-Si photocathodes, the overpotential for proton reduction is over 1 V. In principle, p-Si/Co-catalyst junction can reduce proton to hydrogen homogeneously at underpotential. In a concluding effort, a wireless monolithic dual face single photoelectrode (multi junction photovoltaic cell which can generate a voltage higher 1.7 V) based photochemical cell is proposed for direct conversion of solar energy into liquid fuel. In this device, the two faces of the multijunction photoelectrode are serve as an anode and a cathode for water oxidation and fuel generation, respectively, and are separated by proton exchange membrane.
Luan, Chuhao; Shao, Yang; Lu, Qi; Gao, Shenghan; Huang, Kai; Wu, Hui; Yao, Kefu
2018-05-30
An efficient and selective catalyst is in urgent need for carbon dioxide electroreduction and silver is one of the promising candidates with affordable costs. Here we fabricated large-scale vertically standing Ag nanowire arrays with high crystallinity and electrical conductivity as carbon dioxide electroreduction catalysts by a simple nanomolding method that was usually considered not feasible for metallic crystalline materials. A great enhancement of current densities and selectivity for CO at moderate potentials was achieved. The current density for CO ( j co ) of Ag nanowire array with 200 nm in diameter was more than 2500 times larger than that of Ag foil at an overpotential of 0.49 V with an efficiency over 90%. The origin of enhanced performances are attributed to greatly increased electrochemically active surface area (ECSA) and higher intrinsic activity compared to those of polycrystalline Ag foil. More low-coordinated sites on the nanowires which can stabilize the CO 2 intermediate better are responsible for the high intrinsic activity. In addition, the impact of surface morphology that induces limited mass transportation on reaction selectivity and efficiency of nanowire arrays with different diameters was also discussed.
Huan, Tran Ngoc; Simon, Philippe; Rousse, Gwenaëlle; Génois, Isabelle; Artero, Vincent; Fontecave, Marc
2017-01-01
Copper is currently extensively studied because it provides promising electrodes for carbon dioxide electroreduction. The original combination, reported here, of a nanostructured porous dendritic Cu-based material, characterized by electron microcopy (SEM, TEM) and X-ray diffraction methods, and a water/ionic liquid mixture as the solvent, contributing to CO 2 solubilization and activation, results in a remarkably efficient (large current densities at low overpotentials), stable and selective (large faradic yields) electrocatalytic system for the conversion of CO 2 into formic acid, a product with a variety of uses. These results provide new directions for the further improvement of Cu electrodes.
Gadolinia-Doped Ceria Cathodes for Electrolysis of CO2
NASA Technical Reports Server (NTRS)
Adler, Stuart B.
2009-01-01
Gadolinia-doped ceria, or GDC, (Gd(0.4)Ce(0.6)O(2-delta), where the value of delta in this material varies, depending on the temperature and oxygen concentration in the atmosphere in which it is being used) has shown promise as a cathode material for high-temperature electrolysis of carbon dioxide in solid oxide electrolysis cells. The polarization resistance of a GDC electrode is significantly less than that of an otherwise equivalent electrode made of any of several other materials that are now in use or under consideration for use as cathodes for reduction of carbon dioxide. In addition, GDC shows no sign of deterioration under typical temperature and gas-mixture operating conditions of a high-temperature electrolyzer. Electrolysis of CO2 is of interest to NASA as a way of generating O2 from the CO2 in the Martian atmosphere. On Earth, a combination of electrolysis of CO2 and electrolysis of H2O might prove useful as a means of generating synthesis gas (syngas) from the exhaust gas of a coal- or natural-gas-fired power plant, thereby reducing the emission of CO2 into the atmosphere. The syngas a mixture of CO and H2 could be used as a raw material in the manufacture, via the Fisher-Tropsch process, of synthetic fuels, lubrication oils, and other hydrocarbon prod
Emission reductions from woody biomass waste for energy as an alternative to open burning.
Springsteen, Bruce; Christofk, Tom; Eubanks, Steve; Mason, Tad; Clavin, Chris; Storey, Brett
2011-01-01
Woody biomass waste is generated throughout California from forest management, hazardous fuel reduction, and agricultural operations. Open pile burning in the vicinity of generation is frequently the only economic disposal option. A framework is developed to quantify air emissions reductions for projects that alternatively utilize biomass waste as fuel for energy production. A demonstration project was conducted involving the grinding and 97-km one-way transport of 6096 bone-dry metric tons (BDT) of mixed conifer forest slash in the Sierra Nevada foothills for use as fuel in a biomass power cogeneration facility. Compared with the traditional open pile burning method of disposal for the forest harvest slash, utilization of the slash for fuel reduced particulate matter (PM) emissions by 98% (6 kg PM/BDT biomass), nitrogen oxides (NOx) by 54% (1.6 kg NOx/BDT), nonmethane volatile organics (NMOCs) by 99% (4.7 kg NMOCs/BDT), carbon monoxide (CO) by 97% (58 kg CO/BDT), and carbon dioxide equivalents (CO2e) by 17% (0.38 t CO2e/BDT). Emission contributions from biomass processing and transport operations are negligible. CO2e benefits are dependent on the emission characteristics of the displaced marginal electricity supply. Monetization of emissions reductions will assist with fuel sourcing activities and the conduct of biomass energy projects.
NASA Technical Reports Server (NTRS)
Knox, James C.; Campbell, Melissa; Murdoch, Karen; Miller, Lee A.; Jeng, Frank
2005-01-01
Currently on the International Space Station s (ISS) U.S. Segment, carbon dioxide (CO2) scrubbed from the cabin by a 4-Bed Molecular Sieve (4BMS) Carbon Dioxide Removal Assembly (CDRA) is vented overboard as a waste product. Likewise, the product hydrogen (H2) that will be generated by the Oxygen Generation Assembly (OGA) planned for installation will also be vented. A flight experiment has been proposed that will take the waste CO2 removed from the cabin, and via the catalytic Sabatier process, reduce it with waste H2 to generate water and methane. The water produced may provide cost and logistics savings for ISS by reducing the amount of water periodically re-supplied to orbit. To make this concept viable, a mechanical piston compressor and accumulator were developed for collecting and storing the CO2 from the CDRA. The compressor, accumulator and Sabatier system would be packaged together as one unit and referred to as the Carbon Dioxide Reduction Assembly (CRA). Testing was required to evaluate the performance of a 4BMS CDRA, compressor, accumulator, and Sabatier performance along with their operating rules when integrated together. This had been numerically modeled and simulated; however, testing was necessary to verify the results from the engineering analyses. Testing also allowed a better understanding of the practical inefficiencies and control issues involved in a fully integrated system versus the theoretical ideals in the model. This paper presents and discusses the results of an integrated engineering development unit test.
Direct carbon dioxide emissions from civil aircraft
NASA Astrophysics Data System (ADS)
Grote, Matt; Williams, Ian; Preston, John
2014-10-01
Global airlines consume over 5 million barrels of oil per day, and the resulting carbon dioxide (CO2) emitted by aircraft engines is of concern. This article provides a contemporary review of the literature associated with the measures available to the civil aviation industry for mitigating CO2 emissions from aircraft. The measures are addressed under two categories - policy and legal-related measures, and technological and operational measures. Results of the review are used to develop several insights into the challenges faced. The analysis shows that forecasts for strong growth in air-traffic will result in civil aviation becoming an increasingly significant contributor to anthropogenic CO2 emissions. Some mitigation-measures can be left to market-forces as the key-driver for implementation because they directly reduce airlines' fuel consumption, and their impact on reducing fuel-costs will be welcomed by the industry. Other mitigation-measures cannot be left to market-forces. Speed of implementation and stringency of these measures will not be satisfactorily resolved unattended, and the current global regulatory-framework does not provide the necessary strength of stewardship. A global regulator with ‘teeth' needs to be established, but investing such a body with the appropriate level of authority requires securing an international agreement which history would suggest is going to be very difficult. If all mitigation-measures are successfully implemented, it is still likely that traffic growth-rates will continue to out-pace emissions reduction-rates. Therefore, to achieve an overall reduction in CO2 emissions, behaviour change will be necessary to reduce demand for air-travel. However, reducing demand will be strongly resisted by all stakeholders in the industry; and the ticket price-increases necessary to induce the required reduction in traffic growth-rates place a monetary-value on CO2 emissions of approximately 7-100 times greater than other common valuations. It is clear that, whilst aviation must remain one piece of the transport-jigsaw, environmentally a global regulator with ‘teeth' is urgently required.
Basin scale controls on CO2 and CH4 emissions from the Upper Mississippi River
Crawford, John T.; Loken, Luke C.; Stanley, Emily H.; Stets, Edward G.; Dornblaser, Mark M.; Striegl, Robert G.
2016-01-01
The Upper Mississippi River, engineered for river navigation in the 1930s, includes a series of low-head dams and navigation pools receiving elevated sediment and nutrient loads from the mostly agricultural basin. Using high-resolution, spatially resolved water quality sensor measurements along 1385 river kilometers, we show that primary productivity and organic matter accumulation affect river carbon dioxide and methane emissions to the atmosphere. Phytoplankton drive CO2to near or below atmospheric equilibrium during the growing season, while anaerobic carbon oxidation supports a large proportion of the CO2 and CH4 production. Reductions of suspended sediment load, absent of dramatic reductions in nutrients, will likely further reduce net CO2emissions from the river. Large river pools, like Lake Pepin, which removes the majority of upstream sediments, and large agricultural tributaries downstream that deliver significant quantities of sediments and nutrients, are likely to persist as major geographical drivers of greenhouse gas emissions.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Fixen, Kathryn R.; Zheng, Yanning; Harris, Derek F.
Nitrogenase is an ATP-requiring enzyme capable of carrying out multielectron reductions of inert molecules. A purified remodeled nitrogenase containing two amino acid substitutions near the site of its FeMo cofactor was recently described as having the capacity to reduce carbon dioxide (CO 2) to methane (CH 4). Here, we developed the anoxygenic phototroph, Rhodopseudomonas palustris, as a biocatalyst capable of light-driven CO 2 reduction to CH 4 in vivo using this remodeled nitrogenase. Conversion of CO 2 to CH 4 by R. palustris required constitutive expression of nitrogenase, which was achieved by using a variant of the transcription factor NifAmore » that is able to activate expression of nitrogenase under all growth conditions. Also, light was required for generation of ATP by cyclic photophosphorylation. CH 4 production by R. palustris could be controlled by manipulating the distribution of electrons and energy available to nitrogenase. Furthermore, this work shows the feasibility of using microbes to generate hydrocarbons from CO 2 in one enzymatic step using light energy.« less
Federal Register 2010, 2011, 2012, 2013, 2014
2012-02-24
... CO 2 carbon dioxide CO 2 e carbon dioxide equivalent CBI confidential business information CFR Code... RFA Regulatory Flexibility Act T-D transmission--distribution UIC Underground Injection Control UMRA... to or greater than 25,000 metric tons carbon dioxide equivalent (mtCO 2 e). The proposed...
Olah, George A; Goeppert, Alain; Prakash, G K Surya
2009-01-16
Nature's photosynthesis uses the sun's energy with chlorophyll in plants as a catalyst to recycle carbon dioxide and water into new plant life. Only given sufficient geological time can new fossil fuels be formed naturally. In contrast, chemical recycling of carbon dioxide from natural and industrial sources as well as varied human activities or even from the air itself to methanol or dimethyl ether (DME) and their varied products can be achieved via its capture and subsequent reductive hydrogenative conversion. The present Perspective reviews this new approach and our research in the field over the last 15 years. Carbon recycling represents a significant aspect of our proposed Methanol Economy. Any available energy source (alternative energies such as solar, wind, geothermal, and atomic energy) can be used for the production of needed hydrogen and chemical conversion of CO(2). Improved new methods for the efficient reductive conversion of CO(2) to methanol and/or DME that we have developed include bireforming with methane and ways of catalytic or electrochemical conversions. Liquid methanol is preferable to highly volatile and potentially explosive hydrogen for energy storage and transportation. Together with the derived DME, they are excellent transportation fuels for internal combustion engines (ICE) and fuel cells as well as convenient starting materials for synthetic hydrocarbons and their varied products. Carbon dioxide thus can be chemically transformed from a detrimental greenhouse gas causing global warming into a valuable, renewable and inexhaustible carbon source of the future allowing environmentally neutral use of carbon fuels and derived hydrocarbon products.
TES/Aura L2 Carbon Dioxide (CO2) Nadir V7 (TL2CO2N)
Atmospheric Science Data Center
2018-01-18
... TES/Aura L2 Carbon Dioxide (CO2) Nadir (TL2CO2N) News: TES News Join TES News List Project ... TES Order Tool Parameters: Earth Science Atmosphere Atmospheric Chemistry/Carbon and Hydrocarbon Compounds ...
Thornton, Philip K.; Herrero, Mario
2010-01-01
We estimate the potential reductions in methane and carbon dioxide emissions from several livestock and pasture management options in the mixed and rangeland-based production systems in the tropics. The impacts of adoption of improved pastures, intensifying ruminant diets, changes in land-use practices, and changing breeds of large ruminants on the production of methane and carbon dioxide are calculated for two levels of adoption: complete adoption, to estimate the upper limit to reductions in these greenhouse gases (GHGs), and optimistic but plausible adoption rates taken from the literature, where these exist. Results are expressed both in GHG per ton of livestock product and in Gt CO2-eq. We estimate that the maximum mitigation potential of these options in the land-based livestock systems in the tropics amounts to approximately 7% of the global agricultural mitigation potential to 2030. Using historical adoption rates from the literature, the plausible mitigation potential of these options could contribute approximately 4% of global agricultural GHG mitigation. This could be worth on the order of $1.3 billion per year at a price of $20 per t CO2-eq. The household-level and sociocultural impacts of some of these options warrant further study, however, because livestock have multiple roles in tropical systems that often go far beyond their productive utility. PMID:20823225
Sabel, Clive E; Hiscock, Rosemary; Asikainen, Arja; Bi, Jun; Depledge, Mike; van den Elshout, Sef; Friedrich, Rainer; Huang, Ganlin; Hurley, Fintan; Jantunen, Matti; Karakitsios, Spyros P; Keuken, Menno; Kingham, Simon; Kontoroupis, Periklis; Kuenzli, Nino; Liu, Miaomiao; Martuzzi, Marco; Morton, Katie; Mudu, Pierpaolo; Niittynen, Marjo; Perez, Laura; Sarigiannis, Denis; Stahl-Timmins, Will; Tobollik, Myriam; Tuomisto, Jouni; Willers, Saskia
2016-03-08
Climate change is a global threat to health and wellbeing. Here we provide findings of an international research project investigating the health and wellbeing impacts of policies to reduce greenhouse gas emissions in urban environments. Five European and two Chinese city authorities and partner academic organisations formed the project consortium. The methodology involved modelling the impact of adopted urban climate-change mitigation transport, buildings and energy policy scenarios, usually for the year 2020 and comparing them with business as usual (BAU) scenarios (where policies had not been adopted). Carbon dioxide emissions, health impacting exposures (air pollution, noise and physical activity), health (cardiovascular, respiratory, cancer and leukaemia) and wellbeing (including noise related wellbeing, overall wellbeing, economic wellbeing and inequalities) were modelled. The scenarios were developed from corresponding known levels in 2010 and pre-existing exposure response functions. Additionally there were literature reviews, three longitudinal observational studies and two cross sectional surveys. There are four key findings. Firstly introduction of electric cars may confer some small health benefits but it would be unwise for a city to invest in electric vehicles unless their power generation fuel mix generates fewer emissions than petrol and diesel. Second, adopting policies to reduce private car use may have benefits for carbon dioxide reduction and positive health impacts through reduced noise and increased physical activity. Third, the benefits of carbon dioxide reduction from increasing housing efficiency are likely to be minor and co-benefits for health and wellbeing are dependent on good air exchange. Fourthly, although heating dwellings by in-home biomass burning may reduce carbon dioxide emissions, consequences for health and wellbeing were negative with the technology in use in the cities studied. The climate-change reduction policies reduced CO2 emissions (the most common greenhouse gas) from cities but impact on global emissions of CO2 would be more limited due to some displacement of emissions. The health and wellbeing impacts varied and were often limited reflecting existing relatively high quality of life and environmental standards in most of the participating cities; the greatest potential for future health benefit occurs in less developed or developing countries.
Okada, Takashi; Yonezawa, Susumu
2014-08-01
With large quantity of flux (Na2CO3), lead can be recovered from the funnel glass of waste cathode-ray tubes via reduction-melting at 1000°C. To reduce flux cost, a technique to recover added flux from the generated oxide phase is also important in order to recycle the flux recovered from the reduction-melting process. In this study, the phase separation of sodium and the crystallization of water-soluble sodium silicates were induced after the reduction-melting process to enhance the leachability of sodium in the oxide phase and to extract the sodium from the phase for the recovery of Na2CO3 as flux. A reductive atmosphere promoted the phase separation and crystallization, and the leachability of sodium from the oxide phase was enhanced. The optimum temperature and treatment time for increasing the leachability were 700°C and 2h, respectively. After treatment, more than 90% of the sodium in the oxide phase was extracted in water. NaHCO3 can be recovered by carbonization of the solution containing sodium ions using carbon dioxide gas, decomposed to Na2CO3 at 50°C and recycled for use in the reduction-melting process. Copyright © 2014 Elsevier Ltd. All rights reserved.
Grills, David Charles; Lymar, Sergei
2018-03-29
In this study, the solvated electron in CH 3CN is scavenged by CO 2 with a rate constant of 3.2 × 10 10 M –1 s –1 to produce the carbon dioxide radical anion (CO 2 •–), a strong and versatile reductant. Using pulse radiolysis with time-resolved IR detection, this radical is unambiguously identified by its absorption band at 1650 cm –1 corresponding to the antisymmetric CO 2 •– stretch. This assignment is confirmed by 13C isotopic labelling experiments and DFT calculations. In neat CH 3CN, CO 2 •– decays on a ~10 μs time scale via recombination with solvent-derivedmore » radicals (R•) and solvated protons. Upon addition of formate (HCO 2 –), the radiation yield of CO 2 •– is substantially increased due to H-atom abstraction by R• from HCO 2 – (R• + HCO 2 – → RH + CO 2 •–), which occurs in two kinetically separated steps. The rapid step involves the stronger H-abstracting CN•, CH 3•, and possibly, H• primary radicals, while the slower step is due to the less reactive, but more abundant radical, CH 2CN•. The removal of solvent radicals by HCO 2 – also results in over a hundredfold increase in the CO 2 •– lifetime. CO 2 •– scavenging experiments suggest that at 50 mM HCO 2 –, about 60% of the solvent-derived radicals are engaged in CO 2 •– generation. Finally, even under CO 2 saturation, no formation of the radical adduct, (CO 2) 2 •–, could be detected on the microsecond time scale.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Grills, David Charles; Lymar, Sergei
In this study, the solvated electron in CH 3CN is scavenged by CO 2 with a rate constant of 3.2 × 10 10 M –1 s –1 to produce the carbon dioxide radical anion (CO 2 •–), a strong and versatile reductant. Using pulse radiolysis with time-resolved IR detection, this radical is unambiguously identified by its absorption band at 1650 cm –1 corresponding to the antisymmetric CO 2 •– stretch. This assignment is confirmed by 13C isotopic labelling experiments and DFT calculations. In neat CH 3CN, CO 2 •– decays on a ~10 μs time scale via recombination with solvent-derivedmore » radicals (R•) and solvated protons. Upon addition of formate (HCO 2 –), the radiation yield of CO 2 •– is substantially increased due to H-atom abstraction by R• from HCO 2 – (R• + HCO 2 – → RH + CO 2 •–), which occurs in two kinetically separated steps. The rapid step involves the stronger H-abstracting CN•, CH 3•, and possibly, H• primary radicals, while the slower step is due to the less reactive, but more abundant radical, CH 2CN•. The removal of solvent radicals by HCO 2 – also results in over a hundredfold increase in the CO 2 •– lifetime. CO 2 •– scavenging experiments suggest that at 50 mM HCO 2 –, about 60% of the solvent-derived radicals are engaged in CO 2 •– generation. Finally, even under CO 2 saturation, no formation of the radical adduct, (CO 2) 2 •–, could be detected on the microsecond time scale.« less
Plasma Methane Pyrolysis for Spacecraft Oxygen Loop Closure
NASA Technical Reports Server (NTRS)
Greenwood, Z. W.
2018-01-01
Life support is a critical function of any crewed space vehicle or habitat. Human life support systems on the International Space Station (ISS) include a number of atmosphere revitalization (AR) technologies to provide breathable air and a comfortable living environment to the crew. The Trace Contaminant Control System removes harmful volatile organic compounds and other trace contaminants from the circulating air. The Carbon Dioxide Removal Assembly (CDRA) removes metabolic carbon dioxide (CO2) and returns air to the cabin. Humidity is kept at comfortable levels by a number of condensing heat exchangers. The Oxygen Generation Assembly (OGA) electrolyzes water to produce oxygen for the crew and hydrogen (H2) as a byproduct. A Sabatier reaction-based CO2 Reduction Assembly (CRA) was launched to the ISS in 2009 and became fully operational in June 2011.The CRA interfaces with both the OGA and CDRA. Carbon dioxide from the CDRA is compressed and stored in tanks until hydrogen is available from OGA water electrolysis. When the OGA is operational and there is CO2 available, the CRA is activated and produces methane and water via the Sabatier reaction shown in Equation 1... One approach to achieve these higher recovery rates builds upon the ISS AR architecture and includes adding a methane post-processor to recover H2 from CRA methane. NASA has been developing the Plasma Pyrolysis Assembly (PPA) to fill the role of a methane post-processor.
The influence of food supply on the response of Olympia oyster larvae to ocean acidification
NASA Astrophysics Data System (ADS)
Hettinger, A.; Sanford, E.; Hill, T. M.; Hosfelt, J. D.; Russell, A. D.; Gaylord, B.
2013-10-01
Increases in atmospheric carbon dioxide drive accompanying changes in the marine carbonate system as carbon dioxide (CO2) enters seawater and alters ocean pH (termed "ocean acidification"). However, such changes do not occur in isolation, and other environmental factors have the potential to modulate the consequences of altered ocean chemistry. Given that physiological mechanisms used by organisms to confront acidification can be energetically costly, we explored the potential for food supply to influence the response of Olympia oyster (Ostrea lurida) larvae to ocean acidification. In laboratory experiments, we reared oyster larvae under a factorial combination of pCO2 and food level. Elevated pCO2 had negative effects on larval growth, total dry weight, and metamorphic success, but high food availability partially offset these influences. The combination of elevated pCO2 and low food availability led to the greatest reduction in larval performance. However, the effects of food and pCO2 interacted additively rather than synergistically, indicating that they operated independently. Despite the potential for abundant resources to counteract the consequences of ocean acidification, impacts were never completely negated, suggesting that even under conditions of enhanced primary production and elevated food availability, impacts of ocean acidification may still accrue in some consumers.
Sabatier Catalyst Poisoning Investigation
NASA Technical Reports Server (NTRS)
Nallette, Tim; Perry, Jay; Abney, Morgan; Knox, Jim; Goldblatt, Loel
2013-01-01
The Carbon Dioxide Reduction Assembly (CRA) on the International Space Station (ISS) has been operational since 2010. The CRA uses a Sabatier reactor to produce water and methane by reaction of the metabolic CO2 scrubbed from the cabin air and the hydrogen byproduct from the water electrolysis system used for metabolic oxygen generation. Incorporating the CRA into the overall air revitalization system has facilitated life support system loop closure on the ISS reducing resupply logistics and thereby enhancing longer term missions. The CRA utilizes CO2 which has been adsorbed in a 5A molecular sieve within the Carbon Dioxide Removal Assembly, CDRA. There is a potential of compounds with molecular dimensions similar to, or less than CO2 to also be adsorbed. In this fashion trace contaminants may be concentrated within the CDRA and subsequently desorbed with the CO2 to the CRA. Currently, there is no provision to remove contaminants prior to entering the Sabatier catalyst bed. The risk associated with this is potential catalyst degradation due to trace organic contaminants in the CRA carbon dioxide feed acting as catalyst poisons. To better understand this risk, United Technologies Aerospace System (UTAS) has teamed with MSFC to investigate the impact of various trace contaminants on the CRA catalyst performance at relative ISS cabin air concentrations and at about 200/400 times of ISS concentrations, representative of the potential concentrating effect of the CDRA molecular sieve. This paper summarizes our initial assessment results.
The researches on energy sustainability in Northern China
NASA Astrophysics Data System (ADS)
Wang, Ping; Zhu, Zhiqiang; Zhang, Shuang
2018-06-01
Energy, which accounts for two-thirds of today's greenhouse gas emissions, is the key to reducing greenhouse gas emissions and slowing global warming. In this paper, the IPCC-recommended reference approach and scenario analysis were applied to evaluate dynamic change of the energy supply and energy-related carbon dioxide emissions within the period of 2000-2025 in Northern China (NC). The results show that energy importing reliance reached 85% in 2015 and the energy structure has become more diversified in NC. In addition, the per-capita CO2 emission is significantly higher while carbon intensity is lower than those of the national average. Under the LC scenario, CO2 emissions begin to fall for the first time in 2022. Hence, if Energy-Saving and Emission-Reduction strategy and regional planning for NC are implemented fully, NC will achieve the national emission reduction targets in 2025 and will have a large CO2 mitigation potential in the future.
Noman, Efaq; Norulaini Nik Ab Rahman, Nik; Al-Gheethi, Adel; Nagao, Hideyuki; Talip, Balkis A; Ab Kadir, Omar
2018-05-21
The present study aimed to select the best medium for inactivation of Aspergillus fumigatus, Aspergillus spp. in section Nigri, A. niger, A. terreus var. terreus, A. tubingensis, Penicillium waksmanii, P. simplicissimum, and Aspergillus sp. strain no. 145 spores in clinical wastes by using supercritical carbon dioxide (SC-CO 2 ). There were three types of solutions used including normal saline, seawater, distilled water, and physiological saline with 1% of methanol; each solution was tested at 5, 10, and 20 mL of the water contents. The experiments were conducted at the optimum operating parameters of supercritical carbon dioxide (30 MPa, 75 °C, 90 min). The results showed that the inactivation rate was more effective in distilled water with the presence of 1% methanol (6 log reductions). Meanwhile, the seawater decreases inactivation rate more than normal saline (4.5 vs. 5.1 log reduction). On the other hand, the experiments performed with different volumes of distilled water (5, 10, and 20 mL) indicated that A. niger spores were completely inactivated with 10 mL of distilled water. The inactivation rate of fungal spores decreased from 6 to 4.5 log as the amount of distilled water increased from 10 to 20 mL. The analysis for the spore morphology of A. fumigatus and Aspergillus spp. in section Nigri using scanning electron microscopy (SEM) has revealed the role of temperature and pressure in the SC-CO 2 in the destruction of the cell walls of the spores. It can be concluded that the distilled water represent the best medium for inactivation of fungal spores in the clinical solid wastes by SC-CO 2 .
Nucleation of Super-Critical Carbon Dioxide in a Venturi Nozzle
NASA Astrophysics Data System (ADS)
Jarrahbashi, Dorrin; Pidaparti, Sandeep; Ranjan, Devesh
2015-11-01
The supercritical carbon dioxide (S-CO2) Brayton cycle combines the primary advantages of the ideal Brayton and Rankine cycles by utilizing CO2 above its critical pressure. In addition to single phase and small back work ratios, supercritical fluids offer other advantages, e.g. heat transfer augmentation and low specific volume. Pressure reduction at the entrance of the compressor may cause homogenous nucleation, vapor production, and collapse of bubbles due to operation near the saturation conditions. Transient behavior of the flow after nucleation may cause serious issues in operation of the cycle and affect the materials used in design. The flow of S-CO2 through a venturi nozzle near the critical point has been studied. A transient compressible 3D Navier-Stokes solver, coupled with continuity, and energy equation has been used. Developed FIT libraries based on a piecewise biquintic spline interpolation of Helmholtz energy have been integrated with OpenFOAM to model S-CO2 properties. The mass fraction of vapor created in the venturi has been calculated using homogeneous equilibrium model (HEM). The flow conditions that lead to nucleation have been investigated. The sensitivity of nucleation to the inlet pressure and temperature, flow rate, and venturi profile has been shown.
Hedstrom, Svante; dos Santos, Egon Campos; Liu, Chang; ...
2018-05-08
Here, the production of useful compounds via the electrochemical carbon dioxide reduction reaction (CO2RR) is a matter of intense research. Although the thermodynamics and kinetic barriers of CO2RR are reported in previous computational studies, the electronic structure details are often overlooked. We study two important CO2RR intermediates: ethylenedione (OCCO) and CO 2 covalently bound to cluster and slab models of the Cu(100) surface. Both molecules exhibit a near-unity negative charge as chemisorbed, but otherwise they behave quite differently, as explained by a spin-uncoupling perspective. OCCO adopts a high-spin, quartetlike geometry, allowing two covalent bonds to the surface with an averagemore » gross interaction energy of –1.82 eV/bond. The energy cost for electronically exciting OCCO– to the quartet state is 1.5 eV which is readily repaid via the formation of its two surface bonds. CO 2, conversely, retains a low-spin, doubletlike structure upon chemisorption, and its single unpaired electron forms a single covalent surface bond of –2.07 eV. The 5.0 eV excitation energy to the CO 2 – quartet state is prohibitively costly and cannot be compensated for by an additional surface bond.« less
Dong, Xiyang; Dröge, Johannes; von Toerne, Christine; Marozava, Sviatlana; McHardy, Alice C; Meckenstock, Rainer U
2017-03-01
The enrichment culture BPL is able to degrade benzene with sulfate as electron acceptor and is dominated by an organism of the genus Pelotomaculum. Members of Pelotomaculum are usually known to be fermenters, undergoing syntrophy with anaerobic respiring microorganisms or methanogens. By using a metagenomic approach, we reconstructed a high-quality genome (∼2.97 Mbp, 99% completeness) for Pelotomaculum candidate BPL. The proteogenomic data suggested that (1) anaerobic benzene degradation was activated by a yet unknown mechanism for conversion of benzene to benzoyl-CoA; (2) the central benzoyl-CoA degradation pathway involved reductive dearomatization by a class II benzoyl-CoA reductase followed by hydrolytic ring cleavage and modified β-oxidation; (3) the oxidative acetyl-CoA pathway was utilized for complete oxidation to CO2. Interestingly, the genome of Pelotomaculum candidate BPL has all the genes for a complete sulfate reduction pathway including a similar electron transfer mechanism for dissimilatory sulfate reduction as in other Gram-positive sulfate-reducing bacteria. The proteome analysis revealed that the essential enzymes for sulfate reduction were all formed during growth with benzene. Thus, our data indicated that, besides its potential to anaerobically degrade benzene, Pelotomaculum candidate BPL is the first member of the genus that can perform sulfate reduction. © FEMS 2016. All rights reserved. For permissions, please e-mail: journals.permissions@oup.com.
Development of a Rapid Cycling CO(sub 2) and H(sub 2)O Removal Sorbent
NASA Technical Reports Server (NTRS)
Paul, Heather; Alptekin, Goekhan; Cates, Matthew; Bernal, Casey; Dubovik, Margarita; Gershanovich, Yevgenia
2007-01-01
The National Aeronautics and Space Administration (NASA) planned future missions set stringent demands on the design of the Portable Life Support System (PLSS), requiring dramatic reductions in weight, decreased reliance on supplies and greater flexibility on the types of missions. Use of regenerable systems that reduce weight and volume of the Extravehicular Mobility Unit (EMU) is of critical importance to NASA, both for low orbit operations and for long duration manned missions. The carbon dioxide and humidity control unit in the existing PLSS design is relatively large, since it has to remove and store 8 hours worth of CO2. If the sorbent regeneration can be carried out during the extravehicular activity (EVA) with a relatively high regeneration frequency, the size of the sorbent canister and weight can be significantly reduced. The progress of regenerable CO2 and humidity control is leading us towards the use of a rapid cycling amine system. TDA Research, Inc. is developing compact, regenerable sorbent materials to control CO2 and humidity in the space suit ventilation loop. The sorbent can be regenerated using space vacuum during the EVA, eliminating all carbon dioxide and humidity duration-limiting elements in the life support system. The material also has applications in other areas of space exploration such as the Orion spacecraft and other longer duration exploration missions requiring regenerable technologies. This paper summarizes the results of the sorbent development, testing, and evaluation efforts to date. The results of a preliminary system analysis are also included, showing the size and volume reductions for PLSS provided by the new system.
NASA Astrophysics Data System (ADS)
Hu, Hanjun; Tang, Yang; Hu, Qing; Wan, Pingyu; Dai, Liming; Yang, Xiao Jin
2018-07-01
In-situ grown nanoporous Zn-Cu catalysts were prepared by simply annealing a commercial brass foil at 500 °C in air, followed by electrochemical reduction. During the annealing process, Zn preferentially melted and migrated out of the framework of the alloy to form a thin layer of ZnO on its surface. Subsequent electroreduction created nanoporous Zn-enriched surface. The Zn concentration increased from 36% to 50% by 10 min, to 81% by 3 h, and to 87% by 12 h annealing treatment while the average pore size decreased from 290 nm to 120 nm as the annealing time increased from 1 h to 12 h. Faradaic efficiency of CO2 reduction to CO and HCOOH was enhanced by nearly 4 and 6 times, respectively, as compared to untreated brass foils. The nanoporous Zn-Cu catalyst presented a stable ratio of CO/H2 and a steady working current density in a continuous electrolysis of 18 h in 0.5 M KHCO3 solution.
NASA Astrophysics Data System (ADS)
Ali, Sardar; Zabidi, Noor Asmawati Mohd; Subbarao, Duvvuri
2014-10-01
Catalysts were prepared via a wet impregnation method. Different physicochemical properties of the samples were revealed by transmission electron microscope (TEM), temperature programmed reduction (H2-TPR) and carbon dioxide desorption (CO2-desorption). Fischer-Tropsch reaction (FTS) was carried out in a fixed-bed microreactor at 220°C and 1 atm, with H2/ CO = 2v / v and space velocity, SV of 12L/g.h for 5 h. Various characterization techniques revealed that there was a stronger interaction between Co and Al2O3 support compared to that of CNTs support. CNTs support increased the reducibility and decreased Co particle size. A significant increase in % CO conversion and FTS reaction rate was observed over CNTs support compared to that of Co / Al2O3. Co/CNTs resulted in higher C5+ hydrocarbons selectivity compared to that of Co / Al2O3 catalyst. CNTs are a better support for Co compared to Al2O3.
How do leaf hydraulics limit stomatal conductance at high water vapour pressure deficits?
Bunce, James A
2006-08-01
A reduction in leaf stomatal conductance (g) with increasing leaf-to-air difference in water vapour pressure (D) is nearly ubiquitous. Ecological comparisons of sensitivity have led to the hypothesis that the reduction in g with increasing D serves to maintain leaf water potentials above those that would cause loss of hydraulic conductance. A reduction in leaf water potential is commonly hypothesized to cause stomatal closure at high D. The importance of these particular hydraulic factors was tested by exposing Abutilon theophrasti, Glycine max, Gossypium hirsutum and Xanthium strumarium to D high enough to reduce g and then decreasing ambient carbon dioxide concentration ([CO2]), and observing the resulting changes in g, transpiration rate and leaf water potential, and their reversibility. Reducing the [CO2] at high D increased g and transpiration rate and lowered leaf water potential. The abnormally high transpiration rates did not result in reductions in hydraulic conductance. Results indicate that low water potential effects on g at high D could be overcome by low [CO2], and that even lower leaf water potentials did not cause a reduction in hydraulic conductance in these well-watered plants. Reduced g at high D in these species resulted primarily from increased stomatal sensitivity to [CO2] at high D, and this increased sensitivity may mediate stomatal responses to leaf hydraulics at high D.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Balbus, John M.; Greenblatt, Jeffery B.; Chari, Ramya
While it has been recognized that actions reducing greenhouse gas (GHG) emissions can have significant positive and negative impacts on human health through reductions in ambient fine particulate matter (PM2.5) concentrations, these impacts are rarely taken into account when analyzing specific policies. This study presents a new framework for estimating the change in health outcomes resulting from implementation of specific carbon dioxide (CO 2) reduction activities, allowing comparison of different sectors and options for climate mitigation activities. Our estimates suggest that in the year 2020, the reductions in adverse health outcomes from lessened exposure to PM2.5 would yield economic benefitsmore » in the range of $6 to $14 billion (in 2008 USD), depending on the specific activity. This equates to between $40 and $93 per metric ton of CO 2 in health benefits. Specific climate interventions will vary in the health co-benefits they provide as well as in potential harms that may result from their implementation. Rigorous assessment of these health impacts is essential for guiding policy decisions as efforts to reduce GHG emissions increase in scope and intensity.« less
Reynolds, Conor C O; Kandlikar, Milind
2008-08-15
Between 2001 and 2003, public transport vehicles in New Delhi were required to switch their fuel to natural gas in an attemptto reduce their air pollution impacts. This study examines the climatic impacts of New Delhi's fuel switching policy, and outlines implications for such efforts in rapidly industrializing countries. Natural gas is mostly composed of methane, an important greenhouse gas. Emitted aerosols (black carbon, particulate organic carbon, and sulfate) also cause radiative forcing. We find that methane and black carbon emissions are critical contributors to the change in carbon dioxide equivalent [CO2(e)] emissions. In New Delhi, the switch to natural gas results in a 30% increase in CO2(e) when the impact of aerosols is not considered. However, when aerosol emissions are taken into account in our model, the net effect of the switch is estimated to be a 10% reduction in CO2(e), and there may be as much as a 30% reduction in CO2(e). There is significant potential for emissions reductions through the United Nations Framework Convention on Climate Change (UNFCCC) Clean Development Mechanism for such fuel switching projects.
Soil respiration contributes substantially to urban carbon fluxes in the greater Boston area.
Decina, Stephen M; Hutyra, Lucy R; Gately, Conor K; Getson, Jackie M; Reinmann, Andrew B; Short Gianotti, Anne G; Templer, Pamela H
2016-05-01
Urban areas are the dominant source of U.S. fossil fuel carbon dioxide (FFCO2) emissions. In the absence of binding international treaties or decisive U.S. federal policy for greenhouse gas regulation, cities have also become leaders in greenhouse gas reduction efforts through climate action plans. These plans focus on anthropogenic carbon flows only, however, ignoring a potentially substantial contribution to atmospheric carbon dioxide (CO2) concentrations from biological respiration. Our aim was to measure the contribution of CO2 efflux from soil respiration to atmospheric CO2 fluxes using an automated CO2 efflux system and to use these measurements to model urban soil CO2 efflux across an urban area. We find that growing season soil respiration is dramatically enhanced in urban areas and represents levels of CO2 efflux of up to 72% of FFCO2 within greater Boston's residential areas, and that soils in urban forests, lawns, and landscaped cover types emit 2.62 ± 0.15, 4.49 ± 0.14, and 6.73 ± 0.26 μmolCO2 m(-2) s(-1), respectively, during the growing season. These rates represent up to 2.2 times greater soil respiration than rates found in nearby rural ecosystems in central Massachusetts (MA), a potential consequence of imported carbon amendments, such as mulch, within a general regime of landowner management. As the scientific community moves rapidly towards monitoring, reporting, and verification of CO2 emissions using ground based approaches and remotely-sensed observations to measure CO2 concentrations, our results show that measurement and modeling of biogenic urban CO2 fluxes will be a critical component for verification of urban climate action plans. Copyright © 2016 Elsevier Ltd. All rights reserved.
Hyperthermic-induced hyperventilation and associated respiratory alkalosis in humans.
Abbiss, Chris R; Nosaka, Kazunori; Laursen, Paul B
2007-05-01
The purpose of this study was to determine if increased environmental heat leads to hyperthermic-induced hypocapnia and associated alkalosis during prolonged self-paced cycling. Nine male cyclists completed three 100 km stochastic time trials in hot (34 degrees C), neutral (22 degrees C) and cold (10 degrees C) environments. Intermittent measurements of rectal and skin temperature, expired gases, blood pH, PaCO(2), PaO(2), and bicarbonate were made throughout. Rectal temperature increased significantly throughout all trials (P < 0.001) and was significantly correlated with increases in the ventilatory equivalent for carbon dioxide (Ve/ VCo2; r = 0.77; P < 0.001) and blood pH (r = 0.69; P < 0.05). Rectal temperature was also negatively correlated with a reduction in PaCO(2) (r = -0.80; P < 0.001). PaO(2) and bicarbonate concentration remained constant throughout all trials. This study has shown that prolonged self-paced cycling is associated with a hyperthermic-induced hyperventilation, causing a decrease in arterialized carbon dioxide tension and consequential respiratory alkalosis.
De Angelis, Chiara; Sardanelli, Francesco; Perego, Matteo; Alì, Marco; Casilli, Francesco; Inglese, Luigi; Mauri, Giovanni
2017-11-01
To assess feasibility, efficacy and safety of carbon dioxide (CO 2 ) digital subtraction angiography (DSA) to guide endovascular aneurysm repair (EVAR) in a cohort of patients with chronic kidney disease (CKD). After Ethical Committee approval, the records of 13 patients (all male, mean age 74.6 ± 8.0 years) with CKD, who underwent EVAR to exclude an abdominal aortic aneurysm (AAA) under CO 2 angiography guidance, were reviewed. The AAA to be excluded had a mean diameter of 52.0 ± 8.0 mm. CO 2 angiography was performed by automatic (n = 7) or hand (n = 6) injection. The endograft was correctly placed and the AAA was excluded in all cases, without any surgical conversions. Two patients (15.4%) had an endoleak: one type-Ia, detected by CO 2 -DSA and effectively treated with prosthesis dilatation; one type-III, detected by CO 2 -DSA, confirmed using 10 ml of ICM, and conservatively managed. In one patient, CO 2 angiograms were considered of too low quality for guiding the procedure and 200 ml of ICM were administered. Overall, 11 patients (84.6%) underwent a successful EVAR under the guidance of the sole CO 2 angiography. No patients suffered from major complications, including those typically CO 2 -related. Two patients suffered from abdominal pain during the procedure secondary to a transient splanchnic perfusion's reduction due to CO 2 , and one patient had a worsening of renal function probably caused by a cholesterol embolization during the procedure. In patients with CKD, EVAR under CO 2 angiography guidance is feasible, effective, and safe.
On the development of a methodology for extensive in-situ and continuous atmospheric CO2 monitoring
NASA Astrophysics Data System (ADS)
Wang, K.; Chang, S.; Jhang, T.
2010-12-01
Carbon dioxide is recognized as the dominating greenhouse gas contributing to anthropogenic global warming. Stringent controls on carbon dioxide emissions are viewed as necessary steps in controlling atmospheric carbon dioxide concentrations. From the view point of policy making, regulation of carbon dioxide emissions and its monitoring are keys to the success of stringent controls on carbon dioxide emissions. Especially, extensive atmospheric CO2 monitoring is a crucial step to ensure that CO2 emission control strategies are closely followed. In this work we develop a methodology that enables reliable and accurate in-situ and continuous atmospheric CO2 monitoring for policy making. The methodology comprises the use of gas filter correlation (GFC) instrument for in-situ CO2 monitoring, the use of CO2 working standards accompanying the continuous measurements, and the use of NOAA WMO CO2 standard gases for calibrating the working standards. The use of GFC instruments enables 1-second data sampling frequency with the interference of water vapor removed from added dryer. The CO2 measurements are conducted in the following timed and cycled manner: zero CO2 measurement, two standard CO2 gases measurements, and ambient air measurements. The standard CO2 gases are calibrated again NOAA WMO CO2 standards. The methodology is used in indoor CO2 measurements in a commercial office (about 120 people working inside), ambient CO2 measurements, and installed in a fleet of in-service commercial cargo ships for monitoring CO2 over global marine boundary layer. These measurements demonstrate our method is reliable, accurate, and traceable to NOAA WMO CO2 standards. The portability of the instrument and the working standards make the method readily applied for large-scale and extensive CO2 measurements.
NASA Technical Reports Server (NTRS)
Schaefer, C.; Young, M.; Mason, S.; Coble, C.; Wear, M. L.; Sargsyan, A.; Garcia, K.; Patel, N.; Gibson, C.; Alexander, D.;
2017-01-01
Enhanced screening for the Visual Impairment/Intracranial Pressure (VIIP) syndrome has been implemented to better characterize the ocular and vision changes observed in some long-duration crewmembers. This includes implementation of in-flight ultrasound in 2010 and optical coherence tomography (OCT) in 2013. Potential risk factors for VIIP include cardiovascular health, diet, anatomical and genetic factors, and environmental conditions. Carbon dioxide (CO2), a potent vasodilator, is chronically elevated on the International Space Station (ISS) relative to ambient levels on Earth, and is a plausible risk factor for VIIP. In an effort to understand the possible associations between CO2 and VIIP, this study explores the relationship of ambient CO2 levels on ISS compared to inflight ultrasound and OCT measures of the eye obtained from ISS crewmembers. CO2 measurements were aggregated from Operational Data Reduction Complex and Node 3 major constituent analyzers (MCAs) on ISS or from sensors located in the European Columbus module, as available. CO2 levels in the periods between each ultrasound and OCT session are summarized using timeseries metrics, including time-weighted means and variances. Partial least squares regression analyses are used to quantify the complex relationship between specific ultrasound and OCT measures and the CO2 metrics simulataneously. These analyses will enhance our understanding of the possible associations between CO2 levels and structural changes to the eye which will in turn inform future analysis of inflight VIIP data.
21 CFR 868.2480 - Cutaneous carbon dioxide (PcCO2) monitor.
Code of Federal Regulations, 2012 CFR
2012-04-01
... 21 Food and Drugs 8 2012-04-01 2012-04-01 false Cutaneous carbon dioxide (PcCO2) monitor. 868.2480 Section 868.2480 Food and Drugs FOOD AND DRUG ADMINISTRATION, DEPARTMENT OF HEALTH AND HUMAN SERVICES (CONTINUED) MEDICAL DEVICES ANESTHESIOLOGY DEVICES Monitoring Devices § 868.2480 Cutaneous carbon dioxide (PcCO2) monitor. (a) Identification. A...
Federal Register 2010, 2011, 2012, 2013, 2014
2010-09-02
... long-lived and directly emitted GHGs--carbon dioxide (CO 2 ), methane (CH 4 ), nitrous oxide (N 2 O... carbon dioxide equivalent (CO 2 e) but only if the project also significantly increase emissions of at... emissions must be calculated on both a mass basis and, as alluded to above, a carbon dioxide equivalent (CO...
DOE Office of Scientific and Technical Information (OSTI.GOV)
Niu Dongjie, E-mail: niudongjie@tongji.edu.cn; UNEP-Tongji Institute of Environment for Sustainable Development, 1239 Siping Road, Shanghai 200092; Huang Hui
2013-01-15
Highlights: Black-Right-Pointing-Pointer GHGs emissions from sludge digestion + residue land use in China were calculated. Black-Right-Pointing-Pointer The AD unit contributes more than 97% of total biogenic GHGs emissions. Black-Right-Pointing-Pointer AD with methane recovery is attractive for sludge GHGs emissions reduction. - Abstract: About 20 million tonnes of sludge (with 80% moisture content) is discharged by the sewage treatment plants per year in China, which, if not treated properly, can be a significant source of greenhouse gases (GHGs) emissions. Anaerobic digestion is a conventional sewage sludge treatment method and will continue to be one of the main technologies in the followingmore » years. This research has taken into consideration GHGs emissions from typical processes of sludge thickening + anaerobic digestion + dewatering + residue land application in China. Fossil CO{sub 2}, biogenic CO{sub 2}, CH{sub 4,} and avoided CO{sub 2} as the main objects is discussed respectively. The results show that the total CO{sub 2}-eq is about 1133 kg/t DM (including the biogenic CO{sub 2}), while the net CO{sub 2}-eq is about 372 kg/t DM (excluding the biogenic CO{sub 2}). An anaerobic digestion unit as the main GHGs emission source occupies more than 91% CO{sub 2}-eq of the whole process. The use of biogas is important for achieving carbon dioxide emission reductions, which could reach about 24% of the total CO{sub 2}-eq reduction.« less
Anaerobic oxidation of acetylene by estuarine sediments and enrichment cultures
Culbertson, Charles W.; Zehnder, Alexander J. B.; Oremland, Ronald S.
1981-01-01
Acetylene disappeared from the gas phase of anaerobically incubated estuarine sediment slurries, and loss was accompanied by increased levels of carbon dioxide. Acetylene loss was inhibited by chloramphenicol, air, and autoclaving. Addition of 14C2H2 to slurries resulted in the formation of 14CO2 and the transient appearance of 14C-soluble intermediates, of which acetate was a major component. Acetylene oxidation stimulated sulfate reduction; however, sulfate reduction was not required for the loss of C2H2 to occur. Enrichment cultures were obtained which grew anaerobically at the expense of C2H2.
Frey, H Christopher; Kuo, Po-Yao
2009-07-01
Long-haul freight trucks typically idle for 2000 or more hours per year, motivating interest in reducing idle fuel use and emissions using auxiliary power units (APUs) and shore-power (SP). Fuel-use rates are estimated based on electronic control unit (ECU) data for truck engines and measurements for APU engines. Engine emission factors were measured using a portable emission measurement system. Indirect emissions from SP were based on average utility grid emission factors. Base engine fuel use and APU and SP electrical load were analyzed for 20 trucks monitored for more than 1 yr during 2.76 million mi of activity within 42 U.S. states. The average base engine fuel use varied from 0.46 to 0.65 gal/hr. The average APU fuel use varied from 0.24 to 0.41 gal/hr. Fuel-use rates are typically lowest in mild weather, highest in hot or cold weather, and depend on engine speed (revolutions per minute [RPM]). Compared with the base engine, APU fuel use and emissions of carbon dioxide (CO2) and sulfur dioxide (SO2) are lower by 36-47%. Oxides of nitrogen (NO(x)) emissions are lower by 80-90%. Reductions in particulate matter (PM), carbon monoxide (CO), and hydrocarbon emissions vary from approximately 10 to over 50%. SP leads to more substantial reductions, except for SO2. The actual achievable reductions will be lower because only a fraction of base engine usage will be replaced by APUs, SP, or both. Recommendations are made for reducing base engine fuel use and emissions, accounting for variability in fuel use and emissions reductions, and further work to quantify real-world avoided fuel use and emissions.
Alteration of Oceanic Nitrification Under Elevated Carbon Dioxide Concentrations
NASA Astrophysics Data System (ADS)
Beman, J.; Chow, C. E.; Popp, B. N.; Fuhrman, J. A.; Feng, Y.; Hutchins, D. A.
2008-12-01
Atmospheric carbon dioxide (CO2) concentrations are increasing exponentially and expected to double by the year 2100. Dissolution of excess CO2 in the upper ocean reduces pH, alters carbonate chemistry, and also represents a potential resource for autotrophic organisms that convert inorganic carbon into biomass--including a broad spectrum of marine microbes. These bacteria and archaea drive global biogeochemical cycles of carbon and nitrogen and constitute the vast majority of biomass in the sea, yet their responses to reduced pH and increased pCO2 remain largely undocumented. Here we show that elevated pCO2 may sharply reduce nitrification rates and populations of nitrifying microorganisms in the ocean. Multiple experiments were performed in the Sargasso Sea and the Southern California Bight under glacial maximum (193 ppm), present day (390 ppm), and projected (750 ppm) pCO2 concentrations, over time scales from hours to multiple days, and at depths of 45 m to 240 m. Measurement of nitrification rates using isotopically-labeled nitrogen showed 2-5 fold reduction under elevated pCO2--as well as an increase under glacial maximum pCO2. Marine Crenarchaeota are likely involved in nitrification as ammonia-oxidizing archaea (AOA) and are among the most abundant microbial groups in the ocean, yet this group decreased by 40-80% under increased pCO2, based on quantification of both 16S rRNA and ammonia monooxygenase (amoA) gene copies. Crenarchaeota also steadily declined over the course of multiple days under elevated pCO2, whereas ammonia-oxidizing (AOB) and nitrite-oxidizing bacteria (NOB) were more variable in their responses or were not detected. These findings suggest that projected increases in pCO2 and subsequent decreases in pH may strongly influence marine biogeochemistry and microbial community structure in the sea.
How Can CO2 Help Agriculture in the Face of Climate Change?
NASA Technical Reports Server (NTRS)
Delphine, Deryng; Elliott, Joshua; Folberth, Christian; Mueller, Christoph; Pugh, Thomas A. M.; Boote, Kenneth J.; Conway, Declan; Ruane, Alexander C.; Gerten, Dieter; Jones, James W.;
2017-01-01
Humans are increasing the amount of carbon dioxide (CO2) in the air through CO2 emissions. This is changing the climate, making life harder for many plants in areas that suffer from heat and drought. However, plants need CO2 to grow, and more CO2 can make them grow better. So will plants overall benefit from increased CO2 level or suffer from it? We wanted to test if the positive effect would offset the negative ones. To do so, we used scientific models to calculate future crop production and water use of four important crops all over the world under different scenarios of CO2 emissions and climate change. Our calculations show that although there will be large reductions in crop yield due to climate change over the next century, some crops will still be able to grow well. This is also because crops can grow with less water when CO2 levels are raised.
Dimitrakis, Dimitrios A; Syrigou, Maria; Lorentzou, Souzana; Kostoglou, Margaritis; Konstandopoulos, Athanasios G
2017-10-11
This study aims at developing a kinetic model that can adequately describe solar thermochemical water and carbon dioxide splitting with nickel ferrite powder as the active redox material. The kinetic parameters of water splitting of a previous study are revised to include transition times and new kinetic parameters for carbon dioxide splitting are developed. The computational results show a satisfactory agreement with experimental data and continuous multicycle operation under varying operating conditions is simulated. Different test cases are explored in order to improve the product yield. At first a parametric analysis is conducted, investigating the appropriate duration of the oxidation and the thermal reduction step that maximizes the hydrogen yield. Subsequently, a non-isothermal oxidation step is simulated and proven as an interesting option for increasing the hydrogen production. The kinetic model is adapted to simulate the production yields in structured solar reactor components, i.e. extruded monolithic structures, as well.
NASA Technical Reports Server (NTRS)
Green, Robert D.; Matter, Paul H.; Holt, Chris; Beachy, Michael; Gaydos, James; Farmer, Serene C.; Setlock, John
2016-01-01
A critical component in spacecraft life support loop closure is the removal of carbon dioxide (CO2, produced by the crew) from the cabin atmosphere and chemical reduction of this CO2 to recover the oxygen. In 2015, we initiated development of an oxygen recovery system for life support applications consisting of a solid oxide co-electrolyzer (SOCE) and a carbon formation reactor (CFR). The SOCE electrolyzes a combined stream of carbon dioxide (CO2) and water (H2O) gas mixtures to produce synthesis gas (e.g., CO and H2 gas) and pure dry oxygen as separate products. This SOCE is being developed from a NASA GRC solid oxide fuel cell and stack design originally developed for aeronautics long-duration power applications. The CFR, being developed by pHMatter LLC, takes the CO and H2 output from the SOCE, and converts it primarily to solid carbon (C(s)) and H2O and CO2. Although the solid carbon accumulates in the CFR, the innovative design allows easy removal of the carbon product, requiring minimal crew member (CM) time and low resupply mass (1.0 kg/year/CM) for replacement of the solid carbon catalyst, a significant improvement over previous Bosch reactor approaches. In this work, we will provide a status of our Phase I efforts in the development and testing of both the SOCE and CFR prototype units, along with an initial assessment of the combined SOCE-CFR system, including a mass and power projections, along with an estimate of the oxygen recovery rate.
Research, Development and Demonstration of Bio-Mass Boiler for Food Industry
DOE Office of Scientific and Technical Information (OSTI.GOV)
Fisher, Steve; Knapp, David
2012-07-01
Frito-Lay is working to reduce carbon emissions from their manufacturing plants. As part of this effort, they invested in a biomass-fired boiler at the Topeka, Kansas, plant. Frito-Lay partnered with Burns & McDonnell Engineering, Inc. and CPL Systems, Inc., to design and construct a steam producing boiler using carbon neutral fuels such as wood wastes (e.g. tree bark), shipping pallets, and used rubber vehicle tires. The U.S. Department of Energy (DOE) joined with Frito-Lay, Burns & McDonnell, and CPL to analyze the reductions in carbon dioxide (CO 2) emissions that result from use of biomass-fired boilers in the food manufacturingmore » environment. DOE support provided for the data collection and analysis, and reporting necessary to evaluate boiler efficiencies and reductions in CO 2 emissions. The Frito-Lay biomass-fired boiler has resulted in significant reductions in CO 2 emissions from the Topeka production facility. The use of natural gas has been reduced by 400 to 420 million standard cubic feet per year with corresponding reductions of 24,000 to 25,000 tons of CO 2. The boiler does require auxiliary functions, however, that are unnecessary for a gas-fired boiler. These include heavy motors and fans for moving fuel and firing the boiler, trucks and equipment for delivering the fuel and moving at the boiler plant, and chippers for preparing the fuel prior to delivery. Each of these operations requires the combustion of fossil fuels or electricity and has associated CO 2 emissions. Even after accounting for each of these auxiliary processes, however, the biomass-fired boiler results in net emission reductions of 22,500 to 23,500 tons of CO 2 per year.« less
Gibbons, William T; Venstrom, Luke J; De Smith, Robert M; Davidson, Jane H; Jackson, Gregory S
2014-07-21
Zirconium-doped ceria (Ce(1-x)Zr(x)O2) was synthesized through a controlled electrospinning process as a promising approach to cost-effective, sinter-resistant material structures for high-temperature, solar-driven thermochemical redox cycles. To approximate a two-step redox cycle for solar fuel production, fibrous Ce(1-x)Zr(x)O2 with relatively low levels of Zr-doping (0 < x < 0.1) were cycled in an infrared-imaging furnace with high-temperature (up to 1500 °C) partial reduction and lower-temperature (∼800 °C) reoxidation via CO2 splitting to produce CO. Increases in Zr content improve reducibility and sintering resistance, and, for x≤ 0.05, do not significantly slow reoxidation kinetics for CO production. Cycle stability of the fibrous Ce(1-x)Zr(x)O2 (with x = 0.025) was assessed for a range of conditions by measuring rates of O2 release during reduction and CO production during reoxidation and by assessing post-cycling fiber crystallite sizes and surface areas. Sintering increases with reduction temperature but occurs primarily along the fiber axes. Even after 108 redox cycles with reduction at 1400 °C and oxidation with CO2 at 800 °C, the fibers maintain their structure with surface areas of ∼0.3 m(2) g(-1), higher than those observed in the literature for other ceria-based structures operating at similarly high temperature conditions. Total CO production and peak production rate stabilize above 3.0 mL g(-1) and 13.0 mL min(-1) g(-1), respectively. The results show the potential for electrospun oxides as sinter-resistant material structures with adequate surface area to support rapid CO2 splitting in solar thermochemical redox cycles.
USDA-ARS?s Scientific Manuscript database
Soil carbon dioxide (CO2) flux is an important component of the terrestrial carbon cycle. Accurate measurements of soil CO2 flux aids determinations of carbon budgets. In this study, we investigated soil CO2 fluxes with time and depth and above ground CO2 fluxes in a bare field. CO2 concentrations w...
Uzunova, Ellie L; Mikosch, Hans
2012-03-29
The dimers of cobalt oxide (CoO)(2) with cyclic and open bent structure are studied with the B1LYP density functional; the ordering of states is validated by the CCSD(T) method. The D(2h)-symmetry rhombic dioxide Co(2)O(2) with antiferromagnetically ordered electrons on cobalt centers is the global minimum. The cyclic peroxide Co(2)(O(2)) with side-on-bonded dioxygen in (7)B(2) ground state is separated from the global minimum by an energy gap of 3.15 eV. The dioxide is highly reactive as indicated by the high value of proton affinity and chemical reactivity indices. The four-member ring structures are more stable than those with three-member ring or chain configuration. The thermodynamic stability toward dissociation to CoO increases upon carbonylation, whereas proton affinity and reactivity with release of molecular oxygen also increase. The global minimum of Co(2)O(2)(CO)(6) corresponds to a triplet state (3)A" with oxygen atoms shifted above the molecular plane of the rhombic dioxide Co(2)O(2). The SOMO-LUMO gap in the ground-state carbonylated dioxide is wider, compared to the same gap in the bare dicobalt dioxide. The peroxo-isomer Co(2)(O(2))(CO)(6) retains the planar Co(2)(O(2)) ring and is only stable in a high-spin state (7)A". The carbonylated clusters have increased reactivity in both redox and nucleophilic reactions, as a result of the increased electron density in the Co(2)O(2)-ring area.
Chen, Mengmeng; Han, Lu; Zhou, Jie; Sun, Chunyi; Hu, Chengying; Wang, Xinlong; Su, Zhongmin
2018-07-13
Metal-organic frameworks (MOFs) are well-known porous materials able to adsorb CO 2 , and their performance in CO 2 reduction has attracted much attention from researchers. A classical Co-MOF, Co-ZIF-9, has been proposed as a novel photocatalyst for reducing CO 2 into chemical feedstocks. Herein, Co-ZIF-9 with a rod-like structure was obtained through reflux. Ultra-small silver nanoparticles (Ag NPs, smaller than 5 nm) were doped into Co-ZIF-9 by the photodeposition method. With the assistance of a photosensitizer, the resultant composite Ag@Co-ZIF-9 shows catalytic reactivity in converting CO 2 into CO under visible light irradiation. Compared with bare Co-ZIF-9, the photocatalytic performance of Ag@Co-ZIF-9 increases by more than twofold (around 28.4 μmol CO) and the selectivity is enhanced by about 20% (22.9 μmol H 2 ) for 0.5 h of irradiation. This demonstrates that Ag NPs doping may provide a possible way to promote the efficiency and selectivity of MOF materials in CO 2 photoreduction.
NASA Astrophysics Data System (ADS)
Chen, Mengmeng; Han, Lu; Zhou, Jie; Sun, Chunyi; Hu, Chengying; Wang, Xinlong; Su, Zhongmin
2018-07-01
Metal–organic frameworks (MOFs) are well-known porous materials able to adsorb CO2, and their performance in CO2 reduction has attracted much attention from researchers. A classical Co-MOF, Co-ZIF-9, has been proposed as a novel photocatalyst for reducing CO2 into chemical feedstocks. Herein, Co-ZIF-9 with a rod-like structure was obtained through reflux. Ultra-small silver nanoparticles (Ag NPs, smaller than 5 nm) were doped into Co-ZIF-9 by the photodeposition method. With the assistance of a photosensitizer, the resultant composite Ag@Co-ZIF-9 shows catalytic reactivity in converting CO2 into CO under visible light irradiation. Compared with bare Co-ZIF-9, the photocatalytic performance of Ag@Co-ZIF-9 increases by more than twofold (around 28.4 μmol CO) and the selectivity is enhanced by about 20% (22.9 μmol H2) for 0.5 h of irradiation. This demonstrates that Ag NPs doping may provide a possible way to promote the efficiency and selectivity of MOF materials in CO2 photoreduction.
Yehezkeli, Omer; Bedford, Nicholas M; Park, Eunsol; Ma, Ke; Cha, Jennifer N
2016-11-23
There has been active interest to identify new methods to reduce CO 2 into usable fuel sources. In this work, we demonstrate two types of photo-electrochemical cells (PECs) that photoreduce CO 2 directly to formate in aqueous solutions both in the presence and absence of external bias or additional electron sources. The photocathodes were either a CuFeO 2 /CuO electrode or a bilayer of CdTe on NiO, whereas the photoanode was a bilayer of NiO x on CdS. The PECs were characterized by using both electrochemistry and spectroscopy, and the products formed from CO 2 reduction were characterized and quantified by using 1 H NMR spectroscopy and ESI-MS. In addition, an organohydride catalyst was tested in conjunction with the PECs, which not only showed a significant gain of 85 times in CO 2 reduction (27 μm formate without the catalyst, 2.3 mm formate with it) compared to the NiO/CdTe photocathode system but could also generate methanol under an external bias (10 μm). © 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.
Xu, Yan-Jun; Elimban, Vijayan; Dhalla, Naranjan S
2017-08-01
In this study, we investigated the effects of CO 2 water-bath therapy on blood flow and angiogenesis in the ischemic hind limb, as well as some plasma angiogenic factors in peripheral ischemic model. The hind limb ischemia was induced by occluding the femoral artery for 2 weeks in rats and treated with or without CO 2 water-bath therapy at 37 °C for 4 weeks (20 min treatment every day for 5 days per week). The peak blood flow and minimal and mean blood flow in the ischemic skeletal muscle were markedly increased by the CO 2 water-bath therapy. This increase in blood flow was associated with development of angiogenesis in the muscle, as well as reduction in the ischemia-induced increase in plasma malondialdehyde levels. Although plasma vascular endothelial growth factor and nitric oxide levels were increased in animals with peripheral ischemia, the changes in these biomarkers were not affected by CO 2 water-bath therapy. These results suggest that augmentation of blood flow in the ischemic hind limb by CO 2 water-bath therapy may be due to the development of angiogenesis and reduction in oxidative stress.
Carbon dioxide separation with a two-dimensional polymer membrane.
Schrier, Joshua
2012-07-25
Carbon dioxide gas separation is important for many environmental and energy applications. Molecular dynamics simulations are used to characterize a two-dimensional hydrocarbon polymer, PG-ES1, that uses a combination of surface adsorption and narrow pores to separate carbon dioxide from nitrogen, oxygen, and methane gases. The CO2 permeance is 3 × 10(5) gas permeation units (GPU). The CO2/N2 selectivity is 60, and the CO2/CH4 selectivity exceeds 500. The combination of high CO2 permeance and selectivity surpasses all known materials, enabling low-cost postcombustion CO2 capture, utilization of landfill gas, and horticulture applications.
Asphalt-derived high surface area activated porous carbons for carbon dioxide capture.
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.
Climate-driven changes to the atmospheric CO2 sink in the subtropical North Pacific Ocean.
Dore, John E; Lukas, Roger; Sadler, Daniel W; Karl, David M
2003-08-14
The oceans represent a significant sink for atmospheric carbon dioxide. Variability in the strength of this sink occurs on interannual timescales, as a result of regional and basin-scale changes in the physical and biological parameters that control the flux of this greenhouse gas into and out of the surface mixed layer. Here we analyse a 13-year time series of oceanic carbon dioxide measurements from station ALOHA in the subtropical North Pacific Ocean near Hawaii, and find a significant decrease in the strength of the carbon dioxide sink over the period 1989-2001. We show that much of this reduction in sink strength can be attributed to an increase in the partial pressure of surface ocean carbon dioxide caused by excess evaporation and the accompanying concentration of solutes in the water mass. Our results suggest that carbon dioxide uptake by ocean waters can be strongly influenced by changes in regional precipitation and evaporation patterns brought on by climate variability.
Kaewmai, Roihatai; H-Kittikun, Aran; Suksaroj, Chaisri; Musikavong, Charongpun
2013-01-01
Alternative methodologies for the reduction of greenhouse gas (GHG) emissions from crude palm oil (CPO) production by a wet extraction mill in Thailand were developed. The production of 1 t of CPO from mills with biogas capture (four mills) and without biogas capture (two mills) in 2010 produced GHG emissions of 935 kg carbon dioxide equivalent (CO2eq), on average. Wastewater treatment plants with and without biogas capture produced GHG emissions of 64 and 47% of total GHG emission, respectively. The rest of the emissions mostly originated from the acquisition of fresh fruit bunches. The establishment of a biogas recovery system must be the first step in the reduction of GHG emissions. It could reduce GHG emissions by 373 kgCO2eq/t of CPO. The main source of GHG emission of 163 kgCO2eq/t of CPO from the mills with biogas capture was the open pond used for cooling of wastewater before it enters the biogas recovery system. The reduction of GHG emissions could be accomplished by (i) using a wastewater-dispersed unit for cooling, (ii) using a covered pond, (iii) enhancing the performance of the biogas recovery system, and (iv) changing the stabilization pond to an aerated lagoon. By using options i-iv, reductions of GHG emissions of 216, 208, 92.2, and 87.6 kgCO2eq/t of CPO, respectively, can be achieved.
Advanced Oxygen Recovery via Series-Bosch Technology
NASA Technical Reports Server (NTRS)
Abney, Morgan B.; Mansell, J. Matthew; Atkins, Bobby; Evans, Chris; Nur, Mononita; Beassie, Rockford D.
2015-01-01
Oxygen recovery from metabolically-produced carbon dioxide (CO2) is of critical importance for long-duration manned space missions beyond low Earth orbit. On the International Space Station (ISS), oxygen is provided to the crew through electrolysis of water in the Oxygen Generation Assembly (OGA). Prior to 2011, this water was entirely resupplied from Earth. A CO2 Reduction Assembly based on the Sabatier reaction (1) was developed by Hamilton Sundstrand and delivered to ISS in 2010. The unit recovers oxygen by reducing metabolic CO2 with diatomic hydrogen (H2) to produce methane and product water. The water is cleaned by the Water Purification Assembly and recycled to the OGA for continued oxygen production. The methane product is vented overboard.
Yoshimoto, Makoto; Yamashita, Takayuki; Yamashiro, Takuya
2010-01-01
Formate dehydrogenase from Candida boidinii (CbFDH) is potentially applicable in reduction of CO(2) through oxidation of cofactor NADH into NAD(+). For this, the CbFDH activity needs to be maintained under practical reaction conditions, such as CO(2) gas-liquid flow. In this work, CbFDH and cofactor were encapsulated in liposomes and the liposomal enzymes were characterized in an external loop airlift bubble column. The airlift was operated at 45 degrees C with N(2) or CO(2) as gas phase at the superficial gas velocity U(G) of 2.0 or 3.0 cm/s. The activities of liposomal CbFDH/cofactor systems were highly stable in the airlift regardless of the type of gas phase because liposome membranes prevented interactions of the encapsulated enzyme and cofactor molecules with the gas-liquid interface of bubbles. On the other hand, free CbFDH was deactivated in the airlift especially at high U(G) with CO(2) bubbles. The liposomal CbFDH/NADH could catalyze reduction of CO(2) in the airlift giving the fractional oxidation of the liposomal NADH of 23% at the reaction time of 360 min. The cofactor was kept inside liposomes during the reaction operation with less than 10% of leakage. All of the results obtained demonstrate that the liposomal CbFDH/NADH functions as a stable catalyst for reduction of CO(2) in the airlift. (c) 2010 American Institute of Chemical Engineers
NASA Astrophysics Data System (ADS)
Tan, Lling-Lling; Ong, Wee-Jun; Chai, Siang-Piao; Mohamed, Abdul Rahman
2013-11-01
Photocatalytic reduction of carbon dioxide (CO2) into hydrocarbon fuels such as methane is an attractive strategy for simultaneously harvesting solar energy and capturing this major greenhouse gas. Incessant research interest has been devoted to preparing graphene-based semiconductor nanocomposites as photocatalysts for a variety of applications. In this work, reduced graphene oxide (rGO)-TiO2 hybrid nanocrystals were fabricated through a novel and simple solvothermal synthetic route. Anatase TiO2 particles with an average diameter of 12 nm were uniformly dispersed on the rGO sheet. Slow hydrolysis reaction was successfully attained through the use of ethylene glycol and acetic acid mixed solvents coupled with an additional cooling step. The prepared rGO-TiO2 nanocomposites exhibited superior photocatalytic activity (0.135 μmol gcat -1 h-1) in the reduction of CO2 over graphite oxide and pure anatase. The intimate contact between TiO2 and rGO was proposed to accelerate the transfer of photogenerated electrons on TiO2 to rGO, leading to an effective charge anti-recombination and thus enhancing the photocatalytic activity. Furthermore, our photocatalysts were found to be active even under the irradiation of low-power energy-saving light bulbs, which renders the entire process economically and practically feasible.
Tan, Lling-Lling; Ong, Wee-Jun; Chai, Siang-Piao; Mohamed, Abdul Rahman
2013-11-06
Photocatalytic reduction of carbon dioxide (CO2) into hydrocarbon fuels such as methane is an attractive strategy for simultaneously harvesting solar energy and capturing this major greenhouse gas. Incessant research interest has been devoted to preparing graphene-based semiconductor nanocomposites as photocatalysts for a variety of applications. In this work, reduced graphene oxide (rGO)-TiO2 hybrid nanocrystals were fabricated through a novel and simple solvothermal synthetic route. Anatase TiO2 particles with an average diameter of 12 nm were uniformly dispersed on the rGO sheet. Slow hydrolysis reaction was successfully attained through the use of ethylene glycol and acetic acid mixed solvents coupled with an additional cooling step. The prepared rGO-TiO2 nanocomposites exhibited superior photocatalytic activity (0.135 μmol gcat-1 h-1) in the reduction of CO2 over graphite oxide and pure anatase. The intimate contact between TiO2 and rGO was proposed to accelerate the transfer of photogenerated electrons on TiO2 to rGO, leading to an effective charge anti-recombination and thus enhancing the photocatalytic activity. Furthermore, our photocatalysts were found to be active even under the irradiation of low-power energy-saving light bulbs, which renders the entire process economically and practically feasible.
Hyperventilation, cerebral perfusion, and syncope.
Immink, R V; Pott, F C; Secher, N H; van Lieshout, J J
2014-04-01
This review summarizes evidence in humans for an association between hyperventilation (HV)-induced hypocapnia and a reduction in cerebral perfusion leading to syncope defined as transient loss of consciousness (TLOC). The cerebral vasculature is sensitive to changes in both the arterial carbon dioxide (PaCO2) and oxygen (PaO2) partial pressures so that hypercapnia/hypoxia increases and hypocapnia/hyperoxia reduces global cerebral blood flow. Cerebral hypoperfusion and TLOC have been associated with hypocapnia related to HV. Notwithstanding pronounced cerebrovascular effects of PaCO2 the contribution of a low PaCO2 to the early postural reduction in middle cerebral artery blood velocity is transient. HV together with postural stress does not reduce cerebral perfusion to such an extent that TLOC develops. However when HV is combined with cardiovascular stressors like cold immersion or reduced cardiac output brain perfusion becomes jeopardized. Whether, in patients with cardiovascular disease and/or defect, cerebral blood flow cerebral control HV-induced hypocapnia elicits cerebral hypoperfusion, leading to TLOC, remains to be established.
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.
Application of end-tidal carbon dioxide monitoring via distal gas samples in ventilated neonates.
Jin, Ziying; Yang, Maoying; Lin, Ru; Huang, Wenfang; Wang, Jiangmei; Hu, Zhiyong; Shu, Qiang
2017-08-01
Previous research has suggested correlations between the end-tidal partial pressure of carbon dioxide (P ET CO 2 ) and the partial pressure of arterial carbon dioxide (PaCO 2 ) in mechanically ventilated patients, but both the relationship between P ET CO 2 and PaCO 2 and whether P ET CO 2 accurately reflects PaCO 2 in neonates and infants are still controversial. This study evaluated remote sampling of P ET CO 2 via an epidural catheter within an endotracheal tube to determine the procedure's clinical safety and efficacy in the perioperative management of neonates. Abdominal surgery was performed under general anesthesia in 86 full-term newborns (age 1-30 days, weight 2.55-4.0 kg, American Society of Anesthesiologists class I or II). The infants were divided into 2 groups (n = 43 each), and carbon dioxide (CO 2 ) gas samples were collected either from the conventional position (the proximal end) or a modified position (the distal end) of the epidural catheter. The P ET CO 2 measured with the new method was significantly higher than that measured with the traditional method, and the difference between P ET CO 2 and PaCO 2 was also reduced. The accuracy of P ET CO 2 measured increased from 78.7% to 91.5% when the modified sampling method was used. The moderate correlation between P ET CO 2 and PaCO 2 by traditional measurement was 0.596, which significantly increased to 0.960 in the modified sampling group. Thus, the P ET CO 2 value was closer to that of PaCO 2 . P ET CO 2 detected via modified carbon dioxide monitoring had a better accuracy and correlation with PaCO 2 in neonates. Copyright © 2017. Published by Elsevier B.V.
NASA Astrophysics Data System (ADS)
Strahl, J.; Fabricius, K.; de Beer, D.
2016-02-01
Ocean acidification due to rising partial pressure of carbon dioxide (pCO2) in the atmosphere is predicted to profoundly affect marine ecosystems. Studies on coral reef communities at volcanic CO2 seeps in Papua New Guinea (PNG) show reductions in coral diversity and structural complexity where mean pH is reduced by 0.3 units. For example, the abundance of the scleractinian coral Seriatopora hystrix is significantly reduced at seep sites in PNG. To assess the physiological mechanisms for these community shifts in response to ocean acidification, we collected branches of S. hystrix at a seep (pCO2= 803, pHTotal = 7.8) and a control site (pCO2 = 323, pHTotal = 8.1) in PNG. We determined rates of oxygen production, oxygen consumption and calcification of live coral branches in light and dark incubation experiments. While net photosynthesis and dark respiration rates in the corals remained similar at high and low pCO2, their rates of light and dark calcification considerably decreased at high pCO2. In order to investigate the mechanism of calcification under acidified and ambient conditions and its coupling to photosynthesis and respiration, we further studied Ca2+, pH and O2 dynamics with microsensors. The results of these analyses will allow us to determine whether limited capacity for physiological acclimatization rather than lower recruitment success have led to reduced densities of sensitive corals such as S. hystrix at high pCO2 sites.
NASA Astrophysics Data System (ADS)
Johnson, Timothy Lawrence
2002-09-01
Stabilization of atmospheric greenhouse gas concentrations will likely require significant cuts in electric sector carbon dioxide (CO2) emissions. The ability to capture and sequester CO2 in a manner compatible with today's fossil-fuel based power generating infrastructure offers a potentially low-cost contribution to a larger climate change mitigation strategy. This thesis fills a niche between economy-wide studies of CO 2 abatement and plant-level control technology assessments by examining the contribution that carbon capture and sequestration (CCS) might make toward reducing US electric sector CO2 emissions. The assessment's thirty year perspective ensures that costs sunk in current infrastructure remain relevant and allows time for technological diffusion, but remains free of assumptions about the emergence of unidentified radical innovations. The extent to which CCS might lower CO2 mitigation costs will vary directly with the dispatch of carbon capture plants in actual power-generating systems, and will depend on both the retirement of vintage capacity and competition from abatement alternatives such as coal-to-gas fuel switching and renewable energy sources. This thesis therefore adopts a capacity planning and dispatch model to examine how the current distribution of generating units, natural gas prices, and other industry trends affect the cost of CO2 control via CCS in an actual US electric market. The analysis finds that plants with CO2 capture consistently provide significant reductions in base-load emissions at carbon prices near 100 $/tC, but do not offer an economical means of meeting peak demand unless CO2 reductions in excess of 80 percent are required. Various scenarios estimate the amount by which turn-over of the existing generating infrastructure and the severity of criteria pollutant constraints reduce mitigation costs. A look at CO2 sequestration in the seabed beneath the US Outer Continental Shelf (OCS) complements this model-driven assessment by considering issues of risk, geological storage capacity, and regulation. Extensive experience with offshore oil and gas operations suggests that the technical uncertainties associated with OCS sequestration are not large. The legality of seabed CO 2 disposal under US law and international environmental agreements, however, is ambiguous, and the OCS may be the first region where these regulatory regimes clash over CO2 sequestration.
Haworth, Matthew; Elliott-Kingston, Caroline; McElwain, Jennifer C
2011-09-01
The inverse relationship between the number of stomata on a leaf surface and the atmospheric carbon dioxide concentration ([CO(2)]) in which the leaf developed allows plants to optimise water-use efficiency (WUE), but it also permits the use of fossil plants as proxies of palaeoatmospheric [CO(2)]. The ancient conifer family Araucariaceae is often represented in fossil floras and may act as a suitable proxy of palaeo-[CO(2)], yet little is known regarding the stomatal index (SI) responses of extant Araucariaceae to [CO(2)]. Four Araucaria species (Araucaria columnaris, A. heterophylla, A. angustifolia and A. bidwillii) and Agathis australis displayed no significant relationship in SI to [CO(2)] below current ambient levels (~380 ppm). However, representatives of the three extant genera within the Araucariaceae (A. bidwillii, A. australis and Wollemia nobilis) all exhibited significant reductions in SI when grown in atmospheres of elevated [CO(2)] (1,500 ppm). Stomatal conductance was reduced and WUE increased when grown under elevated [CO(2)]. Stomatal pore length did not increase alongside reduced stomatal density (SD) and SI in the three araucariacean conifers when grown at elevated [CO(2)]. These pronounced SD and SI reductions occur at higher [CO(2)] levels than in other species with more recent evolutionary origins, and may reflect an evolutionary legacy of the Araucariaceae in the high [CO(2)] world of the Mesozoic Era. Araucariacean conifers may therefore be suitable stomatal proxies of palaeo-[CO(2)] during periods of "greenhouse" climates and high [CO(2)] in the Earth's history.
Darbah, Joseph N T; Kubiske, Mark E; Nelson, Neil; Oksanen, Elina; Vapaavuori, Elina; Karnosky, David F
2008-10-01
We studied the effects of long-term exposure (nine years) of birch (Betula papyrifera) trees to elevated CO(2) and/or O(3) on reproduction and seedling development at the Aspen FACE (Free-Air Carbon Dioxide Enrichment) site in Rhinelander, WI. We found that elevated CO(2) increased both the number of trees that flowered and the quantity of flowers (260% increase in male flower production), increased seed weight, germination rate, and seedling vigor. Elevated O(3) also increased flowering but decreased seed weight and germination rate. In the combination treatment (elevated CO(2)+O(3)) seed weight is decreased (20% reduction) while germination rate was unaffected. The evidence from this study indicates that elevated CO(2) may have a largely positive impact on forest tree reproduction and regeneration while elevated O(3) will likely have a negative impact.
A microfluidic study of liquid-liquid extraction mediated by carbon dioxide.
Lestari, Gabriella; Salari, Alinaghi; Abolhasani, Milad; Kumacheva, Eugenia
2016-07-05
Liquid-liquid extraction is an important separation and purification method; however, it faces a challenge in reducing the energy consumption and the environmental impact of solvent (extractant) recovery. The reversible chemical reactions of switchable solvents (nitrogenous bases) with carbon dioxide (CO2) can be implemented in reactive liquid-liquid extraction to significantly reduce the cost and energy requirements of solvent recovery. The development of new effective switchable solvents reacting with CO2 and the optimization of extraction conditions rely on the ability to evaluate and screen the performance of switchable solvents in extraction processes. We report a microfluidic strategy for time- and labour-efficient studies of CO2-mediated solvent extraction. The platform utilizes a liquid segment containing an aqueous extractant droplet and a droplet of a solution of a switchable solvent in a non-polar liquid, with gaseous CO2 supplied to the segment from both sides. Following the reaction of the switchable solvent with CO2, the solvent becomes hydrophilic and transfers from the non-polar solvent to the aqueous droplet. By monitoring the time-dependent variation in droplet volumes, we determined the efficiency and extraction time for the CO2-mediated extraction of different nitrogenous bases in a broad experimental parameter space. The platform enables a significant reduction in the amount of switchable solvents used in these studies, provides accurate temporal characterization of the liquid-liquid extraction process, and offers the capability of high-throughput screening of switchable solvents.
Exploration Analysis of Carbon Dioxide Levels and Ultrasound Measures of the Eye During ISS Missions
NASA Technical Reports Server (NTRS)
Young, M.; Mason, S.; Schaefer, C.; Wear, M. L.; Sargsyan, A.; Garcia, K.; Coble, C.; Gruschkus, S.; Law, J.; Alexander, D.;
2016-01-01
Enhanced screening for the Visual Impairment/Intracranial Pressure (VIIP) Syndrome, including in-flight ultrasound, was implemented in 2010 to better characterize the changes in vision observed in some long-duration crewmembers. Suggested possible risk factors for VIIP include cardiovascular changes, diet, anatomical and genetic factors, and environmental conditions. As a potent vasodilator, carbon dioxide (CO (sub 2)), which is chronically elevated on the International Space Station (ISS) relative to typical indoor and outdoor ambient levels on Earth, seems a plausible contributor to VIIP. In an effort to understand the possible associations between CO (sub 2) and VIIP, this study analyzes the relationship between ambient CO (sub 2) levels on ISS and ultrasound measures of the eye obtained from ISS fliers. CO (sub 2) measurements will be pulled directly from Operational Data Reduction Complex for the Lab and Node 3 major constituent analyzers (MCAs) on ISS or from sensors located in the European Columbus module, as available. CO (sub 2) measures between ultrasound sessions will be summarized using standard time series class metrics in MATLAB including time-weighted means and variances. Cumulative CO (sub 2) exposure metrics will also be developed. Regression analyses will be used to quantify the relationships between the CO (sub 2) metrics and specific ultrasound measures. Generalized estimating equations will adjust for the repeated measures within individuals. Multiple imputation techniques will be used to adjust for any possible biases in missing data for either CO (sub 2) or ultrasound measures. These analyses will elucidate the possible relationship between CO (sub 2) and changes in vision and also inform future analysis of inflight VIIP data.
Series Bosch System Development
NASA Technical Reports Server (NTRS)
Abney, Morgan B.; Evans, Christopher; Mansell, Matt; Swickrath, Michael
2012-01-01
State-of-the-art (SOA) carbon dioxide (CO2) reduction technology for the International Space Station produces methane as a byproduct. This methane is subsequently vented overboard. The associated loss of hydrogen ultimately reduces the mass of oxygen that can be recovered from CO2 in a closed-loop life support system. As an alternative to SOA CO2 reduction technology, NASA is exploring a Series-Bosch system capable of reducing CO2 with hydrogen to form water and solid carbon. This results in 100% theoretical recovery of oxygen from metabolic CO2. In the past, Bosch-based technology did not trade favorably against SOA technology due to a high power demand, low reaction efficiencies, concerns with carbon containment, and large resupply requirements necessary to replace expended catalyst cartridges. An alternative approach to Bosch technology, labeled "Series-Bosch," employs a new system design with optimized multi-stage reactors and a membrane-based separation and recycle capability. Multi-physics modeling of the first stage reactor, along with chemical process modeling of the integrated system, has resulted in a design with potential to trade significantly better than previous Bosch technology. The modeling process and resulting system architecture selection are discussed.
Ma, Weiguang; Wang, Hong; Yu, Wei; Wang, Xiaomei; Xu, Zhiqiang; Zong, Xu; Li, Can
2018-03-19
Carbon dioxide (CO 2 ) and hydrogen sulfide (H 2 S) are generally concomitant with methane (CH 4 ) in natural gas and traditionally deemed useless or even harmful. Developing strategies that can simultaneously convert both CO 2 and H 2 S into value-added products is attractive; however it has not received enough attention. A solar-driven electrochemical process is demonstrated using graphene-encapsulated zinc oxide catalyst for CO 2 reduction and graphene catalyst for H 2 S oxidation mediated by EDTA-Fe 2+ /EDTA-Fe 3+ redox couples. The as-prepared solar-driven electrochemical system can realize the simultaneous conversion of CO 2 and H 2 S into carbon monoxide and elemental sulfur at near neutral conditions with high stability and selectivity. This conceptually provides an alternative avenue for the purification of natural gas with added economic and environmental benefits. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.
Migration of carbon dioxide included micro-nano bubble water in porous media and its monitoring
NASA Astrophysics Data System (ADS)
Takemura, T.; Hamamoto, S.; Suzuki, K.; Koichi, O.
2017-12-01
The distributed CO2 storage is the small scale storage and its located near the emission areas. In the distributed CO2 storage, the CO2 is neutralized by sediment and underground water in the subsurface region (300-500m depth). Carbon dioxide (CO2) included micro-nano bubbles is one approach in neutralizing CO2 and sediments by increasing CO2 volume per unit volume of water and accelerating the chemical reaction. In order to design underground treatment for CO2 gas in the subsurface, it is required to elucidate the behavior of CO2 included micro-nano bubbles in the water. In this study, we carried out laboratory experiment using the soil tank, and measure the amount of leakage of CO2 gas at the surface. In addition, the process of migration of carbon dioxide included micro-nano bubble was monitored by the nondestructive method, wave velocity and resistivity.
Performance and emissions of an engine fuelled by biogas of palm oil mill effluent
NASA Astrophysics Data System (ADS)
Arjuna, J.; Sitorus, T. B.; Ambarita, H.; Abda, S.
2018-02-01
This research investigates the performance and emissions of an engine by biogas and gasoline. The experiments use biogas of palm oil mill effluent (POME) with turbocharger at engine loading conditions (100, 200, 300, 400, and 500 Watt). Specific fuel consumption and thermal efficiency are used to compare engine performance, and emission analysis is based on parameters such as carbon monoxide (CO), hydrocarbon (HC), carbon dioxide (CO2) and oxide (O2). The experimental data show that the maximum thermal efficiency when engine use biogas and gasoline is 20.44% and 22.22% respectively. However, there was CO emission reduction significantly when the engine using POME biogas.
Feaster, Jeremy T.; Shi, Chuan; Cave, Etosha R.; ...
2017-06-22
Increases in energy demand and in chemical production, together with the rise in CO 2 levels in the atmosphere, motivate the development of renewable energy sources. Electrochemical CO 2 reduction to fuels and chemicals is an appealing alternative to traditional pathways to fuels and chemicals due to its intrinsic ability to couple to solar and wind energy sources. Formate (HCOO –) is a key chemical for many industries; however, greater understanding is needed regarding the mechanism and key intermediates for HCOO – production. This work reports a joint experimental and theoretical investigation of the electrochemical reduction of CO 2 tomore » HCOO – on polycrystalline Sn surfaces, which have been identified as promising catalysts for selectively producing HCOO –. Our results show that Sn electrodes produce HCOO –, carbon monoxide (CO), and hydrogen (H 2) across a range of potentials and that HCOO – production becomes favored at potentials more negative than –0.8 V vs RHE, reaching a maximum Faradaic efficiency of 70% at –0.9 V vs RHE. Scaling relations for Sn and other transition metals are examined using experimental current densities and density functional theory (DFT) binding energies. While *COOH was determined to be the key intermediate for CO production on metal surfaces, we suggest that it is unlikely to be the primary intermediate for HCOO – production. Instead, *OCHO is suggested to be the key intermediate for the CO 2RR to HCOO – transformation, and Sn’s optimal *OCHO binding energy supports its high selectivity for HCOO –. Lastly, these results suggest that oxygen-bound intermediates are critical to understand the mechanism of CO 2 reduction to HCOO – on metal surfaces.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Feaster, Jeremy T.; Shi, Chuan; Cave, Etosha R.
Increases in energy demand and in chemical production, together with the rise in CO 2 levels in the atmosphere, motivate the development of renewable energy sources. Electrochemical CO 2 reduction to fuels and chemicals is an appealing alternative to traditional pathways to fuels and chemicals due to its intrinsic ability to couple to solar and wind energy sources. Formate (HCOO –) is a key chemical for many industries; however, greater understanding is needed regarding the mechanism and key intermediates for HCOO – production. This work reports a joint experimental and theoretical investigation of the electrochemical reduction of CO 2 tomore » HCOO – on polycrystalline Sn surfaces, which have been identified as promising catalysts for selectively producing HCOO –. Our results show that Sn electrodes produce HCOO –, carbon monoxide (CO), and hydrogen (H 2) across a range of potentials and that HCOO – production becomes favored at potentials more negative than –0.8 V vs RHE, reaching a maximum Faradaic efficiency of 70% at –0.9 V vs RHE. Scaling relations for Sn and other transition metals are examined using experimental current densities and density functional theory (DFT) binding energies. While *COOH was determined to be the key intermediate for CO production on metal surfaces, we suggest that it is unlikely to be the primary intermediate for HCOO – production. Instead, *OCHO is suggested to be the key intermediate for the CO 2RR to HCOO – transformation, and Sn’s optimal *OCHO binding energy supports its high selectivity for HCOO –. Lastly, these results suggest that oxygen-bound intermediates are critical to understand the mechanism of CO 2 reduction to HCOO – on metal surfaces.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Flynn, Kristen
2015-08-18
Carbon dioxide (CO 2) emission into the atmosphere has increased tremendously through burning of fossil fuels, forestry, etc.. The increased concentration has made CO 2 reductions very attractive though the reaction is considered uphill. Utilizing the sun as a potential energy source, CO 2 has the possibility to undergo six electron and four proton transfers to produce methanol, a useable resource. This reaction has been shown to occur selectively in an aqueous pyridinium solution with a gallium phosphide (GaP) electrode. Though this reaction has a high faradaic efficiency, it was unclear as to what role the GaP surface played duringmore » the reaction. In this work, we aim to address the fundamental role of GaP during the catalytic conversion, by investigating the interaction between a clean GaP surface with the reactants, products, and intermediates of this reaction using X-ray photoelectron spectroscopy. We have determined a procedure to prepare atomically clean GaP and our initial CO 2 adsorption studies have shown that there is evidence of chemisorption and reaction to form carbonate on the clean surface at LN2 temperatures (80K), in contrast to previous theoretical calculations. These findings will enable future studies on CO 2 catalysis.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Flynn, Kristen
2015-08-19
Carbon dioxide (CO 2) emission into the atmosphere has increased tremendously through burning of fossil fuels, forestry, etc.. The increased concentration has made CO 2 reductions very attractive though the reaction is considered uphill. Utilizing the sun as a potential energy source, CO 2 has the possibility to undergo six electron and four proton transfers to produce methanol, a useable resource. This reaction has been shown to occur selectively in an aqueous pyridinium solution with a gallium phosphide (GaP) electrode. Though this reaction has a high faradaic efficiency, it was unclear as to what role the GaP surface played duringmore » the reaction. In this work, we aim to address the fundamental role of GaP during the catalytic conversion, by investigating the interaction between a clean GaP surface with the reactants, products, and intermediates of this reaction using X-ray photoelectron spectroscopy. We have determined a procedure to prepare atomically clean GaP and our initial CO 2 adsorption studies have shown that there is evidence of chemisorption and reaction to form carbonate on the clean surface at LN2 temperatures (80K), in contrast to previous theoretical calculations. These findings will enable future studies on CO 2 catalysis.« less
Bajracharya, Suman; Vanbroekhoven, Karolien; Buisman, Cees J N; Strik, David P B T B; Pant, Deepak
2017-09-21
The recent concept of microbial electrosynthesis (MES) has evolved as an electricity-driven production technology for chemicals from low-value carbon dioxide (CO 2 ) using micro-organisms as biocatalysts. MES from CO 2 comprises bioelectrochemical reduction of CO 2 to multi-carbon organic compounds using the reducing equivalents produced at the electrically-polarized cathode. The use of CO 2 as a feedstock for chemicals is gaining much attention, since CO 2 is abundantly available and its use is independent of the food supply chain. MES based on CO 2 reduction produces acetate as a primary product. In order to elucidate the performance of the bioelectrochemical CO 2 reduction process using different operation modes (batch vs. continuous), an investigation was carried out using a MES system with a flow-through biocathode supplied with 20 : 80 (v/v) or 80 : 20 (v/v) CO 2 : N 2 gas. The highest acetate production rate of 149 mg L -1 d -1 was observed with a 3.1 V applied cell-voltage under batch mode. While running in continuous mode, high acetate production was achieved with a maximum rate of 100 mg L -1 d -1 . In the continuous mode, the acetate production was not sustained over long-term operation, likely due to insufficient microbial biocatalyst retention within the biocathode compartment (i.e. suspended micro-organisms were washed out of the system). Restarting batch mode operations resulted in a renewed production of acetate. This showed an apparent domination of suspended biocatalysts over the attached (biofilm forming) biocatalysts. Long term CO 2 reduction at the biocathode resulted in the accumulation of acetate, and more reduced compounds like ethanol and butyrate were also formed. Improvements in the production rate and different biomass retention strategies (e.g. selecting for biofilm forming micro-organisms) should be investigated to enable continuous biochemical production from CO 2 using MES. Certainly, other process optimizations will be required to establish MES as an innovative sustainable technology for manufacturing biochemicals from CO 2 as a next generation feedstock.
Cavusoglu, Halit; Buyukbekar, Burak Zafer; Sakalak, Huseyin; Kohsakowski, Sebastian
2017-02-13
This study involves the preparation and catalytic properties of anatase titanium dioxide nanofibers (TiO2 NFs) supported gold nanoparticles (Au NPs) using a model reaction based on the reduction of 4-nitrophenol (NP) into 4-aminophenol (AP) by sodium borohydride (NaBH4). The fabrication of surfactant-free Au NPs was performed using pulsed laser ablation in liquid (PLAL) technique. The TiO2 NFs were fabricated by a combination of electrospinning and calcination process using a solution containing poly(vinyl pyrolidone)(PVP) and titanium isopropoxide. The adsorption efficiency of laser-generated surfactant-free Au NPs to TiO2 NF supports as a function of pH was analyzed. Our results show that the electrostatic interaction mainly controls the adsorption of the nanoparticles. Au NPs/TiO2 NFs composite exhibited good catalytic activity for the reduction of 4-NP to 4-AP. The unique combination of these materials leads to the development of highly efficient catalysts. Our heterostructured nanocatalysts possibly form an efficient path to fabricate various metal NP/metal-oxide supported catalysts. Thus the applications of PLAL-noble metal NPs can widely broaden. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
CO.sub.2 separation from low-temperature flue gases
Dilmore, Robert; Allen, Douglas; Soong, Yee; Hedges, Sheila
2010-11-30
Two methods are provide for the separation of carbon dioxide from the flue gases. The first method utilizes a phase-separating moiety dissolved in an aqueous solution of a basic moiety to capture carbon dioxide. The second method utilizes a phase-separating moiety as a suspended solid in an aqueous solution of a basic moiety to capture carbon dioxide. The first method takes advantage of the surface-independent nature of the CO.sub.2 absorption reactions in a homogeneous aqueous system. The second method also provides permanent sequestration of the carbon dioxide. Both methods incorporate the kinetic rate enhancements of amine-based scrubbing while eliminating the need to heat the entire amine solution (80% water) in order to regenerate and release CO.sub.2. Both methods also take advantage of the low-regeneration temperatures of CO.sub.2-bearing mineral systems such as Na.sub.2CO.sub.3/NaHCO.sub.3 and K.sub.2CO.sub.3/KHCO.sub.3.
Carbon dioxide recycling: emerging large-scale technologies with industrial potential.
Quadrelli, Elsje Alessandra; Centi, Gabriele; Duplan, Jean-Luc; Perathoner, Siglinda
2011-09-19
This Review introduces this special issue of ChemSusChem dedicated to CO(2) recycling. Its aim is to offer an up-to-date overview of CO(2) chemical utilization (inorganic mineralization, organic carboxylation, reduction reactions, and biochemical conversion), as a continuation and extension of earlier books and reviews on this topic, but with a specific focus on large-volume routes and projects/pilot plants that are currently emerging at (pre-)industrial level. The Review also highlights how some of these routes will offer a valuable opportunity to introduce renewable energy into the existing energy and chemical infrastructure (i.e., "drop-in" renewable energy) by synthesis of chemicals from CO(2) that are easy to transport and store. CO(2) conversion therefore has the potential to become a key pillar of the sustainable and resource-efficient production of chemicals and energy from renewables. Copyright © 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Adaptive Engine Technologies for Aviation CO2 Emissions Reduction
NASA Technical Reports Server (NTRS)
Mercer, Carolyn R.; Haller, William J.; Tong, Michael T.
2006-01-01
Adaptive turbine engine technologies are assessed for their potential to reduce carbon dioxide emissions from commercial air transports.Technologies including inlet, fan, and compressor flow control, compressor stall control, blade clearance control, combustion control, active bearings and enabling technologies such as active materials and wireless sensors are discussed. The method of systems assessment is described, including strengths and weaknesses of the approach. Performance benefit estimates are presented for each technology, with a summary of potential emissions reduction possible from the development of new, adaptively controlled engine components.
Yan, Yibo; Chen, Jie; Li, Nan; Tian, Jingqi; Li, Kaixin; Jiang, Jizhou; Liu, Jiyang; Tian, Qinghua; Chen, Peng
2018-04-24
Graphene quantum dots (GQDs), which is the latest addition to the nanocarbon material family, promise a wide spectrum of applications. Herein, we demonstrate two different functionalization strategies to systematically tailor the bandgap structures of GQDs whereby making them snugly suitable for particular applications. Furthermore, the functionalized GQDs with a narrow bandgap and intramolecular Z-scheme structure are employed as the efficient photocatalysts for water splitting and carbon dioxide reduction under visible light. The underlying mechanisms of our observations are studied and discussed.
Carbon Dioxide Transformation in Imidazolium Salts: Hydroaminomethylation Catalyzed by Ru-Complexes.
Ali, Meher; Gual, Aitor; Ebeling, Gunter; Dupont, Jairton
2016-08-23
The catalytic species generated by dissolving Ru3 (CO)12 in the ionic liquids 1-n-butyl-3-methyl-imidazolium chloride or 1-n-butyl-2,3-dimethyl-imidazolium chloride are efficient multifunctional catalysts for: (a) reverse water-gas shift, (b) hydroformylation of alkenes, and (c) reductive amination of aldehydes. Thus the reaction of alkenes with primary or secondary amines (alkene/amine, 1:1) under CO2 /H2 (1:1) affords the hydroaminomethylations products in high alkene conversions (up to 99 %) and selectivities (up to 96 %). The reaction proceeds under relatively mild reaction conditions (120 °C, 60 bar=6 MPa) and affords selectively secondary and tertiary amines. The presence of amine strongly reduces the alkene hydrogenation competitive pathway usually observed in the hydroformylation of terminal alkenes by Ru complexes. The catalytic system is also highly active for the reductive amination of aldehydes and ketones yielding amines in high yields (>90 %). © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Development of air conditioning technologies to reduce CO2 emissions in the commercial sector
Yoshida, Yukiko
2006-01-01
Background Architectural methods that take into account global environmental conservation generally concentrate on mitigating the heat load of buildings. Here, we evaluate the reduction of carbon dioxide (CO2) emissions that can be achieved by improving heating, ventilating, and air conditioning (HVAC) technologies. Results The Climate Change Research Hall (CCRH) of the National Institute for Environmental Studies (NIES) is used as a case study. CCRH was built in line with the "Green Government Buildings" program of the Government Buildings Department at the Ministry of Land, Infrastructure and Transport in Japan. We have assessed the technology used in this building, and found that there is a possibility to reduce energy consumption in the HVAC system by 30%. Conclusion Saving energy reduces CO2 emissions in the commercial sector, although emission factors depend on the country or region. Consequently, energy savings potential may serve as a criterion in selecting HVAC technologies with respect to emission reduction targets. PMID:17062161
Carbon Capture and Sequestration- A Review
NASA Astrophysics Data System (ADS)
Sood, Akash; Vyas, Savita
2017-08-01
The Drastic increase of CO2 emission in the last 30 years is due to the combustion of fossil fuels and it causes a major change in the environment such as global warming. In India, the emission of fossil fuels is developed in the recent years. The alternate energy sources are not sufficient to meet the values of this emission reduction and the framework of climate change demands the emission reduction, the CCS technology can be used as a mitigation tool which evaluates the feasibility for implementation of this technology in India. CCS is a process to capture the carbon dioxide from large sources like fossil fuel station to avoid the entrance of CO2 in the atmosphere. IPCC accredited this technology and its path for mitigation for the developing countries. In this paper, we present the technologies of CCS with its development and external factors. The main goal of this process is to avoid the release the CO2 into the atmosphere and also investigates the sequestration and mitigation technologies of carbon.
NASA Astrophysics Data System (ADS)
Anand, Madhu
Nanoparticles have received significant attention because of their unusual characteristics including high surface area to volume ratios. Materials built from nanoparticles possess unique chemical, physical, mechanical and optical properties. Due to these properties, they hold potential in application areas such as catalysts, sensors, semiconductors and optics. At the same time, CO 2 in the form of supercritical fluid or CO2 gas-expanded liquid mixtures has gained significant attention in the area of processing nanostructures. This dissertation focuses on the synthesis and processing of nanoparticles using CO2 tunable solvent systems. Nanoparticle properties depend heavily on their size and, as such, the ability to finely control the size and uniformity of nanoparticles is of utmost importance. Solution based nanoparticle formation techniques are attractive due to their simplicity, but they often result in the synthesis of particles with a wide size range. To address this limitation, a post-synthesis technique has been developed in this dissertation to fractionate polydisperse nanoparticles ( s . = 30%) into monodisperse fractions ( s . = 8%) using tunable physicochemical properties of CO 2 expanded liquids, where CO2 is employed as an antisolvent. This work demonstrates that by controlling the addition of CO2 (pressurization) to an organic dispersion of nanoparticles, the ligand stabilized nanoparticles can be size selectively precipitated within a novel high pressure apparatus that confines the particle precipitation to a specified location on a surface. Unlike current techniques, this CO2 expanded liquid approach provides faster and more efficient particle size separation, reduction in organic solvent usage, and pressure tunable size selection in a single process. To improve our fundamental understanding and to further refine the size separation process, a detailed study has been performed to identify the key parameters enabling size separation of various nanoparticle populations. This study details the influence of various factors on the size separation process, such as the types of nanoparticles, ligand type and solvent type as well as the use of recursive fractionation and the time allowed for settling during each fractionation step. This size selective precipitation technique was also applied to fractionate and separate polydisperse dispersions of CdSe/ZnS semiconductor nanocrystals into very distinct size and color fractions based solely on the pressure tunable solvent properties of CO2 expanded liquids. This size selective precipitation of nanoparticles is achieved by finely tuning the solvent strength of the CO2/organic solvent medium by simply adjusting the applied CO2 pressure. These subtle changes affect the balance between osmotic repulsive and van der Waals attractive forces thereby allowing fractionation of the nanocrystals into multiple narrow size populations. Thermodynamic analysis of nanoparticle size selective fractionation was performed to develop a theoretical model based on the thermodynamic properties of gas expanded liquids. We have used the general phenomenon of nanoparticle precipitation with CO2 expanded liquids to create dodecanethiol stabilized gold nanoparticle thin films. This method utilizes CO2 as an anti-solvent for low defect, wide area gold nanoparticle film formation employing monodisperse gold nanoparticles. Dodecanethiol stabilized gold particles are precipitated from hexane by controllably expanding the solution with carbon dioxide. Subsequent addition of carbon dioxide as a dense supercritical fluid then provides for removal of the organic solvent while avoiding the dewetting effects common to evaporating solvents. Unfortunately, the use of carbon dioxide as a neat solvent in nanoparticles synthesis and processing is limited by the very poor solvent strength of dense phase CO2. As a result, most current techniques employed to synthesize and disperse nanoparticles in neat carbon dioxide require the use of environmentally persistent fluorinated compounds as metal precursors and/or stabilizing ligands. This dissertation presents the first report of the simultaneous synthesis and stabilization of metallic nanoparticles in carbon dioxide solvent without the use of any fluorinated compounds thereby further enabling the use of CO 2 as a green solvent medium in nanomaterials synthesis and processing.
Negative Emissions: Where Will the Carbon Come From?
NASA Astrophysics Data System (ADS)
Aines, R. D.; McCoy, S. T.
2017-12-01
The need for energy technologies that remove carbon dioxide from the air grows with each year of delay in acting to address climate change. The most commonly mentioned approach for achieving that, bioenergy with carbon capture and storage (BECCS), today is largely a modeler's concept, not a technology. Thus, in the near term how can we confidently discuss the scale of biomass for energy with a net reduction in CO2 concentrations in the absence of examples? As a first step toward achieving that research objective, this talk frames the likely ways in which net reductions in CO2 concentrations can be achieved from a lifecycle perspective, and the pathways through which biomass can be converted to fuels and materials while removing CO2 from the atmosphere. We will address questions such as: What pathways exist for converting biomass into transportation fuels, electricity, and materials? How can we capture and manage the carbon dioxide emissions from these kinds of activities? And, what are the tradeoffs between pathways? We have conducted preliminary analyses of some of the common biofuel production pathways, such as ethanol from corn with and without carbon capture. These pathways are still uniformly carbon positive, that is to say, they do not achieve the goal of reducing atmospheric CO2, even if they result in lower emissions than do petroleum-based fuels. More advanced pathways appear to have the capacity for minor atmospheric reductions, including those for drop-in replacement transportation fuels and some long-lived materials. Targets and options for improving these technologies to the point that they can, in fact, be carbon negative will be discussed, including pre-processing of the biomass near the production site to reduce transportation emissions, finding ways to manage small CO2 sources associated with processing, and uses of biochar. We will end with a summary of near-term RD&D needs to advance carbon-negative pathways and the associated technologies. This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344.
Promising flame retardant textile in supercritical carbon dioxide
USDA-ARS?s Scientific Manuscript database
Since carbon dioxide is non-toxic, non-flammable and cost-effective, supercritical carbon dioxide (scCO2) is widely used in textile dyeing applications. Due to its environmentally benign character, scCO2 is considered in green chemistry as a substitute for organic solvents in chemical reactions. O...
Graphite-Conjugated Rhenium Catalysts for Carbon Dioxide Reduction
DOE Office of Scientific and Technical Information (OSTI.GOV)
Oh, Seokjoon; Gallagher, James R.; Miller, Jeffrey T.
2016-02-17
Condensation of fac-Re(5,6-diamino-1,10-phenanthroline)(CO)(3)Cl to o-quinone edge defects on graphitic carbon surfaces generates graphite-conjugated rhenium (GCC-Re) catalysts that are highly active for CO2 reduction to CO in acetonitrile electrolyte. X-ray photo-electron and X-ray absorption spectroscopies establish the formation of surface-bound Re centers with well-defined coordination environments. GCC-Re species on glassy carbon surfaces display catalytic currents greater than 50 mA cm(-2) with 96 +/- 3% Faradaic efficiency for CO production. Normalized for the number of Re active sites, GCC-Re catalysts exhibit higher turnover frequencies than that of a soluble molecular analogue, fac-Re(1,10-phenanthroline)(CO)(3)Cl, and turnover numbers greater than 12,000. In contrast to themore » molecular analogue, GCC-Re surfaces display a Tafel slope of 150 mV/decade, indicative of a catalytic mechanism involving rate-limiting one-electron transfer. This work establishes graphite conjugation as a powerful strategy for generating well-defined, tunable, heterogeneous electrocatalysts on ubiquitous graphitic carbon surfaces.« less
Disintegration of Carbon Dioxide Molecules in a Microwave Plasma Torch.
Kwak, Hyoung S; Uhm, Han S; Hong, Yong C; Choi, Eun H
2015-12-17
A pure carbon dioxide torch is generated by making use of 2.45 GHz microwave. Carbon dioxide gas becomes the working gas and produces a stable carbon dioxide torch. The torch volume is almost linearly proportional to the microwave power. Temperature of the torch flame is measured by making use of optical spectroscopy and thermocouple. Two distinctive regions are exhibited, a bright, whitish region of high-temperature zone and a bluish, dimmer region of relatively low-temperature zone. Study of carbon dioxide disintegration and gas temperature effects on the molecular fraction characteristics in the carbon dioxide plasma of a microwave plasma torch under atmospheric pressure is carried out. An analytical investigation of carbon dioxide disintegration indicates that substantial fraction of carbon dioxide molecules disintegrate and form other compounds in the torch. For example, the normalized particle densities at center of plasma are given by nCO2/nN = 6.12 × 10(-3), nCO/nN = 0.13, nC/nN = 0.24, nO/nN = 0.61, nC2/nN = 8.32 × 10(-7), nO2/nN = 5.39 × 10(-5), where nCO2, nCO, nC, nO, nC2, and nO2 are carbon dioxide, carbon monoxide, carbon and oxygen atom, carbon and oxygen molecule densities, respectively. nN is the neutral particle density. Emission profiles of the oxygen and carbon atom radicals and the carbon monoxide molecules confirm the theoretical predictions of carbon dioxide disintegration in the torch.
Comparison of CO2 Photoreduction Systems: A Review
Carbon dioxide (CO2) emissions are a major contributor to the climate change equation. To alleviate concerns of global warming, strategies to mitigate increase of CO2 levels in the atmosphere have to be developed. The most desirable approach is to convert the carbon dioxide to us...
Singh, Meenesh R; Clark, Ezra L; Bell, Alexis T
2015-11-10
Thermodynamic, achievable, and realistic efficiency limits of solar-driven electrochemical conversion of water and carbon dioxide to fuels are investigated as functions of light-absorber composition and configuration, and catalyst composition. The maximum thermodynamic efficiency at 1-sun illumination for adiabatic electrochemical synthesis of various solar fuels is in the range of 32-42%. Single-, double-, and triple-junction light absorbers are found to be optimal for electrochemical load ranges of 0-0.9 V, 0.9-1.95 V, and 1.95-3.5 V, respectively. Achievable solar-to-fuel (STF) efficiencies are determined using ideal double- and triple-junction light absorbers and the electrochemical load curves for CO2 reduction on silver and copper cathodes, and water oxidation kinetics over iridium oxide. The maximum achievable STF efficiencies for synthesis gas (H2 and CO) and Hythane (H2 and CH4) are 18.4% and 20.3%, respectively. Whereas the realistic STF efficiency of photoelectrochemical cells (PECs) can be as low as 0.8%, tandem PECs and photovoltaic (PV)-electrolyzers can operate at 7.2% under identical operating conditions. We show that the composition and energy content of solar fuels can also be adjusted by tuning the band-gaps of triple-junction light absorbers and/or the ratio of catalyst-to-PV area, and that the synthesis of liquid products and C2H4 have high profitability indices.
NASA Astrophysics Data System (ADS)
Singh, Meenesh R.; Clark, Ezra L.; Bell, Alexis T.
2015-11-01
Thermodynamic, achievable, and realistic efficiency limits of solar-driven electrochemical conversion of water and carbon dioxide to fuels are investigated as functions of light-absorber composition and configuration, and catalyst composition. The maximum thermodynamic efficiency at 1-sun illumination for adiabatic electrochemical synthesis of various solar fuels is in the range of 32-42%. Single-, double-, and triple-junction light absorbers are found to be optimal for electrochemical load ranges of 0-0.9 V, 0.9-1.95 V, and 1.95-3.5 V, respectively. Achievable solar-to-fuel (STF) efficiencies are determined using ideal double- and triple-junction light absorbers and the electrochemical load curves for CO2 reduction on silver and copper cathodes, and water oxidation kinetics over iridium oxide. The maximum achievable STF efficiencies for synthesis gas (H2 and CO) and Hythane (H2 and CH4) are 18.4% and 20.3%, respectively. Whereas the realistic STF efficiency of photoelectrochemical cells (PECs) can be as low as 0.8%, tandem PECs and photovoltaic (PV)-electrolyzers can operate at 7.2% under identical operating conditions. We show that the composition and energy content of solar fuels can also be adjusted by tuning the band-gaps of triple-junction light absorbers and/or the ratio of catalyst-to-PV area, and that the synthesis of liquid products and C2H4 have high profitability indices.
Natural sources of greenhouse gases: carbon dioxide emissions from volcanoes
Gerlach, Terrence
1990-01-01
Volcanic degassing of carbon dioxide plays an important role in keeping the atmosphere-ocean portion of the carbon geochemical cycle in balance. The atmosphere-ocean carbon deficit requires replenishment of 6??1012 mol CO2/yr, and places an upper limit on the output of carbon dioxide from volcanoes. The CO2 output of the global mid-oceanic ridge system is ca. 0.7??1012 mol/yr, thus supplying only a fraction of the amount needed to balance the carbon deficit. The carbon dioxide flux from subaerial volcanoes is poorly known, but it appears to be at least as large as the mid-oceanic ridge flux. Much (perhaps most) of the CO2 emitted from volcanoes is degassed noneruptively. This mode of degassing may lead to impacts on the environment and biosphere that are fundamentally different in character from those envisioned in published scenarios, which are based on the assumption that CO2 degassing occurs predominantly by eruptive processes. Although the flux of carbon dioxide from volcanoes is poorly constrained at present, it is clearly two orders of magnitude lower than the anthropogenic output of CO2.
Irreversible climate change due to carbon dioxide emissions.
Solomon, Susan; Plattner, Gian-Kasper; Knutti, Reto; Friedlingstein, Pierre
2009-02-10
The severity of damaging human-induced climate change depends not only on the magnitude of the change but also on the potential for irreversibility. This paper shows that the climate change that takes place due to increases in carbon dioxide concentration is largely irreversible for 1,000 years after emissions stop. Following cessation of emissions, removal of atmospheric carbon dioxide decreases radiative forcing, but is largely compensated by slower loss of heat to the ocean, so that atmospheric temperatures do not drop significantly for at least 1,000 years. Among illustrative irreversible impacts that should be expected if atmospheric carbon dioxide concentrations increase from current levels near 385 parts per million by volume (ppmv) to a peak of 450-600 ppmv over the coming century are irreversible dry-season rainfall reductions in several regions comparable to those of the "dust bowl" era and inexorable sea level rise. Thermal expansion of the warming ocean provides a conservative lower limit to irreversible global average sea level rise of at least 0.4-1.0 m if 21st century CO(2) concentrations exceed 600 ppmv and 0.6-1.9 m for peak CO(2) concentrations exceeding approximately 1,000 ppmv. Additional contributions from glaciers and ice sheet contributions to future sea level rise are uncertain but may equal or exceed several meters over the next millennium or longer.
Irreversible climate change due to carbon dioxide emissions
Solomon, Susan; Plattner, Gian-Kasper; Knutti, Reto; Friedlingstein, Pierre
2009-01-01
The severity of damaging human-induced climate change depends not only on the magnitude of the change but also on the potential for irreversibility. This paper shows that the climate change that takes place due to increases in carbon dioxide concentration is largely irreversible for 1,000 years after emissions stop. Following cessation of emissions, removal of atmospheric carbon dioxide decreases radiative forcing, but is largely compensated by slower loss of heat to the ocean, so that atmospheric temperatures do not drop significantly for at least 1,000 years. Among illustrative irreversible impacts that should be expected if atmospheric carbon dioxide concentrations increase from current levels near 385 parts per million by volume (ppmv) to a peak of 450–600 ppmv over the coming century are irreversible dry-season rainfall reductions in several regions comparable to those of the “dust bowl” era and inexorable sea level rise. Thermal expansion of the warming ocean provides a conservative lower limit to irreversible global average sea level rise of at least 0.4–1.0 m if 21st century CO2 concentrations exceed 600 ppmv and 0.6–1.9 m for peak CO2 concentrations exceeding ≈1,000 ppmv. Additional contributions from glaciers and ice sheet contributions to future sea level rise are uncertain but may equal or exceed several meters over the next millennium or longer. PMID:19179281
Insights into the structure of mixed CO 2/CH 4 in gas hydrates
Everett, S. Michelle; Rawn, Claudia J.; Chakoumakos, Bryan C.; ...
2015-05-12
The exchange of carbon dioxide for methane in natural gas hydrates is an attractive approach to harvesting CH 4 for energy production while simultaneously sequestering CO 2. In addition to the energy and environmental implications, the solid solution of clathrate hydrate (CH 4) 1-x(CO 2) x·5.75H 2O provides a model system to study how the distinct bonding and shapes of CH 4 and CO 2 influence the structure and properties of the compound. In this paper, high-resolution neutron diffraction was used to examine mixed CO 2/CH 4 gas hydrates. CO 2-rich hydrates had smaller lattice parameters, which were attributed tomore » the higher affinity of the CO 2 molecule interacting with H 2O molecules that form the surrounding cages, and resulted in a reduction in the unit-cell volume. Experimental nuclear scattering densities illustrate how the cage occupants and energy landscape change with composition. Finally, these results provide important insights on the impact and mechanisms for the structure of mixed CH 4/CO 2 gas hydrate.« less
Jayan, Nithin; Jacob, Jaya Susan; Mathew, Mohan
2018-04-01
Not many studies have explored the correlation between arterial carbon dioxide tension (PaCO 2 ) and end-tidal carbon dioxide tension (ETCO 2 ) in surgeries requiring pneumoperitoneum of more than 1 hour duration with the patient in non-supine position. The aim of our study was to evaluate the correlation of ETCO 2 with PaCO 2 in patients undergoing laparoscopic nephrectomy under general anaesthesia. A descriptive study was performed in thirty patients undergoing laparoscopic nephrectomy from September 2014 to August 2015. The haemodynamic parameters, minute ventilation, PaCO 2 and ETCO 2 measured at three predetermined points during the procedure were analysed. Correlation was checked using Pearson's Correlation Coefficient Test. P <0.05 was considered statistically significant. Statistical analysis of the values showed a positive correlation between ETCO 2 and PaCO 2 ( P < 0.05). Following carbon dioxide insufflation, both ETCO 2 and PaCO 2 increased by 5.4 and 6.63 mmHg, respectively, at the end of the 1 st hour. The PaCO 2 -ETCO 2 gradient was found to increase during the 1 st hour following insufflation (4.07 ± 2.05 mmHg); it returned to the pre-insufflation values in another hour (2.93 ± 1.43 mmHg). Continuous ETCO 2 monitoring is a reliable indicator of the trend in arterial CO 2 fluctuations in the American Society of Anesthesiologists Grades 1 and 2 patients undergoing laparoscopic nephrectomy under general anaesthesia.
NASA Astrophysics Data System (ADS)
Patra, P. K.; Crisp, D.; W Kaiser, J.; Wunch, D.; Saeki, T.; Ichii, K.; Sekiya, T.; Wenneberg, P.; Griffith, D. W. T.; Feist, D. G.; Pollard, D.; Velazco, V. A.; De Maziere, M.; Sha, M. K.; Roehl, C. M.; Chatterjee, A.
2016-12-01
Uncertainties in estimates of regional fluxes of carbon dioxide (CO2) and other greenhouse gases derived from direct inventory methods or inferred from atmospheric observations has hindered the implementation of effective policy for reduction of emissions from anthropogenic activity. To improve the resolution and coverage of the atmospheric CO2 measurements for reducing CO2 flux uncertainty, NASA launched the OCO-2 satellite in 2014, and OCO-2 has been routinely returning almost one million soundings each day over the sunlit hemisphere. A powerful El Niño event in 2015-2016 - the third most intense since the 1950s - has exerted a large impact on the Earth's natural climate system. Here, we analyze column-averaged CO2 dry-air mole fraction (XCO2) observations during the period from September 2014 to February 2016 (18 months) together with ground-based remote sensing and in situ observations. From the differences between observations and simulations from an atmospheric chemistry-transport model, we estimated, that relative to the mean annual fluxes for 2011-2013, this El Niño has contributed to an excess CO2 flux from the Earth's surface (land+ocean) to the atmosphere in the range of 2.24-3.32 PgC (1 Pg = 1015 g). This anomalous CO2 flux results primarily from reduction in vegetation uptake due to drought and biomass burning. Improvements in modeling atmospheric-CO2 are required to attribute CO2 source changes at regional scales.
Roy, Lisa; Ghosh, Boyli; Paul, Ankan
2017-07-13
We employ quantum chemical calculations to study the hydrogenation of carbon dioxide by amine boranes, NMe 3 BH 3 ( Me3 AB) and NH 3 BH 3 (AB) weakly bonded to a bulkier Lewis acid, Al(C 6 F 5 ) 3 (LA). Additionally, computations have also been conducted to elucidate the mechanism of hydrogenation of carbon dioxide by Me3 AB while captured between one Lewis base (P(o-tol 3 ), LB) and two Lewis acids, Al(C 6 F 5 ) 3 . In agreement with the experiments, our computational study predicts that hydride transfer to conjugated HCO 2 - , generated in the reaction of Me3 AB-LA with CO 2 , is not feasible. This is in contrast to the potential hydrogenation of bound HCO 2 H, developed in the reduction of CO 2 with AB-LA, to further reduced species like H 2 C(OH) 2 . However, the FLP-trapped CO 2 effortlessly undergoes three hydride (H - ) transfers from Me3 AB to produce a CH 3 O - derivative. DFT calculations reveal that the preference for a H - abstraction by an intrinsically anionic formate moiety is specifically dependent on the electrophilicity of the 2 e - reduced carbon center, which in particular is controlled by the electron-withdrawing capability of the associated substituents on the oxygen. These theoretical predictions are justified by frontier molecular orbitals and molecular electrostatic potential plots. The global electrophicility index, which is a balance of electron affinity and hardness, reveals that the electrophilicity of the formate species undergoing hydrogenation is twice the electrophilicity of the ones where hydrogenation is not feasible. The computed activation energies at M06-2X/6-31++G(d,p) closely predict the observed reactivity. In addition, the possibility of a dissociative channel of the frustrated Lewis pair trapped CO 2 system has been ruled out on the basis of predominantly high endergonicity. Knowledge of the underlying principle of these reactions would be helpful in recruiting appropriate Lewis acids/amine boranes for effective reduction of CO 2 and its hydrogenated forms in a catalytic fashion.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Crandall, Dustin M.; Moore, Johnathan E.; Tudek, John K.
Evaluation of the fate and transport of carbon dioxide (CO 2) in deep reservoirs is crucial to the development of long-term geologic carbon sequestration (GCS) technologies. In this report, various studies using computed tomography (CT) scanning are utilized in conjunction with traditional flow tests to observe the multi-scale phenomena associated with CO 2 injection in geologic media. Pore scale analyses were performed to determine the infiltration characteristics of CO 2 into a brine saturated reservoir rock. Multiphase floods were performed to evaluate the saturation of CO 2 into a brine-saturated reservoir rock and determine how structural changes within the lithologymore » affect such interactions. Additionally, CO 2 induced swelling of unconventional reservoir rock was evaluated with respect to reductions in fracture transmissivity due to matrix swelling. These studies are just a few examples of the benefits of multi-scale CT imaging in conjunction with traditional laboratory methodology to gain a better understanding of the interactions between CO 2 and the lithologies it interacts with during GCS.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Maiti, Debtanu; Daza, Yolanda A.; Yung, Matthew M.
Density functional theory (DFT) based investigation of two parameters of prime interest -- oxygen vacancy and surface terminations along (100) and (110) planes -- has been conducted for La (1-x)Sr xFe(1-y)Co yO (3-more » $$\\delta$$) perovskite oxides in view of their application towards thermochemical carbon dioxide conversion reactions. The bulk oxygen vacancy formation energies for these mixed perovskite oxides are found to increase with increasing lanthanum and iron contents in the 'A' site and 'B' site, respectively. Surface terminations along (100) and (110) crystal planes are studied to probe their stability and their capabilities to accommodate surface oxygen vacancies. Amongst the various terminations, the oxygen-rich (110) surface and strontium-rich (100) surface are the most stable, while transition metal-rich terminations along (100) revealed preference towards the production of oxygen vacancies. The carbon dioxide adsorption strength, a key descriptor for CO 2 conversion reactions, is found to increase on oxygen vacant surfaces thus establishing the importance of oxygen vacancies in CO 2 conversion reactions. Amongst all the surface terminations, the lanthanum-oxygen terminated surface exhibited the strongest CO 2 adsorption strength. Finally, the theoretical prediction of the oxygen vacancy trends and the stability of the samples were corroborated by the temperature-programmed reduction and oxidation reactions and in situ XRD crystallography.« less
Muneer, Sowbiya; Kim, Tae Hwan; Choi, Byung Chul; Lee, Beom Seon; Lee, Jeong Hyun
2013-01-01
A study was conducted to determine the effect of carbon monoxide (CO), nitroxide (NOx) and sulfur dioxide (SO2) on ROS production, photosynthesis and ascorbate–glutathione pathway in strawberry plants. The results showed that both singlet oxygen (O2−1) and hydrogen peroxide (H2O2) content increased in CO, NOx and SO2 treated strawberry leaves. A drastic reduction of primary metabolism of plants (photosynthesis), with the closure of stomata, resulted in a reduction of protein, carbohydrate and sucrose content due to production of reactive oxygen species (ROS) under prolonged exposure of gas stress. The resulting antioxidant enzymes were increased under a low dose of gas stress, whereas they were decreased due to a high dose of gas stress. Our results indicate that increased ROS may act as a signal to induce defense responses to CO, NOx and SO2 gas stress. The increased level of antioxidant enzymes plays a significant role in plant protection due to which strawberry plants can be used as a hyperaccumulator to maintain environmental pollution, however, the defense capacity cannot sufficiently alleviate oxidative damage under prolonged exposure of CO, NOx and SO2 stress. PMID:25460723
Interfacial dynamics and solar fuel formation in dye-sensitized photoelectrosynthesis cells.
Song, Wenjing; Chen, Zuofeng; Glasson, Christopher R K; Hanson, Kenneth; Luo, Hanlin; Norris, Michael R; Ashford, Dennis L; Concepcion, Javier J; Brennaman, M Kyle; Meyer, Thomas J
2012-08-27
Dye-sensitized photoelectrosynthesis cells (DSPECs) represent a promising approach to solar fuels with solar-energy storage in chemical bonds. The targets are water splitting and carbon dioxide reduction by water to CO, other oxygenates, or hydrocarbons. DSPECs are based on dye-sensitized solar cells (DSSCs) but with photoexcitation driving physically separated solar fuel half reactions. A systematic basis for DSPECs is available based on a modular approach with light absorption/excited-state electron injection, and catalyst activation assembled in integrated structures. Progress has been made on catalysts for water oxidation and CO(2) reduction, dynamics of electron injection, back electron transfer, and photostability under conditions appropriate for water splitting. With added reductive scavengers, as surrogates for water oxidation, DSPECs have been investigated for hydrogen generation based on transient absorption and photocurrent measurements. Detailed insights are emerging which define kinetic and thermodynamic requirements for the individual processes underlying DSPEC performance. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Egland, Paul G.; Gibson, Jane; Harwood, Caroline S.
2001-01-01
We isolated a strain of Rhodopseudomonas palustris (RCB100) by selective enrichment in light on 3-chlorobenzoate to investigate the steps that it uses to accomplish anaerobic dechlorination. Analyses of metabolite pools as well as enzyme assays suggest that R. palustris grows on 3-chlorobenzoate by (i) converting it to 3-chlorobenzoyl coenzyme A (3-chlorobenzoyl–CoA), (ii) reductively dehalogenating 3-chlorobenzoyl–CoA to benzoyl-CoA, and (iii) degrading benzoyl-CoA to acetyl-CoA and carbon dioxide. R. palustris uses 3-chlorobenzoate only as a carbon source and thus incorporates the acetyl-CoA that is produced into cell material. The reductive dechlorination route used by R. palustris for 3-chlorobenzoate degradation differs from those previously described in that a CoA thioester, rather than an unmodified aromatic acid, is the substrate for complete dehalogenation. PMID:11229940
DOE Office of Scientific and Technical Information (OSTI.GOV)
Ali, Sardar, E-mail: alikhan-635@yahoo.com; Zabidi, Noor Asmawati Mohd, E-mail: noorasmawati-mzabidi@petronas.com.my; Subbarao, Duvvuri, E-mail: duvvuri-subbarao@petronas.com.my
2014-10-24
Catalysts were prepared via a wet impregnation method. Different physicochemical properties of the samples were revealed by transmission electron microscope (TEM), temperature programmed reduction (H{sub 2}-TPR) and carbon dioxide desorption (CO{sub 2}-desorption). Fischer-Tropsch reaction (FTS) was carried out in a fixed-bed microreactor at 220°C and 1 atm, with H{sub 2}/CO = 2v/v and space velocity, SV of 12L/g.h for 5 h. Various characterization techniques revealed that there was a stronger interaction between Co and Al{sub 2}O{sub 3} support compared to that of CNTs support. CNTs support increased the reducibility and decreased Co particle size. A significant increase in % CO conversion andmore » FTS reaction rate was observed over CNTs support compared to that of Co/Al{sub 2}O{sub 3}. Co/CNTs resulted in higher C{sub 5+} hydrocarbons selectivity compared to that of Co/Al{sub 2}O{sub 3} catalyst. CNTs are a better support for Co compared to Al{sub 2}O{sub 3}.« less
Polymers prepared from plant oils in liquid carbon dioxide
USDA-ARS?s Scientific Manuscript database
Recently, attention has been focused on the preparation of polymers in environmentally friendly media. Supercritical carbon dioxide (scCO2) is a promising candidate. The low toxicity of CO2 and lack of toxic solvent residues in the final products make CO2 an attractive medium for the synthesis of ...
Maiti, Debtanu; Daza, Yolanda A.; Yung, Matthew M.; ...
2016-03-07
Density functional theory (DFT) based investigation of two parameters of prime interest -- oxygen vacancy and surface terminations along (100) and (110) planes -- has been conducted for La (1-x)Sr xFe(1-y)Co yO (3-more » $$\\delta$$) perovskite oxides in view of their application towards thermochemical carbon dioxide conversion reactions. The bulk oxygen vacancy formation energies for these mixed perovskite oxides are found to increase with increasing lanthanum and iron contents in the 'A' site and 'B' site, respectively. Surface terminations along (100) and (110) crystal planes are studied to probe their stability and their capabilities to accommodate surface oxygen vacancies. Amongst the various terminations, the oxygen-rich (110) surface and strontium-rich (100) surface are the most stable, while transition metal-rich terminations along (100) revealed preference towards the production of oxygen vacancies. The carbon dioxide adsorption strength, a key descriptor for CO 2 conversion reactions, is found to increase on oxygen vacant surfaces thus establishing the importance of oxygen vacancies in CO 2 conversion reactions. Amongst all the surface terminations, the lanthanum-oxygen terminated surface exhibited the strongest CO 2 adsorption strength. Finally, the theoretical prediction of the oxygen vacancy trends and the stability of the samples were corroborated by the temperature-programmed reduction and oxidation reactions and in situ XRD crystallography.« less
Koulouris, N G; Latsi, P; Dimitroulis, J; Jordanoglou, B; Gaga, M; Jordanoglou, J
2001-06-01
The lack of methodology for measuring the alveolar carbon dioxide tension (PA,CO2) has forced investigators to make several assumptions, such as that PA,CO2 is equal to end-tidal (PET,CO2) and arterial CO2 tension (Pa,CO2). The present study measured the mean PA,CO2 and Bohr's dead space ratio (Bohr's dead space/tidal volume (VD,Bohr/VT)) during tidal breathing. The method used is a new, simple and noninvasive technique, based on the analysis of the expired CO2 volume per breath (VCO2) versus the exhaled VT. This curve was analysed in 21 normal, healthy subjects and 35 chronic obstructive pulmonary disease (COPD) patients breathing tidally through a mouthpiece apparatus in the sitting position. It is shown that: 1) PA,CO2 is similar to Pa,CO2 in normal subjects, whilst it is significantly lower than Pa,CO2 in COPD patients; 2) PA,CO2 is significantly higher than PET,CO2 in all subjects, especially in COPD patients; 3) VD,Bohr/VT is increased in COPD patients as compared to normal subjects; and 4) VD,Bohr/VT is lower than the "physiological" dead space ratio (VD,phys/VT) in COPD patients. It is concluded that the expired carbon dioxide versus tidal volume curve is a useful tool for research and clinical work, because it permits the noninvasive and accurate measurement of Bohr's dead space and mean alveolar carbon dioxide tension accurately during spontaneous breathing.
da Rosa, Gabriel Martins; Moraes, Luiza; Cardias, Bruna Barcelos; de Souza, Michele da Rosa Andrade Zimmermann; Costa, Jorge Alberto Vieira
2015-09-01
The chemical absorption of carbon dioxide (CO2) is a technique used for the mitigation of the greenhouse effect. However, this process consumes high amounts of energy to regenerate the absorbent and to separate the CO2. CO2 removal by microalgae can be obtained via the photosynthesis process. The objective of this study was to investigate the cultivation and the macromolecules production by Spirulina sp. LEB 18 with the addition of monoethanolamine (MEA) and CO2. In the cultivation with MEA, were obtained higher results of specific growth rate, biomass productivity, CO2 biofixation, CO2 use efficiency, and lower generation time. Besides this, the carbohydrate concentration obtained at the end of this assay was approximately 96.0% higher than the control assay. Therefore, Spirulina can be produced using medium recycle and the addition of MEA, thereby promoting the reduction of CO2 emissions and showing potential for areas that require higher concentrations of carbohydrates, such as in bioethanol production. Copyright © 2015 Elsevier Ltd. All rights reserved.
Allowable exposure limits for carbon dioxide during extravehicular activity
NASA Technical Reports Server (NTRS)
Seter, Andrew J.
1993-01-01
The intent was to review the research pertaining to human exposure to carbon dioxide (CO2) and to recommend allowable exposure limits for extravehicular activity (EVA). Respiratory, renal, and gastrointestinal systems may be adversely affected by chronic low dose CO2 exposure. Ventilation was increased 15 percent with 1 percent CO2 and 50 percent with 2 percent CO2. Chronic exposure to less than 2 percent CO2 led to 20 day cycles of uncompensated and compensated respiratory acidosis. Acid-base changes were small. Histopathologic changes in guinea pig lungs have been noted with long term exposure to 1 percent CO2. No changes were seen with exposure to 0.5 percent CO2. Cycling of bone calcium stores with associated changes in blood and urinary calcium levels occurs with long term CO2 exposure. Histologic changes in bone have been noted in guinea pigs exposed to 1 percent CO2. Renal calcification has been noted in guinea pigs with exposure to as low as 0.5 percent CO2. An increase in gastric acidity was noted in subjects with long term exposure to 1 percent CO2. Cardiovascular and neurologic function were largely unaffected. A decrease in the incidence of respiratory, renal, and gastrointestinal disease was noted in submariners coincident with a decrease in ambient CO2 from 1.2 percent to 0.8-0.9 percent. Oxygen (O2) and CO2 stimulate respiration independently and cumulatively. The addition of CO2 to high dose O2 led to the faster onset of seizure activity in mice. Experiments evaluating the physiologic responses to intermittent, repetitive exposures to low dose CO2 and 100 percent O2 mixtures should be performed. A reduction in the current NASA standard for CO2 exposure during EVA of 1 percent (7.6 mmHg) for nominal and 2 percent (15.2 mmHg) for heavy exertion to 0.5 percent (3.8 mmHg) for nominal and 1 percent (7.6 mmHg) for heavy exertion may be prudent. At a minimum, the current NASA standard should not be liberalized.
Wang, Jing; Zhu, Ting; Ho, Ghim Wei
2016-07-07
Phosphates play significant roles in plant photosynthesis by mediating electron transportation and furnishing energy for CO2 reduction. Motivated by this, we demonstrate herein an artificial solar-to-fuel conversion system, involving versatile copper phosphate microflowers as template and titanium dioxide nanoparticles as host photocatalyst. The elaborate flowerlike architectures, coupled with a unique proton-reduction cycle from interchangeability of different species of orthophosphate ions, not only offer a 2D nanosheet platform for an optimal heterostructure interface but also effectively augment charge-carrier transfer, thereby contributing to enhanced photoactivity and hydrogen generation. These nature-inspired, phosphate-derived nanocomposites advance the synthesis of a large variety of functional materials, which holds great potential for photochemical, photoelectric and catalytic applications. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
The inhibition of marine nitrification by ocean disposal of carbon dioxide.
Huesemann, Michael H; Skillman, Ann D; Crecelius, Eric A
2002-02-01
In an attempt to reduce the threat of global warming, it has been proposed that the rise of atmospheric carbon dioxide concentrations be reduced by the ocean disposal of CO2 from the flue gases of fossil fuel-fired power plants. The release of large amounts of CO2 into mid or deep ocean waters will result in large plumes of acidified seawater with pH values ranging from 6 to 8. In an effort to determine whether these CO2-induced pH changes have any effect on marine nitrification processes, surficial (euphotic zone) and deep (aphotic zone) seawater samples were sparged with CO2 for varying time durations to achieve a specified pH reduction, and the rate of microbial ammonia oxidation was measured spectrophotometrically as a function of pH using an inhibitor technique. For both seawater samples taken from either the euphotic or aphotic zone, the nitrification rates dropped drastically with decreasing pH. Relative to nitrification rates in the original seawater at pH 8, nitrification rates were reduced by ca. 50% at pH 7 and more than 90% at pH 6.5. Nitrification was essentially completely inhibited at pH 6. These findings suggest that the disposal of CO2 into mid or deep oceans will most likely result in a drastic reduction of ammonia oxidation rates within the pH plume and the concomitant accumulation of ammonia instead of nitrate. It is unlikely that ammonia will reach the high concentration levels at which marine aquatic organisms are known to be negatively affected. However, if the ammonia-rich seawater from inside the pH plume is upwelled into the euphotic zone, it is likely that changes in phytoplankton abundance and community structure will occur. Finally, the large-scale inhibition of nitrification and the subsequent reduction of nitrite and nitrate concentrations could also result in a decrease of denitrification rates which, in turn, could lead to the buildup of nitrogen and unpredictable eutrophication phenomena. Clearly, more research on the environmental effects of ocean disposal of CO2 is needed to determine whether the potential costs related to marine ecosystem disturbance and disruption can be justified in terms of the perceived benefits that may be achieved by temporarily delaying global warming.
Basis for the ICRP’s updated biokinetic model for carbon inhaled as CO 2
Leggett, Richard W.
2017-03-02
Here, the International Commission on Radiological Protection (ICRP) is updating its biokinetic and dosimetric models for occupational intake of radionuclides (OIR) in a series of reports called the OIR series. This paper describes the basis for the ICRP's updated biokinetic model for inhalation of radiocarbon as carbon dioxide (CO 2) gas. The updated model is based on biokinetic data for carbon isotopes inhaled as carbon dioxide or injected or ingested as bicarbonatemore » $$({{{\\rm{HCO}}}_{3}}^{-}).$$ The data from these studies are expected to apply equally to internally deposited (or internally produced) carbon dioxide and bicarbonate based on comparison of excretion rates for the two administered forms and the fact that carbon dioxide and bicarbonate are largely carried in a common form (CO 2–H$${{{\\rm{CO}}}_{3}}^{-})$$ in blood. Compared with dose estimates based on current ICRP biokinetic models for inhaled carbon dioxide or ingested carbon, the updated model will result in a somewhat higher dose estimate for 14C inhaled as CO 2 and a much lower dose estimate for 14C ingested as bicarbonate.« less
Basis for the ICRP’s updated biokinetic model for carbon inhaled as CO 2
DOE Office of Scientific and Technical Information (OSTI.GOV)
Leggett, Richard W.
Here, the International Commission on Radiological Protection (ICRP) is updating its biokinetic and dosimetric models for occupational intake of radionuclides (OIR) in a series of reports called the OIR series. This paper describes the basis for the ICRP's updated biokinetic model for inhalation of radiocarbon as carbon dioxide (CO 2) gas. The updated model is based on biokinetic data for carbon isotopes inhaled as carbon dioxide or injected or ingested as bicarbonatemore » $$({{{\\rm{HCO}}}_{3}}^{-}).$$ The data from these studies are expected to apply equally to internally deposited (or internally produced) carbon dioxide and bicarbonate based on comparison of excretion rates for the two administered forms and the fact that carbon dioxide and bicarbonate are largely carried in a common form (CO 2–H$${{{\\rm{CO}}}_{3}}^{-})$$ in blood. Compared with dose estimates based on current ICRP biokinetic models for inhaled carbon dioxide or ingested carbon, the updated model will result in a somewhat higher dose estimate for 14C inhaled as CO 2 and a much lower dose estimate for 14C ingested as bicarbonate.« less
Predicting the Response of Molluscs to the Impact of Ocean Acidification
Parker, Laura M.; Ross, Pauline M.; O’Connor, Wayne A.; Pörtner, Hans O.; Scanes, Elliot; Wright, John M.
2013-01-01
Elevations in atmospheric carbon dioxide (CO2) are anticipated to acidify oceans because of fundamental changes in ocean chemistry created by CO2 absorption from the atmosphere. Over the next century, these elevated concentrations of atmospheric CO2 are expected to result in a reduction of the surface ocean waters from 8.1 to 7.7 units as well as a reduction in carbonate ion (CO32−) concentration. The potential impact that this change in ocean chemistry will have on marine and estuarine organisms and ecosystems is a growing concern for scientists worldwide. While species-specific responses to ocean acidification are widespread across a number of marine taxa, molluscs are one animal phylum with many species which are particularly vulnerable across a number of life-history stages. Molluscs make up the second largest animal phylum on earth with 30,000 species and are a major producer of CaCO3. Molluscs also provide essential ecosystem services including habitat structure and food for benthic organisms (i.e., mussel and oyster beds), purification of water through filtration and are economically valuable. Even sub lethal impacts on molluscs due to climate changed oceans will have serious consequences for global protein sources and marine ecosystems. PMID:24832802
Direct and reversible hydrogenation of CO2 to formate by a bacterial carbon dioxide reductase.
Schuchmann, K; Müller, V
2013-12-13
Storage and transportation of hydrogen is a major obstacle for its use as a fuel. An increasingly considered alternative for the direct handling of hydrogen is to use carbon dioxide (CO2) as an intermediate storage material. However, CO2 is thermodynamically stable, and developed chemical catalysts often require high temperatures, pressures, and/or additives for high catalytic rates. Here, we present the discovery of a bacterial hydrogen-dependent carbon dioxide reductase from Acetobacterium woodii directly catalyzing the hydrogenation of CO2. We also demonstrate a whole-cell system able to produce formate as the sole end product from dihydrogen (H2) and CO2 as well as syngas. This discovery opens biotechnological alternatives for efficient CO2 hydrogenation either by using the isolated enzyme or by employing whole-cell catalysis.
Lovley, D.R.; Lonergan, D.J.
1990-01-01
The dissimilatory Fe(III) reducer, GS-15, is the first microorganism known to couple the oxidation of aromatic compounds to the reduction of Fe(III) and the first example of a pure culture of any kind known to anaerobically oxidize an aromatic hydrocarbon, toluene. In this study, the metabolism of toluene, phenol, and p-cresol by GS-15 was investigated in more detail. GS-15 grew in an anaerobic medium with toluene as the sole electron donor and Fe(III) oxide as the electron acceptor. Growth coincided with Fe(III) reduction. [ring-14C]toluene was oxidized to 14CO2, and the stoichiometry of 14CO2 production and Fe(III) reduction indicated that GS-15 completely oxidized toluene to carbon dioxide with Fe(III) as the electron acceptor. Magnetite was the primary iron end product during toluene oxidation. Phenol and p-cresol were also completely oxidized to carbon dioxide with Fe(III) as the sole electron acceptor, and GS-15 could obtain energy to support growth by oxidizing either of these compounds as the sole electron donor. p-Hydroxybenzoate was a transitory extracellular intermediate of phenol and p-cresol metabolism but not of toluene metabolism. GS-15 oxidized potential aromatic intermediates in the oxidation of toluene (benzylalcohol and benzaldehyde) and p-cresol (p-hydroxybenzylalcohol and p-hydroxybenzaldehyde). The metabolism described here provides a model for how aromatic hydrocarbons and phenols may be oxidized with the reduction of Fe(III) in contaminated aquifers and petroleum-containing sediments.
Graphene-Immobilized fac-Re(bipy)(CO)3Cl for Syngas Generation from Carbon Dioxide.
Zhou, Xin; Micheroni, Daniel; Lin, Zekai; Poon, Christopher; Li, Zhong; Lin, Wenbin
2016-02-17
We report the synthesis of fac-M(4-amino-bipy)(CO)3X (M = Mn and X = Br or M = Re and X = Cl, with bipy = 2,2'-bipyridine), their immobilization on graphene oxide (GrO) via diazonium grafting, and the use of Re-functionalized GrO for electrocatalytic syngas production. Infrared (IR) spectroscopy, X-ray absorption fine structure (XAFS) spectroscopy, and electrocatalysis indicated successful grafting of the Re catalyst onto GrO. Re-functionalized GrO was then deposited onto a glassy carbon electrode (GCE) for CO2 reduction. Investigation of the Re-functionalized GCE for syngas production was performed in a CO2-saturated acetonitrile solution with 3.1 M H2O as the proton source and 0.1 M tetrabutylammonium hexafluorophosphate (TBAPF6) as the supporting electrolyte. Cyclic voltammetry (CV), controlled potential electrolysis (CPE), and gas chromatography (GC) were employed to determine its CO2-to-CO conversion performance. The Re catalyst shows a turnover frequency (TOF) for generating CO up to 4.44 s(-1) with a CO/H2 ratio of 7:5.
Development of a Rapid Cycling CO2 and H2O Removal Sorbent
NASA Technical Reports Server (NTRS)
Alptekin, Gokhan; Cates, Matthew; Bernal, Casey; Dubovik, Margarita; Paul, Heather L.
2007-01-01
The National Aeronautics and Space Administration (NASA) planned future missions set stringent demands on the design of the Portable Life Support System (PLSS), requiring dramatic reductions in weight, decreased reliance on supplies and greater flexibility on the types of missions. Use of regenerable systems that reduce weight and volume of the Extravehicular Mobility Unit (EMU) is of critical importance to NASA, both for low orbit operations and for long duration manned missions. The carbon dioxide and humidity control unit in the existing PLSS design is relatively large, since it has to remove and store eight hours worth of carbon dioxide (CO2). If the sorbent regeneration can be carried out during the Extravehicular Activity (EVA) with a relatively high regeneration frequency, the size of the sorbent canister and weight can be significantly reduced. TDA Research, Inc. is developing compact, regenerable sorbent materials to control CO2 and humidity in the space suit ventilation loop. The sorbent can be regenerated using space vacuum during the EVA, eliminating all CO2 and humidity duration-limiting elements in the life support system. The material also has applications in other areas of space exploration including long duration exploration missions requiring regenerable technologies and possibly the Crew Exploration Vehicle (CEV) spacecraft. This paper summarizes the results of the sorbent development, testing, and evaluation efforts to date.
NASA Astrophysics Data System (ADS)
Nezzal, Ghania; Benammar, Souad; Hamouni, Samia; Meziane, Dalila; Naama, Sabrina; Abdessemed, Djamel
2015-04-01
Referring to the last World Conference COPENHAGEN (2010), endorsed by the United Nations,to '' RISKS OF CLIMATE CHANGES ', states had not reached an agreement to work fairly, in an international program, to limit Carbon dioxide emissions into the atmosphere, to put off it, to the next (in 2015), the right decisions, despite the recommendations of the 'IPCC'. Based on the natural reaction of photosynthesis, which converts carbon dioxide in the presence of water and sun, to '' OSA'' ', it is natural that scientists believe to implement an artificial conversion of CO2 in a renewable energy faster. Our contribution focuses on the same goals, by a different line. In this perspective, nano-materials, catalysts, pervaporation membranes, pervaporation unit, and a photo-reactor prototype, have been made. A summary of the preliminary results presented: For example, are given the concentrations of the various species present in a aqueous solution of sodium hydrogen carbonate, 0.5M, saturated with CO2, at standard temperature and pressure: (CO2) = 1M; (H2CO3) = 0,038M; (HCO3-) = 0,336M; (CO3 --) = 0,34M; pH = 7.33, an overall concentration = 1,714M, more than three times that of the initial solution. It is in such conditions that the conversion of carbon dioxide by the hydrogen produced in situ by electrolysis, in fuel, must be done in the presence of catalyst, under UV radiation. For electrodes, a nano-porous layer was formed on their surface to receive the suitable catalyst. These lats prepared, are made of porous supports (montmorillonite, aluminum and silicon oxides) into which are inserted the metal precursor, by impregnation interactive, in Iron, cobalt, nickel salt solutions, cobalt, nickel. Their performance has been identified by the reduction of para- nitrophenol, to para-aminophenol in aqueous medium in the presence of sodium borohydride. This is the catalyst 'Cobalt supported by SiO2'' that gave the best conversion, 99.5% instead of 99.7%, for a platinum catalyst. The separation of hydrocarbon products, in the considered aqueous medium, continuously, has been studied to determine optimum conditions by pervaporation. For this purpose, membranes of poly-sulfone and poly-dimethylsiloxane, were prepared and characterized in terms of flow pervaporat (J), and solute / solvent separation factor (α). Thus, the developed membranes have equivalent performance to commercial membranes. More accurate results will be the subject of this communication.
Carbon dioxide-water clathrate as a reservoir of CO2 on Mars
NASA Technical Reports Server (NTRS)
Dobrovolskis, A.; Ingersell, A. P.
1975-01-01
It has been suggested that the residual polar caps of Mars contain a resorvoir of permanently frozen carbon dioxide which is controlling the atmospheric pressure. However, observational data and models of the polar heat balance suggest that the temperatures of the Martian poles are too high for solid CO2 to survive permanently. On the other hand, the icelike compound carbon dioxide-water clathrate could function as a CO2 reservoir instead of solid CO2, because it is stable at higher temperatures. This paper shows that the permanent polar caps may contain several millibars of CO2 in the form of clathrate, and discusses the implications of this permanent clathrate reservoir for the present and past atmospheric pressure on Mars.
NASA Astrophysics Data System (ADS)
Helfter, Carole; Tremper, Anja H.; Halios, Christoforos H.; Kotthaus, Simone; Bjorkegren, Alex; Grimmond, C. Sue B.; Barlow, Janet F.; Nemitz, Eiko
2016-08-01
We report on more than 3 years of measurements of fluxes of methane (CH4), carbon monoxide (CO) and carbon dioxide (CO2) taken by eddy-covariance in central London, UK. Mean annual emissions of CO2 in the period 2012-2014 (39.1 ± 2.4 ktons km-2 yr-1) and CO (89 ± 16 tons km-2 yr-1) were consistent (within 1 and 5 % respectively) with values from the London Atmospheric Emissions Inventory, but measured CH4 emissions (72 ± 3 tons km-2 yr-1) were over two-fold larger than the inventory value. Seasonal variability was large for CO with a winter to summer reduction of 69 %, and monthly fluxes were strongly anti-correlated with mean air temperature. The winter increment in CO emissions was attributed mainly to vehicle cold starts and reduced fuel combustion efficiency. CO2 fluxes were 33 % higher in winter than in summer and anti-correlated with mean air temperature, albeit to a lesser extent than for CO. This was attributed to an increased demand for natural gas for heating during the winter. CH4 fluxes exhibited moderate seasonality (21 % larger in winter), and a spatially variable linear anti-correlation with air temperature. Differences in resident population within the flux footprint explained up to 90 % of the spatial variability of the annual CO2 fluxes and up to 99 % for CH4. Furthermore, we suggest that biogenic sources of CH4, such as wastewater, which is unaccounted for by the atmospheric emissions inventories, make a substantial contribution to the overall budget and that commuting dynamics in and out of central business districts could explain some of the spatial and temporal variability of CO2 and CH4 emissions. To our knowledge, this study is unique given the length of the data sets presented, especially for CO and CH4 fluxes. This study offers an independent assessment of "bottom-up" emissions inventories and demonstrates that the urban sources of CO and CO2 are well characterized in London. This is however not the case for CH4 emissions which are heavily underestimated by the inventory approach. Our results and others point to opportunities in the UK and abroad to identify and quantify the "missing" sources of urban methane, revise the methodologies of the emission inventories and devise emission reduction strategies for this potent greenhouse gas.
DOE Office of Scientific and Technical Information (OSTI.GOV)
BEST-Cities is designed to provide city authorities with strategies they can follow to reduce city-wide carbon dioxide (CO2) and methane (CH4) emissions. The tool quickly assesses local energy use and energy-related CO2 emissions across nine sectors (i.e., industry, public and commercial buildings, residential buildings, transportation, power and heat, street lighting, water & wastewater, solid waste, and urban green space), giving officials a comprehensive perspective on their local carbon performance. Cities can also use the tool to benchmark their energy and emissions performance to other cities inside and outside China, and identify those sectors with the greatest energy saving and emissionsmore » reduction potential.« less
Role of Marine Biology in Glacial-Interglacial CO2 Cycles
NASA Astrophysics Data System (ADS)
Kohfeld, Karen E.; Le Quéré, Corinne; Harrison, Sandy P.; Anderson, Robert F.
2005-04-01
It has been hypothesized that changes in the marine biological pump caused a major portion of the glacial reduction of atmospheric carbon dioxide by 80 to 100 parts per million through increased iron fertilization of marine plankton, increased ocean nutrient content or utilization, or shifts in dominant plankton types. We analyze sedimentary records of marine productivity at the peak and the middle of the last glacial cycle and show that neither changes in nutrient utilization in the Southern Ocean nor shifts in plankton dominance explain the CO2 drawdown. Iron fertilization and associated mechanisms can be responsible for no more than half the observed drawdown.
NASA Astrophysics Data System (ADS)
Lucich, Stephen M.
In the United States, the buildings sector is responsible for approximately 40% of the national carbon dioxide (CO2) emissions. CO2 is created during the generation of heat and electricity, and has been linked to climate change, acid rain, a variety of health threats, surface water depletion, and the destruction of natural habitats. Building energy modeling is a powerful educational tool that building owners, architects, engineers, city planners, and policy makers can use to make informed decisions. The aim of this thesis is to simulate the reduction in CO2 emissions that may be achieved for three commercial buildings located in Salt Lake City, UT. The following two questions were used to guide this process: 1. How much can a building's annual CO2 emissions be reduced through a specific energy efficiency upgrade or policy? 2. How much can a building's annual CO2 emissions be reduced through the addition of a photovoltaic (PV) array? How large should the array be? Building energy simulations were performed with the Department of Energy's EnergyPlus software, commercial reference building models, and TMY3 weather data. The chosen models were a medium office building, a primary school, and a supermarket. Baseline energy consumption data were simulated for each model in order to identify changes that would have a meaningful impact. Modifications to the buildings construction and operation were considered before a PV array was incorporated. These modifications include (1) an improved building envelope, (2) reduced lighting intensity, and (3) modified HVAC temperature set points. The PV array sizing was optimized using a demand matching approach based on the method of least squares. The arrays tilt angle was optimized using the golden section search algorithm. Combined, energy efficiency upgrades and the PV array reduced building CO2 emissions by 58.6, 54.0, and 52.2% for the medium office, primary school, and supermarket, respectively. However, for these models, it was determined that the addition of a PV array is not feasible from a purely economic viewpoint. Several avenues for expansion of this research are presented in Chapter 5.
Delgado-Abad, Thais; Martínez-Ferrer, Jaime; Acerete, Rafael; Asensio, Gregorio; Mello, Rossella; González-Núñez, María Elena
2016-07-06
Ethanol () inhibits SN1 reactions of alkyl halides in supercritical carbon dioxide (scCO2) and gives no ethers as products. The unexpected behaviour of alcohols in the reaction of alkyl halides with 1,3-dimethoxybenzene () in scCO2 under different conditions is rationalised in terms of Brønsted and Lewis acid-base equilibria of reagents, intermediates, additives and products in a singular solvent characterised by: (i) the strong quadrupole and Lewis acid character of carbon dioxide, which hinders SN2 paths by strongly solvating basic solutes; (ii) the weak Lewis base character of carbon dioxide, which prevents it from behaving as a proton sink; (iii) the compressible nature of scCO2, which enhances the impact of preferential solvation on carbon dioxide availability for the solvent-demanding rate determining step.
Disintegration of Carbon Dioxide Molecules in a Microwave Plasma Torch
Kwak, Hyoung S.; Uhm, Han S.; Hong, Yong C.; Choi, Eun H.
2015-01-01
A pure carbon dioxide torch is generated by making use of 2.45 GHz microwave. Carbon dioxide gas becomes the working gas and produces a stable carbon dioxide torch. The torch volume is almost linearly proportional to the microwave power. Temperature of the torch flame is measured by making use of optical spectroscopy and thermocouple. Two distinctive regions are exhibited, a bright, whitish region of high-temperature zone and a bluish, dimmer region of relatively low-temperature zone. Study of carbon dioxide disintegration and gas temperature effects on the molecular fraction characteristics in the carbon dioxide plasma of a microwave plasma torch under atmospheric pressure is carried out. An analytical investigation of carbon dioxide disintegration indicates that substantial fraction of carbon dioxide molecules disintegrate and form other compounds in the torch. For example, the normalized particle densities at center of plasma are given by nCO2/nN = 6.12 × 10−3, nCO/nN = 0.13, nC/nN = 0.24, nO/nN = 0.61, nC2/nN = 8.32 × 10−7, nO2/nN = 5.39 × 10−5, where nCO2, nCO, nC, nO, nC2, and nO2 are carbon dioxide, carbon monoxide, carbon and oxygen atom, carbon and oxygen molecule densities, respectively. nN is the neutral particle density. Emission profiles of the oxygen and carbon atom radicals and the carbon monoxide molecules confirm the theoretical predictions of carbon dioxide disintegration in the torch. PMID:26674957
Xiang, Tianyu; Xin, Feng; Zhao, Can; Lou, Shuo; Qu, Wenxiu; Wang, Yong; Song, Yuexiao; Zhang, Shuangfang; Yin, Xiaohong
2018-05-15
A synthetic process was exploited to fabricate patchy CuO evenly planted on cubic NaTaO 3 for photocatalytically reducing CO 2 in isopropanol. The nano patches of CuO with about 15 nm in size were uniformly distributed on the surface of NaTaO 3 via a phase-transfer protocol and solvothermal synthesis. The crystal phase, morphology, composition, optical absorption and charge separation of as-prepared CuO-NaTaO 3 were characterized by XRD, SEM, TEM, EDX, XPS, UV-Vis and PL. The results of photocatalytic reduction of CO 2 confirmed that the CuO patched NaTaO 3 possessed better ability to separate charge carriers and selectively reduce CO 2 to methanol than CuO directly loaded NaTaO 3 using the traditional liquid phase reduction procedure after comparing the methanol yields. Furthermore, 5 wt% CuO patched NaTaO 3 led to the highest methanol yield of 1302.22 μmol g -1 h -1 . A redox mechanism was proposed and illustrated in a schematic diagram. Copyright © 2018 Elsevier Inc. All rights reserved.
The need for carbon dioxide disposal: A threat and an opportunity
DOE Office of Scientific and Technical Information (OSTI.GOV)
Lackner, K.S.; Butt, D.P.; Wendt, C.H.
Ready energy is a cornerstone of modern society. The policies outlined at the recent Kyoto conference have put in question the largest, most readily available and most cost-effective energy resource available. Even if a doubling of atmospheric CO{sub 2} is deemed acceptable, emission reductions worldwide would have to be drastic. For 10 billion people to share equally into the 1990 emission level would allow a per capita emission of 10% of the current US level. Substantial reductions in CO{sub 2} emissions to the atmosphere are unavoidable. Uncertain is the time available to accomplish this reduction. There are also reasons tomore » be optimistic about the future of coal and other fossil fuels. Barring a surprise technological breakthrough in alternative energies, fossil energy consumption is bound to grow. Political and economic drivers even stronger than the threat of climate change favor economic growth and therefore increased energy consumption. To resolve this apparent contradiction requires new technologies that prevent CO{sub 2} generated by combustion from entering the atmosphere. The authors will outline available technologies and show how the coal industry can adapt to them.« less
Late Miocene decoupling of oceanic warmth and atmospheric carbon dioxide forcing.
LaRiviere, Jonathan P; Ravelo, A Christina; Crimmins, Allison; Dekens, Petra S; Ford, Heather L; Lyle, Mitch; Wara, Michael W
2012-06-06
Deep-time palaeoclimate studies are vitally important for developing a complete understanding of climate responses to changes in the atmospheric carbon dioxide concentration (that is, the atmospheric partial pressure of CO(2), p(co(2))). Although past studies have explored these responses during portions of the Cenozoic era (the most recent 65.5 million years (Myr) of Earth history), comparatively little is known about the climate of the late Miocene (∼12-5 Myr ago), an interval with p(co(2)) values of only 200-350 parts per million by volume but nearly ice-free conditions in the Northern Hemisphere and warmer-than-modern temperatures on the continents. Here we present quantitative geochemical sea surface temperature estimates from the Miocene mid-latitude North Pacific Ocean, and show that oceanic warmth persisted throughout the interval of low p(co(2)) ∼12-5 Myr ago. We also present new stable isotope measurements from the western equatorial Pacific that, in conjunction with previously published data, reveal a long-term trend of thermocline shoaling in the equatorial Pacific since ∼13 Myr ago. We propose that a relatively deep global thermocline, reductions in low-latitude gradients in sea surface temperature, and cloud and water vapour feedbacks may help to explain the warmth of the late Miocene. Additional shoaling of the thermocline after 5 Myr ago probably explains the stronger coupling between p(co(2)), sea surface temperatures and climate that is characteristic of the more recent Pliocene and Pleistocene epochs.
A regenerative process for carbon dioxide removal and hydrogen production in IGCC
NASA Astrophysics Data System (ADS)
Hassanzadeh Khayyat, Armin
Advanced power generation technologies, such as Integrated Gasification-Combined Cycles (IGCC) processes, are among the leading contenders for power generation conversion because of their significantly higher efficiencies and potential environmental advantages, compared to conventional coal combustion processes. Although the increased in efficiency in the IGCC processes will reduce the emissions of carbon dioxide per unit of power generated, further reduction in CO2 emissions is crucial due to enforcement of green house gases (GHG) regulations. In IGCC processes to avoid efficiency losses, it is desirable to remove CO2 in the temperature range of 300° to 500°C, which makes regenerable MgO-based sorbents ideal for such operations. In this temperature range, CO2 removal results in the shifting of the water-gas shift (WGS) reaction towards significant reduction in carbon monoxide (CO), and enhancement in hydrogen production. However, regenerable, reactive and attrition resistant sorbents are required for such application. In this work, a highly reactive and attrition resistant regenerable MgO-based sorbent is prepared through dolomite modification, which can simultaneously remove carbon dioxide and enhance hydrogen production in a single reactor. The results of the experimental tests conducted in High-Pressure Thermogravimetric Analyzer (HP-TGA) and high-pressure packed-bed units indicate that in the temperature range of 300° to 500°C at 20 atm more than 95 molar percent of CO2 can be removed from the simulated coal gas, and the hydrogen concentration can be increased to above 70 percent. However, a declining trend is observed in the capacity of the sorbent exposed to long-term durability analysis, which appears to level off after about 20 cycles. Based on the physical and chemical analysis of the sorbent, a two-zone expanding grain model was applied to obtain an excellent fit to the carbonation reaction rate data at various operating conditions. The modeling results indicate that more than 90 percent purification of hydrogen is achievable, either by increasing the activity of the sorbent towards water-gas shift reaction or by mixing the sorbent bed with a commercialized water-gas shift catalyst. The preliminary economical evaluation of the MgO-based process indicates that this process can be economically viable compared to the commercially available WGS/Selexol(TM) processes.
Fixation of carbon dioxide by a hydrogen-oxidizing bacterium for value-added products.
Yu, Jian
2018-06-09
With rapid technology progress and cost reduction, clean hydrogen from water electrolysis driven by renewable powers becomes a potential feedstock for CO 2 fixation by hydrogen-oxidizing bacteria. Cupriavidus necator (formally Ralstonia eutropha), a representative member of the lithoautotrophic prokaryotes, is a promising producer of polyhydroxyalkanoates and single cell proteins. This paper reviews the fundamental properties of the hydrogen-oxidizing bacterium, the metabolic activities under limitation of individual gases and nutrients, and the value-added products from CO 2 , including the products with large potential markets. Gas fermentation and bioreactor safety are discussed for achieving high cell density and high productivity of desired products under chemolithotrophic conditions. The review also updates the recent research activities in metabolic engineering of C. necator to produce novel metabolites from CO 2 .
Costentin, Cyrille; Robert, Marc; Savéant, Jean-Michel
2015-12-15
Recent attention aroused by the reduction of carbon dioxide has as main objective the production of useful products, the "solar fuels", in which solar energy would be stored. One route to this goal is the design of photochemical schemes that would operate this conversion using directly sun light energy. An indirect approach consists in first converting sunlight energy into electricity then using it to reduce CO2 electrochemically. Conversion of carbon dioxide into carbon monoxide is thus a key step through the classical dihydrogen-reductive Fischer-Tropsch chemistry. Direct and catalytic electrochemical CO2 reduction already aroused active interest during the 1980-1990 period. The new wave of interest for these matters that has been growing since 2012 is in direct conjunction with modern energy issues. Among molecular catalysts, electrogenerated Fe(0) porphyrins have proved to be particularly efficient and robust. Recent progress in this field has closely associated the search of more and more efficient catalysts in the iron porphyrin family with an unprecedentedly rigorous deciphering of mechanisms. Accordingly, the coupling of proton transfer with electron transfer and breaking of one of the two C-O bonds of CO2 have been the subjects of relentless scrutiny and mechanistic analysis with systematic investigation of the degree of concertedness of these three events. Catalysis of the electrochemical CO2-to-CO conversion has thus been a good testing ground for the mechanism diagnostic strategies and the all concerted reactivity model proposed then. The role of added Brönsted acids, both as H-bond providers and proton donors, has been elucidated. These efforts have been a preliminary to the inclusion of the acid functionalities within the catalyst molecule, giving rise to considerable increase of the catalytic efficiency. The design of more and more efficient catalysts made it necessary to propose "catalytic Tafel plots" relating the turnover frequency to the overpotential as a rational way of benchmarking the catalysts within iron porphyrins and among all available molecular catalysts, independently of the characteristics of the electrolytic cell in use. To be reliable, such assignments of the intrinsic characteristics of catalysts are grounded in the accurate elucidation of mechanisms. Without forgetting the importance of large scale electrolysis, not only mobilization of all resources of nondestructive techniques such as cyclic voltammetry was necessary to achieve this challenge, but also new approaches, such as foot-of-the-wave analysis combined with raising of scan rate, had to be applied. The latest improvement in catalyst design was to render it water-soluble while preserving, or even augmenting, its catalytic efficiency. The replacement of the nonaqueous solvents so far used by water makes the CO2-to-CO half-cell reaction much more attractive for applications, allowing its association with a water-oxidation anode through a proton-exchange membrane. Manipulation of pH and buffering then allow CO2-to-CO conversions from those involving complete CO-selectivity to ones with prescribed CO-H2 mixtures. Overall, it appears that not only are iron porphyrins the most efficient catalysts of the CO2-to-CO electrochemical conversion but also they can serve to illustrate general issues concerning the field of molecular catalysis as a whole, including other reductive or oxidative processes.
NASA Astrophysics Data System (ADS)
Barry, J. P.; Buck, K. R.; Lovera, C.; Brewer, P. G.; Seibel, B. A.; Drazen, J. C.; Tamburri, M. N.; Whaling, P. J.; Kuhnz, L.; Pane, E. F.
2013-08-01
The effects of low-pH, high-pCO2 conditions on deep-sea organisms were examined during four deep-sea CO2 release experiments simulating deep-ocean C sequestration by the direct injection of CO2 into the deep sea. We examined the survival of common deep-sea, benthic organisms (microbes; macrofauna, dominated by Polychaeta, Nematoda, Crustacea, Mollusca; megafauna, Echinodermata, Mollusca, Pisces) exposed to low-pH waters emanating as a dissolution plume from pools of liquid carbon dioxide released on the seabed during four abyssal CO2-release experiments. Microbial abundance in deep-sea sediments was unchanged in one experiment, but increased under environmental hypercapnia during another, where the microbial assemblage may have benefited indirectly from the negative impact of low-pH conditions on other taxa. Lower abyssal metazoans exhibited low survival rates near CO2 pools. No urchins or holothurians survived during 30-42 days of exposure to episodic, but severe environmental hypercapnia during one experiment (E1; pH reduced by as much as ca. 1.4 units). These large pH reductions also caused 75% mortality for the deep-sea amphipod, Haploops lodo, near CO2 pools. Survival under smaller pH reductions (ΔpH<0.4 units) in other experiments (E2, E3, E5) was higher for all taxa, including echinoderms. Gastropods, cephalopods, and fish were more tolerant than most other taxa. The gastropod Retimohnia sp. and octopus Benthoctopus sp. survived exposure to pH reductions that episodically reached -0.3 pH units. Ninety percent of abyssal zoarcids (Pachycara bulbiceps) survived exposure to pH changes reaching ca. -0.3 pH units during 30-42 day-long experiments.
NASA Technical Reports Server (NTRS)
Gopalakrishnan, Ranjith; Bala, Govindsamy; Jayaraman, Mathangi; Cao, Long; Nemani, Ramakrishna; Ravindranath, N. H.
2011-01-01
Increasing concentrations of atmospheric carbon dioxide (CO2) influence climate by suppressing canopy transpiration in addition to its well-known greenhouse gas effect. The decrease in plant transpiration is due to changes in plant physiology (reduced opening of plant stomata). Here, we quantify such changes in water flux for various levels of CO2 concentrations using the National Center for Atmospheric Research s (NCAR) Community Land Model. We find that photosynthesis saturates after 800 ppmv (parts per million, by volume) in this model. However, unlike photosynthesis, canopy transpiration continues to decline at about 5.1% per 100 ppmv increase in CO2 levels. We also find that the associated reduction in latent heat flux is primarily compensated by increased sensible heat flux. The continued decline in canopy transpiration and subsequent increase in sensible heat flux at elevated CO2 levels implies that incremental warming associated with the physiological effect of CO2 will not abate at higher CO2 concentrations, indicating important consequences for the global water and carbon cycles from anthropogenic CO2 emissions. Keywords: CO2-physiological effect, CO2-fertilization, canopy transpiration, water cycle, runoff, climate change 1.
CARBON DIOXIDE SEPARATION BY PHASE ENHANCED GAS-LIQUID ABSORPTION
DOE Office of Scientific and Technical Information (OSTI.GOV)
Liang Hu
A new process called phase enhanced gas-liquid absorption has been developed in its early stage. It was found that adding another phase into the absorption system of gas/aqueous phase could enhance the absorption rate. A system with three phases was studied. In the system, gas phase was carbon dioxide. Two liquid phases were used. One was organic phase. Another was aqueous phase. By addition of organic phase into the absorption system of CO{sub 2}-aqueous phase, the absorption rate of CO{sub 2} was increased significantly. CO{sub 2} finally accumulated into aqueous phase. The experimental results proved that (1) Absorption rate ofmore » carbon dioxide was enhanced by adding organic phase into gas aqueous phase system; (2) Organic phase played the role of transportation of gas solute (CO{sub 2}). Carbon dioxide finally accumulated into aqueous phase.« less
NASA Astrophysics Data System (ADS)
Ogutu, K. B. Z.; D'Andrea, F.; Ghil, M.; Nyandwi, C.; Manene, M. M.; Muthama, J. N.
2015-04-01
This study uses the global climate-economy-biosphere (CoCEB) model developed in Part 1 to investigate economic aspects of deforestation control and carbon sequestration in forests, as well as the efficiency of carbon capture and storage (CCS) technologies as policy measures for climate change mitigation. We assume - as in Part 1 - that replacement of one technology with another occurs in terms of a logistic law, so that the same law also governs the dynamics of reduction in carbon dioxide emission using CCS technologies. In order to take into account the effect of deforestation control, a slightly more complex description of the carbon cycle than in Part 1 is needed. Consequently, we add a biomass equation into the CoCEB model and analyze the ensuing feedbacks and their effects on per capita gross domestic product (GDP) growth. Integrating biomass into the CoCEB and applying deforestation control as well as CCS technologies has the following results: (i) low investment in CCS contributes to reducing industrial carbon emissions and to increasing GDP, but further investment leads to a smaller reduction in emissions, as well as in the incremental GDP growth; and (ii) enhanced deforestation control contributes to a reduction in both deforestation emissions and in atmospheric carbon dioxide concentration, thus reducing the impacts of climate change and contributing to a slight appreciation of GDP growth. This effect is however very small compared to that of low-carbon technologies or CCS. We also find that the result in (i) is very sensitive to the formulation of CCS costs, while to the contrary, the results for deforestation control are less sensitive.
Abolhasani, Milad; Singh, Mayank; Kumacheva, Eugenia; Günther, Axel
2012-05-07
We present an automated microfluidic (MF) approach for the systematic and rapid investigation of carbon dioxide (CO(2)) mass transfer and solubility in physical solvents. Uniformly sized bubbles of CO(2) with lengths exceeding the width of the microchannel (plugs) were isothermally generated in a co-flowing physical solvent within a gas-impermeable, silicon-based MF platform that is compatible with a wide range of solvents, temperatures and pressures. We dynamically determined the volume reduction of the plugs from images that were accommodated within a single field of view, six different downstream locations of the microchannel at any given flow condition. Evaluating plug sizes in real time allowed our automated strategy to suitably select inlet pressures and solvent flow rates such that otherwise dynamically self-selecting parameters (e.g., the plug size, the solvent segment size, and the plug velocity) could be either kept constant or systematically altered. Specifically, if a constant slug length was imposed, the volumetric dissolution rate of CO(2) could be deduced from the measured rate of plug shrinkage. The solubility of CO(2) in the physical solvent was obtained from a comparison between the terminal and the initial plug sizes. Solubility data were acquired every 5 min and were within 2-5% accuracy as compared to literature data. A parameter space consisting of the plug length, solvent slug length and plug velocity at the microchannel inlet was established for different CO(2)-solvent pairs with high and low gas solubilities. In a case study, we selected the gas-liquid pair CO(2)-dimethyl carbonate (DMC) and volumetric mass transfer coefficients 4-30 s(-1) (translating into mass transfer times between 0.25 s and 0.03 s), and Henry's constants, within the range of 6-12 MPa.
Wilkins, Michael J.; Hoyt, David W.; Marshall, Matthew J.; Alderson, Paul A.; Plymale, Andrew E.; Markillie, L. Meng; Tucker, Abby E.; Walter, Eric D.; Linggi, Bryan E.; Dohnalkova, Alice C.; Taylor, Ron C.
2014-01-01
Geologic carbon dioxide (CO2) sequestration drives physical and geochemical changes in deep subsurface environments that impact indigenous microbial activities. The combined effects of pressurized CO2 on a model sulfate-reducing microorganism, Desulfovibrio vulgaris, have been assessed using a suite of genomic and kinetic measurements. Novel high-pressure NMR time-series measurements using 13C-lactate were used to track D. vulgaris metabolism. We identified cessation of respiration at CO2 pressures of 10 bar, 25 bar, 50 bar, and 80 bar. Concurrent experiments using N2 as the pressurizing phase had no negative effect on microbial respiration, as inferred from reduction of sulfate to sulfide. Complementary pressurized batch incubations and fluorescence microscopy measurements supported NMR observations, and indicated that non-respiring cells were mostly viable at 50 bar CO2 for at least 4 h, and at 80 bar CO2 for 2 h. The fraction of dead cells increased rapidly after 4 h at 80 bar CO2. Transcriptomic (RNA-Seq) measurements on mRNA transcripts from CO2-incubated biomass indicated that cells up-regulated the production of certain amino acids (leucine, isoleucine) following CO2 exposure at elevated pressures, likely as part of a general stress response. Evidence for other poorly understood stress responses were also identified within RNA-Seq data, suggesting that while pressurized CO2 severely limits the growth and respiration of D. vulgaris cells, biomass retains intact cell membranes at pressures up to 80 bar CO2. Together, these data show that geologic sequestration of CO2 may have significant impacts on rates of sulfate reduction in many deep subsurface environments where this metabolism is a key respiratory process. PMID:25309528
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hasanbeigi, Ali; Price, Lynn; Lin, Elina
2012-04-06
Globally, the cement industry accounts for approximately 5 percent of current anthropogenic carbon dioxide (CO{sub 2}) emissions. World cement demand and production are increasing significantly, leading to an increase in this industry's absolute energy use and CO{sub 2} emissions. Development of new energy-efficiency and CO{sub 2} emission-reduction technologies and their deployment in the market will be key for the cement industry's mid- and long-term climate change mitigation strategies. This report is an initial effort to compile available information on process description, energy savings, environmental and other benefits, costs, commercialization status, and references for emerging technologies to reduce the cement industry'smore » energy use and CO{sub 2} emissions. Although studies from around the world identify a variety of sector-specific and cross-cutting energy-efficiency technologies for the cement industry that have already been commercialized, information is scarce and/or scattered regarding emerging or advanced energy-efficiency and low-carbon technologies that are not yet commercialized. This report consolidates available information on nineteen emerging technologies for the cement industry, with the goal of providing engineers, researchers, investors, cement companies, policy makers, and other interested parties with easy access to a well-structured database of information on these technologies.« less
Development of Flexi-Burn™ CFB Power Plant to Meet the Challenge of Climate Change
NASA Astrophysics Data System (ADS)
Hackt, Horst; Fant, Zhen; Seltzert, Andrew; Hotta, Arto; Erikssoni, Timo; Sippu, Ossi
Carbon-dioxide capture and storage (CCS) offers the potential for major reductions in carbon- dioxide emissions of fossil fuel-based power generation in the fairly short term, and oxyfuel combustion is one of the identified CCS technology options. Foster Wheeler (FW) is working on reduction of carbon-dioxide with its integrated Flexi-Burn™ CFB technology. The proven high efficiency circulating fluidized-bed (CFB) technology, when coupled with air separation units and carbon purification units, offers a solution for carbon dioxide reduction both in re-powering and in greenfield power plants. CFB technology has the advantages over pulverized coal technology of a more uniform furnace heat flux, increased fuel flexibility and offers the opportunity to further reduce carbon dioxide emissions by co-firing coal with bio-fuels. Development and design of an integrated Flexi-Bum™ CFB steam generator and balance of plant system was conducted for both air mode and oxyfuel mode. Through proper configuration and design, the same steam generator can be switched from air mode to oxyfuel mode without the need for unit shutdown for modifications. The Flexi-Burn™ CFB system incorporates features to maximize plant efficiency and power output when operating in the oxy-firing mode through firing more fuel in the same boiler.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Wilkins, Michael J.; Hoyt, David W.; Marshall, Matthew J.
Geologic carbon dioxide (CO2) sequestration drives physical and geochemical changes in deep subsurface environments that impact indigenous microbial activities. The combined effects of pressurized CO2 on a model sulfate-reducing microorganism, Desulfovibrio vulgaris, have been assessed using a suite of genomic and kinetic measurements. Novel high-pressure NMR time-series measurements using 13C-lactate were used to track D. vulgaris metabolism. We identified cessation of respiration at CO2 pressures of 10 bar, 25 bar, 50 bar, and 80 bar. Concurrent experiments using N2 as the pressurizing phase had no negative effect on microbial respiration, as inferred from reduction of sulfate to sulfide. Complementary pressurizedmore » batch incubations and fluorescence microscopy measurements supported NMR observations, and indicated that non-respiring cells were mostly viable at 50 bar CO2 for at least four hours, and at 80 bar CO2 for two hours. The fraction of dead cells increased rapidly after four hours at 80 bar CO2. Transcriptomic (RNA-Seq) measurements on mRNA transcripts from CO2-incubated biomass indicated that cells up-regulated the production of certain amino acids (leucine, isoleucine) following CO2 exposure at elevated pressures, likely as part of a general stress response. Evidence for other poorly understood stress responses were also identified within RNA-Seq data, suggesting that while pressurized CO2 severely limits the growth and respiration of D. vulgaris cells, biomass retains intact cell membranes at pressures up to 80 bar CO2. Together, these data show that geologic sequestration of CO2 may have significant impacts on rates of sulfate reduction in many deep subsurface environments where this metabolism is a key respiratory process.« less
CO2 emissions, natural gas and renewables, economic growth: Assessing the evidence from China.
Dong, Kangyin; Sun, Renjin; Dong, Xiucheng
2018-05-31
This study aims to test the environmental Kuznets curve (EKC) for carbon dioxide (CO 2 ) emissions in China by developing a new framework based on the suggestion of Narayan and Narayan (2010). The dynamic effect of natural gas and renewable energy consumption on CO 2 emissions is also analyzed. Considering the structural break observed in the sample, a series of econometric techniques allowing for structural breaks is utilized for the period 1965-2016. The empirical results confirm the existence of the EKC for CO 2 emissions in China. Furthermore, in both the long-run and the short-run, the beneficial effects of natural gas and renewables on CO 2 emission reduction are observable. In addition, the mitigation effect of natural gas on CO 2 emissions will be weakened over time, while renewables will become progressively more important. Finally, policy suggestions are highlighted not only for mitigating CO 2 emissions, but also for promoting growth in the natural gas and renewable energy industries. Copyright © 2018 Elsevier B.V. All rights reserved.
Bhattacharyya, P; Roy, K S; Das, M; Ray, S; Balachandar, D; Karthikeyan, S; Nayak, A K; Mohapatra, T
2016-01-15
Carbon (C) and nitrogen (N) mineralization is one of the key processes of biogeochemical cycling in terrestrial ecosystem in general and rice ecology in particular. Rice rhizosphere is a rich niche of microbial diversity influenced by change in atmospheric temperature and concentration of carbon dioxide (CO2). Structural changes in microbial communities in rhizosphere influence the nutrient cycling. In the present study, the bacterial diversity and population dynamics were studied under ambient CO2 (a-CO2) and elevated CO2+temperature (e-CO2T) in lowland rice rhizosphere using whole genome metagenomic approach. The whole genome metagenomic sequence data of lowland rice exhibited the dominance of bacterial communities including Proteobacteria, Firmicutes, Acidobacteria, Actinobacteria and Planctomycetes. Interestingly, four genera related to methane production namely, Methanobacterium, Methanosphaera, Methanothermus and Methanothermococcus were absent in a-CO2 but noticed under e-CO2T. The acetoclastic pathway was found as the predominant pathway for methanogenesis, whereas, the serine pathway was found as the principal metabolic pathway for CH4 oxidation in lowland rice. The abundances of reads of enzymes in the acetoclastic methanogenesis pathway and serine pathways of methanotrophy were much higher in e-CO2T (328 and 182, respectively) as compared with a-CO2 (118 and 98, respectively). Rice rhizosphere showed higher structural diversities and functional activities in relation to N metabolism involving nitrogen fixation, assimilatory and dissimilatory nitrate reduction and denitrification under e-CO2T than that of a-CO2. Among the three pathways of N metabolism, dissimilarity pathways were predominant in lowland rice rhizosphere and more so under e-CO2T. Consequently, under e-CO2T, CH4 emission, microbial biomass nitrogen (MBN) and dehydrogenase activities were 45%, 20% and 35% higher than a-CO2, respectively. Holistically, a high bacterial diversity and abundances of C and N decomposing bacteria in lowland rice rhizosphere were found under e-CO2T, which could be explored further for their specific role in nutrient cycling, sustainable agriculture and environment management. Copyright © 2015 Elsevier B.V. All rights reserved.
Supercritical carbon dioxide for textile applications and recent developments
NASA Astrophysics Data System (ADS)
Eren, H. A.; Avinc, O.; Eren, S.
2017-10-01
In textile industry, supercritical carbon dioxide (scCO2), possessing liquid-like densities, mostly find an application on textile dyeing processes such as providing hydrophobic dyes an advantage on dissolving. Their gas-like low viscosities and diffusion properties can result in shorter dyeing periods in comparison with the conventional water dyeing process. Supercritical carbon dioxide dyeing is an anhydrous dyeing and this process comprises the usage of less energy and chemicals when compared to conventional water dyeing processes leading to a potential of up to 50% lower operation costs. The advantages of supercritical carbon dioxide dyeing method especially on synthetic fiber fabrics hearten leading textile companies to alter their dyeing method to this privileged waterless dyeing technology. Supercritical carbon dioxide (scCO2) waterless dyeing is widely known and applied green method for sustainable and eco-friendly textile industry. However, not only the dyeing but also scouring, desizing and different finishing applications take the advantage of supercritical carbon dioxide (scCO2). In this review, not only the principle, advantages and disadvantages of dyeing in supercritical carbon dioxide but also recent developments of scCO2 usage in different textile processing steps such as scouring, desizing and finishing are explained and commercial developments are stated and summed up.
Liquid carbon dioxide absorbents, methods of using the same, and related system
DOE Office of Scientific and Technical Information (OSTI.GOV)
Perry, Robert James; Soloveichik, Grigorii Lev; Rubinsztajn, Malgorzata Iwona
A carbon dioxide absorbent composition is described, including (i) a liquid, nonaqueous silicon-based material, functionalized with one or more groups that either reversibly react with CO 2 or have a high-affinity for CO 2, and (ii) a hydroxy-containing solvent that is capable of dissolving both the silicon-based material and a reaction product of the silicon-based material and CO 2. The absorbent may be utilized in methods to reduce carbon dioxide in an exhaust gas, and finds particular utility in power plants.
Liquid carbon dioxide absorbents, methods of using the same, and related systems
O'Brien, Michael Joseph; Perry, Robert James; Lam, Tunchiao Hubert; Soloveichik, Grigorii Lev; Kniajanski, Sergei; Lewis, Larry Neil; Rubinsztajn, Malgorzata Iwona; Hancu, Dan
2016-09-13
A carbon dioxide absorbent composition is described, including (i) a liquid, nonaqueous silicon-based material, functionalized with one or more groups that either reversibly react with CO.sub.2 or have a high-affinity for CO.sub.2; and (ii) a hydroxy-containing solvent that is capable of dissolving both the silicon-based material and a reaction product of the silicon-based material and CO.sub.2. The absorbent may be utilized in methods to reduce carbon dioxide in an exhaust gas, and finds particular utility in power plants.
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.
Dai, X R; Blanes-Vidal, V
2013-01-30
This study aimed at evaluating the effect of swine slurry acidification and acidification-aeration treatments on ammonia (NH(3)), carbon dioxide (CO(2)) and hydrogen sulfide (H(2)S) emissions during slurry treatment and subsequent undisturbed storage. The study was conducted in an experimental setup consisting of nine dynamic flux chambers. Three pH levels (pH = 6.0, pH = 5.8 and pH = 5.5), combined with short-term aeration and venting (with an inert gas) treatments were studied. Acidification reduced average NH(3) emissions from swine slurry stored after acidification treatment compared to emissions during storage of non-acidified slurry. The reduction were 50%, 62% and 77% when pH was reduce to 6.0, 5.8 and 5.5, respectively. However, it had no significant effect on average CO(2) and H(2)S emissions during storage of slurry after acidification. Aeration of the slurry for 30 min had no effect on average NH(3), CO(2) and H(2)S emissions both during the process and from stored slurry after venting treatments. During aeration treatment, the NH(3), CO(2) and H(2)S release pattern observed was related to the liquid turbulence caused by the gas bubbles rather than to biological oxidation processes in this study. Copyright © 2012 Elsevier Ltd. All rights reserved.
Koelkebeck, K W; Odom, T W
1994-04-01
Exposure to heat stress lowered partial pressure of arterial blood carbon dioxide (paCO2), arterial blood bicarbonate ion (HCO3-), but increased arterial blood pH (pHa) and plasma lactate (LA). Increasing ambient carbon dioxide (CO2) to 1.5% increased paCO2 from hypocapnic levels to normocapnic levels, raised HCO3-, lowered pHa and plasma LA to pre-heat stress levels. Following CO2 treatment, respiratory alkalosis conditions returned. It was evident in this study that increasing ambient chamber CO2 to 1.5% was effective in ameliorating acid-base disturbances and reducing elevated levels of plasma LA which normally develops when laying hens are subjected to an acute heat stress exposure.
This study examines using the threshold critical pressure increase and the extent of the carbon dioxide (CO2) plume to delineate the area of potential impact (AoPI) for geologic CO2 storage projects. The combined area covering both the CO2 plume and the region where the pressure ...
Response of sugarcane to carbon dioxide enrichment and elevated air temperature
USDA-ARS?s Scientific Manuscript database
Four sugarcane cultivars (CP 72-2086, CP 73-1547, CP 88-1508, and CP 80-1827) were grown in elongated temperature-gradient greenhouses (TGG) at ambient or elevated carbon dioxide (CO2) of 360 or 720 µmol CO2 mol-1 air (ppm, mole fraction basis), respectively. Elevated CO2 was maintained by injection...
21 CFR 868.2480 - Cutaneous carbon dioxide (PcCO2) monitor.
Code of Federal Regulations, 2010 CFR
2010-04-01
... 21 Food and Drugs 8 2010-04-01 2010-04-01 false Cutaneous carbon dioxide (PcCO2) monitor. 868.2480 Section 868.2480 Food and Drugs FOOD AND DRUG ADMINISTRATION, DEPARTMENT OF HEALTH AND HUMAN SERVICES... (PcCO2) and Oxygen (PcO2) Monitors; Guidance for Industry and FDA.” See § 868.1(e) for the...
Feng, Jin-Xing; Liu, Xiao-Hong; Huang, Hui-Jun; Yu, Zhen-Zhu; Yang, Hui; He, Liu-Fang
2014-05-01
To study the correlation between end-tidal carbon dioxide (PetCO2) and partial pressure of arterial carbon dioxide (PaCO2) in ventilated newborns. Thirty-one ventilated newborn underwent mainstream PetCO2 monitoring; meanwhile, arterial blood gas analysis was performed. The correlation and consistency between PetCO2 and PaCO2 were assessed. A total of 85 end-tidal and arterial CO2 pairs were obtained from 31 ventilated newborns. The mean PetCO2 (41±10 mm Hg) was significantly lower than the corresponding mean PaCO2 (46±11 mm Hg) (P<0.01). There was a significant positive correlation between PetCO2 and PaCO2 (r=0.92, P<0.01). The overall PetCO2 bias was 5.1±4.3 mm Hg (95% limits of consistency, -3.3 to 13.6 mmHg), and 5% (4/85) of the points were beyond the 95%CI. When the oxygenation index (OI) was less than 300 mm Hg (n=48), there was a significant positive correlation between PetCO2 and PaCO2 (r=0.85, P<0.01); the PetCO2 bias was 5.9±4.3 mm Hg (95% limits of consistency, -2.6 to 14.5 mm Hg), and 4.2% (2/48) of the points were beyond the 95%CI. When the OI was more than 300 mm Hg (n=37), there was also a significant positive correlation between PetCO2 and PaCO2 (r=0.91, P<0.01); the PetCO2 bias was 4.1±4.1 mm Hg (95% limits of consistency, -3.9 to 12.1 mm Hg), and 5% (2/37) of the points were beyond the 95%CI. There is a good correlation and consistency between PetCO2 and PaCO2 in ventilated newborns.
Cadmium-Aluminum Layered Double Hydroxide Microspheres for Photocatalytic CO2 Reduction.
Saliba, Daniel; Ezzeddine, Alaa; Sougrat, Rachid; Khashab, Niveen M; Hmadeh, Mohamad; Al-Ghoul, Mazen
2016-04-21
We report the synthesis of cadmium-aluminum layered double hydroxide (CdAl LDH) using the reaction-diffusion framework. As the hydroxide anions diffuse into an agar gel matrix containing the mixture of aluminum and cadmium salts at a given ratio, they react to give the LDH. The LDH self-assembles inside the pores of the gel matrix into a unique spherical-porous shaped microstructure. The internal and external morphologies of the particles are studied by electron microscopy and tomography revealing interconnected channels and a high surface area. This material is shown to exhibit a promising performance in the photoreduction of carbon dioxide using solar light. Moreover, the palladium-decorated version shows a significant improvement in its reduction potential at room temperature. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Ichikawa, Shinichiro; Tada, Mizuki; Iwasawa, Yasuhiro; Ikariya, Takao
2005-02-21
Chemoselective hydrogenation of halogenated nitrobenzenes over Pt/C catalysts proceeds effectively in supercritical carbon dioxide (scCO2) to produce halogenated anilines with excellent selectivity; the rate of the hydrogenation of nitro groups is markedly enhanced in scCO2 compared to the neat reaction, and the dehalogenation reaction is significantly suppressed.
NASA launches carbon dioxide research satellite
NASA Astrophysics Data System (ADS)
Wendel, JoAnna
2014-07-01
Last week NASA launched a new satellite to study atmospheric carbon dioxide (CO2). Once in orbit, the Orbiting Carbon Observatory-2 (OCO-2) satellite, launched from Vandenberg Air Force Base in California, will take more than 100,000 individual measurements of atmospheric CO2 per day.
NASA Astrophysics Data System (ADS)
Wu, Jingjie; Ma, Sichao; Sun, Jing; Gold, Jake I.; Tiwary, Chandrasekhar; Kim, Byoungsu; Zhu, Lingyang; Chopra, Nitin; Odeh, Ihab N.; Vajtai, Robert; Yu, Aaron Z.; Luo, Raymond; Lou, Jun; Ding, Guqiao; Kenis, Paul J. A.; Ajayan, Pulickel M.
2016-12-01
Electroreduction of carbon dioxide into higher-energy liquid fuels and chemicals is a promising but challenging renewable energy conversion technology. Among the electrocatalysts screened so far for carbon dioxide reduction, which includes metals, alloys, organometallics, layered materials and carbon nanostructures, only copper exhibits selectivity towards formation of hydrocarbons and multi-carbon oxygenates at fairly high efficiencies, whereas most others favour production of carbon monoxide or formate. Here we report that nanometre-size N-doped graphene quantum dots (NGQDs) catalyse the electrochemical reduction of carbon dioxide into multi-carbon hydrocarbons and oxygenates at high Faradaic efficiencies, high current densities and low overpotentials. The NGQDs show a high total Faradaic efficiency of carbon dioxide reduction of up to 90%, with selectivity for ethylene and ethanol conversions reaching 45%. The C2 and C3 product distribution and production rate for NGQD-catalysed carbon dioxide reduction is comparable to those obtained with copper nanoparticle-based electrocatalysts.
Haworth, Matthew; Elliott-Kingston, Caroline; McElwain, Jennifer C
2013-01-01
Plant stomata display a wide range of short-term behavioural and long-term morphological responses to atmospheric carbon dioxide concentration ([CO(2)]). The diversity of responses suggests that plants may have different strategies for controlling gas exchange, yet it is not known whether these strategies are co-ordinated in some way. Here, we test the hypothesis that there is co-ordination of physiological (via aperture change) and morphological (via stomatal density change) control of gas exchange by plants. We examined the response of stomatal conductance (G(s)) to instantaneous changes in external [CO(2)] (C(a)) in an evolutionary cross-section of vascular plants grown in atmospheres of elevated [CO(2)] (1,500 ppm) and sub-ambient [O(2)] (13.0 %) compared to control conditions (380 ppm CO(2), 20.9 % O(2)). We found that active control of stomatal aperture to [CO(2)] above current ambient levels was not restricted to angiosperms, occurring in the gymnosperms Lepidozamia peroffskyana and Nageia nagi. The angiosperm species analysed appeared to possess a greater respiratory demand for stomatal movement than gymnosperm species displaying active stomatal control. Those species with little or no control of stomatal aperture (termed passive) to C(a) were more likely to exhibit a reduction in stomatal density than species with active stomatal control when grown in atmospheres of elevated [CO(2)]. The relationship between the degree of stomatal aperture control to C(a) above ambient and the extent of any reduction in stomatal density may suggest the co-ordination of physiological and morphological responses of stomata to [CO(2)] in the optimisation of water use efficiency. This trade-off between stomatal control strategies may have developed due to selective pressures exerted by the costs associated with passive and active stomatal control.
Supercritical carbon dioxide: a solvent like no other
Peach, Jocelyn
2014-01-01
Summary Supercritical carbon dioxide (scCO2) could be one aspect of a significant and necessary movement towards green chemistry, being a potential replacement for volatile organic compounds (VOCs). Unfortunately, carbon dioxide has a notoriously poor solubilising power and is famously difficult to handle. This review examines attempts and breakthroughs in enhancing the physicochemical properties of carbon dioxide, focusing primarily on factors that impact solubility of polar and ionic species and attempts to enhance scCO2 viscosity. PMID:25246947
Morris, Megan M.; Brown, Matt; Doane, Michael; Edwards, Matthew S.; Michael, Todd P.; Dinsdale, Elizabeth A.
2018-01-01
Global climate change includes rising temperatures and increased pCO2 concentrations in the ocean, with potential deleterious impacts on marine organisms. In this case study we conducted a four-week climate change incubation experiment, and tested the independent and combined effects of increased temperature and partial pressure of carbon dioxide (pCO2), on the microbiomes of a foundation species, the giant kelp Macrocystis pyrifera, and the surrounding water column. The water and kelp microbiome responded differently to each of the climate stressors. In the water microbiome, each condition caused an increase in a distinct microbial order, whereas the kelp microbiome exhibited a reduction in the dominant kelp-associated order, Alteromondales. The water column microbiomes were most disrupted by elevated pCO2, with a 7.3 fold increase in Rhizobiales. The kelp microbiome was most influenced by elevated temperature and elevated temperature in combination with elevated pCO2. Kelp growth was negatively associated with elevated temperature, and the kelp microbiome showed a 5.3 fold increase Flavobacteriales and a 2.2 fold increase alginate degrading enzymes and sulfated polysaccharides. In contrast, kelp growth was positively associated with the combination of high temperature and high pCO2 ‘future conditions’, with a 12.5 fold increase in Planctomycetales and 4.8 fold increase in Rhodobacteriales. Therefore, the water and kelp microbiomes acted as distinct communities, where the kelp was stabilizing the microbiome under changing pCO2 conditions, but lost control at high temperature. Under future conditions, a new equilibrium between the kelp and the microbiome was potentially reached, where the kelp grew rapidly and the commensal microbes responded to an increase in mucus production. PMID:29474389
NASA Astrophysics Data System (ADS)
Butman, D. E.; Holtgrieve, G. W.
2017-12-01
Recent modelling studies in large catchments have estimated that in excess of 74% of the dissolved carbon dioxide found in first and second order streams originate from allochthonous sources. Stable isotopes of carbon-13 in carbon dioxide have been used to identify ground water seeps in stream systems, where decreases in δ13CO2 occur along gaining stream reaches, suggesting that carbon dioxide in ground water is more depleted than what is found in surface water due to fractionation of CO2 during emissions across the air water interface. Although isotopes represent a chemical tracer in stream systems for potential groundwater contribution, the temporal resolution of discrete samples make partitioning allochthonous versus autochthonous sources of CO2 difficult on hydrologically relevant time scales. Here we show results of field deployments of high frequent dissolved CO2, O2, PAR, Temperature and pH from the Thornton Creek Watershed, the largest urban watershed in Seattle, WA. We present an exploration into using high resolution time series of dissolved oxygen and carbon dioxide in a dual gas approach to separate the contribution of in stream respiration from external sources. We extend upon previous efforts to model stream metabolism across diel cycles by incorporating simultaneous direct measurements of dissolved oxygen, PCO2, and pH within an inverse modeling framework and Bayesian parameter estimation. With an initial assumption of a stoichiometric ratio of 1:1 for O2 and CO2 for autochthonous driven metabolism, we investigate positive or negative departures from this ratio as an indicator of external CO2 to the stream (terrestrial or atmospheric) and factors contributing to this flux.
Watten, B.J.; Sibrell, P.L.; Schwartz, M.F.
2004-01-01
Limestone has potential for reducing reagent costs and sludge volume associated with the treatment of acid mine drainage (AMD), but its use has been restricted by slow dissolution rates and sensitivity to scale forming reactions that retard transport of H+ at the solid-liquid interface. We evaluated a pulsed limestone bed (PLB) remediation process designed to circumvent these problems through use of intermittently fluidized beds of granular limestone and elevated carbon dioxide pressure. PLB limestone dissolution (LD, mg/L), and effluent alkalinity (Alk, mg/L) were correlated with reactor pressure (PCO2, kPa), influent acidity (Acy, mg/L) and reactor bed height (H, cm) using a prototype capable of processing 10 L/min. The PLB process effectively neutralized sulfuric acid acidity over the range of 6-1033 mg/L (as CaCO3) while generating high concentrations of alkalinity (36-1086 mg/L) despite a hydraulic residence time of just 4.2-5.0 min. Alk and LD (mg/L CaCO3) rose with increases in influent acidity and PCO2 (p < 0.001) according to the models: Alk = 58 + 38.4 (PCO2)0.5 + 0.080 (Acy) - 0.0059(PCO2) 0.5 (Acy); LD = 55 + 38.3 (PCO2)0.5 + 1.08 (Acy) - 0.0059 (PCO2)0.5 (Acy). Alkalinity decreased at an increasing rate with reductions in H over the range of 27.3-77.5 cm (p < 0.001). Carbon dioxide requirements (Q(avg)CO2, L/min) increased with PCO2 (p < 0.001) following the model Q(avg)CO2 = 0.858 (PCO2)0.620, resulting in a greater degree of pH buffering (depression) within the reactors, a rise in limestone solubility and an increase in limestone dissolution related to carbonic acid attack. Corresponding elevated concentrations of effluent alkalinity allow for sidestream treatment with blending. Numerical modeling demonstrated that carbon dioxide requirements are reduced as influent acidity rises and when carbon dioxide is recovered from system effluent and recycled. Field trials demonstrated that the PLB process is capable of raising the pH of AMD above that required for hydrolysis and precipitation of Fe3+ and Al 3+ but not Fe2+ and Mn2+.
Singh, Meenesh R.; Clark, Ezra L.; Bell, Alexis T.
2015-01-01
Thermodynamic, achievable, and realistic efficiency limits of solar-driven electrochemical conversion of water and carbon dioxide to fuels are investigated as functions of light-absorber composition and configuration, and catalyst composition. The maximum thermodynamic efficiency at 1-sun illumination for adiabatic electrochemical synthesis of various solar fuels is in the range of 32–42%. Single-, double-, and triple-junction light absorbers are found to be optimal for electrochemical load ranges of 0–0.9 V, 0.9–1.95 V, and 1.95–3.5 V, respectively. Achievable solar-to-fuel (STF) efficiencies are determined using ideal double- and triple-junction light absorbers and the electrochemical load curves for CO2 reduction on silver and copper cathodes, and water oxidation kinetics over iridium oxide. The maximum achievable STF efficiencies for synthesis gas (H2 and CO) and Hythane (H2 and CH4) are 18.4% and 20.3%, respectively. Whereas the realistic STF efficiency of photoelectrochemical cells (PECs) can be as low as 0.8%, tandem PECs and photovoltaic (PV)-electrolyzers can operate at 7.2% under identical operating conditions. We show that the composition and energy content of solar fuels can also be adjusted by tuning the band-gaps of triple-junction light absorbers and/or the ratio of catalyst-to-PV area, and that the synthesis of liquid products and C2H4 have high profitability indices. PMID:26504215
Singh, Meenesh R.; Clark, Ezra L.; Bell, Alexis T.
2015-10-26
Thermodynamic, achievable, and realistic efficiency limits of solar-driven electrochemical conversion of water and carbon dioxide to fuels are investigated as functions of light-absorber composition and configuration, and catalyst composition. The maximum thermodynamic efficiency at 1-sun illumination for adiabatic electrochemical synthesis of various solar fuels is in the range of 32–42%. Single-, double-, and triple-junction light absorbers are found to be optimal for electrochemical load ranges of 0–0.9 V, 0.9–1.95 V, and 1.95–3.5 V, respectively. Achievable solar-to-fuel (STF) efficiencies are determined using ideal double- and triple-junction light absorbers and the electrochemical load curves for CO 2 reduction on silver and coppermore » cathodes, and water oxidation kinetics over iridium oxide. The maximum achievable STF efficiencies for synthesis gas (H 2 and CO) and Hythane (H 2 and CH 4) are 18.4% and 20.3%, respectively. Whereas the realistic STF efficiency of photoelectrochemical cells (PECs) can be as low as 0.8%, tandem PECs and photovoltaic (PV)-electrolyzers can operate at 7.2% under identical operating conditions. Finally, we show that the composition and energy content of solar fuels can also be adjusted by tuning the band-gaps of triple-junction light absorbers and/or the ratio of catalyst-to-PV area, and that the synthesis of liquid products and C 2H 4 have high profitability indices.« less
49 CFR 173.217 - Carbon dioxide, solid (dry ice).
Code of Federal Regulations, 2011 CFR
2011-10-01
... 49 Transportation 2 2011-10-01 2011-10-01 false Carbon dioxide, solid (dry ice). 173.217 Section... Class 7 § 173.217 Carbon dioxide, solid (dry ice). (a) Carbon dioxide, solid (dry ice), when offered for... marked on two sides “WARNING CO2 SOLID (DRY ICE).” (2) Other packagings containing solid carbon dioxide...
49 CFR 173.217 - Carbon dioxide, solid (dry ice).
Code of Federal Regulations, 2012 CFR
2012-10-01
... 49 Transportation 2 2012-10-01 2012-10-01 false Carbon dioxide, solid (dry ice). 173.217 Section... Class 7 § 173.217 Carbon dioxide, solid (dry ice). (a) Carbon dioxide, solid (dry ice), when offered for... marked on two sides “WARNING CO2 SOLID (DRY ICE).” (2) Other packagings containing solid carbon dioxide...
49 CFR 173.217 - Carbon dioxide, solid (dry ice).
Code of Federal Regulations, 2010 CFR
2010-10-01
... 49 Transportation 2 2010-10-01 2010-10-01 false Carbon dioxide, solid (dry ice). 173.217 Section... Class 7 § 173.217 Carbon dioxide, solid (dry ice). (a) Carbon dioxide, solid (dry ice), when offered for... marked on two sides “WARNING CO2 SOLID (DRY ICE).” (2) Other packagings containing solid carbon dioxide...
49 CFR 173.217 - Carbon dioxide, solid (dry ice).
Code of Federal Regulations, 2014 CFR
2014-10-01
... 49 Transportation 2 2014-10-01 2014-10-01 false Carbon dioxide, solid (dry ice). 173.217 Section... Class 7 § 173.217 Carbon dioxide, solid (dry ice). (a) Carbon dioxide, solid (dry ice), when offered for... marked on two sides “WARNING CO2 SOLID (DRY ICE).” (2) Other packagings containing solid carbon dioxide...
49 CFR 173.217 - Carbon dioxide, solid (dry ice).
Code of Federal Regulations, 2013 CFR
2013-10-01
... 49 Transportation 2 2013-10-01 2013-10-01 false Carbon dioxide, solid (dry ice). 173.217 Section... Class 7 § 173.217 Carbon dioxide, solid (dry ice). (a) Carbon dioxide, solid (dry ice), when offered for... marked on two sides “WARNING CO2 SOLID (DRY ICE).” (2) Other packagings containing solid carbon dioxide...
Puig, Sebastià; Ganigué, Ramon; Batlle-Vilanova, Pau; Balaguer, M Dolors; Bañeras, Lluís; Colprim, Jesús
2017-03-01
This study reveals that reduction of carbon dioxide (CO 2 ) to commodity chemicals can be functionally compartmentalized in bioelectrochemical systems. In the present example, a syntrophic consortium composed by H 2 -producers (Rhodobacter sp.) in the biofilm is combined with carboxidotrophic Clostridium species, mainly found in the bulk liquid. The performance of these H 2 -mediated electricity-driven systems could be tracked by the activity of a biological H 2 sensory protein identified at cathode potentials between -0.2V and -0.3V vs SHE. This seems to point out that such signal is not strain specific, but could be detected in any organism containing hydrogenases. Thus, the findings of this work open the door to the development of a biosensor application or soft sensors for monitoring such systems. Copyright © 2016 Elsevier Ltd. All rights reserved.
Meujo, Damaris A F; Kevin, Dion A; Peng, Jiangnan; Bowling, John J; Liu, Jianping; Hamann, Mark T
2010-03-31
An innovative approach to Post-Harvest Processing (PHP) of oysters is introduced focusing on the effects of supercritical carbon dioxide (scCO(2)) on bacterial contaminants trapped in the digestive system of oysters. Oysters were exposed to scCO(2) under two conditions: (1) 100 bar and 37 degrees C for 30 min and (2) 172 bar and 60 degrees C for 60 min. Using FDA standard guidelines for food analysis, variations in the Aerobic Plate Count (APC) were assessed. It was established that exposing oysters to CO(2) at 100 bar and 37 degrees C for 30 min and at 172 bar and 60 degrees C for 60 min induced 2-log and 3-log reductions in the APC respectively. The decrease in the microbial load as a result of treatment with scCO(2) was found to be significant (P=0.002). A release of adductor muscles from the shell was noted in oysters treated at 172 bar and 60 degrees C for 60 min; this was not the case for oysters treated at 100 bar and 37 degrees C for 30 min. A blind study allowing sensory analysis of treated vs. untreated oysters was also completed and no significant change in the physical appearance, smell, or texture was recorded. In this paper, we also report the effect of scCO(2) on several bacterial isolates, including a referenced ATCC strain of a non-pathogenic Vibrio (Vibrio fischeri) as well as several other bacterial isolates cultured from oyster' tissues and found to share biochemical features common to pathogenic Vibrio strains. A complete inactivation (minimum 7-log reduction) was achieved with these latter bacterial isolates. A 6-log reduction was observed with V. fischeri. Copyright 2009 Elsevier B.V. All rights reserved.
Meujo, Damaris A.F.; Kevin, Dion; Peng, Jiangnan; Bowling, John J.; Liu, Jianping; Hamann, Mark T.
2010-01-01
An innovative approach to Post-Harvest Processing (PHP) of oysters is introduced focusing on the effects of supercritical carbon dioxide (scCO2) on bacterial contaminants trapped in the digestive system of oysters. Oysters were exposed to scCO2 under two conditions: (1) 100 bar and 37 °C for 30 minutes and (2) 172 bar and 60 °C for 60 minutes. Using FDA standard guidelines for food analysis, variations in the Aerobic Plate Count (APC) was assessed. It was established that exposing oysters to CO2 at 100 bar and 37 °C for 30 minutes and at 172 bar and 60°C for 60 minutes induced 2-log and 3-log reductions in the APC respectively. The decrease in the microbial load as a result of treatment with scCO2 was found to be significant (P=0.002). A release of adductor muscles from the shell was noted in oysters treated at 172 bar and 60 °C for 60 minutes; this was not the case for oysters treated at 100 bar and 37 °C for 30 minutes. A blind study allowing sensory analysis of treated vs. untreated oysters was also completed and no significant change in the physical appearance, smell, or texture was recorded. In this paper, we also report the effect of scCO2 on several bacterial isolates, including a referenced ATCC strain of a non pathogenic Vibrio (V. fisherii) as well as several other bacterial isolates cultured from oyster’ tissues and found to share biochemical features common to pathogenic Vibrio strains. A complete inactivation (minimum 7-log reduction) was achieved with these latter bacterial isolates. A 6-log reduction was observed with V. fisherii. PMID:20022650
USDA-ARS?s Scientific Manuscript database
Nutrients such as phosphorus availability may exert a major control over plant response to rising atmospheric carbon dioxide concentration (CO2), which is projected to double by the end of 21st century. Elevated CO2 may overcome the diffusional limitation to photosynthesis posed by stomata and mesop...
Aquifer disposal of carbon dioxide for greenhouse effect mitigation
DOE Office of Scientific and Technical Information (OSTI.GOV)
Gupta, N.; Naymik, T.G.; Bergman, P.
1998-07-01
Deep aquifer sequestration of carbon dioxide (CO{sup 2}), generated from power plant and other industrial emissions, is being evaluated as one of the potential options for the reduction of atmospheric greenhouse gas emissions. The major advantages of using deep aquifers are that the disposal facilities may be located close to the sources, thus reducing the CO{sub 2} transport costs. The potential capacity is much larger than the projected CO{sub 2} emissions over the next century, and it is a long-term/permanent sequestration option, because a large portion of the injected CO{sub 2} may be fixed into the aquifer by dissolution ormore » mineralization. The major limitations include the potentially high cost, the risk of upward migration, and the public perception of risk. Most of the cost is due to the need to separate CO{sub 2} from other flue gases, rather than the actual cost of disposal. Hazardous liquid waste and acid gas disposal in deep sedimentary formations is a well-established practice. There are also numerous facilities for storage of natural gases in depleted oil and gas reservoirs. The only current facility for aquifer disposal of CO{sub 2} is the offshore injection well at Sleipner Vest in the North Sea in Norway operated by Statoil. Exxon and Pertamina are planning an offshore aquifer disposal facility at Natuna gas field in Indonesia. A major evaluation of the feasibility of CO{sub 2} disposal in the European Union and Norway has been conducted under project Joule II. The data and experience obtained from the existing deep-waste disposal facilities and from the Sleipner Vest site form a strong foundation for further research and development on CO{sub 2} sequestration. Federal Energy Technology Center (FETC) is currently leading a project that uses data from an existing hazardous waste disposal facility injecting in the Mt. Simon Sandstone aquifer in Ohio to evaluate hydrogeologic, geochemical, and social issues related to CO{sub 2} disposal.« less
Aquifer disposal of carbon dioxide for greenhouse effect mitigation
DOE Office of Scientific and Technical Information (OSTI.GOV)
Gupta, N.; Naymik, T.G.; Bergman, P.
1998-04-01
Deep aquifer sequestration of carbon dioxide (CO{sub 2}) generated from power plant and other industrial emissions, is being evaluated as one of the potential options for the reduction of atmospheric greenhouse gas emissions. The major advantages of using deep aquifers are that the disposal facilities may be located close to the sources, thus reducing the CO{sub 2} transport costs. The potential capacity is much larger than the projected CO{sub 2} emissions over the next century, and it is a long-term/permanent sequestration option, because a large portion of the injected CO{sub 2} may be fixed into the aquifer by dissolution ormore » mineralization. The major limitations include the potentially high cost, the risk of upward migration, and the public perception of risk. Most of the cost is due to the need to separate CO{sub 2} from other flue gases, rather than the actual cost of disposal. Hazardous liquid waste and acid gas disposal in deep sedimentary formations is a well-established practice. There are also numerous facilities for storage of natural gases in depleted oil and gas reservoirs. The only current facility for aquifer disposal of CO{sub 2} is the offshore injection well at Sleipner Vest in the North Sea in Norway operated by Statoil. Exxon and Pertamina are planning an offshore aquifer disposal facility at Natuna gas field in Indonesia. A major evaluation of the feasibility of CO{sub 2} disposal in the European Union and Norway has been conducted under project Joule II. The data and experience obtained from the existing deep-waste disposal facilities and from the Sleipner Vest site form a strong foundation for further research and development on CO{sub 2} sequestration. Federal Energy Technology Center (FETC) is currently leading a project that uses data from an existing hazardous waste disposal facility injecting in the Mt. Simon Sandstone aquifer in Ohio to evaluate hydrogeologic, geochemical, and social issues related to CO{sub 2} disposal.« less
Carbon Dioxide and Nitrogen Infused Compressed Air Foam for Depopulation of Caged Laying Hens
Gurung, Shailesh; White, Dima; Archer, Gregory; Styles, Darrel; Zhao, Dan; Farnell, Yuhua; Byrd, James; Farnell, Morgan
2018-01-01
Simple Summary Compressed air, detergent, and water make up compressed air foam. Our laboratory has previously reported that compressed air foam may be an effective method for mass depopulation of caged layer hens. Gases, such as carbon dioxide and nitrogen, have also been used for poultry euthanasia and depopulation. The objective of this study was to produce compressed air foam infused with carbon dioxide or nitrogen to compare its efficacy against foam with air and gas inhalation methods (carbon dioxide or nitrogen) for depopulation of caged laying hens. The study showed that a carbon dioxide-air mixture or 100% nitrogen can replace air to make compressed air foam. However, the foam with carbon dioxide had poor foam quality compared to the foam with air or nitrogen. The physiological stress response of hens subjected to foam treatments with and without gas infusion did not differ significantly. Hens exposed to foam with nitrogen died earlier as compared to methods such as foam with air and carbon dioxide. The authors conclude that infusion of nitrogen into compressed air foam results in better foam quality and shortened time to death as compared to the addition of carbon dioxide. Abstract Depopulation of infected poultry flocks is a key strategy to control and contain reportable diseases. Water-based foam, carbon dioxide inhalation, and ventilation shutdown are depopulation methods available to the poultry industry. Unfortunately, these methods have limited usage in caged layer hen operations. Personnel safety and welfare of birds are equally important factors to consider during emergency depopulation procedures. We have previously reported that compressed air foam (CAF) is an alternative method for depopulation of caged layer hens. We hypothesized that infusion of gases, such as carbon dioxide (CO2) and nitrogen (N2), into the CAF would reduce physiological stress and shorten time to cessation of movement. The study had six treatments, namely a negative control, CO2 inhalation, N2 inhalation, CAF with air (CAF Air), CAF with 50% CO2 (CAF CO2), and CAF with 100% N2 (CAF N2). Four spent hens were randomly assigned to one of these treatments on each of the eight replication days. A total of 192 spent hens were used in this study. Serum corticosterone and serotonin levels were measured and compared between treatments. Time to cessation of movement of spent hens was determined using accelerometers. The addition of CO2 in CAF significantly reduced the foam quality while the addition of N2 did not. The corticosterone and serotonin levels of spent hens subjected to foam (CAF, CAF CO2, CAF N2) and gas inhalation (CO2, N2) treatments did not differ significantly. The time to cessation of movement of spent hens in the CAF N2 treatment was significantly shorter than CAF and CAF CO2 treatments but longer than the gas inhalation treatments. These data suggest that the addition of N2 is advantageous in terms of shortening time to death and improved foam quality as compared to the CAF CO2 treatment. PMID:29301340
Electrocatalytic process for carbon dioxide conversion
DOE Office of Scientific and Technical Information (OSTI.GOV)
Masel, Richard I.; Salehi-Khojin, Amin; Kutz, Robert
An electrocatalytic process for carbon dioxide conversion includes combining a Catalytically Active Element and a Helper Polymer in the presence of carbon dioxide, allowing a reaction to proceed to produce a reaction product, and applying electrical energy to said reaction to achieve electrochemical conversion of said carbon dioxide reactant to said reaction product. The Catalytically Active Element can be a metal in the form of supported or unsupported particles or flakes with an average size between 0.6 nm and 100 nm. The reaction products comprise at least one of CO, HCO.sup.-, H.sub.2CO, (HCO.sub.2).sup.-, H.sub.2CO.sub.2, CH.sub.3OH, CH.sub.4, C.sub.2H.sub.4, CH.sub.3CH.sub.2OH, CH.sub.3COO.sup.-, CH.sub.3COOH,more » C.sub.2H.sub.6, (COOH).sub.2, (COO.sup.-).sub.2, and CF.sub.3COOH.« less
Recuperative supercritical carbon dioxide cycle
Sonwane, Chandrashekhar; Sprouse, Kenneth M; Subbaraman, Ganesan; O'Connor, George M; Johnson, Gregory A
2014-11-18
A power plant includes a closed loop, supercritical carbon dioxide system (CLS-CO.sub.2 system). The CLS-CO.sub.2 system includes a turbine-generator and a high temperature recuperator (HTR) that is arranged to receive expanded carbon dioxide from the turbine-generator. The HTR includes a plurality of heat exchangers that define respective heat exchange areas. At least two of the heat exchangers have different heat exchange areas.
NASA Astrophysics Data System (ADS)
Wohlfahrt, Georg; Cremonese, Edoardo; Hammerle, Albin; Hörtnagl, Lukas; Galvagno, Marta; Gianelle, Damiano; Marcolla, Barbara; Cella, Umberto Morra
2013-12-01
is well established that warming leads to longer growing seasons in seasonally cold ecosystems. Whether this goes along with an increase in the net ecosystem carbon dioxide (CO2) uptake is much more controversial. We studied the effects of warming on the start of the carbon uptake period (CUP) of three mountain grasslands situated along an elevational gradient in the Alps. To this end, we used a simple empirical model of the net ecosystem CO2 exchange, calibrated, and forced with multiyear empirical data from each site. We show that reductions in the quantity and duration of daylight associated with earlier snowmelts were responsible for diminishing returns, in terms of carbon gain, from longer growing seasons caused by reductions in daytime photosynthetic uptake and increases in nighttime losses of CO2. This effect was less pronounced at high, compared to low, elevations, where the start of the CUP occurred closer to the summer solstice when changes in day length and incident radiation are minimal.
Wohlfahrt, Georg; Cremonese, Edoardo; Hammerle, Albin; Hörtnagl, Lukas; Galvagno, Marta; Gianelle, Damiano; Marcolla, Barbara; di Cella, Umberto Morra
2013-12-16
It is well established that warming leads to longer growing seasons in seasonally cold ecosystems. Whether this goes along with an increase in the net ecosystem carbon dioxide (CO 2 ) uptake is much more controversial. We studied the effects of warming on the start of the carbon uptake period (CUP) of three mountain grasslands situated along an elevational gradient in the Alps. To this end we used a simple empirical model of the net ecosystem CO 2 exchange, calibrated and forced with multi-year empirical data from each site. We show that reductions in the quantity and duration of daylight associated with earlier snowmelts were responsible for diminishing returns, in terms of carbon gain, from longer growing seasons caused by reductions in daytime photosynthetic uptake and increases in nighttime losses of CO 2 . This effect was less pronounced at high, compared to low, elevations, where the start of the CUP occurred closer to the summer solstice when changes in day length and incident radiation are minimal.
NASA Astrophysics Data System (ADS)
Du, Juan; Liu, Jiqiao; Bi, Decang; Ma, Xiuhua; Hou, Xia; Zhu, Xiaolei; Chen, Weibiao
2018-04-01
A ground-based double-pulse 1572 nm integrated path differential absorption (IPDA) lidar was developed for carbon dioxide (CO2) column concentrations measurement. The lidar measured the CO2 concentrations continuously by receiving the scattered echo signal from a building about 1300 m away. The other two instruments of TDLAS and in-situ CO2 analyzer measured the CO2 concentrations on the same time. A CO2 concentration measurement of 430 ppm with 1.637 ppm standard error was achieved.
Sterilizing Bacillus pumilus spores using supercritical carbon dioxide.
Zhang, Jian; Burrows, Sarah; Gleason, Courtney; Matthews, Michael A; Drews, Michael J; Laberge, Martine; An, Yuehuei H
2006-09-01
Supercritical carbon dioxide (SC CO(2)) has been evaluated as a new sterilization technology. Results are presented on killing of B. pumilus spores using SC CO(2) containing trace levels of additives. Complete killing was achieved with 200 part per million (ppm) hydrogen peroxide in SC CO(2) at 60 degrees C, 27.5 MPa. Addition of water to SC CO(2) resulted in greater than three-log killing, but this is insufficient to claim sterilization. Neither ethanol nor isopropanol when added to SC CO(2) affected killing.
Chemical reactions occurring during direct solar reduction of CO2.
Lyma, J L; Jensen, R J
2001-09-28
At high temperatures carbon dioxide may absorb solar radiation and react to form carbon monoxide and molecular oxygen. The CO, so produced, may be converted by well-established means to a combustible fuel, such as methanol. We intend to make a future demonstration of the solar reduction of CO2 based on these processes. This paper, however, addresses only the problem of preserving, or even enhancing, the initial photolytic CO by quenching the hot gas with colder H2O or CO2. We present model calculations with a reaction mechanism used extensively in other calculations. If a CO2 gas stream is heated and photolyzed by intense solar radiation and then allowed to cool slowly, it will react back to the initial CO2 by a series of elementary chemical reactions. The back reaction to CO2 can be terminated with the rapid addition of CO2, water, or a mixture. Calculations show that a three-fold quench with pure CO2 will stop the reactions and preserve over 90% of the initial photolytic CO. We find that water has one of two effects. It can either increase the CO level, or it can catalyze the recombination of O and CO to CO2. The gas temperature is the determining factor. If the quench gas is not sufficient to keep the temperature below approximately 1100 K, a chain-branching reaction dominates and the reaction to CO2 occurs. If the temperature stays below that level a chain terminating reaction dominates and the CO is increased. The former case occurs below approximately a fourfold quench with a water/CO2 mixture. The later case occurs when the quench is greater than fourfold. We conclude that CO2, H2O, or a mixture may quench the hot gas stream photolyzed by solar radiation and preserve the photolytic CO.
Method for carbon dioxide sequestration
Wang, Yifeng; Bryan, Charles R.; Dewers, Thomas; Heath, Jason E.
2015-09-22
A method for geo-sequestration of a carbon dioxide includes selection of a target water-laden geological formation with low-permeability interbeds, providing an injection well into the formation and injecting supercritical carbon dioxide (SC--CO.sub.2) into the injection well under conditions of temperature, pressure and density selected to cause the fluid to enter the formation and splinter and/or form immobilized ganglia within the formation. This process allows for the immobilization of the injected SC--CO.sub.2 for very long times. The dispersal of scCO2 into small ganglia is accomplished by alternating injection of SC--CO.sub.2 and water. The injection rate is required to be high enough to ensure the SC--CO.sub.2 at the advancing front to be broken into pieces and small enough for immobilization through viscous instability.
Performance of Charcoal Cookstoves for Haiti, Part 2: Results from the Controlled Cooking Test
DOE Office of Scientific and Technical Information (OSTI.GOV)
Lask, Kathleen; Jones, Jennifer; Booker, Kayje
2011-11-30
Five charcoal cookstoves were tested using a Controlled Cooking Test (CCT) developed from cooking practices in Haiti. Cookstoves were tested for total burn time, specific fuel consumption, and emissions of carbon monoxide (CO), carbon dioxide (CO 2), and the ratio of carbon monoxide to carbon dioxide (CO/CO 2). These results are presented in this report along with LBNL testers’ observations regarding the usability of the stoves.
Six-man, self-contained carbon dioxide concentrator system
NASA Technical Reports Server (NTRS)
Powell, J. D.; Schubert, F. H.; Marshall, R. D.; Shumar, J. W.
1974-01-01
A six man, self contained electrochemical carbon dioxide concentrating subsystem was successfully designed and fabricated. It was a preprototype engineering model designed to nominally remove 6.0 kg (13.2 lb) CO2/day with an inlet air CO2 partial pressure of 400 N/sq m (3 mm Hg) and an overcapacity removal capability of 12.0 kg (26.4 lb) CO2/day. The design specifications were later expanded to allow operation at space station prototype CO2 collection subsystem operating conditions.
Cerebrovascular response to the cold pressor test - the critical role of carbon dioxide.
Tymko, Michael M; Kerstens, Thijs P; Wildfong, Kevin W; Ainslie, Philip N
2017-12-01
What is the central question of this study? What is the role of carbon dioxide in the cerebral blood flow (CBF) response to the cold pressor test (CPT)? What is the main finding and its importance? The CBF response was elevated during the isocapnic (controlled CO 2 ) CPT in the middle cerebral artery and the internal carotid artery compared with the poikilocapnic (uncontrolled CO 2 ) CPT, owing to ventilation-associated reductions in end-tidal CO 2 . Furthermore, the common carotid artery vasodilated to a greater extent during the isocapnic compared with the poikilocapnic CPT, whereas the internal carotid artery vasoconstricted during both CPTs. Our data highlight the importance of CO 2 control when investigating the CBF response to the CPT. In addition to increasing sympathetic nervous activity, blood pressure and cerebral blood flow (CBF), the cold pressor test (CPT) stimulates pain receptors, which may increase ventilation above metabolic demand; this response is likely to reduce the partial pressure of end-tidal carbon dioxide (P ET ,CO2) and will attenuate elevations in CBF. Our hypotheses were as follows: (i) the CPT will elicit hyperventilation, effectively lowering P ET ,CO2; (ii) the CBF response will be elevated during an isocapnic (controlled P ET ,CO2) compared with a poikilocapnic CPT (uncontrolled P ET ,CO2); and (iii) in response to the CPT, the common carotid artery (CCA) will vasodilate, while the internal carotid artery (ICA) will remain unchanged to help regulate CBF. Using a new, randomized experimental design, we measured the cerebrovascular response in the middle cerebral artery (MCA), CCA and internal carotid artery (ICA), during an isocapnic and poikilocapnic CPT in 15 participants. Blood pressure and cardiac output (finger photoplethysmography), heart rate (ECG), MCA mean velocity (transcranial Doppler ultrasound) and CCA and ICA CBF (Duplex ultrasound) were recorded during both CPT trials. Our findings were as follows: (i) ventilation increased, which reduced P ET ,CO2 (-5.3 ± 6.4 mmHg) during the poikilocapnic compared with the isocapnic CPT; (ii) the CBF response was elevated during the isocapnic compared with the poikilocapnic CPT in the MCA and ICA, but not in the CCA; and (iii) the CCA dilated to a greater extent during the isocapnic compared with the poikilocapnic CPT, and the ICA vasoconstricted during both trials. Our data emphasize the importance of P ET ,CO2 control in the CBF response to the CPT and in the differential vasomotor regulation between the CCA and ICA. © 2017 The Authors. Experimental Physiology © 2017 The Physiological Society.
Carbon dioxide stripping in aquaculture. part 1: terminology and reporting
Colt, John; Watten, Barnaby; Pfeiffer, Tim
2012-01-01
The removal of carbon dioxide gas in aquacultural systems is much more complex than for oxygen or nitrogen gas because of liquid reactions of carbon dioxide and their kinetics. Almost all published carbon dioxide removal information for aquaculture is based on the apparent removal value after the CO2(aq) + HOH ⇔ H2CO3 reaction has reached equilibrium. The true carbon dioxide removal is larger than the apparent value, especially for high alkalinities and seawater. For low alkalinity freshwaters (<2000 μeq/kg), the difference between the true and apparent removal is small and can be ignored for many applications. Analytical and reporting standards are recommended to improve our understanding of carbon dioxide removal.
Development of a low cost unmanned aircraft system for atmospheric carbon dioxide leak detection
NASA Astrophysics Data System (ADS)
Mitchell, Taylor Austin
Carbon sequestration, the storage of carbon dioxide gas underground, has the potential to reduce global warming by removing a greenhouse gas from the atmosphere. These storage sites, however, must first be monitored to detect if carbon dioxide is leaking back out to the atmosphere. As an alternative to traditional large ground-based sensor networks to monitor CO2 levels for leaks, unmanned aircraft offer the potential to perform in-situ atmospheric leak detection over large areas for a fraction of the cost. This project developed a proof-of-concept sensor system to map relative carbon dioxide levels to detect potential leaks. The sensor system included a Sensair K-30 FR CO2 sensor, GPS, and altimeter connected an Arduino microcontroller which logged data to an onboard SD card. Ground tests were performed to verify and calibrate the system including wind tunnel tests to determine the optimal configuration of the system for the quickest response time (4-8 seconds based upon flowrate). Tests were then conducted over a controlled release of CO 2 in addition to over controlled rangeland fires which released carbon dioxide over a large area as would be expected from a carbon sequestration source. 3D maps of carbon dioxide were developed from the system telemetry that clearly illustrated increased CO2 levels from the fires. These tests demonstrated the system's ability to detect increased carbon dioxide concentrations in the atmosphere.
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.
Pan, Shu-Yuan; Chung, Tai-Chun; Ho, Chang-Ching; Hou, Chin-Jen; Chen, Yi-Hung; Chiang, Pen-Chi
2017-12-08
Both steelmaking via an electric arc furnace and manufacturing of portland cement are energy-intensive and resource-exploiting processes, with great amounts of carbon dioxide (CO 2 ) emission and alkaline solid waste generation. In fact, most CO 2 capture and storage technologies are currently too expensive to be widely applied in industries. Moreover, proper stabilization prior to utilization of electric arc furnace slag are still challenging due to its high alkalinity, heavy metal leaching potentials and volume instability. Here we deploy an integrated approach to mineralizing flue gas CO 2 using electric arc furnace slag while utilizing the reacted product as supplementary cementitious materials to establish a waste-to-resource supply chain toward a circular economy. We found that the flue gas CO 2 was rapidly mineralized into calcite precipitates using electric arc furnace slag. The carbonated slag can be successfully utilized as green construction materials in blended cement mortar. By this modulus, the global CO 2 reduction potential using iron and steel slags was estimated to be ~138 million tons per year.
Formation and decomposition of siderite for CO2 treatment
NASA Astrophysics Data System (ADS)
Y Mora, E.; Sarmiento, A.; Vera, E.; Drozd, V.; Durigyn, A.; Saxena, S.
2017-12-01
In this research work, we studied the conditions for formation and decomposition of siderite FeCO3 from hematite Fe2O3 along with carbon dioxide CO2 at suitable thermodynamic conditions. As reductant agents were used mixtures of two elements, metallic iron and graphite. Best levels of carbonation were found in mixtures with bigger amounts of metallic iron. It was demonstrated that CO2 capture capacity by hematite depends of temperature, CO2 pressure, and reaction time. Temperatures between 100 and 150°C, pressures between 10 and 30bar and reaction times between 1 and 4h were adjusted for analyse the carbonation behaviour; siderite formation was improved by increases of these three variables. There was no carbonation without water in the mixtures, due to kinetic limitations. CO2 capture capacity was calculated from Rietveld refinement results. Using vacuum system and Dielectric Barrier Discharge, DBD plasma, the siderite was decomposed at 300°C, and 320°C respectively. Techniques as X-ray diffraction, and surface area analysis were employed to study the material.
An advanced carbon reactor subsystem for carbon dioxide reduction
NASA Technical Reports Server (NTRS)
Noyes, Gary P.; Cusick, Robert J.
1986-01-01
An evaluation is presented of the development status of an advanced carbon-reactor subsystem (ACRS) for the production of water and dense, solid carbon from CO2 and hydrogen, as required in physiochemical air revitalization systems for long-duration manned space missions. The ACRS consists of a Sabatier Methanation Reactor (SMR) that reduces CO2 with hydrogen to form methane and water, a gas-liquid separator to remove product water from the methane, and a Carbon Formation Reactor (CFR) to pyrolize methane to carbon and hydrogen; the carbon is recycled to the SMR, while the produce carbon is periodically removed from the CFR. A preprototype ACRS under development for the NASA Space Station is described.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Kuc, T.; Rozanski, K.; Zimnoch, M.
2007-07-01
Time series are presented of radiocarbon and C-13 contents in atmospheric carbon dioxide over eastern Europe (southern Poland), covering the periods 1983-1994 and 2000-2004. The carbon isotope composition was measured in biweekly composite samples of atmospheric CO{sub 2}, collected about 20 m above the local ground level. The data for 2 observational sites are presented: I) city of Krakow (50{sup o} 04'N, 19{sup o} 55'E; 220 m asl; for 1983-1994 and 2000-2004); and ii) Kasprowy Wierch, Tatra Mountains (49{sup o} 14'N, 19{sup o} 56'E; 1989 m asl; for 2000-2004). The latter site is considered a regional reference station, relatively freemore » of anthropogenic influences. During the period 1983-1994, observations in the Krakow area revealed a gradual decrease of C-14 content with a broad minimum around 1991 and a small increase by about 10 parts per thousand in the subsequent years. {delta}C-13 also changes with time, showing a decreasing trend from approximately -9.6 parts per thousand in 1983, with a slope of -0.02 parts per thousand/yr. The observed trends for both isotopes coincide well with a substantial reduction of coal consumption in Poland and partial replacement of coal by natural gas, especially in urban regions. After 2000, the {delta}C-13 slightly increases, reaching a mean value of -10 parts per thousand in 2004, while {delta}C-14 is below the reference level by similar to 3.5 parts per thousand. Observations at Kasprowy Wierch (regional reference station) also reflect a diminishing input of fossil carbon into the regional atmosphere. The fossil component in atmospheric CO{sub 2}, calculated with the aid of C-14 data available for the 2 study periods, shows a reduction of anthropogenic input by a factor of 2, which is confirmed by annual statistics of coal consumption.« less
NASA Astrophysics Data System (ADS)
Schmidt, Andres; Rella, Chris W.; Göckede, Mathias; Hanson, Chad; Yang, Zhenlin; Law, Beverly E.
2014-11-01
In recent years, measurements of atmospheric carbon dioxide with high precision and accuracy have become increasingly important for climate change research, in particular to inform terrestrial biosphere models. Anthropogenic carbon dioxide emissions from fossil fuel burning have long been recognized to contribute a significant portion of the carbon dioxide in the atmosphere. Here, we present an approach to remove the traffic related carbon dioxide emissions from mole fractions measured at a tall tower by using the corresponding carbon monoxide measurements in combination with footprint analyses and transport modeling. This technique improves the suitability of the CO2 data to be used in inverse modeling approaches of atmosphere-biosphere exchange that do not account for non-biotic portions of CO2. In our study region in Oregon, road traffic emissions are the biggest source of anthropogenic carbon dioxide and carbon monoxide. A three-day mobile campaign covering 1700 km of roads in northwestern Oregon was performed during summer of 2012 using a laser-based Cavity Ring-Down Spectrometer. The mobile measurements incorporated different roads including main highways, urban streets, and back-roads, largely within the typical footprint of a tall CO/CO2 observation tower in Oregon's Willamette Valley. For the first time, traffic related CO:CO2 emission ratios were measured directly at the sources during an on-road campaign under a variety of different driving conditions. An average emission ratio of 7.43 (±1.80) ppb CO per ppm CO2 was obtained for the study region and applied to separate the traffic related portion of CO2 from the mole fraction time series. The road traffic related portion of the CO2 mole fractions measured at the tower site reached maximum values ranging from 9.8 to 12 ppm, depending on the height above the surface, during summer 2012.
Synthesis of TiO2/functionalized graphene sheets (FGSs) nanocomposites in super critical CO2
NASA Astrophysics Data System (ADS)
Farhangi, Nasrin; Medina-Gonzalez, Yaocihuatl; Chen, Bo; Charpentier, Paul A.
2010-06-01
Highly ordered TiO2 nanowire arrays were prepared on the surface of Functionalized Graphene sheets (FGSs) by solgel method using titanium isopropoxide monomer with acetic acid as the polycondensation agent in the green solvent, supercritical carbon dioxide (sc-CO2). Morphology of synthesized materials was studied by SEM and TEM. Optical properties of the nanocomposites studied by UV spectroscopy which showed high absorption in visible area as well as reduction in their band gap compared to TiO2. By high resolution XPS, chelating bidentate structure of TiO2 with carboxylic group on the surface of graphene sheets can be confirmed. Improvement in the optical properties of the synthesized composites compared to TiO2 alone was confirmed by photocurrent measurements.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Jones, Brant M.; Kaiser, Ralf I.; Strazzulla, Giovanni, E-mail: brantmj@hawaii.edu
Carbon dioxide (CO{sub 2}) has been detected on the surface of several icy moons of Jupiter and Saturn via observation of the ν{sub 3} band with the Near-Infrared Mapping Spectrometer on board the Galileo spacecraft and the Visible-Infrared Mapping Spectrometer on board the Cassini spacecraft. Interestingly, the CO{sub 2} band for several of these moons exhibits a blueshift along with a broader profile than that seen in laboratory studies and other astrophysical environments. As such, numerous attempts have been made in order to clarify this abnormal behavior; however, it currently lacks an acceptable physical or chemical explanation. We present amore » rather surprising result pertaining to the synthesis of carbon dioxide in a polar environment. Here, carbonic acid was synthesized in a water (H{sub 2}O)-carbon dioxide (CO{sub 2}) (1:5) ice mixture exposed to ionizing radiation in the form of 5 keV electrons. The irradiated ice mixture was then annealed, producing pure carbonic acid which was then subsequently irradiated, recycling water and carbon dioxide. However, the observed carbon dioxide ν{sub 3} band matches almost exactly with that observed on Callisto; subsequent temperature program desorption studies reveal that carbon dioxide synthesized under these conditions remains in solid form until 160 K, i.e., the sublimation temperature of water. Consequently, our results suggest that carbon dioxide on Callisto as well as other icy moons is indeed complexed with water rationalizing the shift in peak frequency, broad profile, and the solid state existence on these relatively warm moons.« less
NASA Technical Reports Server (NTRS)
Bishop, Phillip; Greenisen, M. C.
1997-01-01
The Launch and Entry Suit (LES) and Advanced Crew Escape Suit (ACES) are worn by astronauts for launch and entry. Previous work by Waligora, et al., 1992, Waligora and Gilbert, 1992, and Dalrymple 1996, have found that carbon dioxide (CO2) accumulation in the LES/ACES helmet may be problematic. CO2 accumulation is important because high inspired levels of CO2 reduce physical function and pose a safety hazard (e.g. levels of CO2 accumulation of 3.6% in the Extravehicular Mobility Unit are sufficient to terminate Extra Vehicular Activities). My task was to design a suitable test protocol for determining the important physiological aspects of LES/ACES use. Three basic issues arose. First was the determination of the astronaut's CO2 inspiration during visor-down use at rest and during walking at 3.5 mph. A sub-issue was the impact of a pneumotach on CO2 since it has been previously observed that when the Aerosport pneumotach was used, performance seemed improved, which might be attributable to a lowered respiration rate when using the pneumotach. The second issue was the energy costs of waLking in the LES/ACES with various G-suit inflation levels, since G-suit inflation increases metabolic costs and metabolic costs influence the C02 production in the LES/ACES helmet. Since G-suit inflation improves orthostatic tolerance after space flight, but likely increases the energy costs of walking, the balance between G-suit inflation and C02 accumulation is an important safety consideration. The third issue which arose from pilot work was the substantial reduction in physical function after a 10 min visor-down period prior to walk.
NASA Astrophysics Data System (ADS)
Kornhuber, Kai; Rybski, Diego; Costa, Luis; Reusser, Dominik E.; Kropp, Jürgen P.
2014-05-01
The Environmental Kuznets Curves (EKC) postulates that pollution increases with the income per capita up to a maximum, above which it decreases with the further increase in income per capita, i.e. following an inverse U-shape in the pollution vs. income per capita. It is commonly believed that EKC occurs for "local" pollutants such as nitrogen oxide and sulfur dioxide, but does not hold for CO2 emissions. This is attributed to the fact that while "local" pollutants cause a visible environmental damage on the local/regional scale (which authorities/governments seek to avoid), the consequences of CO2 emission have no immediate attributable local/regional consequences. We review EKC for CO2 exploring its relation between CO2 per capita and the Human Development Index (HDI) between 1990 and 2010 obtained from the World Bank database. We find evidence for a reduction in CO2 emissions per capita in highly developed countries. We propose a model according to which the emissions per capita of a country are composed of a component related to the actual state of development and a component related to the change of development. The model leads to four distinct cases of which two have EKC shape and two imply saturation. This outcome is in line with previously suggested qualitative relations. Our analysis indicates that the EKC shaped cases better describes the empirical values. We explore the less extreme version corresponding to the so-called conventional EKC and study the maximum of the fitted curve, providing a threshold-value for the HDI and a typical maximum value for the emissions per capita. We find that approx. 5 countries have crossed the CO2-HDI maximum, corresponding to approx. 1.5% of the world population.
Diaztagle Fernández, J J; Rodríguez Murcia, J C; Sprockel Díaz, J J
2017-10-01
The way to assess tissue perfusion during the resuscitation of patients with severe sepsis and septic shock is a current subject of research and debate. Venous oxygen saturation and lactate concentration have been the most frequently used criteria, though they involve known limitations. The venous-to-arterial difference of carbon dioxide (pCO 2 delta) is a parameter than can be used to indicate tissue perfusion, and its determination therefore may be useful in these patients. A qualitative systematic review of the literature was made, comprising studies that assessed pCO 2 delta in adult patients with severe sepsis or septic shock, and published between January 1966 and November 2016 in the Medline-PubMed, Embase-Elsevier, Cochrane Library, and LILACS databases. There was no language restriction. The PRISMA statement was followed, and methodological quality was evaluated. Twelve articles were included, all of an observational nature, and including 10 prospective studies (9 published since 2010). Five documented greater mortality among patients with high pCO 2 delta values, in 3 cases even when achieving venous oxygen saturation targets. In 4 studies, a high pCO 2 delta was related to lower venous oxygen saturation and higher lactate levels, and another 3 documented lesser percentage lactate reductions. The parameter pCO 2 delta has been more frequently assessed in the management of patients with severe sepsis during the last few years. The studies demonstrate its correlation to mortality and other clinical outcomes, defining pCO 2 delta as a useful tool in the management of these patients. Copyright © 2017 Elsevier España, S.L.U. y SEMICYUC. All rights reserved.
Capacitance-Assisted Sustainable Electrochemical Carbon Dioxide Mineralisation.
Lamb, Katie J; Dowsett, Mark R; Chatzipanagis, Konstantinos; Scullion, Zhan Wei; Kröger, Roland; Lee, James D; Aguiar, Pedro M; North, Michael; Parkin, Alison
2018-01-10
An electrochemical cell comprising a novel dual-component graphite and Earth-crust abundant metal anode, a hydrogen producing cathode and an aqueous sodium chloride electrolyte was constructed and used for carbon dioxide mineralisation. Under an atmosphere of 5 % carbon dioxide in nitrogen, the cell exhibited both capacitive and oxidative electrochemistry at the anode. The graphite acted as a supercapacitive reagent concentrator, pumping carbon dioxide into aqueous solution as hydrogen carbonate. Simultaneous oxidation of the anodic metal generated cations, which reacted with the hydrogen carbonate to give mineralised carbon dioxide. Whilst conventional electrochemical carbon dioxide reduction requires hydrogen, this cell generates hydrogen at the cathode. Carbon capture can be achieved in a highly sustainable manner using scrap metal within the anode, seawater as the electrolyte, an industrially relevant gas stream and a solar panel as an effective zero-carbon energy source. © 2017 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.
Pathways limiting warming to 1.5°C: a tale of turning around in no time?
NASA Astrophysics Data System (ADS)
Kriegler, Elmar; Luderer, Gunnar; Bauer, Nico; Baumstark, Lavinia; Fujimori, Shinichiro; Popp, Alexander; Rogelj, Joeri; Strefler, Jessica; van Vuuren, Detlef P.
2018-05-01
We explore the feasibility of limiting global warming to 1.5°C without overshoot and without the deployment of carbon dioxide removal (CDR) technologies. For this purpose, we perform a sensitivity analysis of four generic emissions reduction measures to identify a lower bound on future CO2 emissions from fossil fuel combustion and industrial processes. Final energy demand reductions and electrification of energy end uses as well as decarbonization of electricity and non-electric energy supply are all considered. We find the lower bound of cumulative fossil fuel and industry CO2 emissions to be 570 GtCO2 for the period 2016-2100, around 250 GtCO2 lower than the lower end of available 1.5°C mitigation pathways generated with integrated assessment models. Estimates of 1.5°C-consistent CO2 budgets are highly uncertain and range between 100 and 900 GtCO2 from 2016 onwards. Based on our sensitivity analysis, limiting warming to 1.5°C will require CDR or terrestrial net carbon uptake if 1.5°C-consistent budgets are smaller than 650 GtCO2. The earlier CDR is deployed, the more it neutralizes post-2020 emissions rather than producing net negative emissions. Nevertheless, if the 1.5°C budget is smaller than 550 GtCO2, temporary overshoot of the 1.5°C limit becomes unavoidable if CDR cannot be ramped up faster than to 4 GtCO2 in 2040 and 10 GtCO2 in 2050. This article is part of the theme issue `The Paris Agreement: understanding the physical and social challenges for a warming world of 1.5°C above pre-industrial levels'.
Pathways limiting warming to 1.5°C: a tale of turning around in no time?
Kriegler, Elmar; Luderer, Gunnar; Bauer, Nico; Baumstark, Lavinia; Fujimori, Shinichiro; Popp, Alexander; Rogelj, Joeri; Strefler, Jessica; van Vuuren, Detlef P
2018-05-13
We explore the feasibility of limiting global warming to 1.5°C without overshoot and without the deployment of carbon dioxide removal (CDR) technologies. For this purpose, we perform a sensitivity analysis of four generic emissions reduction measures to identify a lower bound on future CO 2 emissions from fossil fuel combustion and industrial processes. Final energy demand reductions and electrification of energy end uses as well as decarbonization of electricity and non-electric energy supply are all considered. We find the lower bound of cumulative fossil fuel and industry CO 2 emissions to be 570 GtCO 2 for the period 2016-2100, around 250 GtCO 2 lower than the lower end of available 1.5°C mitigation pathways generated with integrated assessment models. Estimates of 1.5°C-consistent CO 2 budgets are highly uncertain and range between 100 and 900 GtCO 2 from 2016 onwards. Based on our sensitivity analysis, limiting warming to 1.5°C will require CDR or terrestrial net carbon uptake if 1.5°C-consistent budgets are smaller than 650 GtCO 2 The earlier CDR is deployed, the more it neutralizes post-2020 emissions rather than producing net negative emissions. Nevertheless, if the 1.5°C budget is smaller than 550 GtCO 2 , temporary overshoot of the 1.5°C limit becomes unavoidable if CDR cannot be ramped up faster than to 4 GtCO 2 in 2040 and 10 GtCO 2 in 2050.This article is part of the theme issue 'The Paris Agreement: understanding the physical and social challenges for a warming world of 1.5°C above pre-industrial levels'. © 2018 The Author(s).
Experimental Investigation of Mechanical Properties of Black Shales after CO2-Water-Rock Interaction
Lyu, Qiao; Ranjith, Pathegama Gamage; Long, Xinping; Ji, Bin
2016-01-01
The effects of CO2-water-rock interactions on the mechanical properties of shale are essential for estimating the possibility of sequestrating CO2 in shale reservoirs. In this study, uniaxial compressive strength (UCS) tests together with an acoustic emission (AE) system and SEM and EDS analysis were performed to investigate the mechanical properties and microstructural changes of black shales with different saturation times (10 days, 20 days and 30 days) in water dissoluted with gaseous/super-critical CO2. According to the experimental results, the values of UCS, Young’s modulus and brittleness index decrease gradually with increasing saturation time in water with gaseous/super-critical CO2. Compared to samples without saturation, 30-day saturation causes reductions of 56.43% in UCS and 54.21% in Young’s modulus for gaseous saturated samples, and 66.05% in UCS and 56.32% in Young’s modulus for super-critical saturated samples, respectively. The brittleness index also decreases drastically from 84.3% for samples without saturation to 50.9% for samples saturated in water with gaseous CO2, to 47.9% for samples saturated in water with super-critical carbon dioxide (SC-CO2). SC-CO2 causes a greater reduction of shale’s mechanical properties. The crack propagation results obtained from the AE system show that longer saturation time produces higher peak cumulative AE energy. SEM images show that many pores occur when shale samples are saturated in water with gaseous/super-critical CO2. The EDS results show that CO2-water-rock interactions increase the percentages of C and Fe and decrease the percentages of Al and K on the surface of saturated samples when compared to samples without saturation. PMID:28773784
Homogeneously Catalyzed Electroreduction of Carbon Dioxide-Methods, Mechanisms, and Catalysts.
Francke, Robert; Schille, Benjamin; Roemelt, Michael
2018-05-09
The utilization of CO 2 via electrochemical reduction constitutes a promising approach toward production of value-added chemicals or fuels using intermittent renewable energy sources. For this purpose, molecular electrocatalysts are frequently studied and the recent progress both in tuning of the catalytic properties and in mechanistic understanding is truly remarkable. While in earlier years research efforts were focused on complexes with rare metal centers such as Re, Ru, and Pd, the focus has recently shifted toward earth-abundant transition metals such as Mn, Fe, Co, and Ni. By application of appropriate ligands, these metals have been rendered more than competitive for CO 2 reduction compared to the heavier homologues. In addition, the important roles of the second and outer coordination spheres in the catalytic processes have become apparent, and metal-ligand cooperativity has recently become a well-established tool for further tuning of the catalytic behavior. Surprising advances have also been made with very simple organocatalysts, although the mechanisms behind their reactivity are not yet entirely understood. Herein, the developments of the last three decades in electrocatalytic CO 2 reduction with homogeneous catalysts are reviewed. A discussion of the underlying mechanistic principles is included along with a treatment of the experimental and computational techniques for mechanistic studies and catalyst benchmarking. Important catalyst families are discussed in detail with regard to mechanistic aspects, and recent advances in the field are highlighted.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Tilmes, S.; Fasullo, John; Lamarque, J.-F.
2013-10-14
Abstract: The hydrologic impact of enhancing Earth’s albedo due to solar radiation management (SRM) is investigated using simulations from 12 models contributing to the Geoengineering Model Intercomparison Project (GeoMIP). An artificial experiment is investigated, where global mean temperature is preserved at pre-industrial conditions, while atmospheric carbon dioxide concentrations are quadrupled. The associated reduction of downwelling surface solar radiation in a high CO2 environment leads to a reduction of global evaporation of 10% and 4% and precipitation of 6.1% and 6.3% over land and ocean, respectively. An initial reduction of latent heat flux at the surface is largely driven by reducedmore » evapotranspiration over land with instantly increasing CO2 concentrations in both experiments. A warming surface associated with the transient adjustment in the 4xCO2 experiment further generates an increase of global precipitation, with considerable regional changes, such as a significant precipitation reduction of 7% for the North American summer monsoon. Reduced global precipitation persists in the geoengineered experiment where temperatures are stabilized, with considerable regional rainfall deficits. Precipitation reductions that are consistent in sign across models are identified in the geoengineered experiment over monsoonal land regions of East Asia (6%), North America (7%), South America (6%) and South Africa (5%). In contrast to the 4xCO2 experiment, where the frequency of months with heavy precipitation intensity is increased by over 50%, it is reduced by up to 20% in the geoengineering scenario . The reduction in heavy precipitation is more pronounced over land than over the ocean, and accompanies a stronger reduction in evaporation over land. For northern mid-latitudes, maximum precipitation reduction over land ranges from 1 to 16% for individual models. For 45-65°N, the frequency of median to high intensity precipitation in summer is strongly reduced. These changes in precipitation in both total amount and frequency of extremes, point to a considerable weakening of the hydrological cycle in a geoengineered world.« less
Conversion of carbon dioxide to carbon monoxide by pulse dielectric barrier discharge plasma
NASA Astrophysics Data System (ADS)
Wang, Taobo; Liu, Hongxia; Xiong, Xiang; Feng, Xinxin
2017-01-01
The conversion of carbon dioxide (CO2) to carbon monoxide (CO) was investigated in a non-thermal plasma dielectric barrier discharge (DBD) reactor, and the effects of different process conditions on the CO2 conversion were investigated. The results showed that the increase of input power could optimize the conversion of CO2 to CO. The CO2 conversion and CO yield were negatively correlated with the gas flow rate, but there was an optimum gas flow rate, that made the CO selectivity best. The carrier gas (N2, Ar) was conducive to the conversion of CO2, and the effect of N2 as carrier gas was better than Ar. The conversion of CO2 to CO was enhanced by addition of the catalyst (5A molecular sieve).
A simple method for isocapnic hyperventilation evaluated in a lung model.
Hallén, K; Stenqvist, O; Ricksten, S-E; Lindgren, S
2016-05-01
Isocapnic hyperventilation (IHV) has the potential to increase the elimination rate of anaesthetic gases and has been shown to shorten time to wake-up and post-operative recovery time after inhalation anaesthesia. In this bench test, we describe a technique to achieve isocapnia during hyperventilation (HV) by adding carbon dioxide (CO2) directly to the breathing circuit of a standard anaesthesia apparatus with standard monitoring equipment. Into a mechanical lung model, carbon dioxide was added to simulate a CO2 production (V(CO2)) of 175, 200 and 225 ml/min. Dead space (V(D)) volume could be set at 44, 92 and 134 ml. From baseline ventilation (BLV), HV was achieved by doubling the minute ventilation and fresh gas flow for each level of V(CO2), and dead space. During HV, CO2 was delivered (D(CO2)) by a precision flow meter via a mixing box to the inspiratory limb of the anaesthesia circuit to achieve isocapnia. During HV, the alveolar ventilation increased by 113 ± 6%. Tidal volume increased by 20 ± 0.1% during IHV irrespective of V(D) and V(CO2) level. D(CO2) varied between 147 ± 8 and 325 ± 13 ml/min. Low V(CO2) and large V(D) demanded a greater D(CO2) administration to achieve isocapnia. The FICO2 level during IHV varied between 2.3% and 3.3%. It is possible to maintain isocapnia during HV by delivering carbon dioxide through a standard anaesthesia circuit equipped with modern monitoring capacities. From alveolar ventilation, CO2 production and dead space, the amount of carbon dioxide that is needed to achieve IHV can be estimated. © 2015 The Acta Anaesthesiologica Scandinavica Foundation. Published by John Wiley & Sons Ltd.
Will Transition of Staple Food Strategy in China Really Mitigate Global Climate Change?
NASA Astrophysics Data System (ADS)
Liu, B.; Zhao, D.
2017-12-01
With the increase in agricultural demand, reducing greenhouse gas (GHG) emissions is a vital challenge in mitigating climate change. Potato staple food strategy in China introduced by Ministry of Agriculture in 2015 is to gradually adjust staple food structure, which provides an opportunity to meet with the challenge. Apart from staple food structure, difference on energy, material input, geography, and crop management are essential to determine agriculture's contribution to climate change. In this study, we conduct a life cycle analysis of four staple foods in China, namely rice, wheat, maize, and potato, to develop crop-specific estimates of GHG emissions and GHG intensity by using `Production intensity' (carbon dioxide equivalent emissions per kilocalorie produced), to help us understand potential synergies and frictions between food producing and climate mitigation. Data used in this study is on city / province levels if city level is unavailable in 2015. First, we evaluate GHG reductions due to transition of staple food structure in China. Staple food GHG emissions in China are 546.90 Tg CO2e yr-1 in 2015, with 47.6%, 21.9%, 27.3% and 3.2% from rice, wheat, maize and potato. Mean production intensity of staple food is 0.45 Mg CO2e M kcal-1 in 2015. Maize leads the intensity with 0.77 Mg CO2e M kcal-1, followed by rice (0.49 Mg CO2e M kcal-1), wheat (0.28 Mg CO2e M kcal-1) and potato (0.24 Mg CO2e M kcal-1). After staple food structure adjustment, 25 Tg CO2e yr-1 (4.2%) reduction will be accomplished in 2020 without any crop management improvement. Further reduction (33.3% - 40.4%) could be achieved with crop management improvement. In addition, because of staple food structure switching, native rice production will decline, which might lead to more export from countries with higher production intensity. Estimated emission leakage from rice import is 30.10 Tg CO2e yr-1, exceeds emission reduction in native China. Therefore, potato staple food strategy could meet the demand for food in China, but it increases risk of global climate change.
Manolis, Evangelos N; Tsakris, Athanassios; Kaklamanos, Ioannis; Markogiannakis, Antonios; Siomos, Konstadinos
2006-03-01
Although beam-scanning carbon dioxide (CO2) lasers have provided a highly efficient tool for esthetic skin rejuvenation there has been no comprehensive animal studies looking into microbial skin changes following CO2 laser skin resurfacing. To evaluate the in vivo effects of CO2 laser skin resurfacing in an experimental rat model in comparison with mechanical abrasion on the skin microbial flora. Four separate cutaneous sections of the right dorsal surface of 10 Wistar rats were treated with a CO2 laser, operating at 18 W and delivering a radiant energy of 5.76 J/cm2, while mechanical abrasions of the skin were created on four sections of the left dorsal surface using a scalpel. Samples for culture and biopsies were obtained from the skin surfaces of the rats on day 1 of application of the CO2 laser or mechanical abrasion, as well as 10, 30, and 90 days after the procedure. The presence of four microorganisms (staphylococci, streptococci, diphtheroids, and yeasts) was evaluated as a microbe index for the skin flora, and colony counts were obtained using standard microbiological methods. Skin biopsy specimens, following CO2 laser treatment, initially showed epidermal and papillary dermal necrosis and later a re-epithelization of the epidermis as well as the generation of new collagen on the upper papillary dermis. The reduction in microbial counts on day 1 of the CO2 laser-inflicted wound was statistically significant for staphylococci and diphtheroids compared with the baseline counts (p=.004 and p<.001, respectively), and for staphylococci, diphtheroids, and yeasts compared with the scalpel-inflicted wound on the same day (p=0.029, p<.001, and p=.030, respectively). Skin resurfacing using CO2 lasers considerably reduces microbial counts of most microorganisms in comparison with either normal skin flora or a scalpel-inflicted wound. This might contribute to the positive clinical outcome of laser skin resurfacing.
Spray process for the recovery of CO.sub.2 from a gas stream and a related apparatus
Soloveichik, Grigorii Lev; Perry, Robert James; Wood, Benjamin Rue; Genovese, Sarah Elizabeth
2014-02-11
A method for recovering carbon dioxide (CO.sub.2) from a gas stream is disclosed. The method includes the step of reacting CO.sub.2 in the gas stream with fine droplets of a liquid absorbent, so as to form a solid material in which the CO.sub.2 is bound. The solid material is then transported to a desorption site, where it is heated, to release substantially pure CO.sub.2 gas. The CO.sub.2 gas can then be collected and used or transported in any desired way. A related apparatus for recovering carbon dioxide (CO.sub.2) from a gas stream is also described herein.
Carbon dioxide (CO2) sequestration in deep saline aquifers and formations: Chapter 3
Rosenbauer, Robert J.; Thomas, Burt
2010-01-01
Carbon dioxide (CO2) capture and sequestration in geologic media is one among many emerging strategies to reduce atmospheric emissions of anthropogenic CO2. This chapter looks at the potential of deep saline aquifers – based on their capacity and close proximity to large point sources of CO2 – as repositories for the geologic sequestration of CO2. The petrochemical characteristics which impact on the suitability of saline aquifers for CO2 sequestration and the role of coupled geochemical transport models and numerical tools in evaluating site feasibility are also examined. The full-scale commercial CO2 sequestration project at Sleipner is described together with ongoing pilot and demonstration projects.
Chemical approaches to carbon dioxide utilization for manned Mars missions
NASA Technical Reports Server (NTRS)
Hepp, Aloysius F.; Landis, Geoffrey A.; Kubiak, Clifford P.
1991-01-01
Use of resources available in situ is a critical enabling technology for a permanent human presence in space. A permanent presence on Mars, e.g., requires a large infrastructure to sustain life under hostile conditions. As a resource on Mars, atmospheric CO2 is as follows: abundant; available at all points on the surface; of known presence; chemically simple; and can be obtained by simple compression. Many studies focus on obtaining O2 and the various uses for O2 including life support and fuel; discussion of CO, the coproduct from CO2 fixation revolves around its uses as a fuel, being oxidized back to CO2. Several new proposals are studied for CO2 fixation through chemical, photochemical, and photoelectrochemical means. For example, the reduction of CO2 to hydrocarbons such as acetylene (C2H2) can be accomplished with H2. C2H2 has a theoretical vacuum specific impulse of approx. 375 secs. Potential uses were also studied of CO2, as obtained or further reduced to carbon, as a reducing agent in metal oxide processing to form metals or metal carbides for use as structural or power materials; the CO2 can be recycled to generate O2 and CO.
Wu, Jingjie; Ma, Sichao; Sun, Jing; Gold, Jake I.; Tiwary, ChandraSekhar; Kim, Byoungsu; Zhu, Lingyang; Chopra, Nitin; Odeh, Ihab N.; Vajtai, Robert; Yu, Aaron Z.; Luo, Raymond; Lou, Jun; Ding, Guqiao; Kenis, Paul J. A.; Ajayan, Pulickel M.
2016-01-01
Electroreduction of carbon dioxide into higher-energy liquid fuels and chemicals is a promising but challenging renewable energy conversion technology. Among the electrocatalysts screened so far for carbon dioxide reduction, which includes metals, alloys, organometallics, layered materials and carbon nanostructures, only copper exhibits selectivity towards formation of hydrocarbons and multi-carbon oxygenates at fairly high efficiencies, whereas most others favour production of carbon monoxide or formate. Here we report that nanometre-size N-doped graphene quantum dots (NGQDs) catalyse the electrochemical reduction of carbon dioxide into multi-carbon hydrocarbons and oxygenates at high Faradaic efficiencies, high current densities and low overpotentials. The NGQDs show a high total Faradaic efficiency of carbon dioxide reduction of up to 90%, with selectivity for ethylene and ethanol conversions reaching 45%. The C2 and C3 product distribution and production rate for NGQD-catalysed carbon dioxide reduction is comparable to those obtained with copper nanoparticle-based electrocatalysts. PMID:27958290
NASA Astrophysics Data System (ADS)
Dong, Feng; Heinbuch, Scott; Bernstein, Elliot; Rocca, Jorge
2006-05-01
A desk-top soft x-ray laser is applied to the study of water, methanol, ammonia, sulfur dioxide, carbon dioxide, mixed sulfur dioxide-water, and mixed carbon dioxide-water clusters through single photon ionization time of flight mass spectroscopy. Almost all of the energy above the vertical ionization energy is removed by the ejected electron. Protonated water, methanol, and ammonia clusters dominate the mass spectra for the first three systems. The temperatures of the neutral water and methanol clusters can be estimated. In the case of pure SO2 and CO2, the mass spectra are dominated by (SO2)n^+ and (CO2)n^+ cluster series. When a high or low concentration of SO2/CO2 is mixed with water, we observe (SO2/CO2)nH2O^+ or SO2/CO2(H2O)nH^+ in the mass spectra, respectively. The unimolecular dissociation rate constants for reactions involving loss of one neutral molecule are calculated for the protonated water, methanol, and ammonia clusters as well as for SO2 and CO2 clusters. We find that the 26.5 eV soft x-ray laser is a nearly ideal tool for the study of hydrogen bonded and van der Waals cluster systems and we are currently exploring its usefulness for other more strongly bound systems.
Liu, Qiang; Wu, Lipeng; Fleischer, Ivana; Selent, Detlef; Franke, Robert; Jackstell, Ralf; Beller, Matthias
2014-06-02
An efficient domino ruthenium-catalyzed reverse water-gas-shift (RWGS)-hydroformylation-reduction reaction of olefins to alcohols is reported. Key to success is the use of specific bulky phosphite ligands and triruthenium dodecacarbonyl as the catalyst. Compared to the known ruthenium/chloride system, the new catalyst allows for a more efficient hydrohydroxymethylation of terminal and internal olefins with carbon dioxide at lower temperature. Unwanted hydrogenation of the substrate is prevented. Preliminary mechanism investigations uncovered the homogeneous nature of the active catalyst and the influence of the ligand and additive in individual steps of the reaction sequence. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Rain events decrease boreal peatland net CO2 uptake through reduced light availability.
Nijp, Jelmer J; Limpens, Juul; Metselaar, Klaas; Peichl, Matthias; Nilsson, Mats B; van der Zee, Sjoerd E A T M; Berendse, Frank
2015-06-01
Boreal peatlands store large amounts of carbon, reflecting their important role in the global carbon cycle. The short-term exchange and the long-term storage of atmospheric carbon dioxide (CO2 ) in these ecosystems are closely associated with the permanently wet surface conditions and are susceptible to drought. Especially, the single most important peat forming plant genus, Sphagnum, depends heavily on surface wetness for its primary production. Changes in rainfall patterns are expected to affect surface wetness, but how this transient rewetting affects net ecosystem exchange of CO2 (NEE) remains unknown. This study explores how the timing and characteristics of rain events during photosynthetic active periods, that is daytime, affect peatland NEE and whether rain event associated changes in environmental conditions modify this response (e.g. water table, radiation, vapour pressure deficit, temperature). We analysed an 11-year time series of half-hourly eddy covariance and meteorological measurements from Degerö Stormyr, a boreal peatland in northern Sweden. Our results show that daytime rain events systematically decreased the sink strength of peatlands for atmospheric CO2 . The decrease was best explained by rain associated reduction in light, rather than by rain characteristics or drought length. An average daytime growing season rain event reduced net ecosystem CO2 uptake by 0.23-0.54 gC m(-2) . On an annual basis, this reduction of net CO2 uptake corresponds to 24% of the annual net CO2 uptake (NEE) of the study site, equivalent to a 4.4% reduction of gross primary production (GPP) during the growing season. We conclude that reduced light availability associated with rain events is more important in explaining the NEE response to rain events than rain characteristics and changes in water availability. This suggests that peatland CO2 uptake is highly sensitive to changes in cloud cover formation and to altered rainfall regimes, a process hitherto largely ignored. © 2015 John Wiley & Sons Ltd.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Paul Imhoff; Ramin Yazdani; Don Augenstein
Methane is an important contributor to global warming with a total climate forcing estimated to be close to 20% that of carbon dioxide (CO2) over the past two decades. The largest anthropogenic source of methane in the US is 'conventional' landfills, which account for over 30% of anthropogenic emissions. While controlling greenhouse gas emissions must necessarily focus on large CO2 sources, attention to reducing CH4 emissions from landfills can result in significant reductions in greenhouse gas emissions at low cost. For example, the use of 'controlled' or bioreactor landfilling has been estimated to reduce annual US greenhouse emissions by aboutmore » 15-30 million tons of CO2 carbon (equivalent) at costs between $3-13/ton carbon. In this project we developed or advanced new management approaches, landfill designs, and landfill operating procedures for bioreactor landfills. These advances are needed to address lingering concerns about bioreactor landfills (e.g., efficient collection of increased CH4 generation) in the waste management industry, concerns that hamper bioreactor implementation and the consequent reductions in CH4 emissions. Collectively, the advances described in this report should result in better control of bioreactor landfills and reductions in CH4 emissions. Several advances are important components of an Intelligent Bioreactor Management Information System (IBM-IS).« less
NASA Astrophysics Data System (ADS)
Schmidt, A.; Rella, C.; Goeckede, M.; Hanson, C. V.; Yang, Z.; Law, B. E.
2014-12-01
In recent years, measurements of atmospheric carbon dioxide with high precision and accuracy have become increasingly important for climate change research, in particular to inform terrestrial biosphere models. Anthropogenic carbon dioxide emissions from fossil fuel burning have long been recognized to contribute a significant portion of the carbon dioxide in the atmosphere. Here, we present an approach to remove the traffic related carbon dioxide emissions from mole fractions measured at a tall tower by using the corresponding carbon monoxide measurements in combination with footprint analyses and transport modeling. This technique improves the suitability of the CO2 data to be used in inverse modeling approaches of atmosphere-biosphere exchange that do not account for non-biotic portions of CO2. In our study region in Oregon, road traffic emissions are the biggest source of anthropogenic carbon dioxide and carbon monoxide. A three-day mobile campaign covering 1700 km of roads in northwestern Oregon was performed during summer of 2012 using a laser-based Cavity Ring Down Spectrometer. The mobile measurements incorporated different roads including main highways, urban streets, and back-roads, largely within the typical footprint of a tall CO2 observation tower in Oregon's Willamette Valley. For the first time, traffic related CO:CO2 emission ratios were measured directly at the sources during an on-road campaign under a variety of different driving conditions. An average emission ratio of 7.43 (±1.80) ppb CO per ppm CO2 was obtained for the study region and applied to separate the traffic related portion of CO2 from the mole fraction time series. The road traffic related portion of the CO2 mole fractions measured at the tower site reached maximum values from 9.8 to 12 ppm, depending on the height above the surface, during summer 2012.
Lucas, Rebekah A I; Pearson, James; Schlader, Zachary J; Crandall, Craig G
2015-11-01
What is the central question of this study? Does baroreceptor unloading during passive hyperthermia contribute to increases in ventilation and decreases in end-tidal carbon dioxide during that exposure? What is the main finding and its importance? Hyperthermic hyperventilation is not mitigated by expanding central blood volume and reloading the cardiopulmonary baroreceptors via rapid saline infusion or by reloading the arterial baroreceptors via phenylephrine administration. The absence of a reduction in ventilation upon reloading the baroreceptors to pre-hyperthermic levels indicates that cardiopulmonary and arterial baroreceptor unloading with hyperthermia is unlikely to contribute to hyperthermic hyperventilation in humans. This study tested the hypothesis that baroreceptor unloading during passive hyperthermia contributes to increases in ventilation and decreases in end-tidal partial pressure of carbon dioxide (P ET ,CO2) during that exposure. Two protocols were performed, in which healthy subjects underwent passive hyperthermia (increasing intestinal temperature by ∼1.8°C) to cause a sustained increase in ventilation and reduction in P ET ,CO2. Upon attaining hyperthermic hyperventilation, in protocol 1 (n = 10; three females) a bolus (19 ± 2 ml kg(-1) ) of warm (∼38°C) isotonic saline was rapidly (5-10 min) infused intravenously to restore reductions in central venous pressure, whereas in protocol 2 (n = 11; five females) phenylephrine was infused intravenously (60-120 μg min(-1) ) to return mean arterial pressure to normothermic levels. In protocol 1, hyperthermia increased ventilation (by 2.2 ± 1.7 l min(-1) , P < 0.01), while reducing P ET ,CO2 (by 4 ± 3 mmHg, P = 0.04) and central venous pressure (by 5 ± 1 mmHg, P <0.01). Saline infusion increased central venous pressure by 5 ± 1 mmHg (P < 0.01), restoring it to normothermic values, but did not change ventilation or P ET ,CO2 (P > 0.05). In protocol 2, hyperthermia increased ventilation (by 5.0 ± 2.7 l min(-1) , P <0.01) and reduced P ET ,CO2 (by 5 ± 2 mmHg, P < 0.01) and mean arterial pressure (by 9 ± 7 mmHg, P <0.01). Phenylephrine infusion increased mean arterial pressure by 12 ± 3 mmHg (P < 0.01), restoring it to normothermic values, but did not change ventilation or P ET ,CO2 (P > 0.05). The absence of a reduction in ventilation upon reloading the cardiopulmonary and arterial baroreceptors to pre-hyperthermic levels indicates that baroreceptor unloading with hyperthermia is unlikely to contribute to hyperthermic hyperventilation in humans. © 2015 The Authors. Experimental Physiology © 2015 The Physiological Society.
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
NASA Astrophysics Data System (ADS)
Semprini, L.; Azizian, M.
2012-12-01
The demonstration of transformation of chlorinated aliphatic compounds (CAHs) in the subsurface is a challenge, especially when the products are carbon dioxide (CO2) and chloride ion. The groundwater contaminant carbon tetrachloride (CT) is of particular interest since a broad range of transformation products can be potentially formed under anaerobic conditions. The ability to demonstrate the transformation of CT to CO2 as a non toxic endproduct, is also of great interest. Results will be presented from a continuous flow column study where 13C labeled CT was used to demonstrate its transformation to CO2. The column was packed with a quartz sand and bioaugmented the Evanite Culture (EV) that is capable of transforming tetrachloroethene (PCE) to ethene. The column was continously fed a synthetic groundwater that was amended with PCE (0.10 mM) and either formate (1.5 mM) or lactate (1.1 mM), which ferments to produce hydrogen (H2) as the ultimate electron donor. Earlier CT transformation studies with the column, in the absence of sulfate reduction, and with formate added as a donor found CT (0.015 mM) was over 98% transformed with about 20% converted to chloroform (CF) (0.003 mM) and with a transient detection of chloromethane (CM). Methane and carbon disulfide, as potential products, were not detected. Neither CT nor CF inhibited the reductive dehalogenation of PCE to ethene. A series of transient studies conducted after these initial CT transformation tests, but in the absence of CT, showed formate remained an effective substrate for maintaining sulfate reduction and PCE transformation. Lactate, which was effectively fermented prior to CT addition, was not effectively fermented, with propionate accumulating as a fermentation product. When lactate was added, PCE was mainly transformed to cis-dichloroethene (cis-DCE) and VC, and sulfate reduction did not occur. In order to restore effective lactate fermentation the column was then bioaugmented with an EV culture that was capable of lactate fermentation. After bioaugmentation, effective lactate fermentation, sulfate reduction and PCE transformation to ethene was achieved. Unlabeled CT (0.015 mM) addition was then started and complete transformation was achieved with a transient build-up of CF and chloromethane, which were subsequently removed below their detection limits. CT continued to be completely transformed after the influent concentration was increased to 0.03 mM. 13C labeled CT (0.03 mM) was then added to the column. GC-MS analysis showed that 13C labeled CO2 was formed at near stoichiometric levels to the CT that was transformed. The results clearly demonstrate that CT can being transformed to CO2 at high CT concentrations, while maintaining effective PCE dehalogenation, sulfate reduction and lactate fermentation. The results also illustrate the great potential of using 13C labeled compounds in subsurface investigations.
Warwick, Peter D.; Verma, Mahendra K.; Attanasi, Emil; Olea, Ricardo A.; Blondes, Madalyn S.; Freeman, Philip; Brennan, Sean T.; Merrill, Matthew; Jahediesfanjani, Hossein; Roueche, Jacqueline; Lohr, Celeste D.
2017-01-01
The U.S. Geological Survey (USGS) has developed an assessment methodology for estimating the potential incremental technically recoverable oil resources resulting from carbon dioxide-enhanced oil recovery (CO2-EOR) in reservoirs with appropriate depth, pressure, and oil composition. The methodology also includes a procedure for estimating the CO2 that remains in the reservoir after the CO2-EOR process is complete. The methodology relies on a reservoir-level database that incorporates commercially available geologic and engineering data. The mathematical calculations of this assessment methodology were tested and produced realistic results for the Permian Basin Horseshoe Atoll, Upper Pennsylvanian-Wolfcampian Play (Texas, USA). The USGS plans to use the new methodology to conduct an assessment of technically recoverable hydrocarbons and associated CO2 sequestration resulting from CO2-EOR in the United States.
Atmospheric CO2 capture by algae: Negative carbon dioxide emission path.
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.
NASA Technical Reports Server (NTRS)
Matty, Christopher M.; Cover, John M.
2009-01-01
The International Space Station (ISS) represents a largely closed-system habitable volume which requires active control of atmospheric constituents, including removal of exhaled Carbon Dioxide (CO2). The ISS provides a unique opportunity to observe system requirements for (CO2) removal. CO2 removal is managed by the Carbon Dioxide Removal Assembly (CDRA) aboard the US segment of ISS and by Lithium Hydroxide (LiOH) aboard the Space Shuttle (STS). While the ISS and STS are docked, various methods are used to balance the CO2 levels between the two vehicles, including mechanical air handling and management of general crew locations. Over the course of ISS operation, several unexpected anomalies have occurred which have required troubleshooting, including possible compromised performance of the CDRA and LiOH systems, and possible imbalance in CO2 levels between the ISS and STS while docked. This paper will cover efforts to troubleshoot the CO2 removal systems aboard the ISS and docked STS.
Early Implementation of Large Scale Carbon Dioxide Removal Projects through the Cement Industry
NASA Astrophysics Data System (ADS)
Zeman, F. S.
2014-12-01
The development of large-scale carbon dioxide reduction projects requires high purity CO2and a reactive cation source. A project seeking to provide both of these requirements will likely face cost barriers with current carbon prices. The cement industry is a suitable early implementation site for such projects by virtue of the properties of its exhaust gases and those of waste concrete. Cement plants are the second largest source of industrial CO2 emissions, globally. It is also the second largest commodity after water, has no ready substitute and is literally the foundation of society. Finally, half of the CO2 emissions originate from process reactions rather than fossil fuel combustion resulting in higher flue gas CO2concentrations. These properties, with the co-benefits of oxygen combustion, create a favorable environment for spatially suitable projects. Oxygen combustion involves substituting produced oxygen for air in a combustion reaction. The absence of gaseous N2 necessitates the recirculation of exhaust gases to maintain kiln temperatures, which increase the CO2 concentrations from 28% to 80% or more. Gas exit temperatures are also elevated (>300oC) and can reach higher temperatures if the multi stage pre-heater towers, that recover heat, are re-designed in light of FGR. A ready source of cations can be found in waste concrete, a by-product of construction and demolition activities. These wastes can be processed to remove cations and then reacted with atmospheric CO2 to produce carbonate minerals. While not carbon negative, they represent a demonstration opportunity for binding atmospheric CO2while producing a saleable product (precipitated calcium carbonate). This paper will present experimental results on PCC production from waste concrete along with modeling results for oxygen combustion at cement facilities. The results will be presented with a view to mineral sequestration process design and implementation.
Electrochemical reduction of carbon dioxide. Final report
DOE Office of Scientific and Technical Information (OSTI.GOV)
LaConti, A.B.; Molter, T.M.; Zagaja, J.A.
1986-05-01
Many researchers have studied the electrochemical reduction of carbon dioxide and related organic species to form concentrated liquid/gaseous products in laboratory-scale hardware. Hamilton Standard has developed a high pressure SPE electrolysis cell capable of reducing carbon dioxide streams to form pure, concentrated alcohols, carboxylic acids, and other hydrocarbons. The process is unique in that the byproducts of reaction include oxygen and, under some test conditions water. In addition, a relatively simple test system was designed and constructed permitting both batch and semibatch type electrochemical reduction studies. In this study, cathode materials were developed which 1) had a characteristic high hydrogenmore » overvoltage, and 2) possessed the intrinsic affinity for electrochemical reduction of the carbon dioxide species. In addition, suitable anode electrocatalyst materials were identified. Studies involving the electrochemical reduction of carbon dioxide required the ability to identify and quantify reaction products obtained during cell evaluation. Gas chromatographic techniques were developed along with the establishment of ion chromatographic methods permitting the analysis of organic reaction products. Hamilton Standard has evaluated electrochemical carbon dioxide reduction cells under a variety of test conditions.« less
Farhangi, Nasrin; Medina-Gonzalez, Yaocihuatl; Chowdhury, Rajib Roy; Charpentier, Paul A
2012-07-27
Tremendous interest exists towards synthesizing nanoassemblies for dye-sensitized solar cells (DSSCs) using earth-abundant and -friendly materials with green synthetic approaches. In this work, high surface area TiO(2) nanowire arrays were grown on the surface of functionalized graphene sheets (FGSs) containing -COOH functionalities acting as a template by using a sol-gel method in the green solvent, supercritical carbon dioxide (scCO(2)). The effect of scCO(2) pressure (1500, 3000 and 5000 psi), temperature (40, 60 and 80 °C), acetic acid/titanium isopropoxide monomer ratios (HAc/TIP = 2, 4 and 6), functionalized graphene sheets (FGSs)/TIP weight ratios (1:20, 1:40 and 1:60 w/w) and solvents (EtOH, hexane) were investigated. Increasing the HAc/TIPweight ratio from 4 to 6 in scCO(2) resulted in increasing the TiO(2) nanowire diameter from 10 to 40 nm. Raman and high resolution XPS showed the interaction of TiO(2) with the -COOH groups on the surface of the graphene sheets, indicating that graphene acted as a template for polycondensation growth. UV-vis diffuse reflectance and photoluminescence spectroscopy showed a reduction in titania's bandgap and also a significant reduction in electron-hole recombination compared to bare TiO(2) nanowires. Photocurrent measurements showed that the TiO(2)nanowire/graphene composites prepared in scCO(2) gave a 5× enhancement in photoefficiency compared to bare TiO(2) nanowires.
NASA Astrophysics Data System (ADS)
Farhangi, Nasrin; Medina-Gonzalez, Yaocihuatl; Chowdhury, Rajib Roy; Charpentier, Paul A.
2012-07-01
Tremendous interest exists towards synthesizing nanoassemblies for dye-sensitized solar cells (DSSCs) using earth-abundant and -friendly materials with green synthetic approaches. In this work, high surface area TiO2 nanowire arrays were grown on the surface of functionalized graphene sheets (FGSs) containing -COOH functionalities acting as a template by using a sol-gel method in the green solvent, supercritical carbon dioxide (scCO2). The effect of scCO2 pressure (1500, 3000 and 5000 psi), temperature (40, 60 and 80 °C), acetic acid/titanium isopropoxide monomer ratios (HAc/TIP = 2, 4 and 6), functionalized graphene sheets (FGSs)/TIP weight ratios (1:20, 1:40 and 1:60 w/w) and solvents (EtOH, hexane) were investigated. Increasing the HAc/TIPweight ratio from 4 to 6 in scCO2 resulted in increasing the TiO2 nanowire diameter from 10 to 40 nm. Raman and high resolution XPS showed the interaction of TiO2 with the -COOH groups on the surface of the graphene sheets, indicating that graphene acted as a template for polycondensation growth. UV-vis diffuse reflectance and photoluminescence spectroscopy showed a reduction in titania’s bandgap and also a significant reduction in electron-hole recombination compared to bare TiO2 nanowires. Photocurrent measurements showed that the TiO2nanowire/graphene composites prepared in scCO2 gave a 5× enhancement in photoefficiency compared to bare TiO2 nanowires.
Yin, Ge; Sako, Hiroshi; Gubbala, Ramesh V; Ueda, Shigenori; Yamaguchi, Akira; Abe, Hideki; Miyauchi, Masahiro
2018-04-17
Selective carbon dioxide photoreduction to produce formic acid was achieved under visible light irradiation using water molecules as electron donors, similar to natural plants, based on the construction of a Z-scheme light harvesting system modified with a Cu-Zn alloy nanoparticle co-catalyst. The faradaic efficiency of our Z-scheme system for HCOOH generation was over 50% under visible light irradiation.
NASA Technical Reports Server (NTRS)
White, James H. (Inventor); Taylor, Jesse W. (Inventor)
2008-01-01
Catalyst compositions and methods for F-T synthesis which exhibit high CO conversion with minor levels (preferably less than 35% and more preferably less than 5%) or no measurable carbon dioxide generation. F-T active catalysts are prepared by reduction of certain oxygen deficient mixed metal oxides.
A memory structure adapted simulated annealing algorithm for a green vehicle routing problem.
Küçükoğlu, İlker; Ene, Seval; Aksoy, Aslı; Öztürk, Nursel
2015-03-01
Currently, reduction of carbon dioxide (CO2) emissions and fuel consumption has become a critical environmental problem and has attracted the attention of both academia and the industrial sector. Government regulations and customer demands are making environmental responsibility an increasingly important factor in overall supply chain operations. Within these operations, transportation has the most hazardous effects on the environment, i.e., CO2 emissions, fuel consumption, noise and toxic effects on the ecosystem. This study aims to construct vehicle routes with time windows that minimize the total fuel consumption and CO2 emissions. The green vehicle routing problem with time windows (G-VRPTW) is formulated using a mixed integer linear programming model. A memory structure adapted simulated annealing (MSA-SA) meta-heuristic algorithm is constructed due to the high complexity of the proposed problem and long solution times for practical applications. The proposed models are integrated with a fuel consumption and CO2 emissions calculation algorithm that considers the vehicle technical specifications, vehicle load, and transportation distance in a green supply chain environment. The proposed models are validated using well-known instances with different numbers of customers. The computational results indicate that the MSA-SA heuristic is capable of obtaining good G-VRPTW solutions within a reasonable amount of time by providing reductions in fuel consumption and CO2 emissions.
Rehder, G.; Kirby, S.H.; Durham, W.B.; Stern, L.A.; Peltzer, E.T.; Pinkston, J.; Brewer, P.G.
2004-01-01
To help constrain models involving the chemical stability and lifetime of gas clathrate hydrates exposed at the seafloor, dissolution rates of pure methane and carbon-dioxide hydrates were measured directly on the seafloor within the nominal pressure-temperature (P/T) range of the gas hydrate stability zone. Other natural boundary conditions included variable flow velocity and undersaturation of seawater with respect to the hydrate-forming species. Four cylindrical test specimens of pure, polycrystalline CH4 and CO2 hydrate were grown and fully compacted in the laboratory, then transferred by pressure vessel to the seafloor (1028 m depth), exposed to the deep ocean environment, and monitored for 27 hours using time-lapse and HDTV cameras. Video analysis showed diameter reductions at rates between 0.94 and 1.20 ??m/s and between 9.0 and 10.6 ?? 10-2 ??m/s for the CO2 and CH4 hydrates, respectively, corresponding to dissolution rates of 4.15 ?? 0.5 mmol CO2/m2s and 0.37 ?? 0.03 mmol CH4/m2s. The ratio of the dissolution rates fits a diffusive boundary layer model that incorporates relative gas solubilities appropriate to the field site, which implies that the kinetics of the dissolution of both hydrates is diffusion-controlled. The observed dissolution of several mm (CH4) or tens of mm (CO2) of hydrate from the sample surfaces per day has major implications for estimating the longevity of natural gas hydrate outcrops as well as for the possible roles of CO2 hydrates in marine carbon sequestration strategies. ?? 2003 Elsevier Ltd.
Monitoring gaseous exchange: implications for nursing care.
Martin, Susan; Wilson, Michael
2002-02-01
The purpose of this study is to examine whether a relationship exists between arterial and end-tidal carbon dioxide tension (PaCO2 and PETCO2 respectively) in patients admitted to intensive care units (ICUs), and what the implications it has for nursing care. PaCO2 and PETCO2 are indicators of ventilatory adequacy which is an important aspect of respiratory function. These measures of carbon dioxide tension are obtained via invasive and non-invasive monitoring tools. Measurement of PETCO2 has only recently been introduced into ICUs and its usefulness in these environments is open to debate. A population of 30 intubated patients had 214 simultaneous measurements of PaCO2 and PETCO2 taken over a period of 10 months. The findings indicate that, despite strong significant correlations, PETCO2 cannot be used safely as a substitute for PaCO2 as the arterial/end-tidal carbon dioxide gradient is not constant, nor does capnography provide a consistently reliable indicator of PaCO2.
Chambers, Matthew B; Wang, Xia; Elgrishi, Noémie; Hendon, Christopher H; Walsh, Aron; Bonnefoy, Jonathan; Canivet, Jérôme; Quadrelli, Elsje Alessandra; Farrusseng, David; Mellot-Draznieks, Caroline; Fontecave, Marc
2015-02-01
The first photosensitization of a rhodium-based catalytic system for CO2 reduction is reported, with formate as the sole carbon-containing product. Formate has wide industrial applications and is seen as valuable within fuel cell technologies as well as an interesting H2 -storage compound. Heterogenization of molecular rhodium catalysts is accomplished via the synthesis, post-synthetic linker exchange, and characterization of a new metal-organic framework (MOF) Cp*Rh@UiO-67. While the catalytic activities of the homogeneous and heterogeneous systems are found to be comparable, the MOF-based system is more stable and selective. Furthermore it can be recycled without loss of activity. For formate production, an optimal catalyst loading of ∼10 % molar Rh incorporation is determined. Increased incorporation of rhodium catalyst favors thermal decomposition of formate into H2 . There is no precedent for a MOF catalyzing the latter reaction so far. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Compatibility of Medical-Grade Polymers with Dense CO2
Jiménez, A; Thompson, G L; Matthews, M A; Davis, T A; Crocker, K; Lyons, J S; Trapotsis, A
2009-01-01
This study reports the effect of exposure to liquid carbon dioxide on the mechanical properties of selected medical polymers. The tensile strengths and moduli of fourteen polymers are reported. Materials were exposed to liquid CO2, or CO2 + trace amounts of aqueous H2O2, at 6.5 MPa and ambient temperature. Carbon dioxide uptake, swelling, and distortion were observed for the more amorphous polymers while polymers with higher crystallinity showed little effect from CO2 exposure. Changes in tensile strength were not statistically significant for most plastics, and most indicated good tolerance to liquid CO2. These results are relevant to evaluating the potential of liquid CO2-based sterilization technology. PMID:19756235
Müller, Marius N; Trull, Thomas W; Hallegraeff, Gustaaf M
2017-08-01
Future oceanic conditions induced by anthropogenic greenhouse gas emissions include warming, acidification and reduced nutrient supply due to increased stratification. Some parts of the Southern Ocean are expected to show rapid changes, especially for carbonate mineral saturation. Here we compare the physiological response of the model coccolithophore Emiliania huxleyi (strain EHSO 5.14, originating from 50 o S, 149 o E) with pH/CO 2 gradients (mimicking ocean acidification ranging from 1 to 4 × current pCO 2 levels) under nutrient-limited (nitrogen and phosphorus) and -replete conditions. Both nutrient limitations decreased per cell photosynthesis (particulate organic carbon (POC) production) and calcification (particulate inorganic carbon (PIC) production) rates for all pCO 2 levels, with more than 50% reductions under nitrogen limitation. These impacts, however, became indistinguishable from nutrient-replete conditions when normalized to cell volume. Calcification decreased three-fold and linearly with increasing pCO 2 under all nutrient conditions, and was accompanied by a smaller ~30% nonlinear reduction in POC production, manifested mainly above 3 × current pCO 2 . Our results suggest that normalization to cell volume allows the major impacts of nutrient limitation (changed cell sizes and reduced PIC and POC production rates) to be treated independently of the major impacts of increasing pCO 2 and, additionally, stresses the importance of including cell volume measurements to the toolbox of standard physiological analysis of coccolithophores in field and laboratory studies.
Müller, Marius N; Trull, Thomas W; Hallegraeff, Gustaaf M
2017-01-01
Future oceanic conditions induced by anthropogenic greenhouse gas emissions include warming, acidification and reduced nutrient supply due to increased stratification. Some parts of the Southern Ocean are expected to show rapid changes, especially for carbonate mineral saturation. Here we compare the physiological response of the model coccolithophore Emiliania huxleyi (strain EHSO 5.14, originating from 50oS, 149oE) with pH/CO2 gradients (mimicking ocean acidification ranging from 1 to 4 × current pCO2 levels) under nutrient-limited (nitrogen and phosphorus) and -replete conditions. Both nutrient limitations decreased per cell photosynthesis (particulate organic carbon (POC) production) and calcification (particulate inorganic carbon (PIC) production) rates for all pCO2 levels, with more than 50% reductions under nitrogen limitation. These impacts, however, became indistinguishable from nutrient-replete conditions when normalized to cell volume. Calcification decreased three-fold and linearly with increasing pCO2 under all nutrient conditions, and was accompanied by a smaller ~30% nonlinear reduction in POC production, manifested mainly above 3 × current pCO2. Our results suggest that normalization to cell volume allows the major impacts of nutrient limitation (changed cell sizes and reduced PIC and POC production rates) to be treated independently of the major impacts of increasing pCO2 and, additionally, stresses the importance of including cell volume measurements to the toolbox of standard physiological analysis of coccolithophores in field and laboratory studies. PMID:28430186
Stratospheric ozone depletion due to nitrous oxide: influences of other gases
Portmann, R. W.; Daniel, J. S.; Ravishankara, A. R.
2012-01-01
The effects of anthropogenic emissions of nitrous oxide (N2O), carbon dioxide (CO2), methane (CH4) and the halocarbons on stratospheric ozone (O3) over the twentieth and twenty-first centuries are isolated using a chemical model of the stratosphere. The future evolution of ozone will depend on each of these gases, with N2O and CO2 probably playing the dominant roles as halocarbons return towards pre-industrial levels. There are nonlinear interactions between these gases that preclude unambiguously separating their effect on ozone. For example, the CH4 increase during the twentieth century reduced the ozone losses owing to halocarbon increases, and the N2O chemical destruction of O3 is buffered by CO2 thermal effects in the middle stratosphere (by approx. 20% for the IPCC A1B/WMO A1 scenario over the time period 1900–2100). Nonetheless, N2O is expected to continue to be the largest anthropogenic emission of an O3-destroying compound in the foreseeable future. Reductions in anthropogenic N2O emissions provide a larger opportunity for reduction in future O3 depletion than any of the remaining uncontrolled halocarbon emissions. It is also shown that 1980 levels of O3 were affected by halocarbons, N2O, CO2 and CH4, and thus may not be a good choice of a benchmark of O3 recovery. PMID:22451111
Oh, Heung-Il; Ye, Sang-Ho; Johnson, Carl A.; Woolley, Joshua R.; Federspiel, William J.; Wagner, William R.
2011-01-01
Hollow fiber membrane (HFM)-based artificial lungs can require a large blood-contacting membrane surface area to provide adequate gas exchange. However, such a large surface area presents significant challenges to hemocompatibility. One method to improve carbon dioxide (CO2) transfer efficiency might be to immobilize carbonic anhydrase (CA) onto the surface of conventional HFMs. By catalyzing the dehydration of bicarbonate in blood, CA has been shown to facilitate diffusion of CO2 toward the fiber membranes. This study evaluated the impact of surface modifying a commercially available microporous HFM-based artificial lung on fiber blood biocompatibility. A commercial poly(propylene) Celgard HFM surface was coated with a siloxane, grafted with amine groups, and then attached with CA which has been shown to facilitate diffusion of CO2 toward the fiber membranes. Results following acute ovine blood contact indicated no significant reduction in platelet deposition or activation with the siloxane coating or the siloxane coating with grafted amines relative to base HFMs. However,HFMs with attached CA showed a significant reduction in both platelet deposition and activation compared with all other fiber types. These findings, along with the improved CO2 transfer observed in CA modified fibers, suggest that its incorporation into HFM design may potentiate the design of a smaller, more biocompatible HFM-based artificial lung. PMID:20633159
USDA Agriculture and Forestry Greenhouse Gas Inventory: 1990-2013
USDA-ARS?s Scientific Manuscript database
Carbon dioxide (CO2), methane (CH4), and nitrous oxide (N2O) concentrations in the atmosphere have increased by approximately 43%, 152%, and 20% respectively since about 1750. In 2013, total U.S. greenhouse gas emissions were 6,673 million metric tons of carbon dioxide equivalents (MMT CO2 eq.), ris...
Hierarchical Inorganic Assemblies for Artificial Photosynthesis
DOE Office of Scientific and Technical Information (OSTI.GOV)
Kim, Wooyul; Edri, Eran; Frei, Heinz
Artificial photosynthesis is an attractive approach for renewable fuel generation because it offers the prospect of a technology suitable for deployment on highly abundant, non-arable land. Recent leaps forward in the development of efficient and durable light absorbers and catalysts for oxygen evolution and the growing attention to catalysts for carbon dioxide activation brings into focus the tasks of hierarchically integrating the components into assemblies for closing of the photosynthetic cycle. A particular challenge is the efficient coupling of the multi-electron processes of CO 2 reduction and H 2O oxidation. Among the most important requirements for a complete integrated systemmore » are catalytic rates that match the solar flux, efficient charge transport between the various components, and scalability of the photosynthetic assembly on the unprecedented scale of terawatts in order to have impact on fuel consumption. To address these challenges, we have developed in this paper a heterogeneous inorganic materials approach with molecularly precise control of light absorption and charge transport pathways. Oxo-bridged heterobinuclear units with metal-to-metal charge-transfer transitions absorbing deep in the visible act as single photon, single charge transfer pumps for driving multi-electron catalysts. A photodeposition method has been introduced for the spatially directed assembly of nanoparticle catalysts for selective coupling to the donor or acceptor metal of the light absorber. For CO 2 reduction, a Cu oxide cluster is coupled to the Zr center of a ZrOCo light absorber, while coupling of an Ir nanoparticle catalyst for water oxidation to the Co donor affords closing of the photosynthetic cycle of CO 2 conversion by H 2O to CO and O 2. Optical, vibrational, and X-ray spectroscopy provide detailed structural knowledge of the polynuclear assemblies. Time resolved visible and rapid-scan FT-IR studies reveal charge transfer mechanisms and transient surface intermediates under photocatalytic conditions for guiding performance improvements. Separation of the water oxidation and carbon dioxide reduction half reactions by a membrane is essential for efficient photoreduction of CO 2 by H 2O to liquid fuel products. A concept of a macroscale artificial photosystem consisting of arrays of Co oxide–silica core–shell nanotubes is introduced in which each tube operates as a complete, independent photosynthetic unit with built-in membrane separation. The ultrathin amorphous silica shell with embedded molecular wires functions as a proton conducting, molecule impermeable membrane. Photoelectrochemical and transient optical measurements confirm tight control of charge transport through the membrane by the orbital energetics of the wire molecules. Finally, hierarchical arrangement of the components is accomplished by a combination of photodeposition, controlled anchoring, and atomic layer deposition methods.« less
CO2 Removal and Atmosphere Revitalization Systems for Next Generation Space Flight
NASA Technical Reports Server (NTRS)
Luna, Bernadette; Mulloth, Lila M.; Varghese, Mini M.; Hogan, John Andrew
2010-01-01
Removal of metabolic CO2 from breathing air is a vital process for life support in all crewed space missions. A CO2 removal processor called the Low Power CO2 Removal (LPCOR) system is being developed in the Bioengineering Branch at NASA Ames Research Center. LPCOR utilizes advanced adsorption and membrane gas separation processes to achieve substantial power and mass reduction when compared to the state-of-the-art carbon dioxide removal assembly (CORA) of the US segment of the International Space Station (ISS). LPCOR is an attractive alternative for use in commercial spacecraft for short-duration missions and can easily be adapted for closed-loop life support applications. NASA envisions a next-generation closed-loop atmosphere revitalization system that integrates advanced CO2 removal, O2 recovery, and trace contaminant control processes to improve overall system efficiency. LPCOR will serve as the front end to such a system. LPCOR is a reliable air revitalization technology that can serve both the near-term and long-term human space flight needs of NASA and its commercial partners.
Tang, Lin; Guo, Xuefeng; Yang, Yu; Zha, Zhenggen; Wang, Zhiyong
2014-06-11
A highly efficient and selective reaction for the synthesis of 2-substituted benzoxazoles and benzimidazoles catalyzed by Au/TiO2 has been developed via two hydrogen-transfer processes. This reaction has a good tolerance to air and water, a wide substrate scope, and represents a new avenue for practical C-N and C-O bond formation. More importantly, no additional additives, oxidants and reductants are required for the reaction and the catalyst can be recovered and reused readily.
Parati, Gianfranco; Agostoni, Piergiuseppe; Basnyat, Buddha; Bilo, Grzegorz; Brugger, Hermann; Coca, Antonio; Festi, Luigi; Giardini, Guido; Lironcurti, Alessandra; Luks, Andrew M; Maggiorini, Marco; Modesti, Pietro A; Swenson, Erik R; Williams, Bryan; Bärtsch, Peter; Torlasco, Camilla
2018-01-01
Abstract Take home figureAdapted from Bärtsch and Gibbs2 Physiological response to hypoxia. Life-sustaining oxygen delivery, in spite of a reduction in the partial pressure of inhaled oxygen between 25% and 60% (respectively at 2500 m and 8000 m), is ensured by an increase in pulmonary ventilation, an increase in cardiac output by increasing heart rate, changes in vascular tone, as well as an increase in haemoglobin concentration. BP, blood pressure; HR, heart rate; PaCO2, partial pressure of arterial carbon dioxide. PMID:29340578
Mobile source CO2 mitigation through smart growth development and vehicle fleet hybridization.
Stone, Brian; Mednick, Adam C; Holloway, Tracey; Spak, Scott N
2009-03-15
This paper presents the results of a study on the effectiveness of smart growth development patterns and vehicle fleet hybridization in reducing mobile source emissions of carbon dioxide (CO2) across 11 major metropolitan regions of the Midwestern U.S. over a 50-year period. Through the integration of a vehicle travel activity modeling framework developed by researchers atthe Oak Ridge National Laboratory with small area population projections, we model mobile source emissions of CO2 associated with alternative land development and technology change scenarios between 2000 and 2050. Our findings suggest that under an aggressive smart growth scenario, growth in emissions expected to occur under a business as usual scenario is reduced by 34%, while the full dissemination of hybrid-electric vehicles throughout the light vehicle fleet is found to offset the expected growth in emissions by 97%. Our results further suggest that high levels of urban densification could achieve reductions in 2050 CO2 emissions equivalent to those attainable through the full dissemination of hybrid-electric vehicle technologies.
Virus infection mediates the effects of elevated CO2 on plants and vectors.
Trębicki, Piotr; Vandegeer, Rebecca K; Bosque-Pérez, Nilsa A; Powell, Kevin S; Dader, Beatriz; Freeman, Angela J; Yen, Alan L; Fitzgerald, Glenn J; Luck, Jo E
2016-03-04
Atmospheric carbon dioxide (CO2) concentration has increased significantly and is projected to double by 2100. To increase current food production levels, understanding how pests and diseases respond to future climate driven by increasing CO2 is imperative. We investigated the effects of elevated CO2 (eCO2) on the interactions among wheat (cv. Yitpi), Barley yellow dwarf virus and an important pest and virus vector, the bird cherry-oat aphid (Rhopalosiphum padi), by examining aphid life history, feeding behavior and plant physiology and biochemistry. Our results showed for the first time that virus infection can mediate effects of eCO2 on plants and pathogen vectors. Changes in plant N concentration influenced aphid life history and behavior, and N concentration was affected by virus infection under eCO2. We observed a reduction in aphid population size and increased feeding damage on noninfected plants under eCO2 but no changes to population and feeding on virus-infected plants irrespective of CO2 treatment. We expect potentially lower future aphid populations on noninfected plants but no change or increased aphid populations on virus-infected plants therefore subsequent virus spread. Our findings underscore the complexity of interactions between plants, insects and viruses under future climate with implications for plant disease epidemiology and crop production.
Virus infection mediates the effects of elevated CO2 on plants and vectors
Trębicki, Piotr; Vandegeer, Rebecca K.; Bosque-Pérez, Nilsa A.; Powell, Kevin S.; Dader, Beatriz; Freeman, Angela J.; Yen, Alan L.; Fitzgerald, Glenn J.; Luck, Jo E.
2016-01-01
Atmospheric carbon dioxide (CO2) concentration has increased significantly and is projected to double by 2100. To increase current food production levels, understanding how pests and diseases respond to future climate driven by increasing CO2 is imperative. We investigated the effects of elevated CO2 (eCO2) on the interactions among wheat (cv. Yitpi), Barley yellow dwarf virus and an important pest and virus vector, the bird cherry-oat aphid (Rhopalosiphum padi), by examining aphid life history, feeding behavior and plant physiology and biochemistry. Our results showed for the first time that virus infection can mediate effects of eCO2 on plants and pathogen vectors. Changes in plant N concentration influenced aphid life history and behavior, and N concentration was affected by virus infection under eCO2. We observed a reduction in aphid population size and increased feeding damage on noninfected plants under eCO2 but no changes to population and feeding on virus-infected plants irrespective of CO2 treatment. We expect potentially lower future aphid populations on noninfected plants but no change or increased aphid populations on virus-infected plants therefore subsequent virus spread. Our findings underscore the complexity of interactions between plants, insects and viruses under future climate with implications for plant disease epidemiology and crop production. PMID:26941044
Virus infection mediates the effects of elevated CO2 on plants and vectors
NASA Astrophysics Data System (ADS)
Trębicki, Piotr; Vandegeer, Rebecca K.; Bosque-Pérez, Nilsa A.; Powell, Kevin S.; Dader, Beatriz; Freeman, Angela J.; Yen, Alan L.; Fitzgerald, Glenn J.; Luck, Jo E.
2016-03-01
Atmospheric carbon dioxide (CO2) concentration has increased significantly and is projected to double by 2100. To increase current food production levels, understanding how pests and diseases respond to future climate driven by increasing CO2 is imperative. We investigated the effects of elevated CO2 (eCO2) on the interactions among wheat (cv. Yitpi), Barley yellow dwarf virus and an important pest and virus vector, the bird cherry-oat aphid (Rhopalosiphum padi), by examining aphid life history, feeding behavior and plant physiology and biochemistry. Our results showed for the first time that virus infection can mediate effects of eCO2 on plants and pathogen vectors. Changes in plant N concentration influenced aphid life history and behavior, and N concentration was affected by virus infection under eCO2. We observed a reduction in aphid population size and increased feeding damage on noninfected plants under eCO2 but no changes to population and feeding on virus-infected plants irrespective of CO2 treatment. We expect potentially lower future aphid populations on noninfected plants but no change or increased aphid populations on virus-infected plants therefore subsequent virus spread. Our findings underscore the complexity of interactions between plants, insects and viruses under future climate with implications for plant disease epidemiology and crop production.
Annual soil CO_{2} production in Moscow Botanical Garden (Russia).
NASA Astrophysics Data System (ADS)
Udovenko, Maria; Goncharova, Olga; Matyshak, Georgy
2017-04-01
Soil respiration is an essential component of the carbon cycle, determining 25-40 % of carbon dioxide in the atmosphere. Urban soils are subject to significant anthropogenic influences. Anthropogenic impact affects both the plants and the soil microbiota. So, soil CO2 efflux and soil profile CO2 concentration probably differ in urban and natural soils. Influence of abiotic factors on soil carbon dioxide production is explored insufficiently. The research of their impact on soil carbon dioxide production is necessary to predict soil response to anthropogenic climate change. The aim of this study was estimation of annual soil CO2 production and the impact of climatic factors on it. The research took place in Moscow State University Botanical Garden Arboretum (southern taiga). Investigations were carried out at two sites: the areas planted with Picea obovata and Carpinus betulus. The study was conducted with 1-2 weeks intervals between November 2014 and December 2015. Emission measurement were carried out by closed chamber technique, profile concentration were measured by soil air sampling tubes method. Annual carbon dioxide soil surface efflux of soil planted with Picea obovata was 1370 gCO2/(m2 * year), soil planted with Carpinus betulus - 1590 gCO2/(m2 * year). Soil CO2 concentration increased with depth in average of 3300 to 12000 ppm (at 80 cm depth). Maximum concentration values are confined to the end of vegetation period (high biological activity) and to beginning of spring (spring ice cover of soil prevents CO2 emission). Soil CO2 efflux depends on soil temperature at 10 cm depth (R = 0.89; p <0.05), in a less degree it correlate with soil surface temperature and with soil temperature at 20 cm depth (r=0.88; p<0.05). Soil moisture has a little effect on CO2 efflux in the annual cycle (r=-0.16; p<0.05). However in vegetation period efflux of carbon dioxide largely depends on soil moisture, due to the fact, that soil moisture is limiting factor for soil microbiota activity and plant respiration.
Carbon dioxide: Global warning for nephrologists
Marano, Marco; D’Amato, Anna; Cantone, Alessandra
2016-01-01
The large prevalence of respiratory acid-base disorders overlapping metabolic acidosis in hemodialysis population should prompt nephrologists to deal with the partial pressure of carbon dioxide (pCO2) complying with the reduced bicarbonate concentration. What the most suitable formula to compute pCO2 is reviewed. Then, the neglected issue of CO2 content in the dialysis fluid is under the spotlight. In fact, a considerable amount of CO2 comes to patients’ bloodstream every hemodialysis treatment and “acidosis by dialysate” may occur if lungs do not properly clear away this burden of CO2. Moreover, vascular access recirculation may be easy diagnosed by detecting CO2 in the arterial line of extracorporeal circuit if CO2-enriched blood from the filter reenters arterial needle. PMID:27648406
Carbon dioxide: Global warning for nephrologists.
Marano, Marco; D'Amato, Anna; Cantone, Alessandra
2016-09-06
The large prevalence of respiratory acid-base disorders overlapping metabolic acidosis in hemodialysis population should prompt nephrologists to deal with the partial pressure of carbon dioxide (pCO2) complying with the reduced bicarbonate concentration. What the most suitable formula to compute pCO2 is reviewed. Then, the neglected issue of CO2 content in the dialysis fluid is under the spotlight. In fact, a considerable amount of CO2 comes to patients' bloodstream every hemodialysis treatment and "acidosis by dialysate" may occur if lungs do not properly clear away this burden of CO2. Moreover, vascular access recirculation may be easy diagnosed by detecting CO2 in the arterial line of extracorporeal circuit if CO2-enriched blood from the filter reenters arterial needle.
Liu, Shijiang; Sun, Jie; Chen, Xing; Yu, Yingying; Liu, Xuan; Liu, Cunming
2014-01-01
To investigate the correlation and accuracy of transcutaneous carbon dioxide partial pressure (PTCCO2) with regard to arterial carbon dioxide partial pressure (PaCO2) in severe obese patients undergoing laparoscopic bariatric surgery. Twenty-one patients with BMI>35 kg/m2 were enrolled in our study. Their PaCO2, end-tidal carbon dioxide partial pressure (PetCO2), as well as PTCCO2 values were measured at before pneumoperitoneum and 30 min, 60 min, 120 min after pneumoperitoneum respectively. Then the differences between each pair of values (PetCO2–PaCO2) and. (PTCCO2–PaCO2) were calculated. Bland–Altman method, correlation and regression analysis, as well as exact probability method and two way contingency table were employed for the data analysis. 21 adults (aged 19–54 yr, mean 29, SD 9 yr; weight 86–160 kg, mean119.3, SD 22.1 kg; BMI 35.3–51.1 kg/m2, mean 42.1,SD 5.4 kg/m2) were finally included in this study. One patient was eliminated due to the use of vaso-excitor material phenylephrine during anesthesia induction. Eighty-four sample sets were obtained. The average PaCO2–PTCCO2 difference was 0.9±1.3 mmHg (mean±SD). And the average PaCO2–PetCO2 difference was 10.3±2.3 mmHg (mean±SD). The linear regression equation of PaCO2–PetCO2 is PetCO2 = 11.58+0.57×PaCO2 (r2 = 0.64, P<0.01), whereas the one of PaCO2–PTCCO2 is PTCCO2 = 0.60+0.97×PaCO2 (r2 = 0.89). The LOA (limits of agreement) of 95% average PaCO2–PetCO2 difference is 10.3±4.6 mmHg (mean±1.96 SD), while the LOA of 95% average PaCO2–PTCCO2 difference is 0.9±2.6 mmHg (mean±1.96 SD). In conclusion, transcutaneous carbon dioxide monitoring provides a better estimate of PaCO2 than PetCO2 in severe obese patients undergoing laparoscopic bariatric surgery. PMID:24699267
Ca-Embedded C2N: an efficient adsorbent for CO2 capture.
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.
Reduction of fuel consumption and exhaust pollutant using intelligent transport systems.
Nasir, Mostofa Kamal; Md Noor, Rafidah; Kalam, M A; Masum, B M
2014-01-01
Greenhouse gas emitted by the transport sector around the world is a serious issue of concern. To minimize such emission the automobile engineers have been working relentlessly. Researchers have been trying hard to switch fossil fuel to alternative fuels and attempting to various driving strategies to make traffic flow smooth and to reduce traffic congestion and emission of greenhouse gas. Automobile emits a massive amount of pollutants such as Carbon Monoxide (CO), hydrocarbons (HC), carbon dioxide (CO2), particulate matter (PM), and oxides of nitrogen (NO x ). Intelligent transport system (ITS) technologies can be implemented to lower pollutant emissions and reduction of fuel consumption. This paper investigates the ITS techniques and technologies for the reduction of fuel consumption and minimization of the exhaust pollutant. It highlights the environmental impact of the ITS application to provide the state-of-art green solution. A case study also advocates that ITS technology reduces fuel consumption and exhaust pollutant in the urban environment.
Reduction of Fuel Consumption and Exhaust Pollutant Using Intelligent Transport Systems
Nasir, Mostofa Kamal; Md Noor, Rafidah; Kalam, M. A.; Masum, B. M.
2014-01-01
Greenhouse gas emitted by the transport sector around the world is a serious issue of concern. To minimize such emission the automobile engineers have been working relentlessly. Researchers have been trying hard to switch fossil fuel to alternative fuels and attempting to various driving strategies to make traffic flow smooth and to reduce traffic congestion and emission of greenhouse gas. Automobile emits a massive amount of pollutants such as Carbon Monoxide (CO), hydrocarbons (HC), carbon dioxide (CO2), particulate matter (PM), and oxides of nitrogen (NOx). Intelligent transport system (ITS) technologies can be implemented to lower pollutant emissions and reduction of fuel consumption. This paper investigates the ITS techniques and technologies for the reduction of fuel consumption and minimization of the exhaust pollutant. It highlights the environmental impact of the ITS application to provide the state-of-art green solution. A case study also advocates that ITS technology reduces fuel consumption and exhaust pollutant in the urban environment. PMID:25032239
A Novel Real-time Carbon Dioxide Analyzer for Health and Environmental Applications
Zhao, Di; Miller, Dylan; Xian, Xiaojun; Tsow, Francis
2014-01-01
To be able to detect carbon dioxide (CO2) with high accuracy and fast response time is critical for many health and environmental applications. We report on a pocket-sized CO2 sensor for real-time analysis of end-tidal CO2, and environmental CO2. The sensor shows fast and reversible response to CO2 over a wide concentration range, covering the needs of both environmental and health applications. It is also immune to the presence of various interfering gases in ambient or expired air. Furthermore, the sensor has been used for real-time breath analysis, and the results are in good agreement with those from a commercial CO2 detector. PMID:24659857
A Novel Real-time Carbon Dioxide Analyzer for Health and Environmental Applications.
Zhao, Di; Miller, Dylan; Xian, Xiaojun; Tsow, Francis; Forzani, Erica S
2014-05-01
To be able to detect carbon dioxide (CO 2 ) with high accuracy and fast response time is critical for many health and environmental applications. We report on a pocket-sized CO 2 sensor for real-time analysis of end-tidal CO 2, and environmental CO 2 . The sensor shows fast and reversible response to CO 2 over a wide concentration range, covering the needs of both environmental and health applications. It is also immune to the presence of various interfering gases in ambient or expired air. Furthermore, the sensor has been used for real-time breath analysis, and the results are in good agreement with those from a commercial CO 2 detector.
Soil respiration in northern forests exposed to elevated atmospheric carbon dioxide and ozone
Kurt Pregitzer; Wendy Loya; Mark Kubiske; Donald Zak
2006-01-01
The aspen free-air CO2 and O3 enrichment (FACTS II-FACE) study in Rhinelander, Wisconsin, USA, is designed to understand the mechanisms by which young northern deciduous forest ecosystems respond to elevated atmospheric carbon dioxide (CO2) and elevated tropospheric ozone (O3)...
USDA-ARS?s Scientific Manuscript database
In plantation crops perennial tropical legumes are grown as understory plants, receive limited irradiance, and are subjected to elevated levels of CO2 and temperature. Independent short-term effects of photosynthetic photon flux density (PPFD), external carbon dioxide concentration [CO2] and temper...
Arbuscular mycorrhizal fungi increase organic carbon decomposition under elevated carbon dioxide
USDA-ARS?s Scientific Manuscript database
A major goal of climate change research is to understand whether and how terrestrial ecosystems can sequester more carbon to mitigate rising atmospheric carbon dioxide (CO2) levels. The stimulation of arbuscular mycorrhizal fungi (AMF) by elevated atmospheric CO2 has been assumed to be a major mecha...
46 CFR 13.121 - Courses for tankerman endorsements.
Code of Federal Regulations, 2013 CFR
2013-10-01
... (open and closed). (vii) Rules of the Coast Guard governing operations in general and prevention of..., carbon dioxide (CO2), foam... X Halogenated hydrocarbons X Pressure-water spray system in special..., spray, fog, and flooding) X Foam (high, medium and low expansion) X Carbon dioxide (CO2) X X Halon X...