A System Level Mass and Energy Calculation for a Temperature Swing Adsorption Pump Used for In-Situ Resource Utilization (ISRU) on Mars

NASA Technical Reports Server (NTRS)

Hasseeb, Hashmatullah; Iannetti, Anthony

2017-01-01

Mars ISRU converts atmospheric CO2 to generate O2 and CH4. Reduces launch mass, thus mission cost. Increases mission duration and independence. CO2 acquisition system must: a) Reliably extract CO2 over the varying Martian environment. 1) approx. 0.67-0.93 kPa pressure and 2) 125 C to 40 C. b) Provide and compress high purity gas to chemical plants. 1) Separate N2, Ar2, etc. from approx. 95% CO2 atmosphere and 2) Current pressure targets: 50 kPa-500 kPa.

Improvement of CO2/N2 separation performance by polymer matrix cellulose acetate butyrate

NASA Astrophysics Data System (ADS)

Lee, R. J.; Jawad, Z. A.; Ahmad, A. L.; Ngo, J. Q.; Chua, H. B.

2017-06-01

With the rapid development of modern civilization, carbon dioxide (CO2) is produced in large quantities and mainly generated from industrial sectors. The gas emission is the major contributor to global warming. To address this issue, the membrane technology is implemented for the CO2 removal, due to the energy efficiency and economic advantages presented. Cellulose acetate butyrate (CAB) is selected as the polymeric material, due to the excellent film-forming properties and capable of developing a defect-free layer of neat membrane. This study described the fabrication development of CAB using a wet phase inversion method with different casting conditions. Where the composition of the casting solutions (3-5 wt %) and solvent evaporation time (4-6 min) were determined. The outcomes of these dominant parameters were then used to determine the best CAB membrane for CO2/Nitrogen (N2) separation and supported by the characterization i.e. scanning electron micrograph. Gas permeation measurements showed satisfactory performance for CAB membrane fabricated with 5 min evaporation time and 4 wt% polymer composition (M2). Where, its permeance and selectivity are 120.19 GPU and 3.17, respectively. In summary, this study showed a brief outlined of the future direction and perspective of CAB membrane for CO2/N2 separation.

Carbon Dioxide-Free Hydrogen Production with Integrated Hydrogen Separation and Storage.

PubMed

Dürr, Stefan; Müller, Michael; Jorschick, Holger; Helmin, Marta; Bösmann, Andreas; Palkovits, Regina; Wasserscheid, Peter

2017-01-10

An integration of CO 2 -free hydrogen generation through methane decomposition coupled with hydrogen/methane separation and chemical hydrogen storage through liquid organic hydrogen carrier (LOHC) systems is demonstrated. A potential, very interesting application is the upgrading of stranded gas, for example, gas from a remote gas field or associated gas from off-shore oil drilling. Stranded gas can be effectively converted in a catalytic process by methane decomposition into solid carbon and a hydrogen/methane mixture that can be directly fed to a hydrogenation unit to load a LOHC with hydrogen. This allows for a straight-forward separation of hydrogen from CH 4 and conversion of hydrogen to a hydrogen-rich LOHC material. Both, the hydrogen-rich LOHC material and the generated carbon on metal can easily be transported to destinations of further industrial use by established transport systems, like ships or trucks. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Explore various co-substrates for simultaneous electricity generation and Congo red degradation in air-cathode single-chamber microbial fuel cell.

PubMed

Cao, Yunqing; Hu, Yongyou; Sun, Jian; Hou, Bin

2010-08-01

Microbial fuel cell (MFC) holds a great promise to harvest electricity directly from a wide range of ready degradable organic matters and enhance degradation of some recalcitrant contaminants. Glucose, acetate sodium and ethanol were separately examined as co-substrates for simultaneous bioelectricity generation and Congo red degradation in a proton exchange membrane (PEM) air-cathode single-chamber MFC. The batch test results showed that more than 98% decolorization at the dye concentration of 300 mg/L were achieved within 36 h for all tested co-substrates during electricity generation. The decolorization rate was different with the co-substrates used. The fastest decolorization rate was achieved with glucose followed by ethanol and sodium acetate. Accumulated intermediates were observed during Congo red degradation which was demonstrated by UV-Visible spectra and high performance liquid chromatography (HPLC). Electricity generation was sustained and not significantly affected by the Congo red degradation. Glucose, acetate sodium and ethanol produced maximum power densities of 103 mW/m(2), 85.9 mW/m(2) and 63.2 mW/m(2), respectively, and the maximum voltage output decreased by only 7% to 15%. Our results demonstrated the feasibility of using various co-substrates for simultaneous decolorization of Congo red and bioelectricity generation in the MFC and showed that glucose was the preferred co-substrate. Copyright (c) 2009 Elsevier B.V. All rights reserved.

Green separation and characterization of fatty acids from solid wastes of leather industry in supercritical fluid CO2.

PubMed

Onem, Ersin; Renner, Manfred; Prokein, Michael

2018-05-26

Considerable tannery waste is generated by leather industry around the world. Recovery of the value-added products as natural fats from the solid wastes gained interest of many researchers. In this study, supercritical fluid separation method was applied for the fatty acid isolation from leather industry solid wastes. Pre-fleshing wastes of the double-face lambskins were used as natural fat source. Only supercritical CO 2 was used as process media without any solvent additive in high-pressure view cell equipment. The effect of different conditions was investigated for the best separation influence. The parameters of pressure (100 to 200 bar), temperature (40 to 80 °C), and time (1 to 3 h) were considered. Extraction yields and fat yields of the parameters were statistically evaluated after the processes. Maximum 78.57 wt% fat yield was obtained from leather industry fleshings in supercritical fluid CO 2 at 200 bar, 80 °C, and 2 h. Morever, conventional Soxhlet and supercritical CO 2 extracted fatty acids were characterized by using gas chromatography (GC) coupled with mass spectrometry (MS) and flame ionization detector (FID). Fourier transform infrared spectroscopy (FTIR) and differential scanning calorimetry (DSC) characterizations were also done. The results showed that supercritical fluid CO 2 extraction was highly effective for the fat separation as green solvent and leather industry tannery wastes could be used for the value-added products.

Amorphous Silk Fibroin Membranes for Separation of CO2

NASA Technical Reports Server (NTRS)

Aberg, Christopher M.; Patel, Anand K.; Gil, Eun Seok; Spontak, Richard J.; Hagg, May-Britt

2009-01-01

Amorphous silk fibroin has shown promise as a polymeric material derivable from natural sources for making membranes for use in removing CO2 from mixed-gas streams. For most applications of silk fibroin, for purposes other than gas separation, this material is used in its highly crystalline, nearly natural form because this form has uncommonly high tensile strength. However, the crystalline phase of silk fibroin is impermeable, making it necessary to convert the material to amorphous form to obtain the high permeability needed for gas separation. Accordingly, one aspect of the present development is a process for generating amorphous silk fibroin by treating native silk fibroin in an aqueous methanol/salt solution. The resulting material remains self-standing and can be prepared as thin film suitable for permeation testing. The permeability of this material by pure CO2 has been found to be highly improved, and its mixed-gas permeability has been found to exceed the mixed-gas permeabilities of several ultrahigh-CO2-permeable synthetic polymers. Only one of the synthetic polymers poly(trimethylsilylpropyne) [PTMSP] may be more highly permeable by CO2. PTMSP becomes unstable with time, whereas amorphous silk should not, although at the time of this reporting this has not been conclusively proven.

A NOVEL CO{sub 2} SEPARATION SYSTEM

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

Robert J. Copeland

2000-03-01

Because of concern over global climate change, new systems are needed that produce electricity from fossil fuels and emit less CO{sub 2}. The fundamental problem with current systems which recover and concentrate CO{sub 2} from flue gases is the need to separate dilute CO{sub 2} and pressurize it to roughly 35 atm for storage or sequestration. This is an energy intensive process that can reduce plant efficiency by 9-37% and double the cost of electricity. There are two fundamental reasons for the current high costs of power consumption, CO{sub 2} removal, and concentration systems: (1) most disposal, storage and sequesteringmore » systems require high pressure CO{sub 2} (at roughly 35 atm). Thus, assuming 90% removal of the CO{sub 2} from a typical atmospheric pressure flue gas that contains 10% CO{sub 2}, the CO{sub 2} is essentially being compressed from 0.01 atm to 35 atm (a pressure ratio of 3,500). This is a very energy intensive process. (2) The absorption-based (amine) separation processes that are used to remove the CO{sub 2} from the flue gas and compress it to 1 atm consume approximately 10 times as much energy as the theoretical work of compression because they are heat driven cycles working over a very low temperature difference. Thus, to avoid the problems of current systems, we need a power cycle in which the CO{sub 2} produced by the oxidation of the fuel is not diluted with a large excess of nitrogen, a power cycle which would allow us to eliminate the very inefficient thermally driven absorption/desorption step. In addition, we would want the CO{sub 2} to be naturally available at high pressure (approximately 3 to 6 atmospheres), which would allow us to greatly reduce the compression ratio between generation and storage (from roughly 3,500 to approximately 8).« less

A NOVEL CO{sub 2} SEPARATION SYSTEM

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

Robert J. Copeland

2000-05-01

Because of concern over global climate change, new systems are needed that produce electricity from fossil fuels and emit less CO{sub 2}. The fundamental problem with current systems which recover and concentrate CO{sub 2} from flue gases is the need to separate dilute CO{sub 2} and pressurize it to roughly 35 atm for storage or sequestration. This is an energy intensive process that can reduce plant efficiency by 9-37% and double the cost of electricity. There are two fundamental reasons for the current high costs of power consumption, CO{sub 2} removal, and concentration systems: (1) most disposal, storage and sequesteringmore » systems require high pressure CO{sub 2} (at roughly 35 atm). Thus, assuming 90% removal of the CO{sub 2} from a typical atmospheric pressure flue gas that contains 10% CO{sub 2}, the CO{sub 2} is essentially being compressed from 0.01 atm to 35 atm (a pressure ratio of 3,500). This is a very energy intensive process. (2) The absorption-based (amine) separation processes that are used to remove the CO{sub 2} from the flue gas and compress it to 1 atm consume approximately 10 times as much energy as the theoretical work of compression because they are heat driven cycles working over a very low temperature difference. Thus, to avoid the problems of current systems, we need a power cycle in which the CO{sub 2} produced by the oxidation of the fuel is not diluted with a large excess of nitrogen, a power cycle which would allow us to eliminate the very inefficient thermally driven absorption/desorption step. In addition, we would want the CO{sub 2} to be naturally available at high pressure (approximately 3 to 6 atmospheres), which would allow us to greatly reduce the compression ratio between generation and storage (from roughly 3,500 to approximately 8).« less

A NOVEL CO{sub 2} SEPARATION SYSTEM

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

Robert J. Copeland

2000-08-01

Because of concern over global climate change, new systems are needed that produce electricity from fossil fuels and emit less CO{sub 2}. The fundamental problem with current systems which recover and concentrate CO{sub 2} from flue gases is the need to separate dilute CO{sub 2} and pressurize it to roughly 35 atm for storage or sequestration. This is an energy intensive process that can reduce plant efficiency by 9-37% and double the cost of electricity. There are two fundamental reasons for the current high costs of power consumption, CO{sub 2} removal, and concentration systems: (1) most disposal, storage and sequesteringmore » systems require high pressure CO{sub 2} (at roughly 35 atm). Thus, assuming 90% removal of the CO{sub 2} from a typical atmospheric pressure flue gas that contains 10% CO{sub 2}, the CO{sub 2} is essentially being compressed from 0.01 atm to 35 atm (a pressure ratio of 3,500). This is a very energy intensive process. (2) The absorption-based (amine) separation processes that are used to remove the CO{sub 2} from the flue gas and compress it to 1 atm consume approximately 10 times as much energy as the theoretical work of compression because they are heat driven cycles working over a very low temperature difference. Thus, to avoid the problems of current systems, we need a power cycle in which the CO{sub 2} produced by the oxidation of the fuel is not diluted with a large excess of nitrogen, a power cycle which would allow us to eliminate the very inefficient thermally driven absorption/desorption step. In addition, we would want the CO{sub 2} to be naturally available at high pressure (approximately 3 to 6 atmospheres), which would allow us to greatly reduce the compression ratio between generation and storage (from roughly 3,500 to approximately 8).« less

A high stability Ni-La0.5Ce0.5O2-δ asymmetrical metal-ceramic membrane for hydrogen separation and generation

NASA Astrophysics Data System (ADS)

Zhu, Zhiwen; Sun, Wenping; Wang, Zhongtao; Cao, Jiafeng; Dong, Yingchao; Liu, Wei

2015-05-01

In this work, hydrogen permeation properties of Ni-La0.5Ce0.5O2-δ (LDC) asymmetrical cermet membrane are investigated, including hydrogen fluxes (JH2) under different hydrogen partial pressures, the influence of water vapor on JH2 and the long-term stability of the membrane operating under the containing-CO2 atmosphere. Ni-LDC asymmetrical membrane shows the best hydrogen permeability among LDC-based hydrogen separation membranes, inferior to Ni-BaZr0.1Ce0.7Y0.2O3-δ asymmetrical membrane. The water vapor in feed gas is beneficial to hydrogen transport process, which promote an increase of JH2 from 5.64 × 10-8 to 6.83 × 10-8 mol cm-2 s-1 at 900 °C. Stability testing of hydrogen permeation suggests that Ni-LDC membrane remains stable against CO2. A dual function of combining hydrogen separation and generation can be realized by humidifying the sweep gas and enhance the hydrogen output by 1.0-1.5 times. Ni-LDC membrane exhibits desirable performance and durability in dual-function mode. Morphologies and phase structures of the membrane after tests are also characterized by SEM and XRD.

Conversion of CO2 to CO using radio-frequency atmospheric pressure plasmas

NASA Astrophysics Data System (ADS)

Foote, Alexander; Dedrick, James; O'Connell, Deborah; North, Michael; Gans, Timo

2016-09-01

Low temperature plasmas can be used for the in situ generation of CO, from relatively non-toxic CO2 . CO is very useful in many industrial chemical processes and so, via low temperature plasmas, CO2, a waste product, can be converted into a valuable chemical. The key challenges in using this method, for CO production, are optimising the energy efficiency, maximising the conversion of CO2 into CO and then separating the CO from the other species produced in the plasma. Very high yields of CO, greater than 90%, have been achieved at atmospheric pressure using argon as a carrier gas with admixtures up to 1.5% with energy efficiencies of up to 4%. The plasma generated in continuous and spatially homogeneous and is driven at a frequency of 40.68 MHz. A zero dimensional global model has also been used to simulate the chemical kinetics of the plasma to determine the dominant dissociation processes and is in good agreement with the experimentally determined yields. The model is used to determine how important a role the vibrational states of CO2 are, in a highly collisional plasma, to the production of CO and there can provide insight into how to improve the energy efficiency and suppress unwanted reactions.

Fifteen terawatt picosecond CO2 laser system.

PubMed

Haberberger, D; Tochitsky, S; Joshi, C

2010-08-16

The generation of a record peak-power of 15 TW (45 J, 3 ps) in a single CO(2) laser beam is reported. Using a master oscillator-power amplifier laser system, it is shown that up to 100 J of energy can be extracted in a train of 3 ps laser pulses separated by 18 ps, a characteristic time of the CO(2) molecule. The bandwidth required for amplifying the short injected laser pulse train in a 2.5 atm final CO(2) amplifier is provided by field broadening of the medium at intensities of up to 140 GW/cm(2). The measured saturation energy for 3 ps pulses is 120 mJ/cm(2) which confirms that energy is simultaneously extracted from six rovibrational lines.

Static feed water electrolysis module

NASA Technical Reports Server (NTRS)

Powell, J. D.; Schubert, F. H.; Jensen, F. C.

1974-01-01

An advanced static feed water electrolysis module (SFWEM) and associated instrumentation for generating breathable O2 was developed. The system also generates a H2 byproduct for use in an air revitalization system for O2 recovery from metabolic CO2. Special attention was given to: (1) eliminating water feed compartment degassing, (2) eliminating need for zero gravity condenser/separators, (3) increasing current density capability, and (4) providing a self contained module so that operation is independent of laboratory instrumentation and complicated startup/shutdown procedures.

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.

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

PubMed Central

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

2015-01-01

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

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

PubMed

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

2015-03-11

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

A novel process for recycling and resynthesizing LiNi{sub 1/3}Co{sub 1/3}Mn{sub 1/3}O{sub 2} from the cathode scraps intended for lithium-ion batteries

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

Zhang, Xihua; Key Laboratory of Green Process and Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190; Beijing Engineering Research Center of Process Pollution Control, Beijing 100190

Highlights: • A simple process to recycle cathode scraps intended for lithium-ion batteries. • Complete separation of the cathode material from the aluminum foil is achieved. • The recovered aluminum foil is highly pure. • LiNi{sub 1/3}Co{sub 1/3}Mn{sub 1/3}O{sub 2} is directly resynthesized from the separated cathode material. - Abstract: To solve the recycling challenge for aqueous binder based lithium-ion batteries (LIBs), a novel process for recycling and resynthesizing LiNi{sub 1/3}Co{sub 1/3}Mn{sub 1/3}O{sub 2} from the cathode scraps generated during manufacturing process is proposed in this study. Trifluoroacetic acid (TFA) is employed to separate the cathode material from the aluminummore » foil. The effects of TFA concentration, liquid/solid (L/S) ratio, reaction temperature and time on the separation efficiencies of the cathode material and aluminum foil are investigated systematically. The cathode material can be separated completely under the optimal experimental condition of 15 vol.% TFA solution, L/S ratio of 8.0 mL g{sup −1}, reacting at 40 °C for 180 min along with appropriate agitation. LiNi{sub 1/3}Co{sub 1/3}Mn{sub 1/3}O{sub 2} is successfully resynthesized from the separated cathode material by solid state reaction method. Several kinds of characterizations are performed to verify the typical properties of the resynthesized LiNi{sub 1/3}Co{sub 1/3}Mn{sub 1/3}O{sub 2} powder. Electrochemical tests show that the initial charge and discharge capacities of the resynthesized LiNi{sub 1/3}Co{sub 1/3}Mn{sub 1/3}O{sub 2} are 201 mAh g{sup −1} and 155.4 mAh g{sup −1} (2.8–4.5 V, 0.1 C), respectively. The discharge capacity remains at 129 mAh g{sup −1} even after 30 cycles with a capacity retention ratio of 83.01%.« less

Combined Power Generation and Carbon Sequestration Using Direct FuelCell

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

Hossein Ghezel-Ayagh

2006-03-01

The unique chemistry of carbonate fuel cell offers an innovative approach for separation of carbon dioxide from greenhouse gases (GHG). The carbonate fuel cell system also produces electric power at high efficiency. The simultaneous generation of power and sequestration of greenhouse gases offer an attractive scenario for re-powering the existing coal-fueled power plants, in which the carbonate fuel cell would separate the carbon dioxide from the flue gas and would generate additional pollutant-free electric power. Development of this system is concurrent with emergence of Direct FuelCell{reg_sign} (DFC{reg_sign}) technology for generation of electric power from fossil fuels. DFC is based onmore » carbonate fuel cell featuring internal reforming. This technology has been deployed in MW-scale power plants and is readily available as a manufactured product. This final report describes the results of the conceptualization study conducted to assess the DFC-based system concept for separation of CO2 from GHG. Design and development studies were focused on integration of the DFC systems with coal-based power plants, which emit large amounts of GHG. In parallel to the system design and simulation activities, operation of laboratory scale DFC verified the technical concept and provided input to the design activity. The system was studied to determine its effectiveness in capturing more than ninety percent of CO2 from the flue gases. Cost analysis was performed to estimate the change in cost of electricity for a 200 MW pulverized coal boiler steam cycle plant retrofitted with the DFC-based CO2 separation system producing an additional 127 MW of electric power. The cost increments as percentage of levelized cost of electricity were estimated for a range of separation plant installations per year and a range of natural gas cost. The parametric envelope meeting the goal (<20% increase in COE) was identified. Results of this feasibility study indicated that DFC-based separation systems have the potential for capturing at least 90% of the emissions from the greenhouse gases generated by power plants and other industrial exhaust streams, and yet entail in less than 20% increase in the cost of energy services for long-term deployment (beyond 2012). The anticipated cost of energy increase is in line with DOE's goal for post-combustion systems as outlined in the ''Carbon Capture and Sequestration Systems Analysis Guidelines'', published by NETL, April 2005. During the course of this study certain enabling technologies were identified and the needs for further research and development were discussed.« less

Electrochemical CO2 and O2 separation for crew and plant environments

NASA Technical Reports Server (NTRS)

Lee, M. G.; Grigger, David J.; Foerg, Sandra L.

1992-01-01

The study describes a closed ecosystem concept that includes electrochemical CO2 and O2 separators and a moisture condenser/separator for maintaining CO2, O2, and humidity levels in the crew and plant habitats at their respective optimal conditions. The key processes of this concept are aqueous electrolyte-based electrochemical CO2 and O2 separations. The principles and cell characteristics of these electrochemical gas separation processes are described. Also presented are descriptions of test hardware and the test results of the Electrochemical CO2 Separator (ECS) and the Electrochemical O2 Separator (EOS), and the combination of the ECS and the EOS. The test results proved that the ECS and EOS processes for the combined concept are viable.

Solid electrolyte oxygen regeneration system

NASA Technical Reports Server (NTRS)

Shumar, J. W.; See, G. G.; Schubert, F. H.; Powell, J. D.

1976-01-01

A program to design, develop, fabricate and assemble a one-man, self-contained, solid electrolyte oxygen regeneration system (SX-1) incorporating solid electrolyte electrolyzer drums was completed. The SX-1 is a preprototype engineering model designed to produce 0.952 kg (2.1 lb)/day of breathable oxygen (O2) from the electrolysis of metabolic carbon dioxide (CO2) and water vapor. The CO2 supply rate was established based on the metabolic CO2 generation rate for one man of 0.998 kg (2.2 lb)/day. The water supply rate (0.254 kg (0.56 lb)/day) was designed to be sufficient to make up the difference between the 0.952 kg (2.1 lb)/day O2 generation specification and the O2 available through CO2 electrolysis, 0.726 kg (1.6 lb)/day. The SX-1 was successfully designed, fabricated and assembled. Design verification tests (DVT) or the CO Disproportionators, H2 separators, control instrumentation, monitor instrumentation, water feed mechanism were successfully completed. The erratic occurrence of electrolyzer drum leakage prevented the completion of the CO2 electrolyzer module and water electrolyzer module DVT's and also prevented the performance of SX-1 integrated testing. Further development work is required to improve the solid electrolyte cell high temperature seals.

A novel process for recycling and resynthesizing LiNi1/3Co1/3Mn1/3O2 from the cathode scraps intended for lithium-ion batteries.

PubMed

Zhang, Xihua; Xie, Yongbing; Cao, Hongbin; Nawaz, Faheem; Zhang, Yi

2014-09-01

To solve the recycling challenge for aqueous binder based lithium-ion batteries (LIBs), a novel process for recycling and resynthesizing LiNi1/3Co1/3Mn1/3O2 from the cathode scraps generated during manufacturing process is proposed in this study. Trifluoroacetic acid (TFA) is employed to separate the cathode material from the aluminum foil. The effects of TFA concentration, liquid/solid (L/S) ratio, reaction temperature and time on the separation efficiencies of the cathode material and aluminum foil are investigated systematically. The cathode material can be separated completely under the optimal experimental condition of 15vol.% TFA solution, L/S ratio of 8.0 mL g(-1), reacting at 40°C for 180 min along with appropriate agitation. LiNi1/3Co1/3Mn1/3O2 is successfully resynthesized from the separated cathode material by solid state reaction method. Several kinds of characterizations are performed to verify the typical properties of the resynthesized LiNi1/3Co1/3Mn1/3O2 powder. Electrochemical tests show that the initial charge and discharge capacities of the resynthesized LiNi1/3Co1/3Mn1/3O2 are 201 mAh g(-)(1) and 155.4 mAh g(-1) (2.8-4.5 V, 0.1C), respectively. The discharge capacity remains at 129 mAh g(-1) even after 30 cycles with a capacity retention ratio of 83.01%. Copyright © 2014 Elsevier Ltd. All rights reserved.

A Hierarchical Z-Scheme α-Fe2 O3 /g-C3 N4 Hybrid for Enhanced Photocatalytic CO2 Reduction.

PubMed

Jiang, Zhifeng; Wan, Weiming; Li, Huaming; Yuan, Shouqi; Zhao, Huijun; Wong, Po Keung

2018-03-01

The challenge in the artificial photosynthesis of fossil resources from CO 2 by utilizing solar energy is to achieve stable photocatalysts with effective CO 2 adsorption capacity and high charge-separation efficiency. A hierarchical direct Z-scheme system consisting of urchin-like hematite and carbon nitride provides an enhanced photocatalytic activity of reduction of CO 2 to CO, yielding a CO evolution rate of 27.2 µmol g -1 h -1 without cocatalyst and sacrifice reagent, which is >2.2 times higher than that produced by g-C 3 N 4 alone (10.3 µmol g -1 h -1 ). The enhanced photocatalytic activity of the Z-scheme hybrid material can be ascribed to its unique characteristics to accelerate the reduction process, including: (i) 3D hierarchical structure of urchin-like hematite and preferable basic sites which promotes the CO 2 adsorption, and (ii) the unique Z-scheme feature efficiently promotes the separation of the electron-hole pairs and enhances the reducibility of electrons in the conduction band of the g-C 3 N 4 . The origin of such an obvious advantage of the hierarchical Z-scheme is not only explained based on the experimental data but also investigated by modeling CO 2 adsorption and CO adsorption on the three different atomic-scale surfaces via density functional theory calculation. The study creates new opportunities for hierarchical hematite and other metal-oxide-based Z-scheme system for solar fuel generation. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Hydrogen purification: MOF membranes put to the test

DOE PAGES

Nenoff, Tina M.

2015-03-30

Membranes are essential components for the removal of greenhouse gases during fuel generation processes, such as hydrogen production, but simultaneous permeability and selectivity is difficult to obtain. This has now been achieved in ultrathin membranes that use the size-selective porosity of metal–organic frameworks to separate CO 2 from H 2.

The Spatial Expansion of a Discharge in the Generation and the Channel Structure (in German)

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

Schlumbohm, H.

1962-02-01

The spatial expansion of a discharge was investigated under homogeneous field conditions, using an anode with a small central area separated from the remainder and wide band double beam oscillographic techniques. The discharge currents were initiated by electrons released along traces of single alpha particles in the gas between the electrodes. The k particles enter the gap volume through a small hole in the middle of the separated center of the anode. The measurements have shown that a secondary photon emission from the cathode causes a spreading over the total gap volume within the first few electron generations (N 2,more » air, and CO 2 at lower pressures). If a streamer mechanism occurs (O 2 and CO 2 at higher pressures), the discharge remains localized to the trace of the alpha particle, in which the avalanches yielded by the primary electrons have produced a high density of positive ions. New details of steamer mechanism are revealed by analyzing the rapid increase of the current during streamer formation.« less

Porous materials as high performance adsorbents for CO2 capture, gas separation and purification

NASA Astrophysics Data System (ADS)

Wang, Jun

Global warming resulted from greenhouse gases emission has received a widespread attention. Among the greenhouse gases, CO2 contributes more than 60% to global warming due to its huge emission amount. The flue gas contains about 15% CO2 with N2 as the balance. If CO2 can be separated from flue gas, the benefit is not only reducing the global warming effect, but also producing pure CO2 as a very useful industry raw material. Substantial progress is urgent to be achieved in an industrial process. Moreover, energy crisis is one of the biggest challenges for all countries due to the short life of fossil fuels, such as, petroleum will run out in 50 years and coal will run out in 150 years according to today's speed. Moreover, the severe pollution to the environment caused by burning fossil fuels requires us to explore sustainable, environment-friendly, and facile energy sources. Among several alternative energy sources, natural gas is one of the most promising alternative energy sources due to its huge productivity, abundant feed stock, and ease of generation. In order to realize a substantial adsorption process in industry, synthesis of new adsorbents or modification of existing adsorbent with improved properties has become the most critical issue. This dissertation reports systemic characterization and development of five serials of novel adsorbents with advanced adsorption properties. In chapter 2, nitrogen-doped Hypercross-linking Polymers (HCPs) have been synthesized successfully with non-carcinogenic chloromethyl methyl ether (CME) as the cross-linking agent within a single step. Texture properties, surface morphology, CO2/N2 selectivity, and adsorption heat have been presented and demonstrated properly. A comprehensive discussion on factors that affect the CO2 adsorption and CO2/N 2 separation has also been presented. It was found that high micropore proportion and N-content could effectively enhance CO2 uptake and CO2/N2 separation selectivity. In chapter 3, a new series of oxygen-doped ACs were synthesized from polyfuran. Different factors that affect the AC formation were investigated, and two kinds of porogens (ZnC12 and KOH) and two active temperatures (600 and 800 °C) were tested. At 298K and 1bar, an excellent selectivity for separating CO2/N2 (41.7) and CO2/CH 4(6.8) gas mixture pairs was obtained on the PF-600 KOH. A breakthrough simulation was also performed to demonstrate the potential of industrial applications. The PF-600 KOH sample showed the best separation result in the simulated adsorption breakthrough as well. In chapter 4, quinone and hydroquinone on the surface of PF-600 ZnC1 2 were integrated. Significantly pore size shrinkage, improved CO 2/N2 and CO2/CH4 IAST selectivity were observed, which is 58.7% and 28.4 % higher than pristine porous carbon at 298K and 1 atm, respectively. In addition, transient breakthrough simulations for CO2/CH4/N2 binary mixtures were conducted in order to demonstrate the good separation performance in fixed bed adsorbers. In chapter 5, a novel nitrogen doped polymer poly(2-phenyl-1,3,6,8tetraazacyclodecane) will be used as the precursor to produce microporous N-doped activated carbons. Three activation temperatures (600, 700, and 800 °C) has been investigated with KOH as the porogen. High nitrogen content has been remained in the resultant carbon materials. Improved CO2 adsorption capacity and selectivites for the separation of CO2/CH4/N2 binary gas mixtures were achieved by the carbon adsorbents due to their N-containing groups, narrow pore size distribution, and large specific surface area. In chapter 6, MOF-derived activated carbons are developed from MIL-100(Al) as hard-template. Direct carbonization of MIL-100, MIL-100(Al)/F-127 composite, and MIL-100(Al)/KOH mixture has been investigated. Pore structure and surface morphology have been demonstrated. CO2/CH4/N2 binary selectivity, adsorption heats, and kinetic selectivity have been calculated. Breakthrough simulation has been conducted to mimic industrial application. We found that resultant carbons showed better CO2 capture ability and selectivity than parental MIL-100(Al).

Carbon monoxide poisoning from portable electric generators.

PubMed

Hampson, Neil B; Zmaeff, Jennette L

2005-01-01

While the overall death rate from unintentional carbon monoxide (CO) poisoning has decreased in the United States due to improved automobile emissions controls and a decline in CO poisonings from motor vehicles, exposures have not changed from some sources of CO. One of these is the operation of portable electrical generators in poorly ventilated spaces. This study sought to describe the population poisoned from CO produced by portable electric generators, and to determine the reasons that generators are operated in a hazardous fashion. Cases of CO poisoning referred for treatment with hyperbaric oxygen at Virginia Mason Medical Center in Seattle from November 1978 to March 2004 were reviewed. Those cases that resulted from portable generator use were selected for analysis. Sixty-three patients aged 2 to 85 years were treated for CO poisoning from portable electric generators. They included 34 males and 29 females who were poisoned in 37 separate incidents. Thirty-four lost consciousness with the exposure. Of the 63 total patients, 60 spoke English. Generators were typically used when normal electrical service was disrupted by a storm or in remote locations. In 29 of 37 incidents, the generator was operated in the home environment, most commonly in the garage. Lack of awareness of the dangers of CO poisoning or lack of knowledge of ventilation requirements were the most commonly identified reasons. CO poisoning from portable electric generators occurs in a characteristic population, in a few typical locations and for a limited number of reasons. This information may help target prevention efforts for this form of poisoning, such as warning labels or educational programs.

Production and uses of liquefied atmosphere (CO2) on Mars

NASA Technical Reports Server (NTRS)

Waldron, R. D.

1991-01-01

Carbon dioxide is universally accessible on Mars, and can be liquefied and separated from residual atmospheric gases by various compress-refrigeration cycles. Liquid CO2, stored under elevated pressures, can be used as a source of high pressure gas for nighttime power generation at a Martian base powered by solar energy during the daytime. Carbon dioxide can also be used for vehicular power. The extractable energy per unit mass of CO2 can exceed that of commercial lead-acid batteries for operating cycles without heat addition. Improved performance is possible using heat input from the ambient atmosphere or thermochemical agents. A unique vehicular application uses pressurized CO2 as a non-combustion low performance propellant for intermediate distance surface transportation. The thermodynamic properties of CO2 are presented with typical operating cycles for the application classes described above.

Coal desulfurization. [using iron pentacarbonyl

NASA Technical Reports Server (NTRS)

Hsu, G. C. (Inventor)

1979-01-01

Organic sulfur is removed from coal by treatment with an organic solution of iron pentacarbonyl. Organic sulfur compounds can be removed by reaction of the iron pentacarbonyl with coal to generate CO and COS off-gases. The CO gas separated from COS can be passed over hot iron fillings to generate iron pentacarbonyl.

Inorganic Nanoparticles/Metal Organic Framework Hybrid Membrane Reactors for Efficient Photocatalytic Conversion of CO2.

PubMed

Maina, James W; Schütz, Jürg A; Grundy, Luke; Des Ligneris, Elise; Yi, Zhifeng; Kong, Lingxue; Pozo-Gonzalo, Cristina; Ionescu, Mihail; Dumée, Ludovic F

2017-10-11

Photocatalytic conversion of carbon dioxide (CO 2 ) to useful products has potential to address the adverse environmental impact of global warming. However, most photocatalysts used to date exhibit limited catalytic performance, due to poor CO 2 adsorption capacity, inability to efficiently generate photoexcited electrons, and/or poor transfer of the photogenerated electrons to CO 2 molecules adsorbed on the catalyst surface. The integration of inorganic semiconductor nanoparticles across metal organic framework (MOF) materials has potential to yield new hybrid materials, combining the high CO 2 adsorption capacity of MOF and the ability of the semiconductor nanoparticles to generate photoexcited electrons. Herein, controlled encapsulation of TiO 2 and Cu-TiO 2 nanoparticles within zeolitic imidazolate framework (ZIF-8) membranes was successfully accomplished, using rapid thermal deposition (RTD), and their photocatalytic efficiency toward CO 2 conversion was investigated under UV irradiation. Methanol and carbon monoxide (CO) were found to be the only products of the CO 2 reduction, with yields strongly dependent upon the content and composition of the dopant semiconductor particles. CuTiO 2 nanoparticle doped membranes exhibited the best photocatalytic performance, with 7 μg of the semiconductor nanoparticle enhancing CO yield of the pristine ZIF-8 membrane by 233%, and methanol yield by 70%. This work opens new routes for the fabrication of hybrid membranes containing inorganic nanoparticles and MOFs, with potential application not only in catalysis but also in electrochemical, separation, and sensing applications.

Different CO2 absorbents-modified SBA-15 sorbent for highly selective CO2 capture

NASA Astrophysics Data System (ADS)

Liu, Xiuwu; Zhai, Xinru; Liu, Dongyang; Sun, Yan

2017-05-01

Different CO2 absorbents-modified SBA-15 materials are used as CO2 sorbent to improve the selectivity of CH4/CO2 separation. The SBA-15 sorbents modified by physical CO2 absorbents are very limited to increasing CO2 adsorption and present poor selectivity. However, the SBA-15 sorbents modified by chemical CO2 absorbents increase CO2 adsorption capacity obviously. The separation coefficients of CO2/CH4 increase in this case. The adsorption and regeneration properties of the SBA-15 sorbents modified by TEA, MDEA and DIPA have been compared. The SBA-15 modified by triethanolamine (TEA) presents better CO2/CH4 separation performance than the materials modified by other CO2 absorbents.

Study of reverse flotation of calcite from scheelite in acidic media

NASA Astrophysics Data System (ADS)

Deng, Rongdong; Huang, Yuqing; Hu, Yuan; Ku, Jiangang; Zuo, Weiran; Yin, Wanzhong

2018-05-01

A new coated-reactive reverse flotation method based on the generation of CO2 bubbles at a calcite surface in acidic solution was used to separate calcite from scheelite. The dissolution kinetics of coated and uncoated calcite were studied in sulfuric acid. The CO2 bubbles generated on the uncoated calcite particle surface are enough to float the particle. However, most of these bubbles left the surface quickly, preventing calcite from floating. Here, a mixture of polyvinyl alcohol polymer and sodium dodecyl sulfonate was used to coat the mineral particles and form a stable membrane, resulting in the formation of a stable foam layer on the calcite surface. After the calcite is coated, the generated bubbles could be successfully captured on the calcite surface, and calcite particles could float to the air-water interface and remain there for more than one hour. Flotation tests indicated that a high-quality tungsten concentrate with a grade of more than 75% and a recovery of more than 99% could be achieved when the particle size was between 0.3 and 1.5 mm. The present results provide theoretical support for the development of a highly efficient flotation separation for carbonate minerals.

Dual-Channel, Molecular-Sieving Core/Shell ZIF@MOF Architectures as Engineered Fillers in Hybrid Membranes for Highly Selective CO2 Separation.

PubMed

Song, Zhuonan; Qiu, Fen; Zaia, Edmond W; Wang, Zhongying; Kunz, Martin; Guo, Jinghua; Brady, Michael; Mi, Baoxia; Urban, Jeffrey J

2017-11-08

A novel core/shell porous crystalline structure was prepared using a large pore metal organic framework (MOF, UiO-66-NH 2 , pore size, ∼ 0.6 nm) as core surrounded by a small pore zeolitic imidazolate framework (ZIF, ZIF-8, pore size, ∼ 0.4 nm) through a layer-by-layer deposition method and subsequently used as an engineered filler to construct hybrid polysulfone (PSF) membranes for CO 2 capture. Compared to traditional fillers utilizing only one type of porous material with rigid channels (either large or small), our custom designed core/shell fillers possess clear advantages via pore engineering: the large internal channels of the UiO-66-NH 2 MOFs create molecular highways to accelerate molecular transport through the membrane, while the thin shells with small pores (ZIF-8) or even smaller pores generated at the interface by the imperfect registry between the overlapping pores of ZIF and MOF enhance molecular sieving thus serving to distinguish slightly larger N 2 molecules (kinetic diameter, 0.364 nm) from smaller CO 2 molecules (kinetic diameter, 0.33 nm). The resultant core/shell ZIF@MOF and as-prepared hybrid PSF membranes were characterized by transmission electron microscopy, X-ray diffraction, wide-angle X-ray scattering, scanning electron microscopy, Fourier transform infrared, thermogravimetric analysis, differential scanning calorimetry, and contact angle tests. The dependence of the separation performance of the membranes on the MOF/ZIF ratio was also studied by varying the number of layers of ZIF coatings. The integrated PSF-ZIF@MOF hybrid membrane (40 wt % loading) with optimized ZIF coating cycles showed improved hydrophobicity and excellent CO 2 separation performance by simultaneously increasing CO 2 permeability (CO 2 permeability of 45.2 barrer, 710% higher than PSF membrane) and CO 2 /N 2 selectivity (CO 2 /N 2 selectivity of 39, 50% higher than PSF membrane), which is superior to most reported hybrid PSF membranes. The strategy of using dual-channel molecular sieving core/shell porous crystals in hybrid membranes thus provides a promising means for CO 2 capture from flue gas.

Increased CO2 selectivity of asphalt-derived porous carbon through introduction of water into pore space

NASA Astrophysics Data System (ADS)

Jalilov, Almaz S.; Li, Yilun; Kittrell, Carter; Tour, James M.

2017-12-01

The development of inexpensive porous solid sorbents, such as porous carbons, that can selectively capture carbon dioxide (CO2) from natural gas wells is essential to reduce emission of CO2 to the atmosphere. However, at higher pressures, the selectivity for CO2 over that for methane (CH4) remains poor. Here we show that H2O can be imbibed within asphalt-derived porous carbon, with a surface area of 4,200 m2 g-1, to generate a hydrated powder material. While maintaining a high CO2 uptake capacity of 48 mmol g-1 (211 wt%), the molar selectivity for CO2 over CH4 increases to >200:1 and the H2O remains within the pores on repeated cycling. To mimic realistic natural gas wells, we used a 90% CH4 and 10% CO2 gas mixture and showed selective CO2 separation at 20 bar. Furthermore, in situ vibrational spectroscopy reveals the formation of an ordered matrix within the pores consisting of gas hydrates.

Effect of addition of Proline, ionic liquid [Choline][Pro] on CO2 separation properties of poly(amidoamine) dendrimer / poly(ethylene glycol) hybrid membranes

NASA Astrophysics Data System (ADS)

Duan, S. H.; Kai, T.; Chowdhury, F. A.; Taniguchi, I.; Kazama, S.

2018-01-01

Poly(amidoamine) (PAMAM) dendrimers were incorporated into cross-linked poly(ethylene glycol) (PEGDMA) matrix to improve carbon dioxide (CO2) separation performance at elevated pressures. In our previous studies, PAMAM/PEGDMA hybrid membranes showed high CO2 separation properties from CO2/H2 mixed gases. In this study, proline, choline and ionic liquid [Choline][Pro] compounds were selected as rate promoters that were used to prepare PAMAM/PEGDMA hybrid membranes. The effect of addition of proline, choline, IL [Choline][Pro] on separation performance of PAMAM/PEGDMA) hybrid membranes for CO2/H2 separation was investigated. Amino acid proline, choline, and IL [Choline][Pro] were used to promote CO2 and amine reaction. With the addition of [Choline][Pro] into PAMAM/PEG membrane, CO2 permeance of PAMAM/PEG hybrid membranes are increased up to 46% without any change of selectivity of membrane for CO2.

Re-manufacture of cobalt-manganese-bromide as a liquid catalyst from spent catalyst containing cobalt generated from petrochemical processes via hydrometallurgy.

PubMed

Joo, Sung-Ho; Shin, Dong Ju; Oh, Chang Hyun; Wang, Jei-Pil; Shin, Shun Myung

2016-11-15

Cobalt and manganese have been the subject of individual separation studies because their fields of application are different. However, this study shows that high-value products can be manufactured in the form of a cobalt-manganese-bromide (CMB) liquid catalyst by simultaneously recovering cobalt and manganese. Na-bis-(2,4,4-tri-methyl-pentyl)phosphinic acid was employed in order to manufacture the CMB liquid catalyst from the spent catalyst generated from petroleum chemistry processes. The pH-isotherm, degree of saponification of solvent and separation factor values were investigated. ΔpH50 and separation factor values show that Co and Mn can be separated from impurities such as Mg and Ca. Further, the extraction stages and organic/aqueous ratio isotherms were investigated using counter-current simulation extraction batch tests. To prepare CMB from a loaded organic phase obtained in a stripping study using hydrogen bromide, the Co and Mn were completely stripped and concentrated by a factor of 6 using a 2M hydrogen bromide solution. When compared with manufactured and commercial CMB, the CMB liquid catalyst could be produced by supplying a shortage of Mn in the form of manganese bromide. Finally, the method of manufacture of CMB was subjected to a real pilot plant test. Copyright © 2016. Published by Elsevier B.V.

Thermodynamic analysis of the advanced zero emission power plant

NASA Astrophysics Data System (ADS)

Kotowicz, Janusz; Job, Marcin

2016-03-01

The paper presents the structure and parameters of advanced zero emission power plant (AZEP). This concept is based on the replacement of the combustion chamber in a gas turbine by the membrane reactor. The reactor has three basic functions: (i) oxygen separation from the air through the membrane, (ii) combustion of the fuel, and (iii) heat transfer to heat the oxygen-depleted air. In the discussed unit hot depleted air is expanded in a turbine and further feeds a bottoming steam cycle (BSC) through the main heat recovery steam generator (HRSG). Flue gas leaving the membrane reactor feeds the second HRSG. The flue gas consist mainly of CO2 and water vapor, thus, CO2 separation involves only the flue gas drying. Results of the thermodynamic analysis of described power plant are presented.

Database for CO2 Separation Performances of MOFs Based on Computational Materials Screening.

PubMed

Altintas, Cigdem; Avci, Gokay; Daglar, Hilal; Nemati Vesali Azar, Ayda; Velioglu, Sadiye; Erucar, Ilknur; Keskin, Seda

2018-05-23

Metal-organic frameworks (MOFs) are potential adsorbents for CO 2 capture. Because thousands of MOFs exist, computational studies become very useful in identifying the top performing materials for target applications in a time-effective manner. In this study, molecular simulations were performed to screen the MOF database to identify the best materials for CO 2 separation from flue gas (CO 2 /N 2 ) and landfill gas (CO 2 /CH 4 ) under realistic operating conditions. We validated the accuracy of our computational approach by comparing the simulation results for the CO 2 uptakes, CO 2 /N 2 and CO 2 /CH 4 selectivities of various types of MOFs with the available experimental data. Binary CO 2 /N 2 and CO 2 /CH 4 mixture adsorption data were then calculated for the entire MOF database. These data were then used to predict selectivity, working capacity, regenerability, and separation potential of MOFs. The top performing MOF adsorbents that can separate CO 2 /N 2 and CO 2 /CH 4 with high performance were identified. Molecular simulations for the adsorption of a ternary CO 2 /N 2 /CH 4 mixture were performed for these top materials to provide a more realistic performance assessment of MOF adsorbents. The structure-performance analysis showed that MOFs with Δ Q st 0 > 30 kJ/mol, 3.8 Å < pore-limiting diameter < 5 Å, 5 Å < largest cavity diameter < 7.5 Å, 0.5 < ϕ < 0.75, surface area < 1000 m 2 /g, and ρ > 1 g/cm 3 are the best candidates for selective separation of CO 2 from flue gas and landfill gas. This information will be very useful to design novel MOFs exhibiting high CO 2 separation potentials. Finally, an online, freely accessible database https://cosmoserc.ku.edu.tr was established, for the first time in the literature, which reports all of the computed adsorbent metrics of 3816 MOFs for CO 2 /N 2 , CO 2 /CH 4 , and CO 2 /N 2 /CH 4 separations in addition to various structural properties of MOFs.

Zeolites for CO2-CO-O2 Separation to Obtain CO2-Neutral Fuels.

PubMed

Perez-Carbajo, Julio; Matito-Martos, Ismael; Balestra, Salvador R G; Tsampas, Mihalis N; van de Sanden, Mauritius C M; Delgado, José A; Águeda, V Ismael; Merkling, Patrick J; Calero, Sofia

2018-06-20

Carbon dioxide release has become an important global issue due to the significant and continuous rise in atmospheric CO 2 concentrations and the depletion of carbon-based energy resources. Plasmolysis is a very energy-efficient process for reintroducing CO 2 into energy and chemical cycles by converting CO 2 into CO and O 2 utilizing renewable electricity. The bottleneck of the process is that CO remains mixed with O 2 and residual CO 2 . Therefore, efficient gas separation and recuperation are essential for obtaining pure CO, which, via water gas shift and Fischer-Tropsch reactions, can lead to the production of CO 2 -neutral fuels. The idea behind this work is to provide a separation mechanism based on zeolites to optimize the separation of carbon dioxide, carbon monoxide, and oxygen under mild operational conditions. To achieve this goal, we performed a thorough screening of available zeolites based on topology and adsorptive properties using molecular simulation and ideal adsorption solution theory. FAU, BRE, and MTW are identified as suitable topologies for these separation processes. FAU can be used for the separation of carbon dioxide from carbon monoxide and oxygen and BRE or MTW for the separation of carbon monoxide from oxygen. These results are reinforced by pressure swing adsorption simulations at room temperature combining adsorption columns with pure silica FAU zeolite and zeolite BRE at a Si/Al ratio of 3. These zeolites have the added advantage of being commercially available.

Gas separation mechanism of CO 2 selective amidoxime-poly(1-trimethylsilyl-1-propyne) membranes

DOE PAGES

Feng, Hongbo; Hong, Tao; Mahurin, Shannon Mark; ...

2017-05-09

Polymeric membranes for CO 2 separation have drawn significant attention in academia and industry. We prepared amidoxime-functionalized poly(1-trimethylsilyl-1-propyne) (AO-PTMSP) membranes through hydrosilylation and post-polymerization modification. Compared to neat PTMSP membranes, the AO-PTMSP membranes showed significant enhancements in CO 2/N 2 gas separation performance (CO 2 permeability ~6000 Barrer; CO 2/N 2 selectivity 17). This systematic study provides clear guidelines on how to tune the CO 2-philicity within PTMSP matrices and the effects on gas selectivity. Key parameters for elucidating the gas transport mechanism were discussed based on CO 2 sorption measurements and fractional free volume estimates. The effect of themore » AO content on CO 2/N 2 selectivity was further examined by means of density functional theory calculations. Here, both experimental and theoretical data provide consistent results that conclusively show that CO 2/N 2 separation performance is enhanced by increased CO 2 polymer interactions.« less

Gas separation mechanism of CO 2 selective amidoxime-poly(1-trimethylsilyl-1-propyne) membranes

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

Feng, Hongbo; Hong, Tao; Mahurin, Shannon Mark

Polymeric membranes for CO 2 separation have drawn significant attention in academia and industry. We prepared amidoxime-functionalized poly(1-trimethylsilyl-1-propyne) (AO-PTMSP) membranes through hydrosilylation and post-polymerization modification. Compared to neat PTMSP membranes, the AO-PTMSP membranes showed significant enhancements in CO 2/N 2 gas separation performance (CO 2 permeability ~6000 Barrer; CO 2/N 2 selectivity 17). This systematic study provides clear guidelines on how to tune the CO 2-philicity within PTMSP matrices and the effects on gas selectivity. Key parameters for elucidating the gas transport mechanism were discussed based on CO 2 sorption measurements and fractional free volume estimates. The effect of themore » AO content on CO 2/N 2 selectivity was further examined by means of density functional theory calculations. Here, both experimental and theoretical data provide consistent results that conclusively show that CO 2/N 2 separation performance is enhanced by increased CO 2 polymer interactions.« less

Polymer ultrapermeability from the inefficient packing of 2D chains

NASA Astrophysics Data System (ADS)

Rose, Ian; Bezzu, C. Grazia; Carta, Mariolino; Comesaña-Gándara, Bibiana; Lasseuguette, Elsa; Ferrari, M. Chiara; Bernardo, Paola; Clarizia, Gabriele; Fuoco, Alessio; Jansen, Johannes C.; Hart, Kyle E.; Liyana-Arachchi, Thilanga P.; Colina, Coray M.; McKeown, Neil B.

2017-09-01

The promise of ultrapermeable polymers, such as poly(trimethylsilylpropyne) (PTMSP), for reducing the size and increasing the efficiency of membranes for gas separations remains unfulfilled due to their poor selectivity. We report an ultrapermeable polymer of intrinsic microporosity (PIM-TMN-Trip) that is substantially more selective than PTMSP. From molecular simulations and experimental measurement we find that the inefficient packing of the two-dimensional (2D) chains of PIM-TMN-Trip generates a high concentration of both small (<0.7 nm) and large (0.7-1.0 nm) micropores, the former enhancing selectivity and the latter permeability. Gas permeability data for PIM-TMN-Trip surpass the 2008 Robeson upper bounds for O2/N2, H2/N2, CO2/N2, H2/CH4 and CO2/CH4, with the potential for biogas purification and carbon capture demonstrated for relevant gas mixtures. Comparisons between PIM-TMN-Trip and structurally similar polymers with three-dimensional (3D) contorted chains confirm that its additional intrinsic microporosity is generated from the awkward packing of its 2D polymer chains in a 3D amorphous solid. This strategy of shape-directed packing of chains of microporous polymers may be applied to other rigid polymers for gas separations.

Ultrathin graphene oxide-based hollow fiber membranes with brush-like CO2-philic agent for highly efficient CO2 capture.

PubMed

Zhou, Fanglei; Tien, Huynh Ngoc; Xu, Weiwei L; Chen, Jung-Tsai; Liu, Qiuli; Hicks, Ethan; Fathizadeh, Mahdi; Li, Shiguang; Yu, Miao

2017-12-13

Among the current CO 2 capture technologies, membrane gas separation has many inherent advantages over other conventional techniques. However, fabricating gas separation membranes with both high CO 2 permeance and high CO 2 /N 2 selectivity, especially under wet conditions, is a challenge. In this study, sub-20-nm thick, layered graphene oxide (GO)-based hollow fiber membranes with grafted, brush-like CO 2 -philic agent alternating between GO layers are prepared by a facile coating process for highly efficient CO 2 /N 2 separation under wet conditions. Piperazine, as an effective CO 2 -philic agent, is introduced as a carrier-brush into the GO nanochannels with chemical bonding. The membrane exhibits excellent separation performance under simulated flue gas conditions with CO 2 permeance of 1,020 GPU and CO 2 /N 2 selectivity as high as 680, demonstrating its potential for CO 2 capture from flue gas. We expect this GO-based membrane structure combined with the facile coating process to facilitate the development of ultrathin GO-based membranes for CO 2 capture.

Dual Effect of Manganese Oxide Micromotors: Catalytic Degradation and Adsorptive Bubble Separation of Organic Pollutants.

PubMed

Wani, Owies M; Safdar, Muhammad; Kinnunen, Niko; Jänis, Janne

2016-01-22

Manganese oxide (MnO2 ) based micromotors exhibiting a dual effect, that is, catalytic degradation and adsorptive bubble separation, were employed for water remediation. The dual effect of MnO2 microparticles led to a greater than 90 % of decolorization of non-biodegradable organic dyes in just 1 h, without the need for external agitation or bubble generation. These findings suggest high potential of MnO2 micromotors for decontamination of organic pollutants from wastewaters or natural water reserves. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Chemical absorption and CO2 biofixation via the cultivation of Spirulina in semicontinuous mode with nutrient recycle.

PubMed

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.

A Review of Enzymatic Transesterification of Microalgal Oil-Based Biodiesel Using Supercritical Technology

PubMed Central

Taher, Hanifa; Al-Zuhair, Sulaiman; Al-Marzouqi, Ali H.; Haik, Yousef; Farid, Mohammed M.

2011-01-01

Biodiesel is considered a promising replacement to petroleum-derived diesel. Using oils extracted from agricultural crops competes with their use as food and cannot realistically satisfy the global demand of diesel-fuel requirements. On the other hand, microalgae, which have a much higher oil yield per hectare, compared to oil crops, appear to be a source that has the potential to completely replace fossil diesel. Microalgae oil extraction is a major step in the overall biodiesel production process. Recently, supercritical carbon dioxide (SC-CO2) has been proposed to replace conventional solvent extraction techniques because it is nontoxic, nonhazardous, chemically stable, and inexpensive. It uses environmentally acceptable solvent, which can easily be separated from the products. In addition, the use of SC-CO2 as a reaction media has also been proposed to eliminate the inhibition limitations that encounter biodiesel production reaction using immobilized enzyme as a catalyst. Furthermore, using SC-CO2 allows easy separation of the product. In this paper, conventional biodiesel production with first generation feedstock, using chemical catalysts and solvent-extraction, is compared to new technologies with an emphasis on using microalgae, immobilized lipase, and SC-CO2 as an extraction solvent and reaction media. PMID:21915372

Energy Economics of Farm Biogas in Cold Climates

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

Pillay, Pragasen; Grimberg, Stefan; Powers, Susan E

Anaerobic digestion of farm and dairy waste has been shown to be capital intensive. One way to improve digester economics is to co-digest high-energy substrates together with the dairy manure. Cheese whey for example represents a high-energy substrate that is generated during cheese manufacture. There are currently no quantitative tools available that predict performance of co-digestion farm systems. The goal of this project was to develop a mathematical tool that would (1) predict the impact of co-digestion and (2) determine the best use of the generated biogas for a cheese manufacturing plant. Two models were developed that separately could bemore » used to meet both goals of the project. Given current pricing structures of the most economical use of the generated biogas at the cheese manufacturing plant was as a replacement of fuel oil to generate heat. The developed digester model accurately predicted the performance of 26 farm digesters operating in the North Eastern U.S.« less

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

Zhu, Lingxiang; Omid, Maryam; Lin, Haiqing

Cross-linking has been widely utilized to modify polyimide nanostructures for membrane gas separations, such as increasing size sieving ability and diffusivity selectivity for H2/CO2 and CO2/CH4 separation, and improving resistance to plasticization derived from CO2 and heavy hydrocarbons for CO2/CH4 and C3H6/C3H8 separations. However, there is a lack of fundamental understanding of the relationship between cross linked structure and membrane gas separation properties. This chapter critically reviews the effect of cross linking on polymer physical properties (such as glass transition temperature, Tg), and current strategies adopted to cross link polyimides for membrane gas separation. The information is synthesized to elucidatemore » the effect of cross linking on Tg and cross linking density in polyimides, which is then used to interpret the changes of gas permeability and selectivity. The benefits of cross linking in improving gas separation properties are also illustrated in Robeson’s upper bound plots for H2/CO2, CO2/CH4 and C3H6/C3H8 separation.« less

40 CFR 98.443 - Calculating CO2 geologic sequestration.

Code of Federal Regulations, 2013 CFR

2013-07-01

... CO2 that was injected into the well or wells covered by this source category. (1) For each gas-liquid... production data, you must sum the mass of all of the CO2 separated at each gas-liquid separator in accordance... category are produced and not processed through a gas-liquid separator, the concentration of CO2 in the...

40 CFR 98.443 - Calculating CO2 geologic sequestration.

Code of Federal Regulations, 2014 CFR

2014-07-01

... CO2 that was injected into the well or wells covered by this source category. (1) For each gas-liquid... production data, you must sum the mass of all of the CO2 separated at each gas-liquid separator in accordance... category are produced and not processed through a gas-liquid separator, the concentration of CO2 in the...

40 CFR 98.443 - Calculating CO2 geologic sequestration.

Code of Federal Regulations, 2012 CFR

2012-07-01

... CO2 that was injected into the well or wells covered by this source category. (1) For each gas-liquid... production data, you must sum the mass of all of the CO2 separated at each gas-liquid separator in accordance... category are produced and not processed through a gas-liquid separator, the concentration of CO2 in the...

Increased Oxygen Recovery from Sabatier Systems Using Plasma Pyrolysis Technology and Metal Hydride Separation

NASA Technical Reports Server (NTRS)

Greenwood, Zachary W.; Abney, Morgan B.; Perry, Jay L.; Miller, Lee A.; Dahl, Roger W.; Hadley, Neal M.; Wambolt, Spencer R.; Wheeler, Richard R.

2015-01-01

State-of-the-art life support carbon dioxide (CO2) reduction technology is based on the Sabatier reaction where less than 50% of the oxygen required for the crew is recovered from metabolic CO2. The reaction produces water as the primary product and methane as a byproduct. Oxygen recovery is constrained by the limited availability of reactant hydrogen. This is further exacerbated when Sabatier methane (CH4) is vented as a waste product resulting in a continuous loss of reactant hydrogen. Post-processing methane with the Plasma Pyrolysis Assembly (PPA) to recover hydrogen has the potential to dramatically increase oxygen recovery and thus drastically reduce the logistical challenges associated with oxygen resupply. The PPA decomposes methane into predominantly hydrogen and acetylene. Due to the highly unstable nature of acetylene, a separation system is necessary to purify hydrogen before it is recycled back to the Sabatier reactor. Testing and evaluation of a full-scale Third Generation PPA is reported and investigations into metal hydride hydrogen separation technology is discussed.

Fast separation of enantiomers by capillary electrophoresis using a combination of two capillaries with different internal diameters.

PubMed

Šebestová, Andrea; Petr, Jan

2017-12-01

The combination of capillaries with different internal diameters was used to accelerate the separation of enantiomers in capillary electrophoresis. Separation of R,S-1,1'-binaphthalene-2,2'-diyl hydrogen phosphate using isopropyl derivative of cyclofructan 6 was studied as a model system. The best separation conditions included 500 mM sodium borate pH 9.5 with 60 mM concentration of the chiral selector. Separation lasted approx. 1.5 min using the combination of 50 and 100 μm id capillaries of 9.7 cm and 22.9 cm, respectively. It allowed approx. 12-fold acceleration in comparison to the traditional long-end separation mainly due to the higher electroosmotic flow generated in the connected capillaries. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Separation control by vortex generator devices in a transonic channel flow

NASA Astrophysics Data System (ADS)

Bur, Reynald; Coponet, Didier; Carpels, Yves

2009-12-01

An experimental study was conducted in a transonic channel to control by mechanical vortex generator devices the strong interaction between a shock wave and a separated turbulent boundary layer. Control devices—co-rotating and counter-rotating vane-type vortex generators—were implemented upstream of the shock foot region and tested both on a steady shock wave and on a forced shock oscillation configurations. The spanwise spacing of vortex generator devices along the channel appeared to be an important parameter to control the flow separation region. When the distance between each device is decreased, the vortices merging is more efficient to reduce the separation. Their placement upstream of the shock wave is determinant to ensure that vortices have mixed momentum all spanwise long before they reach the separation line, so as to avoid separation cells. Then, vortex generators slightly reduced the amplitude of the forced shock wave oscillation by delaying the upstream displacement of the leading shock.

Mixed-Matrix Membranes Containing Carbon Nanotubes Composite with Hydrogel for Efficient CO2 Separation.

PubMed

Zhang, Haiyang; Guo, Ruili; Hou, Jinpeng; Wei, Zhong; Li, Xueqin

2016-10-26

In this study, a carbon nanotubes composite coated with N-isopropylacrylamide hydrogel (NIPAM-CNTs) was synthesized. Mixed-matrix membranes (MMMs) were fabricated by incorporating NIPAM-CNTs composite filler into poly(ether-block-amide) (Pebax MH 1657) matrix for efficient CO 2 separation. The as-prepared NIPAM-CNTs composite filler mainly plays two roles: (i) The extraordinary smooth one-dimensional nanochannels of CNTs act as the highways to accelerate CO 2 transport through membranes, increasing CO 2 permeability; (ii) The NIPAM hydrogel layer coated on the outer walls of CNTs acts as the super water absorbent to increase water content of membranes, appealing both CO 2 permeability and CO 2 /gas selectivity. MMM containing 5 wt % NIPAM-CNTs exhibited the highest CO 2 permeability of 567 barrer, CO 2 /CH 4 selectivity of 35, and CO 2 /N 2 selectivity of 70, transcending 2008 Robeson upper bound line. The improved CO 2 separation performance of MMMs is mainly attributed to the construction of the efficient CO 2 transport pathways by NIPAM-CNTs. Thus, MMMs incorporated with NIPAM-CNTs composite filler can be used as an excellent membrane material for efficient CO 2 separation.

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

PubMed

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

2003-06-01

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

55Co separation from proton irradiated metallic nickel

NASA Astrophysics Data System (ADS)

Valdovinos, H. F.; Graves, S.; Barnhart, T.; Nickles, R. J.

2014-11-01

55Co with > 97% radionuclidic purity 24 hours after end of bombardment (EoB) was produced from the 58Ni ( p ,α) reaction using proton irradiations of 16 MeV on natural nickel. Two-hour irradiations with 25 μA on a 254 μm thick nickel foil generate 0.18 ± 0.01 GBq (n = 3) 24 hours after EoB. The separation of cobalt from the target material and other metallic contaminants present at trace levels is accomplished in HCl medium by two rounds of anion exchange chromatography (AG1-X8) using an automated module driven by a peristaltic pump. 80 ± 5 % (n = 3) of the activity generated at EoB is ready for labeling in 0.1 M HCl one hour after the start of separation. Using 99.999% pure Ni, the reactivity (decay corrected to EoB) with the bifunctional chelator (BFC) DOTA was 8.5 GBq/μmol; enough for radiolabeling BFC conjugated biomolecules at a nmol scale with > 90% yield. Using 99.9% pure Ni the reactivity with DOTA and NOTA was 0.19 +/- 0.09 GBq/μmol and 2.9 +/- 1.7 GBq/μmol (n = 2), respectively. Both cobalt complexes showed 100% in vitro stability in PBS and mouse serum over 41 hours at room temperature. MicroPET images of a miniature Derenzo phantom show excellent resolution where rods of 1.5 mm were separated by two times their diameter.

High Selectivity Gas Separation Membrane Assemblies

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

Nachlas, Jesse; Corn, Isaac; Wegst, Ulrike

Global energy consumption is projected to be more than double of today’s levels by 2050. Economic and environmental pressures are putting significant limits on fossil fuel resources, and there is a significant push for improved efficiency in many industrial processes. Membranes for gas separation represent a significant opportunity for reduced energy consumption and improved efficiencies in a wide range of industrial applications by replacing typical high temperature processes or energy intensive processes with low temperature energy efficient processes. Carbon membranes represent an attractive class of membrane materials that offer the potential to improve the reliability, corrosion resistance and temperature capabilitymore » of polymeric membranes, which limit their adoption for many industrial applications. However, there are still a number of technical hurdles which must be overcome before carbon membranes can be made commercially ready including elimination of manufacturing defects, and improved performance (permeability and selectivity) relative to polymeric membranes. Examples of potential application of carbon membranes include production of oxygen enriched air (OEA) for combustion applications, separation of carbon dioxide (CO 2) from flue gas to improve the commercial feasibility of CO 2 sequestration, separation of hydrogen from CO/CO 2 during hydrogen manufacturing, and separation of H 2 from hydrocarbons during refinery operations to improve the kinetics of cracking reactions. As a result of these benefits there is a strong driving force to develop processing technologies capable of producing carbon membranes and possessing high reliability, for a wide range of applications. The DOE provides significant support for research and development is this area, as they have recognized the significant impact a low cost carbon membrane technology can have on energy consumption and polluting emissions across a broad range of industrial applications. In this SBIR Phase I project, we developed a novel polymer precursor composition, which led to highly reproducible crack-free porous carbon membranes that were capable of producing 30-50% oxygen for OEA from a pressurized air feed, thereby meeting the primary Phase I objective, and possessing a selectivity of ~20:1 for CO 2/N 2 separation. We also successfully developed a method for fabricating a ceramic support from low-cost fly ash. In general, the effectiveness of a carbon membrane at separating various gases is a function of the pore structure and size. The novel processing method utilized is capable of accurately controlling pore structure during the fabrication process opening the possibility to create a membrane technology platform that can operate across a broad range of gas compositions and applications. Nanoporous carbon membrane technology offers a very attractive option for important industrial gas separation processes that are typically energy intensive and expensive to install and operate. Highly efficient gas separation represents a key enabling technology for increasing efficiency and lowering cost in various applications involving advanced power generation systems, metallurgical operations and chemical processes. These benefits will be translated to the public through lower cost for goods and services in addition to lower cost for energy. Increased national security will come from decreased dependence on imported oil by making local resources, such as coal and natural gas, competitive in energy generation markets. Finally, making low cost oxygen available in these industries results in cleaner power production and reduced emissions of polluting gases.« less

A Taxonomy of Digital Media Types for Learner-Generated Digital Media Assignments

ERIC Educational Resources Information Center

Reyna, Jorge; Hanham, Jose; Meier, Peter

2017-01-01

The notion of students as co-creators of content in higher education is gaining popularity, with an ever-increasing emphasis on the development of digital media assignments. In a separate paper, the authors introduced the Digital Media Literacies Framework, which is composed of three interrelated domains: (1) conceptual, (2) functional, and (3)…

Membraneless water filtration using CO2

NASA Astrophysics Data System (ADS)

Shin, Sangwoo; Shardt, Orest; Warren, Patrick B.; Stone, Howard A.

2017-05-01

Water purification technologies such as microfiltration/ultrafiltration and reverse osmosis utilize porous membranes to remove suspended particles and solutes. These membranes, however, cause many drawbacks such as a high pumping cost and a need for periodic replacement due to fouling. Here we show an alternative membraneless method for separating suspended particles by exposing the colloidal suspension to CO2. Dissolution of CO2 into the suspension creates solute gradients that drive phoretic motion of particles. Due to the large diffusion potential generated by the dissociation of carbonic acid, colloidal particles move either away from or towards the gas-liquid interface depending on their surface charge. Using the directed motion of particles induced by exposure to CO2, we demonstrate a scalable, continuous flow, membraneless particle filtration process that exhibits low energy consumption, three orders of magnitude lower than conventional microfiltration/ultrafiltration processes, and is essentially free from fouling.

Membraneless water filtration using CO2

PubMed Central

Shin, Sangwoo; Shardt, Orest; Warren, Patrick B.; Stone, Howard A.

2017-01-01

Water purification technologies such as microfiltration/ultrafiltration and reverse osmosis utilize porous membranes to remove suspended particles and solutes. These membranes, however, cause many drawbacks such as a high pumping cost and a need for periodic replacement due to fouling. Here we show an alternative membraneless method for separating suspended particles by exposing the colloidal suspension to CO2. Dissolution of CO2 into the suspension creates solute gradients that drive phoretic motion of particles. Due to the large diffusion potential generated by the dissociation of carbonic acid, colloidal particles move either away from or towards the gas–liquid interface depending on their surface charge. Using the directed motion of particles induced by exposure to CO2, we demonstrate a scalable, continuous flow, membraneless particle filtration process that exhibits low energy consumption, three orders of magnitude lower than conventional microfiltration/ultrafiltration processes, and is essentially free from fouling. PMID:28462929

Molecular simulation of separation of CO{sub 2} from flue gases in Cu-BTC metal-organic framework

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

Yang, Q.Y.; Xue, C.Y.; Zhong, C.L.

2007-11-15

In this work, a computational study was performed on the adsorption separation of CO{sub 2} from flue gases (mixtures of CO{sub 2}/N{sub 2}/O{sub 2}) in Cu-BTC metal-organic framework (MOF) to investigate the applicability of MOFs to this important industrial system. The computational results showed that Cu-BTC is a promising material for separation of CO{sub 2} from flue gases, and the macroscopic separation behaviors of the MOF were elucidated at a molecular level to give insight into the underlying mechanisms. The present work not only provided useful information for understanding the separation characteristics of MOFs, but also showed their potential applicationsmore » in chemical industry.« less

Electrochemical separation of hydrogen from reformate using PEM fuel cell technology

NASA Astrophysics Data System (ADS)

Gardner, C. L.; Ternan, M.

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

Carbon footprint assessment of Western Australian Groundwater Recycling Scheme

NASA Astrophysics Data System (ADS)

Simms, Andrew; Hamilton, Stacey; Biswas, Wahidul K.

2017-04-01

This research has determined the carbon footprint or the carbon dioxide equivalent (CO2 eq) of potable water production from a groundwater recycling scheme, consisting of the Beenyup wastewater treatment plant, the Beenyup groundwater replenishment trial plant and the Wanneroo groundwater treatment plant in Western Australia, using a life cycle assessment approach. It was found that the scheme produces 1300 tonnes of CO2 eq per gigalitre (GL) of water produced, which is 933 tonnes of CO2 eq higher than the desalination plant at Binningup in Western Australia powered by 100% renewable energy generated electricity. A Monte Carlo Simulation uncertainty analysis calculated a Coefficient of Variation value of 5.4%, thus confirming the accuracy of the simulation. Electricity input accounts for 83% of the carbon dioxide equivalent produced during the production of potable water. The chosen mitigation strategy was to consider the use of renewable energy to generate electricity for carbon intensive groundwater replenishment trial plant. Depending on the local situation, a maximum of 93% and a minimum of 21% greenhouse gas saving from electricity use can be attained at groundwater replenishment trial plant by replacing grid electricity with renewable electricity. In addition, the consideration of vibrational separation (V-Sep) that helps reduce wastes generation and chemical use resulted in a 4.03 tonne of CO2 eq saving per GL of water produced by the plant.

Carbon footprint assessment of Western Australian Groundwater Recycling Scheme.

PubMed

Simms, Andrew; Hamilton, Stacey; Biswas, Wahidul K

2017-04-01

This research has determined the carbon footprint or the carbon dioxide equivalent (CO 2 eq) of potable water production from a groundwater recycling scheme, consisting of the Beenyup wastewater treatment plant, the Beenyup groundwater replenishment trial plant and the Wanneroo groundwater treatment plant in Western Australia, using a life cycle assessment approach. It was found that the scheme produces 1300 tonnes of CO 2 eq per gigalitre (GL) of water produced, which is 933 tonnes of CO 2 eq higher than the desalination plant at Binningup in Western Australia powered by 100% renewable energy generated electricity. A Monte Carlo Simulation uncertainty analysis calculated a Coefficient of Variation value of 5.4%, thus confirming the accuracy of the simulation. Electricity input accounts for 83% of the carbon dioxide equivalent produced during the production of potable water. The chosen mitigation strategy was to consider the use of renewable energy to generate electricity for carbon intensive groundwater replenishment trial plant. Depending on the local situation, a maximum of 93% and a minimum of 21% greenhouse gas saving from electricity use can be attained at groundwater replenishment trial plant by replacing grid electricity with renewable electricity. In addition, the consideration of vibrational separation (V-Sep) that helps reduce wastes generation and chemical use resulted in a 4.03 tonne of CO 2 eq saving per GL of water produced by the plant.

Advanced Supported Liquid Membranes for Carbon Dioxide Control in Cabin Applications

NASA Technical Reports Server (NTRS)

Wickham, David T.; Gleason, Kevin J.; Engel, Jeffrey R.; Chullen, Cinda

2016-01-01

The development of new, robust, life support systems is critical to NASA's continued progress in space exploration. One vital function is maintaining the carbon dioxide (CO2) concentration in the cabin at levels that do not impair the health or performance of the crew. The CO2 removal assembly (CDRA) is the current CO2 control technology on-board the International Space Station (ISS). Although the CDRA has met the needs of the ISS to date, the repeated cycling of the molecular sieve sorbent causes it to break down into small particles that clog filters or generate dust in the cabin. This reduces reliability and increases maintenance requirements. Another approach that has potential advantages over the current system is a membrane that separates CO2 from air. In this approach, cabin air contacts one side of the membrane while other side of the membrane is maintained at low pressure to create a driving force for CO2 transport across the membrane. In this application, the primary power requirement is for the pump that creates the low pressure and then pumps the CO2 to the oxygen recovery system. For such a membrane to be practical, it must have high CO2 permeation rate and excellent selectivity for CO2 over air. Unfortunately, conventional gas separation membranes do not have adequate CO2 permeability and selectivity to meet the needs of this application. However, the required performance could be obtained with a supported liquid membrane (SLM), which consists of a microporous material filled with a liquid that selectively reacts with CO2 over air. In a recently completed Phase II SBIR project, Reaction Systems, Inc. fabricated an SLM that is very close to meeting permeability and selectivity objectives for use in the advanced space suit portable life support system. This paper describes work carried out to evaluate its potential for use in spacecraft cabin application.

A single-ligand ultra-microporous MOF for precombustion CO2 capture and hydrogen purification.

PubMed

Nandi, Shyamapada; De Luna, Phil; Daff, Thomas D; Rother, Jens; Liu, Ming; Buchanan, William; Hawari, Ayman I; Woo, Tom K; Vaidhyanathan, Ramanathan

2015-12-01

Metal organic frameworks (MOFs) built from a single small ligand typically have high stability, are rigid, and have syntheses that are often simple and easily scalable. However, they are normally ultra-microporous and do not have large surface areas amenable to gas separation applications. We report an ultra-microporous (3.5 and 4.8 Å pores) Ni-(4-pyridylcarboxylate)2 with a cubic framework that exhibits exceptionally high CO2/H2 selectivities (285 for 20:80 and 230 for 40:60 mixtures at 10 bar, 40°C) and working capacities (3.95 mmol/g), making it suitable for hydrogen purification under typical precombustion CO2 capture conditions (1- to 10-bar pressure swing). It exhibits facile CO2 adsorption-desorption cycling and has CO2 self-diffusivities of ~3 × 10(-9) m(2)/s, which is two orders higher than that of zeolite 13X and comparable to other top-performing MOFs for this application. Simulations reveal a high density of binding sites that allow for favorable CO2-CO2 interactions and large cooperative binding energies. Ultra-micropores generated by a small ligand ensures hydrolytic, hydrostatic stabilities, shelf life, and stability toward humid gas streams.

Relationship between fabrication method and chemical stability of Ni-BaZr0.8Y0.2O3-δ membrane

NASA Astrophysics Data System (ADS)

Fang, Shumin; Wang, Siwei; Brinkman, Kyle S.; Su, Qing; Wang, Haiyan; Chen, Fanglin

2015-03-01

NiO effectively promotes the sintering of highly refractory Y-doped BaZrO3 (BZY) through the formation of BaY2NiO5, providing a simple and cost-effective method for the fabrication of dense BZY electrolyte and Ni-BZY hydrogen separation membrane at ∼1400 °C. Unfortunately, insulating BaCO3 and Y2O3 phases formed on the surface of BZY and Ni-BZY prepared by solid state reaction method with NiO after annealing in wet CO2. Ni-BZY membranes prepared from different methods suffered different degree of performance loss in wet H2 at 900 °C. The chemical instability of Ni-BZY is attributed to the formation of a secondary phase (BaY2O4) generated from the reduction of BaY2NiO5 in H2 during the sintering process. Both BaY2O4 and BaY2NiO5 react with H2O, and CO2 at elevated temperatures, generating insulating Ba(OH)2 and BaCO3 phases, respectively. The less BaY2O4 is formed in the fabrication process, the better chemical stability the Ni-BZY membranes possess. Therefore, a new Ni-BZY membrane is prepared through a judicial combination of BZY powders prepared from combined EDTA-citric and solid state reaction methods, and demonstrates exceptional chemical stability in H2O and CO2, enabling stable and even improved hydrogen flux in wet 50% CO2 at 900 °C.

Generating "Good Enough" Evidence for Co-Production

ERIC Educational Resources Information Center

Durose, Catherine; Needham, Catherine; Mangan, Catherine; Rees, James

2017-01-01

Co-production is not a new concept but it is one with renewed prominence and reach in contemporary policy discourse. It refers to joint working between people or groups who have traditionally been separated into categories of user and producer. The article focuses on the co-production of public services, offering theory-based and knowledge-based…

Regression and statistical shape model based substitute CT generation for MRI alone external beam radiation therapy from standard clinical MRI sequences.

PubMed

Ghose, Soumya; Greer, Peter B; Sun, Jidi; Pichler, Peter; Rivest-Henault, David; Mitra, Jhimli; Richardson, Haylea; Wratten, Chris; Martin, Jarad; Arm, Jameen; Best, Leah; Dowling, Jason A

2017-10-27

In MR only radiation therapy planning, generation of the tissue specific HU map directly from the MRI would eliminate the need of CT image acquisition and may improve radiation therapy planning. The aim of this work is to generate and validate substitute CT (sCT) scans generated from standard T2 weighted MR pelvic scans in prostate radiation therapy dose planning. A Siemens Skyra 3T MRI scanner with laser bridge, flat couch and pelvic coil mounts was used to scan 39 patients scheduled for external beam radiation therapy for localized prostate cancer. For sCT generation a whole pelvis MRI (1.6 mm 3D isotropic T2w SPACE sequence) was acquired. Patients received a routine planning CT scan. Co-registered whole pelvis CT and T2w MRI pairs were used as training images. Advanced tissue specific non-linear regression models to predict HU for the fat, muscle, bladder and air were created from co-registered CT-MRI image pairs. On a test case T2w MRI, the bones and bladder were automatically segmented using a novel statistical shape and appearance model, while other soft tissues were separated using an Expectation-Maximization based clustering model. The CT bone in the training database that was most 'similar' to the segmented bone was then transformed with deformable registration to create the sCT component of the test case T2w MRI bone tissue. Predictions for the bone, air and soft tissue from the separate regression models were successively combined to generate a whole pelvis sCT. The change in monitor units between the sCT-based plans relative to the gold standard CT plan for the same IMRT dose plan was found to be [Formula: see text] (mean  ±  standard deviation) for 39 patients. The 3D Gamma pass rate was [Formula: see text] (2 mm/2%). The novel hybrid model is computationally efficient, generating an sCT in 20 min from standard T2w images for prostate cancer radiation therapy dose planning and DRR generation.

Regression and statistical shape model based substitute CT generation for MRI alone external beam radiation therapy from standard clinical MRI sequences

NASA Astrophysics Data System (ADS)

Ghose, Soumya; Greer, Peter B.; Sun, Jidi; Pichler, Peter; Rivest-Henault, David; Mitra, Jhimli; Richardson, Haylea; Wratten, Chris; Martin, Jarad; Arm, Jameen; Best, Leah; Dowling, Jason A.

2017-11-01

In MR only radiation therapy planning, generation of the tissue specific HU map directly from the MRI would eliminate the need of CT image acquisition and may improve radiation therapy planning. The aim of this work is to generate and validate substitute CT (sCT) scans generated from standard T2 weighted MR pelvic scans in prostate radiation therapy dose planning. A Siemens Skyra 3T MRI scanner with laser bridge, flat couch and pelvic coil mounts was used to scan 39 patients scheduled for external beam radiation therapy for localized prostate cancer. For sCT generation a whole pelvis MRI (1.6 mm 3D isotropic T2w SPACE sequence) was acquired. Patients received a routine planning CT scan. Co-registered whole pelvis CT and T2w MRI pairs were used as training images. Advanced tissue specific non-linear regression models to predict HU for the fat, muscle, bladder and air were created from co-registered CT-MRI image pairs. On a test case T2w MRI, the bones and bladder were automatically segmented using a novel statistical shape and appearance model, while other soft tissues were separated using an Expectation-Maximization based clustering model. The CT bone in the training database that was most ‘similar’ to the segmented bone was then transformed with deformable registration to create the sCT component of the test case T2w MRI bone tissue. Predictions for the bone, air and soft tissue from the separate regression models were successively combined to generate a whole pelvis sCT. The change in monitor units between the sCT-based plans relative to the gold standard CT plan for the same IMRT dose plan was found to be 0.3%+/-0.9% (mean  ±  standard deviation) for 39 patients. The 3D Gamma pass rate was 99.8+/-0.00 (2 mm/2%). The novel hybrid model is computationally efficient, generating an sCT in 20 min from standard T2w images for prostate cancer radiation therapy dose planning and DRR generation.

Chemical vapor deposition on chabazite (CHA) zeolite membranes for effective post-combustion CO2 capture.

PubMed

Kim, Eunjoo; Lee, Taehee; Kim, Hyungmin; Jung, Won-Jin; Han, Doug-Young; Baik, Hionsuck; Choi, Nakwon; Choi, Jungkyu

2014-12-16

Chabazite (CHA) zeolites with a pore size of 0.37 × 0.42 nm(2) are expected to separate CO2 (0.33 nm) from larger N2 (0.364 nm) in postcombustion flue gases by recognizing their minute size differences. Furthermore, the hydrophobic siliceous constituent in CHA membranes can allow for maintaining the CO2/N2 separation performance in the presence of H2O in contrast with the CO2 affinity-based membranes. In an attempt to increase the molecular sieving ability, the pore mouth size of all silica CHA (Si-CHA) particles was reduced via the chemical vapor deposition (CVD) of a silica precursor (tetraethyl orthosilicate). Accordingly, an increase of the CVD treatment duration decreased the penetration rate of CO2 into the CVD-treated Si-CHA particles. Furthermore, the CVD process was applied to siliceous CHA membranes in order to improve their CO2/N2 separation performance. Compared to the intact CHA membranes, the CO2/N2 maximum separation factor (max SF) for CVD-treated CHA membranes was increased by ∼ 2 fold under dry conditions. More desirably, the CO2/N2 max SF was increased by ∼ 3 fold under wet conditions at ∼ 50 °C, a representative temperature of the flue gas stream. In fact, the presence of H2O in the feed disfavored the permeation of N2 more than that of CO2 through CVD-modified CHA membranes and thus, contributed to the increased CO2/N2 separation factor.

Preparation of polyhedral oligomeric silsesquioxane based hybrid monoliths by ring-opening polymerization for capillary LC and CEC.

PubMed

Lin, Hui; Zhang, Zhenbin; Dong, Jing; Liu, Zhongshan; Ou, Junjie; Zou, Hanfa

2013-09-01

A new organic-inorganic hybrid monolith was prepared by the ring-opening polymerization of octaglycidyldimethylsilyl polyhedral oligomeric silsesquioxane (POSS) with 1,4-butanediamine (BDA) using 1-propanol, 1,4-butanediol, and PEG 10,000 as a porogenic system. Benefiting from the moderate phase separation process, the resulting poly(POSS-co-BDA) hybrid monolith possessed a uniform microstructure and exhibited excellent performance in chromatographic applications. Neutral, acidic, and basic compounds were successfully separated on the hybrid monolith in capillary LC (cLC), and high column efficiencies were achieved in all of the separations. In addition, as the amino groups could generate a strong EOF, the hybrid monolith was also applied in CEC for the separation of neutral and polar compounds, and a satisfactory performance was obtained. These results demonstrate that the poly(POSS-co-BDA) hybrid monolith is a good separation media in chromatographic separations of various types of compounds by both cLC and CEC. © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Enhanced photoelectrochemical water splitting by oxides heterojunction photocathode coupled with Ag.

PubMed

Lu, Xue; Liu, Zhifeng

2017-08-14

A novel one-dimensional Co 3 O 4 /CuO/Ag composite structure film was directly grown on indium tin oxide glass substrate by a simple hydrothermal method and electrodeposition method. The film was employed for the first time as a photocathode for photoelectrochemical (PEC) water splitting to generate hydrogen. The photocurrent density of the Co 3 O 4 /CuO/Ag composite structure achieved -5.13 mA cm -2 at -0.2 V vs. RHE, which is roughly 12.8 times that of 1D Co 3 O 4 nanowires and 3.31 times Co 3 O 4 /CuO heterojunction photocathodes. The enhanced PEC performance of this Co 3 O 4 /CuO/Ag composite structure ascribes increased light-harvesting and light-absorption, distensible photoresponse range, decreased interface charge transfer resistance, and improved photogenerated electron-hole pairs transfer and separation.

Protein separations using enhanced-fluidity liquid chromatography.

PubMed

Bennett, Raffeal; Olesik, Susan V

2017-11-10

Enhanced-fluidity liquid chromatography (EFLC) methods using methanol/H 2 O/CO 2 and hydrophilic interaction liquid chromatography (HILIC) were explored for the separation of proteins and peptides. EFLC is a separation mode that uses a mobile phase made of conventional solvents combined with liquid carbon dioxide (CO 2 ) in subcritical conditions. The addition of liquid CO 2 enhances diffusivity and decreases viscosity while maintaining mixture polarity, which typically results in reduced time of analysis. TFA additive and elevated temperature were leveraged as key factors in the separation of a 13-analyte intact protein mixture in under 5min. Under these conditions EFLC showed modest improvement in terms of peak asymmetry and analysis time over the competing ACN/H 2 O separation. Protein analytes detected by electrospray ionization - quadrupole time of flight, were shown to be unaffected by the addition of CO 2 in the mobile phase. Herein, the feasibility of separating hydrophilic proteins up to 80kDa (with transferrin) is demonstrated for CO 2 -containing mobile phases. Copyright © 2017 Elsevier B.V. All rights reserved.

Carbon dioxide separation with a two-dimensional polymer membrane.

PubMed

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.

Cross-Linked Poly(vinylidene fluoride-co-hexafluoropropene) (PVDF-co-HFP) Gel Polymer Electrolyte for Flexible Li-Ion Battery Integrated with Organic Light Emitting Diode (OLED)

PubMed Central

Kim, Ilhwan; Kim, Bong Sung; Nam, Seunghoon; Lee, Hoo-Jeong; Chung, Ho Kyoon; Cho, Sung Min; Luu, Thi Hoai Thuong; Hyun, Seungmin; Kang, Chiwon

2018-01-01

Here, we fabricate poly(vinylidene fluoride-co-hexafluoropropene) (PVDF-co-HFP) by electrospinning for a gel polymer electrolyte (GPE) for use in flexible Li-ion batteries (LIBs). As a solvent, we use N-methyl-2-pyrrolidone (NMP), which helps produce the cross-linked morphology of PVDF-co-HFP separator, owing to its low volatility. The cross-linked PVDF-co-HFP separator shows an uptake rate higher than that of a commercialized polypropylene (PP) separator. Moreover, the PVDF-co-HFP separator shows an ionic conductivity of 2.3 × 10−3 S/cm at room temperature, comparable with previously reported values. An LIB full-cell assembled with the PVDF-co-HFP-based GPE shows capacities higher than its counterpart with the commercialized PP separator, confirming that the cross-linked PVDF-co-HFP separator provides highly efficient ionic conducting pathways. In addition, we integrate a flexible LIB cell using the PVDF-co-HFP GPE with a flexible organic light emitting diode (OLED), demonstrating a fully flexible unit of LIB and OLED. PMID:29614800

Cross-Linked Poly(vinylidene fluoride-co-hexafluoropropene) (PVDF-co-HFP) Gel Polymer Electrolyte for Flexible Li-Ion Battery Integrated with Organic Light Emitting Diode (OLED).

PubMed

Kim, Ilhwan; Kim, Bong Sung; Nam, Seunghoon; Lee, Hoo-Jeong; Chung, Ho Kyoon; Cho, Sung Min; Luu, Thi Hoai Thuong; Hyun, Seungmin; Kang, Chiwon

2018-04-02

Here, we fabricate poly(vinylidene fluoride- co -hexafluoropropene) (PVDF- co -HFP) by electrospinning for a gel polymer electrolyte (GPE) for use in flexible Li-ion batteries (LIBs). As a solvent, we use N -methyl-2-pyrrolidone (NMP), which helps produce the cross-linked morphology of PVDF- co -HFP separator, owing to its low volatility. The cross-linked PVDF- co -HFP separator shows an uptake rate higher than that of a commercialized polypropylene (PP) separator. Moreover, the PVDF- co -HFP separator shows an ionic conductivity of 2.3 × 10 -3 S/cm at room temperature, comparable with previously reported values. An LIB full-cell assembled with the PVDF- co -HFP-based GPE shows capacities higher than its counterpart with the commercialized PP separator, confirming that the cross-linked PVDF- co -HFP separator provides highly efficient ionic conducting pathways. In addition, we integrate a flexible LIB cell using the PVDF- co -HFP GPE with a flexible organic light emitting diode (OLED), demonstrating a fully flexible unit of LIB and OLED.

Recent trends in ultra-fast HPLC: new generation superficially porous silica columns.

PubMed

Ali, Imran; Al-Othman, Zeid A; Nagae, Norikaju; Gaitonde, Vinay D; Dutta, Kamlesh K

2012-12-01

New generation columns, i.e. packed with superficially porous silica particles are available as trade names with following manufacturers: Halo, Ascentis Express, Proshell 120, Kinetex, Accucore, Sunshell, and Nucleoshell. These provide ultra-fast HPLC separations for a variety of compounds with moderate sample loading capacity and low back pressure. Chemistries of these columns are C(8), C(18), RP-Amide, hydrophilic interaction liquid chromatography, penta fluorophenyl (PFP), F5, and RP-aqua. Normally, the silica gel particles are of 2.7 and 1.7 μm as total and inner solid core diameters, respectively, with 0.5-μm-thick of outer porous layer having 90 Å pore sizes and 150 m(2)/g surface area. This article describes these new generation columns with special emphasis on their textures and chemistries, separations, optimization, and comparison (inter and intra stationary phases). Besides, future perspectives have also been discussed. © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Optical element for full spectral purity from IR-generated EUV light sources

NASA Astrophysics Data System (ADS)

van den Boogaard, A. J. R.; Louis, E.; van Goor, F. A.; Bijkerk, F.

2009-03-01

Laser produced plasma (LLP) sources are generally considered attractive for high power EUV production in next generation lithography equipment. Such plasmas are most efficiently excited by the relatively long, infrared wavelengths of CO2-lasers, but a significant part of the rotational-vibrational excitation lines of the CO2 radiation will be backscattered by the plasma's critical density surface and consequently will be present as parasitic radiation in the spectrum of such sources. Since most optical elements in the EUV collecting and imaging train have a high reflection coefficient for IR radiation, undesirable heating phenomena at the resist level are likely to occur. In this study a completely new principle is employed to obtain full separation of EUV and IR radiation from the source by a single optical component. While the application of a transmission filter would come at the expense of EUV throughput, this technique potentially enables wavelength separation without loosing reflectance compared to a conventional Mo/Si multilayer coated element. As a result this method provides full spectral purity from the source without loss in EUV throughput. Detailed calculations on the principal of functioning are presented.

Formation of freestanding ZrO{sub 2} nanotubes for Cr(VI) removal

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

Bashirom, Nurulhuda, E-mail: nurulhuda.usm2014@gmail.com; Ye, Beh Chin, E-mail: cyebeh@gmail.com; Razak, Khairunisak Abdul, E-mail: khairunisak@usm.my

2016-07-06

Freestanding ZrO{sub 2} nanotubes (ZNTs) were produced using a simple anodization method in fluorinated ethylene glycol electrolyte containing 1 ml 1 M K{sub 2}CO{sub 3}. The pH of the bath was kept constant at 8. The potassium carbonate (K{sub 2}CO{sub 3}) was added into electrolyte to promote the detachment of anodic ZrO{sub 2} film from the underlying zirconium (Zr) substrate. The poor adherence of ZNTs layer was due to generation of CO{sub 2} gas that was thought to occur between metal|oxide interfaces. The effect of anodization voltages towards the detachment of ZNTs layer was systematically studied at 20 V, 40more » V, 50 V and 60 V for 1 hour. The formation of CO{sub 2} gas is a function of anodization voltage, in which at 60 V, a good anodic film separation seen due to higher formation of CO{sub 2} gas. A preliminary study shown the capability of ZNTs in removing 5 ppm of Cr(VI) aqueous solution under illumination of UV light.« less

Advanced Supported Liquid Membranes for Carbon Dioxide Control in Cabin Applications

NASA Technical Reports Server (NTRS)

Wickham, David T.; Gleason, Kevin J.; Engel, Jeffrey R.; Chullen, Cinda

2016-01-01

The development of new, robust, life support systems is critical to NASA's continued progress in space exploration. One vital function is maintaining the carbon dioxide (CO2) concentration in the cabin at levels that do not impair the health or performance of the crew. The carbon dioxide removal assembly (CDRA) is the current CO2 control technology on-board the International Space Station (ISS). Although the CDRA has met the needs of the ISS to date, the repeated cycling of the molecular sieve sorbent causes it to break down into small particles that clog filters or generate dust in the cabin. This reduces reliability and increases maintenance requirements. Another approach that has potential advantages over the current system is a membrane that separates CO2 from air. In this approach, cabin air contacts one side of the membrane while other side of the membrane is maintained at low pressure to create a driving force for CO2 transport across the membrane. In this application, the primary power requirement is for the pump that creates the low pressure and then pumps the CO2 to the oxygen recovery system. For such a membrane to be practical, it must have high CO2 permeation rate and excellent selectivity for CO2 over air. Unfortunately, conventional gas separation membranes do not have adequate CO2 permeability and selectivity to meet the needs of this application. However, the required performance could be obtained with a supported liquid membrane (SLM), which consists of a microporous material filled with a liquid that selectively reacts with CO2 over air. In a recently completed Phase II SBIR project, Reaction Systems, Inc. fabricated an SLM that is very close to meeting permeability and selectivity objectives for use in the Portable Life Support System (PLSS). This paper describes work carried out to evaluate its potential for use in the cabin.

Molecular beam epitaxy growth and magnetic properties of Cr-Co-Ga Heusler alloy films

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

Feng, Wuwei, E-mail: wfeng@cugb.edu.cn; Wang, Weihua; Zhao, Chenglong

2015-11-15

We have re-investigated growth and magnetic properties of Cr{sub 2}CoGa films using molecular beam epitaxy technique. Phase separation and precipitate formation were observed experimentally again in agreement with observation of multiple phases separation in sputtered Cr{sub 2}CoGa films by M. Meinert et al. However, significant phase separation could be suppressed by proper control of growth conditions. We showed that Cr{sub 2}CoGa Heusler phase, rather than Co{sub 2}CrGa phase, constitutes the majority of the sample grown on GaAs(001) at 450 {sup o}C. The measured small spin moment of Cr{sub 2}CoGa is in agreement with predicted HM-FCF nature; however, its Curie temperaturemore » is not as high as expected from the theoretical prediction probably due to the off-stoichiometry of Cr{sub 2}CoGa and the existence of the disorders and phase separation.« less

Multi-Fluid Geothermal Energy Systems: Using CO2 for Dispatchable Renewable Power Generation and Grid Stabilization

NASA Astrophysics Data System (ADS)

Buscheck, T. A.; Bielicki, J. M.; Randolph, J.; Chen, M.; Hao, Y.; Sun, Y.

2013-12-01

Abstract We present an approach to use CO2 to (1) generate dispatchable renewable power that can quickly respond to grid fluctuations and be cost-competitive with natural gas, (2) stabilize the grid by efficiently storing large quantities of energy, (3) enable seasonal storage of solar thermal energy for grid integration, (4) produce brine for power-plant cooling, all which (5) increase CO2 value, rendering CO2 capture to be commerically viable, while (6) sequestering huge quantities of CO2. These attributes reduce carbon intensity of electric power, and enable cost-competitive, dispatchable power from major sources of renewable energy: wind, solar, and geothermal. Conventional geothermal power systems circulate brine as the working fluid to extract heat, but the parasitic power load for this circulation can consume a large portion of gross power output. Recently, CO2 has been considered as a working fluid because its advantageous properties reduce this parasitic loss. We expand on this idea by using multiple working fluids: brine, CO2, and N2. N2 can be separated from air at lower cost than captured CO2, it is not corrosive, and it will not react with the formation. N2 also can improve the economics of energy production and enable energy storage, while reducing operational risk. Extracting heat from geothermal reservoirs often requires submersible pumps to lift brine, but these pumps consume much of the generated electricity. In contrast, our approach drives fluid circulation by injecting supplemental, compressible fluids (CO2, and N2) with high coefficients of thermal expansion. These fluids augment reservoir pressure, produce artesian flow at the producers, and reduce the parasitic load. Pressure augmentation is improved by the thermosiphon effect that results from injecting cold/dense CO2 and N2. These fluids are heated to reservoir temperature, greatly expand, and increase the artesian flow of brine and supplemental fluid at the producers. Rather than using pumps, the thermosiphon directly converts reservoir thermal energy into mechanical energy for fluid circulation. Because stored pressure drives fluid production, the response time is faster than that of conventional geothermal power, already considered to be dispatchable. For conventional geothermal, the parasitic power load is in phase with gross power output. In contrast, our approach can time-shift much of the parasitic power load, which is dominated by the power required to separate N2 from air and compress it for injection. Because N2 is readily available, it can be injected intermittently. Thus, most of the parasitic power load can be shifted to coincide with minimum power demand or when there is a surplus of renewable power. Such a time-shift also allows net power output to be nearly equal to gross power output during peak demand. Energy storage can be almost 100 percent efficient because it is achieved by shifting the parasitic load, which is more efficient than other methods used to store energy and stabilize the grid. This work was performed under the auspices of the U.S. DOE by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344.

Evaluating the energy performance of a hybrid membrane-solvent process for flue gas carbon dioxide capture

DOE PAGES

Kusuma, Victor A.; Li, Zhiwei; Hopkinson, David; ...

2016-10-13

In this study, a particularly energy intensive step in the conventional amine absorption process to remove carbon dioxide is solvent regeneration using a steam stripping column. An attractive alternative to reduce the energy requirement is gas pressurized stripping, in which a high pressure noncondensable gas is used to strip CO 2 off the rich solvent stream. The gas pressurized stripping column product, having CO 2 at high concentration and high partial pressure, can then be regenerated readily using membrane separation. In this study, we performed an energetic analysis in the form of total equivalent work and found that, for capturingmore » CO 2 from flue gas, this hybrid stripping process consumes 49% less energy compared to the base case conventional MEA absorption/steam stripping process. We also found the amount of membrane required in this process is much less than required for direct CO 2 capture from the flue gas: approximately 100-fold less than a previously published two-stage cross-flow scheme, mostly due to the more favorable pressure ratio and CO 2 concentration. There does exist a trade-off between energy consumption and required membrane area that is most strongly affected by the gas pressurized stripper operating pressure. While initial analysis looks promising from both an energy requirement and membrane unit capital cost, the viability of this hybrid process depends on the availability of advanced, next generation gas separation membranes to perform the stripping gas regeneration.« less

Evaluating the energy performance of a hybrid membrane-solvent process for flue gas carbon dioxide capture

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

Kusuma, Victor A.; Li, Zhiwei; Hopkinson, David

In this study, a particularly energy intensive step in the conventional amine absorption process to remove carbon dioxide is solvent regeneration using a steam stripping column. An attractive alternative to reduce the energy requirement is gas pressurized stripping, in which a high pressure noncondensable gas is used to strip CO 2 off the rich solvent stream. The gas pressurized stripping column product, having CO 2 at high concentration and high partial pressure, can then be regenerated readily using membrane separation. In this study, we performed an energetic analysis in the form of total equivalent work and found that, for capturingmore » CO 2 from flue gas, this hybrid stripping process consumes 49% less energy compared to the base case conventional MEA absorption/steam stripping process. We also found the amount of membrane required in this process is much less than required for direct CO 2 capture from the flue gas: approximately 100-fold less than a previously published two-stage cross-flow scheme, mostly due to the more favorable pressure ratio and CO 2 concentration. There does exist a trade-off between energy consumption and required membrane area that is most strongly affected by the gas pressurized stripper operating pressure. While initial analysis looks promising from both an energy requirement and membrane unit capital cost, the viability of this hybrid process depends on the availability of advanced, next generation gas separation membranes to perform the stripping gas regeneration.« less

Graphene Oxide Membranes with Heterogeneous Nanodomains for Efficient CO2 Separations.

PubMed

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

2017-11-06

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

Experimental parametric study of jet vortex generators for flow separation control

NASA Technical Reports Server (NTRS)

Selby, Gregory

1991-01-01

A parametric wind-tunnel study was performed with jet vortex generators to determine their effectiveness in controlling flow separation associated with low-speed turbulence flow over a two-dimensional rearward-facing ramp. Results indicate that flow-separation control can be accomplished, with the level of control achieved being a function of jet speed, jet orientation (with respect to the free-stream direction), and orifice pattern (double row of jets vs. single row). Compared to slot blowing, jet vortex generators can provide an equivalent level of flow control over a larger spanwise region (for constant jet flow area and speed). Dye flow visualization tests in a water tunnel indicated that the most effective jet vortex generator configurations produced streamwise co-rotating vortices.

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

Lunden, Melissa M.; Delp, William W.

Effective exhaust hoods can mitigate the indoor air quality impacts of pollutant emissions from residential cooking. This study reports capture efficiencies (CE) measured for cooking generated particles for scripted cooking procedures in a 121-m3 chamber with kitchenette. CEs also were measured for burner produced CO2 during cooking and separately for pots and pans containing water. The study used four exhaust hoods previously tested by Delp and Singer (Environ. Sci. Technol., 2012, 46, 6167-6173). For pan-frying a hamburger over medium heat on the back burner, CEs for particles were similar to those for burner produced CO2 and mostly above 80percent. Formore » stir-frying green beans in a wok (high heat, front burner), CEs for burner CO2 during cooking varied by hood and airflow: CEs were 34-38percent for low (51?68 L s-1) and 54?72percent for high (109?138 L s-1) settings. CEs for 0.3?2.0 ?m particles during front burner stir-frying were 3?11percent on low and 16?70percent on high settings. Results indicate that CEs measured for burner CO2 are not predictive of CEs of cooking-generated particles under all conditions, but they may be suitable to identify devices with CEs above 80percent both for burner combustion products and for cooking-related particles.« less

Process boundaries of irreversible scCO2 -assisted phase separation in biphasic whole-cell biocatalysis.

PubMed

Brandenbusch, Christoph; Glonke, Sebastian; Collins, Jonathan; Hoffrogge, Raimund; Grunwald, Klaudia; Bühler, Bruno; Schmid, Andreas; Sadowski, Gabriele

2015-11-01

The formation of stable emulsions in biphasic biotransformations catalyzed by microbial cells turned out to be a major hurdle for industrial implementation. Recently, a cost-effective and efficient downstream processing approach, using supercritical carbon dioxide (scCO2 ) for both irreversible emulsion destabilization (enabling complete phase separation within minutes of emulsion treatment) and product purification via extraction has been proposed by Brandenbusch et al. (2010). One of the key factors for a further development and scale-up of the approach is the understanding of the mechanism underlying scCO2 -assisted phase separation. A systematic approach was applied within this work to investigate the various factors influencing phase separation during scCO2 treatment (that is pressure, exposure of the cells to CO2 , and changes of cell surface properties). It was shown that cell toxification and cell disrupture are not responsible for emulsion destabilization. Proteins from the aqueous phase partially adsorb to cells present at the aqueous-organic interface, causing hydrophobic cell surface characteristics, and thus contribute to emulsion stabilization. By investigating the change in cell-surface hydrophobicity of these cells during CO2 treatment, it was found that a combination of catastrophic phase inversion and desorption of proteins from the cell surface is responsible for irreversible scCO2 mediated phase separation. These findings are essential for the definition of process windows for scCO2 -assisted phase separation in biphasic whole-cell biocatalysis. © 2015 Wiley Periodicals, Inc.

Impact of tuning CO 2-philicity in polydimethylsiloxane-based membranes for carbon dioxide separation

DOE PAGES

Hong, Tao; Chatterjee, Sabornie; Mahurin, Shannon M.; ...

2017-02-22

Amidoxime-functionalized polydimethylsiloxane (AO-PDMSPNB) membranes with various amidoxime compositions were synthesized via ring-opening metathesis polymerization followed by post-polymerization modification. Compared to other previously reported PDMS-based membranes, the amidoxime-functionalized membranes show enhanced CO 2 permeability and CO 2/N 2 selectivity. The overall gas separation performance (CO 2 permeability 6800 Barrer; CO 2/N 2 selectivity 19) of the highest performing membrane exceeds the Robeson upper bound line, and the excellent permeability of the copolymer itself provides great potential for real world applications where huge volumes of gases are separated. This study details how tuning the CO 2-philicity within rubbery polymer matrices influences gasmore » transport properties. Key parameters for tuning gas transport properties are discussed, and the experimental results show good consistency with theoretical calculations. Finally, this study provides a roadmap to enhancing gas separation performance in rubbery polymers by tuning gas solubility selectivity.« less

Catalyst functionalized buffer sorbent pebbles for rapid separation of carbon dioxide from gas mixtures

DOEpatents

Aines, Roger D

2015-03-31

A method for separating CO.sub.2 from gas mixtures uses a slurried media impregnated with buffer compounds and coating the solid media with a catalyst or enzyme that promotes the transformation of CO.sub.2 to carbonic acid. Buffer sorbent pebbles with a catalyst or enzyme coating are provided for rapid separation of CO.sub.2 from gas mixtures.

Catalyst functionalized buffer sorbent pebbles for rapid separation of carbon dioxide from gas mixtures

DOEpatents

Aines, Roger D.

2013-03-12

A method for separating CO.sub.2 from gas mixtures uses a slurried media impregnated with buffer compounds and coating the solid media with a catalyst or enzyme that promotes the transformation of CO.sub.2 to carbonic acid. Buffer sorbent pebbles with a catalyst or enzyme coating are provided for rapid separation of CO.sub.2 from gas mixtures.

Computational Screening of MOFs for Acetylene Separation

NASA Astrophysics Data System (ADS)

Nemati Vesali Azar, Ayda; Keskin, Seda

2018-02-01

Efficient separation of acetylene (C2H2) from CO2 and CH4 is important to meet the requirement of high-purity acetylene in various industrial applications. Metal organic frameworks (MOFs) are great candidates for adsorption-based C2H2/CO2 and C2H2/CH4 separations due to their unique properties such as wide range of pore sizes and tunable chemistries. Experimental studies on the limited number of MOFs revealed that MOFs offer remarkable C2H2/CO2 and C2H2/CH4 selectivities based on single-component adsorption data. We performed the first large-scale molecular simulation study to investigate separation performances of 174 different MOF structures for C2H2/CO2 and C2H2/CH4 mixtures. Using the results of molecular simulations, several adsorbent performance evaluation metrics, such as selectivity, working capacity, adsorbent performance score, sorbent selection parameter and regenerability were computed for each MOF. Based on these metrics, the best adsorbent candidates were identified for both separations. Results showed that the top three most promising MOF adsorbents exhibit C2H2/CO2 selectivities of 49, 47, 24 and C2H2/CH4 selectivities of 824, 684, 638 at 1 bar, 298 K and these are the highest C2H2 selectivities reported to date in the literature. Structure-performance analysis revealed that the best MOF adsorbents have pore sizes between 4-11 Å, surface areas in the range of 600-1,200 m2/g and porosities between 0.4-0.6 for selective separation of C2H2 from CO2 and CH4. These results will guide the future studies for the design of new MOFs with high C2H2 separation potentials.

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

NASA Astrophysics Data System (ADS)

Gao, Wenyang

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

Electrochemical Membrane for Carbon Dioxide Capture and Power Generation

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

Ghezel-Ayagh, Hossein

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

Improved solar-driven photocatalytic performance of Ag{sub 2}CO{sub 3}/(BiO){sub 2}CO{sub 3} prepared in-situ

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

Zhong, Junbo, E-mail: junbozhong@163.com; Li, Jianzhang, E-mail: lschmanuscript@163.com; Huang, Shengtian

Highlights: • Ag{sub 2}CO{sub 3}/(BiO){sub 2}CO{sub 3} photocatalysts were prepared in-situ. • The photo-induced charge separation rate has been greatly increased. • The photocatalytic activity has been greatly promoted. - Abstract: Ag{sub 2}CO{sub 3}/(BiO){sub 2}CO{sub 3} composites have been fabricated in-situ via a facile parallel flaw co-precipitation method. The specific surface area, structure, morphology, and the separation rate of photo-induced charge pairs of the photocatalysts were characterized by Brunauer–Emmett–Teller (BET) method, X-ray diffraction (XRD), UV–vis diffuse reflectance spectroscopy(DRS), scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HRTEM), and surface photovoltage (SPV) spectroscopy, respectively. XRD patterns and DRS demonstrated that Ag{submore » 2}CO{sub 3} has no effect on the crystal phase and bandgap of (BiO){sub 2}CO{sub 3}. The existence of Ag{sub 2}CO{sub 3} in the composites enhances the separation rate of photo-induced charge pairs of the photocatalysts. The photocatalytic performance of Ag{sub 2}CO{sub 3}/(BiO){sub 2}CO{sub 3} was evaluated by the decolorization of methyl orange (MO) aqueous solution under simulated solar irradiation. It was found that the simulated solar-induced photocatalytic activity of Ag{sub 2}CO{sub 3}/(BiO){sub 2}CO{sub 3} copmposites was significantly improved, which was mainly attributed to the enhanced surface area and the separation rate of photo-induced charge pairs.« less

MEMBRANE PROCESS TO SEQUESTER CO2 FROM POWER PLANT FLUE GAS

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

Tim Merkel; Karl Amo; Richard Baker

2009-03-31

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

Synthesis and CO2/CH4 separation peformance of Bio-MOF-1 membranes

NASA Astrophysics Data System (ADS)

Bohrman, Joseph Allen

The separation of carbon dioxide from natural gas is of great interest from the environmental and energy perspective, respectively. From the environmental point of view, capturing CO2 effectively from power plants can have a positive impact on reducing greenhouse gas emissions. From the energy point of view, CO2 is an undesirable impurity in natural gas wells, with concentrations as high as 70%. Membrane technology can play a major role in making natural gas purification processes economically feasible. A novel membrane composed of Metal-organic-framework material Zn 8(Ad)4(BPDC)6O 2Me2NH2 (Bio-MOF-1) was designed and created to effectively separate CO2/CH4 gas mixtures. The crystalline structure, composition, and textural properties of Bio-MOF-1 membranes were confirmed through x-ray diffractometry, CHN analysis, transmission electron microscopy, adsorption measurements and BET surface area. A secondary seeded growth approach was employed to prepare these membranes on tubular stainless steel porous support. These membranes displayed high CO2 permeances (11.5x10-7 mol / m2 s Pa) and moderate CO2/CH4 separation selectivities (1.2--2.5). The observed selectivities are above the Knudsen selectivity and indicate that the separation is promoted by preferential CO2 adsorption over CH4. This preferential adsorption is attributed to the presence of adeninate amino basic sites present in the Bio-MOF-1 structure. The work demonstrated shows the feasibility of the development of a novel type of membrane that could be promising for diverse molecular gas separations.

Enhanced photocatalytic CO2 reduction to CH4 over separated dual co-catalysts Au and RuO2

NASA Astrophysics Data System (ADS)

Dong, Chunyang; Hu, Songchang; Xing, Mingyang; Zhang, Jinlong

2018-04-01

A spatially separated, dual co-catalyst photocatalytic system was constructed by the stepwise introduction of RuO2 and Au nanoparticles (NPs) at the internal and external surfaces of a three dimensional, hierarchically ordered TiO2-SiO2 (HTSO) framework (the final photocatalyst was denoted as Au/HRTSO). Characterization by HR-TEM, EDS-mapping, XRD and XPS confirmed the existence and spatially separated locations of Au and RuO2. In CO2 photocatalytic reduction (CO2PR), Au/HRTSO (0.8%) shows the optimal performance in both the activity and selectivity towards CH4; the CH4 yield is almost twice that of the singular Au/HTSO or HRTSO (0.8%, weight percentage of RuO2) counterparts. Generally, Au NPs at the external surface act as electron trapping agents and RuO2 NPs at the inner surface act as hole collectors. This advanced spatial configuration could promote charge separation and transfer efficiency, leading to enhanced CO2PR performance in both the yield and selectivity toward CH4 under simulated solar light irradiation.

CO.sub.2 separation from low-temperature flue gases

DOEpatents

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.

A single-ligand ultra-microporous MOF for precombustion CO2 capture and hydrogen purification

PubMed Central

Nandi, Shyamapada; De Luna, Phil; Daff, Thomas D.; Rother, Jens; Liu, Ming; Buchanan, William; Hawari, Ayman I.; Woo, Tom K.; Vaidhyanathan, Ramanathan

2015-01-01

Metal organic frameworks (MOFs) built from a single small ligand typically have high stability, are rigid, and have syntheses that are often simple and easily scalable. However, they are normally ultra-microporous and do not have large surface areas amenable to gas separation applications. We report an ultra-microporous (3.5 and 4.8 Å pores) Ni-(4-pyridylcarboxylate)2 with a cubic framework that exhibits exceptionally high CO2/H2 selectivities (285 for 20:80 and 230 for 40:60 mixtures at 10 bar, 40°C) and working capacities (3.95 mmol/g), making it suitable for hydrogen purification under typical precombustion CO2 capture conditions (1- to 10-bar pressure swing). It exhibits facile CO2 adsorption-desorption cycling and has CO2 self-diffusivities of ~3 × 10−9 m2/s, which is two orders higher than that of zeolite 13X and comparable to other top-performing MOFs for this application. Simulations reveal a high density of binding sites that allow for favorable CO2-CO2 interactions and large cooperative binding energies. Ultra-micropores generated by a small ligand ensures hydrolytic, hydrostatic stabilities, shelf life, and stability toward humid gas streams. PMID:26824055

The self-assembly structure and the CO2-philicity of a hybrid surfactant in supercritical CO2: effects of hydrocarbon chain length.

PubMed

Wang, Muhan; Fang, Timing; Wang, Pan; Tang, Xinpeng; Sun, Baojiang; Zhang, Jun; Liu, Bing

2016-10-04

Hybrid surfactants containing both fluorocarbon (FC) and hydrocarbon (HC) chains, as effective CO 2 -philic surfactants, could improve the solubility of polar substances in supercritical CO 2 . Varying the length of the HC of hybrid surfactants is an effective way to improve the CO 2 -philicity. In this paper, we have investigated the effects of the HC length on the self-assembly process and the CO 2 -philicity of hybrid surfactants (F7Hn, n = 1, 4, 7 and 10) in water/CO 2 mixtures using molecular dynamics simulations. It is found that the self-assembly time of F7Hn exhibits a maximum when the length of the HC is equal to that of the FC (F7H7). In this case, the investigation of H-bonds between the water core and CO 2 phase shows that F7H7 has the strongest CO 2 -philicity because it has the best ability to separate water and CO 2 . To explain the origin of the differences in separation ability, the analysis of the structures of the reverse micelles shows that there are two competing mechanisms with a shortening HC. Firstly, the volume of F7Hn is reduced, which thus decreases the separation ability. Moreover, this also leads to the curved conformation of the FC. As a result, the separation ability is enhanced. These two mechanisms are balanced in F7H7, which has the best ability to separate water and CO 2 . Our simulation results demonstrate that the increased volume and the curved conformation of the hybrid surfactant tail could enhance the CO 2 -philicity in F7Hn surfactants. It is expected that this work will provide valuable information for the design of CO 2 -philic surfactants.

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

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

Ghezel-Ayagh, Hossein

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

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

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

Ghezel-Ayagh, Hossein

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

Benzyl-Functionalized Room Temperature Ionic Liquids for CO2/N2 Separation

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

Mahurin, Shannon Mark; Dai, Thomas N; Yeary, Joshua S

2011-01-01

In this work, three classes of room temperature ionic liquids (RTILs), including imidazolium, pyridinium, and pyrrolidinium ionic liquids with a benzyl group appended to the cation, were synthesized and tested for their performance in separating CO{sub 2} and N{sub 2}. All RTILs contained the bis(trifluoromethylsulfonyl)imide anion, permitting us to distinguish the impact of the benzyl moiety attached to the cation on gas separation performance. In general, the attachment of the benzyl group increased the viscosity of the ionic liquid compared with the unfunctionalized analogs and decreased the CO{sub 2} permeability. However, all of the benzyl-modified ionic liquids exhibited enhanced CO{submore » 2}/N{sub 2} selectivities compared with alkyl-based ionic liquids, with values ranging from 22.0 to 33.1. In addition, CO{sub 2} solubilities in the form of Henry's constants were also measured and compared with unfunctionalized analogs. Results of the membrane performance tests and CO{sub 2} solubility measurements demonstrate that the benzyl-functionalized RTILs have significant potential for use in the separation of carbon dioxide from combustion products.« less

Cost and greenhouse gas emission tradeoffs of alternative uses of lignin for second generation ethanol

NASA Astrophysics Data System (ADS)

Pourhashem, Ghasideh; Adler, Paul R.; McAloon, Andrew J.; Spatari, Sabrina

2013-06-01

Second generation ethanol bioconversion technologies are under demonstration-scale development for the production of lignocellulosic fuels to meet the US federal Renewable Fuel Standards (RFS2). Bioconversion technology utilizes the fermentable sugars generated from the cellulosic fraction of the feedstock, and most commonly assumes that the lignin fraction may be used as a source of thermal and electrical energy. We examine the life cycle greenhouse gas (GHG) emission and techno-economic cost tradeoffs for alternative uses of the lignin fraction of agricultural residues (corn stover, and wheat and barley straw) produced within a 2000 dry metric ton per day ethanol biorefinery in three locations in the United States. We compare three scenarios in which the lignin is (1) used as a land amendment to replace soil organic carbon (SOC); (2) separated, dried and sold as a coal substitute to produce electricity; and (3) used to produce electricity onsite at the biorefinery. Results from this analysis indicate that for life cycle GHG intensity, amending the lignin to land is lowest among the three ethanol production options (-25 to -2 g CO2e MJ-1), substituting coal with lignin is second lowest (4-32 g CO2e MJ-1), and onsite power generation is highest (36-41 g CO2e MJ-1). Moreover, the onsite power generation case may not meet RFS2 cellulosic fuel requirements given the uncertainty in electricity substitution. Options that use lignin for energy do so at the expense of SOC loss. The lignin-land amendment option has the lowest capital cost among the three options due to lower equipment costs for the biorefinery’s thermal energy needs and use of biogas generated onsite. The need to purchase electricity and uncertain market value of the lignin-land amendment could raise its cost compared to onsite power generation and electricity co-production. However, assuming a market value (50-100/dry Mg) for nutrient and soil carbon replacement in agricultural soils, and potentially economy of scale residue collection prices at higher collection volumes associated with low SOC loss, the lignin-land amendment option is economically and environmentally preferable, with the lowest GHG abatement costs relative to gasoline among the three lignin co-product options we consider.

FTIR study of CO2 and H2O/CO2 nanoparticles and their temporal evolution at 80 K.

PubMed

Taraschewski, M; Cammenga, H K; Tuckermann, R; Bauerecker, S

2005-04-21

Fourier transform infrared (FTIR) spectroscopy combined with a long-path collisional cooling cell was used to investigate the temporal evolution of CO2 nanoparticles and binary H2O/CO2 nanocomposites in the aerosol phase at 80 K. The experimental conditions for the formation of different CO2 particle shapes as slab, shell, sphere, cube, and needle have been studied by comparison with calculated data from the literature. The H2O/CO2 nanoparticles were generated with a newly developed multiple-pulse injection technique and with the simpler flow-in technique. The carbon dioxide nu3-vibration band at 2360 cm(-1) and the water ice OH-dangling band at 3700 cm(-1) were used to study the evolution of structure, shape, and contact area of the nanocomposites over 150 s. Different stages of binary nanocomposites with primary water ice cores were identified dependent on the injected CO2 portion: (a) disordered (amorphous) CO2 slabs on water particle surfaces, (b) globular crystalline CO2 humps sticking on the water cores, and (c) water cores being completely enclosed in bigger predominantly crystalline CO2 nanoparticles. However, regular CO2 shell structures on primary water particles showing both longitudinal (LO) and transverse (TO) optical mode features of the nu3-vibration band could not be observed. Experiments with reversed nucleation order indicate that H2O/CO2 composite particles with different initial structures evolve toward similar molecular nanocomposites with separated CO2 and H2O regions.

CO2 adsorption using TiO2 composite polymeric membranes: A kinetic study.

PubMed

Hafeez, Sarah; Fan, X; Hussain, Arshad; Martín, C F

2015-09-01

CO2 is the main greenhouse gas which causes global climatic changes on larger scale. Many techniques have been utilised to capture CO2. Membrane gas separation is a fast growing CO2 capture technique, particularly gas separation by composite membranes. The separation of CO2 by a membrane is not just a process to physically sieve out of CO2 through the controlled membrane pore size. It mainly depends upon diffusion and solubility of gases, particularly for composite dense membranes. The blended components in composite membranes have a high capability to adsorb CO2. The adsorption kinetics of the gases may directly affect diffusion and solubility. In this study, we have investigated the adsorption behaviour of CO2 in pure and composite membranes to explore the complete understanding of diffusion and solubility of CO2 through membranes. Pure cellulose acetate (CA) and cellulose acetate-titania nanoparticle (CA-TiO2) composite membranes were fabricated and characterised using SEM and FTIR analysis. The results indicated that the blended CA-TiO2 membrane adsorbed more quantity of CO2 gas as compared to pure CA membrane. The high CO2 adsorption capacity may enhance the diffusion and solubility of CO2 in the CA-TiO2 composite membrane, which results in a better CO2 separation. The experimental data was modelled by Pseudo first-order, pseudo second order and intra particle diffusion models. According to correlation factor R(2), the Pseudo second order model was fitted well with experimental data. The intra particle diffusion model revealed that adsorption in dense membranes was not solely consisting of intra particle diffusion. Copyright © 2015. Published by Elsevier B.V.

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

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

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

Biogas and methane yield in response to co- and separate digestion of biomass wastes.

PubMed

Adelard, Laetitia; Poulsen, Tjalfe G; Rakotoniaina, Volana

2015-01-01

The impact of co-digestion as opposed to separate digestion, on biogas and methane yield (apparent synergetic effects) was investigated for three biomass materials (pig manure, cow manure and food waste) under mesophilic conditions over a 36 day period. In addition to the three biomass materials (digested separately), 13 biomass mixtures (co-digested) were used. Two approaches for modelling biogas and methane yield during co-digestion, based on volatile solids concentration and ultimate gas and methane potentials, were evaluated. The dependency of apparent synergetic effects on digestion time and biomass mixture composition was further assessed using measured cumulative biogas and methane yields and specific biogas and methane generation rates. Results indicated that it is possible, based on known volatile solids concentration and ultimate biogas or methane yields for a set of biomass materials digested separately, to accurately estimate gas yields for biomass mixtures made from these materials using calibrated models. For the biomass materials considered here, modelling indicated that the addition of pig manure is the main cause of synergetic effects. Co-digestion generally resulted in improved ultimate biogas and methane yields compared to separate digestion. Biogas and methane production was furthermore significantly higher early (0-7 days) and to some degree also late (above 20 days) in the digestion process during co-digestion. © The Author(s) 2014.

High Water Tolerance of a Core-Shell-Structured Zeolite for CO2 Adsorptive Separation under Wet Conditions.

PubMed

Miyamoto, Manabu; Ono, Shumpei; Kusukami, Kodai; Oumi, Yasunori; Uemiya, Shigeyuki

2018-06-11

Dehumidification in CO 2 adsorptive separation processes is an important issue, owing to its high energy consumption. However, available adsorbents such as low-silica zeolites show a significant decrease in CO 2 adsorption capacity when water vapor is present. A core-shell-structured MFI-type zeolite with a hydrophilic ZSM-5 coated with a hydrophobic silicalite-1 shell layer was applied in CO 2 adsorptive separation under wet conditions. This hybrid material demonstrated remarkably high water tolerance with stable CO 2 adsorption performance without additional thermal treatment for regeneration, whereas a significant decrease in the CO 2 adsorption amount because of water vapor was observed on the parent ZSM-5. The core-shell structure of zeolites with high pore volumes, such as LTA or CHA, could also be suitable candidates for high CO 2 adsorption capacity and high water tolerance for practical applications. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Polyamidoamine dendrimers as sweeping agent and stationary phase for rapid and sensitive open-tubular capillary electrophoretic determination of heavy metal ions.

PubMed

Ge, Ying; Guo, Yujun; Qin, Weidong

2014-04-01

Polyamidoamine (PAMAM) dendrimer generation 2.5 was synthesized and evaluated as sweeping agent for in-column enrichment and as stationary phase for capillary electrochromatographic separation of heavy metal ions, viz., Pb(II), Cu(II), Hg(II), Zn(II) and Co(II), in a running buffer containing 4-(2-pyridylazo)resorcinol (PAR) as a chromogenic reagent. During experiment, a plug of aqueous PAMAM generation 2.5 solution was first introduced to the capillary, followed by electrokinetic injection of the heavy metal ions under a positive voltage. In this step, PAMAM acted as a sweeping agent, stacking the metal ions on the analyte/PAMAM boundary by forming metal ion-PAMAM complexes. The second preconcentration process occurred when PAR, a stronger ligand, moving toward the injection end under the electric field, reached and re-swept the metal ion-PAMAM zone, forming metal ion-PAR complexes. During separation, the neutral PAMAM moved toward the detector with the electroosmotic flow, dynamically coating the capillary wall, forming stationary phases that affected the separation of the metal ions. Due to the function of PAMAM, the detection sensitivity and resolution of the heavy metal ions improved significantly. Under the optimum conditions, the detection limits were 0.299, 0.184, 0.774, 0.182 and 0.047 μg/L for Pb(II), Cu(II), Hg(II), Zn(II) and Co(II), respectively. The method was successfully applied to the determination of heavy metals in snow, tap and rain water samples. Copyright © 2013 Elsevier B.V. All rights reserved.

Comparison on pore development of activated carbon produced by chemical and physical activation from palm empty fruit bunch

NASA Astrophysics Data System (ADS)

Hidayat, A.; Sutrisno, B.

2016-11-01

It is well-known that activated carbon is considered to be the general adsorbent due to the large range of applications. Numerous works are being continuously published concerning its use as adsorbent for: treatment of potable water; purification of air; retention of toxins by respirators; removal of organic and inorganic pollutants from flue gases and industrial waste gases and water; recuperation of solvents and hydrocarbons volatilized from petroleum derivatives; catalysis; separation of gas mixtures (molecularsieve activated carbons); storage of natural gas and hydrogen; energy storage in supercapacitors; recovery of gold, silver and othernoble metals; etc. This work presents producing activated carbons from palm empty fruit bunch using both physical activation with CO2 and chemical activation with KOH. The resultant activated carbons were characterized by measuring their porosities and pore size distributions. A comparison of the textural characteristics and surface chemistry of the activated carbon from palm empty fruit bunch by the CO2 and the KOH activation leads to the following findings: An activated carbon by the CO2 activation under the optimum conditions has a BET surface area of 717 m2/g, while that by the KOH activation has a BET surface area of 613 m2/g. The CO2 activation generated a highly microporous carbon (92%) with a Type-I isotherm, while the KOH activation generated a mesoporous one (70%) with a type-IV isotherm, the pore volumes are 0.2135 and 0.7426 cm3.g-1 respectively. The average pore size of the activated carbons is 2.72 and 2.56 nm for KOH activation and CO2 activation, respectively. The FT-IR spectra indicated significant variation in the surface functional groups are quite different for the KOH activated and CO2 activated carbons.

Reduction-melting combined with a Na₂CO₃ flux recycling process for lead recovery from cathode ray tube funnel glass.

PubMed

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.

Ionic-Liquid-Based CO2 Capture Systems: Structure, Interaction and Process.

PubMed

Zeng, Shaojuan; Zhang, Xiangping; Bai, Lu; Zhang, Xiaochun; Wang, Hui; Wang, Jianji; Bao, Di; Li, Mengdie; Liu, Xinyan; Zhang, Suojiang

2017-07-26

The inherent structure tunability, good affinity with CO 2 , and nonvolatility of ionic liquids (ILs) drive their exploration and exploitation in CO 2 separation field, and has attracted remarkable interest from both industries and academia. The aim of this Review is to give a detailed overview on the recent advances on IL-based materials, including pure ILs, IL-based solvents, and IL-based membranes for CO 2 capture and separation from the viewpoint of molecule to engineering. The effects of anions, cations and functional groups on CO 2 solubility and selectivity of ILs, as well as the studies on degradability of ILs are reviewed, and the recent developments on functionalized ILs, IL-based solvents, and IL-based membranes are also discussed. CO 2 separation mechanism with IL-based solvents and IL-based membranes are explained by combining molecular simulation and experimental characterization. Taking into consideration of the applications and industrialization, the recent achievements and developments on the transport properties of IL fluids and the process design of IL-based processes are highlighted. Finally, the future research challenges and perspectives of the commercialization of CO 2 capture and separation with IL-based materials are posed.

CO2 Acquisition Membrane (CAM) Project

NASA Technical Reports Server (NTRS)

Mason, Larry W.

2003-01-01

The CO2 Acquisition Membrane (CAM) project was performed to develop, test, and analyze thin film membrane materials for separation and purification of carbon dioxide (CO2) from mixtures of gases, such as those found in the Martian atmosphere. The membranes developed in this project are targeted toward In Situ Resource Utilization (ISRU) applications, such as In Situ Propellant Production (ISPP) and In Situ Consumables Production (ISCP). These membrane materials may be used in a variety of ISRU systems, for example as the atmospheric inlet filter for an ISPP process to enhance the concentration of CO2 for use as a reactant gas, to passively separate argon and nitrogen trace gases from CO2 for habitat pressurization, to provide a system for removal of CO2 from breathing gases in a closed environment, or within a process stream to selectively separate CO2 from other gaseous components. The membranes identified and developed for CAM were evaluated for use in candidate ISRU processes and other gas separation applications, and will help to lay the foundation for future unmanned sample return and human space missions. CAM is a cooperative project split among three institutions: Lockheed Martin Astronautics (LMA), the Colorado School of Mines (CSM), and Marshall Space Flight Center (MSFC).

Extraction and separation of Co(II) and Ni(II) from acidic sulfate solutions using Aliquat 336.

PubMed

Nayl, A A

2010-01-15

Extraction and separation of Co(II) and Ni(II) from acidic sulfate solutions by solvent extraction technique were studied using different forms of Aliquat 336 diluted with kerosene. The extraction percent of each metal ion was found to increase with increasing pH and extractant concentration. Co(II) was preferentially extracted by different forms of Aliquat 336 over Ni(II) under the same extraction conditions. From analysis of the experimental results, the extraction mechanism of R(4)N-forms was proposed with Co(II). It was found that the highest separation factor (S(Co/Ni)) value of 606.7 was obtained with 0.36 M R(4)N-SCN in kerosene from 2.0M H(2)SO(4) solution at pH 4.8 and shaking time of 20 min. Stripping of the two metal ions from the organic phase was also investigated. Based on the experimental results, a separation method was developed and tested to separate high purity Co(II), Ni(II) and Ln(III) from Ni-MH batteries leached by 2.0M H(2)SO(4). Based on the experimental results, a flow sheet was developed and tested and 0.34 g Co, 1.39 g Ln and 5.2g Ni were obtained from the leaching process.

Mars Atmospheric Chemistry in Electrified Dust Devils and Storms

NASA Technical Reports Server (NTRS)

Farrell, W. M.; Delory, G. T.; Atreya, S. K.; Wong, A.-S.; Renno, N. O.; Sentmann, D. D.; Marshall, J. G.; Cummer, S. A.; Rafkin, S.; Catling, D.

2005-01-01

Laboratory studies, simulations and desert field tests all indicate that aeolian mixing dust can generate electricity via contact electrification or "triboelectricity". In convective structures like dust devils or storms, grain stratification (or charge separation) occurs giving rise to an overall electric dipole moment to the aeolian feature, similar in nature to the dipolar electric field generated in terrestrial thunderstorms. Previous simulation studies [1] indicate that this storm electric field on Mars can approach atmospheric breakdown field strength of 20 kV/m. In terrestrial dust devils, coherent dipolar electric fields exceeding 20 kV/m have been measured directly via electric field instrumentation. Given the expected electrostatic fields in Martian dust devils and storms, electrons in the low pressure CO2 gas can be energized via the electric field to values exceeding the electron dissociative attachment energy of both CO2 and H2O, resulting in the formation of new chemical products CO and O- and OH and H- within the storm. Using a collisional plasma physics model we present a calculation of the CO/O- and OH/H- reaction and production rates. We demonstrate that these rates vary geometrically with ambient electric field, with substantial production of dissociative products when fields approach breakdown levels of 20-30 kV/m.

Double heterojunction nanowire photocatalysts for hydrogen generation.

PubMed

Tongying, P; Vietmeyer, F; Aleksiuk, D; Ferraudi, G J; Krylova, G; Kuno, M

2014-04-21

Charge separation and charge transfer across interfaces are key aspects in the design of efficient photocatalysts for solar energy conversion. In this study, we investigate the hydrogen generating capabilities and underlying photophysics of nanostructured photocatalysts based on CdSe nanowires (NWs). Systems studied include CdSe, CdSe/CdS core/shell nanowires and their Pt nanoparticle-decorated counterparts. Femtosecond transient differential absorption measurements reveal how semiconductor/semiconductor and metal/semiconductor heterojunctions affect the charge separation and hydrogen generation efficiencies of these hybrid photocatalysts. In turn, we unravel the role of surface passivation, charge separation at semiconductor interfaces and charge transfer to metal co-catalysts in determining photocatalytic H2 generation efficiencies. This allows us to rationalize why Pt nanoparticle decorated CdSe/CdS NWs, a double heterojunction system, performs best with H2 generation rates of ∼434.29 ± 27.40 μmol h(-1) g(-1) under UV/Visible irradiation. In particular, we conclude that the CdS shell of this double heterojunction system serves two purposes. The first is to passivate CdSe NW surface defects, leading to long-lived charges at the CdSe/CdS interface capable of carrying out reduction chemistries. Upon photoexcitation, we also find that CdS selectively injects charges into Pt NPs, enabling simultaneous reduction chemistries at the Pt NP/solvent interface. Pt nanoparticle decorated CdSe/CdS NWs thus enable reduction chemistries at not one, but rather two interfaces, taking advantage of each junction's optimal catalytic activities.

Process for analyzing CO.sub.2 in seawater

DOEpatents

Atwater, James E.; Akse, James R.; DeHart, Jeffrey

1997-01-01

The process of this invention comprises providing a membrane for separating CO.sub.2 into a first CO.sub.2 sample phase and a second CO.sub.2 analyte phase. CO.sub.2 is then transported through the membrane thereby separating the CO.sub.2 with the membrane into a first CO.sub.2 sample phase and a second CO.sub.2 analyte liquid phase including an ionized, conductive, dissociated CO.sub.2 species. Next, the concentration of the ionized, conductive, dissociated CO.sub.2 species in the second CO.sub.2 analyte liquid phase is chemically amplified using a water-soluble chemical reagent which reversibly reacts with undissociated CO.sub.2 to produce conductivity changes therein corresponding to fluctuations in the partial pressure of CO.sub.2 in the first CO.sub.2 sample phase. Finally, the chemically amplified, ionized, conductive, dissociated CO.sub.2 species is introduced to a conductivity measuring instrument. Conductivity changes in the chemically amplified, ionized, conductive, dissociated CO.sub.2 species are detected using the conductivity measuring instrument.

Microporous metal organic framework [M2(hfipbb)2(ted)] (M=Zn, Co; H2hfipbb=4,4-(hexafluoroisopropylidene)-bis(benzoic acid); ted=triethylenediamine): Synthesis, structure analysis, pore characterization, small gas adsorption and CO2/N2 separation properties

NASA Astrophysics Data System (ADS)

Xu, William W.; Pramanik, Sanhita; Zhang, Zhijuan; Emge, Thomas J.; Li, Jing

2013-04-01

Carbon dioxide is a greenhouse gas that is a major contributor to global warming. Developing methods that can effectively capture CO2 is the key to reduce its emission to the atmosphere. Recent research shows that microporous metal organic frameworks (MOFs) are emerging as a promising family of adsorbents that may be promising for use in adsorption based capture and separation of CO2 from power plant waste gases. In this work we report the synthesis, crystal structure analysis and pore characterization of two microporous MOF structures, [M2(hfipbb)2(ted)] (M=Zn (1), Co (2); H2hfipbb=4,4-(hexafluoroisopropylidene)-bis(benzoic acid); ted=triethylenediamine). The CO2 and N2 adsorption experiments and IAST calculations are carried out on [Zn2(hfipbb)2(ted)] under conditions that mimic post-combustion flue gas mixtures emitted from power plants. The results show that the framework interacts with CO2 strongly, giving rise to relatively high isosteric heats of adsorption (up to 28 kJ/mol), and high adsorption selectivity for CO2 over N2, making it promising for capturing and separating CO2 from CO2/N2 mixtures.

Nanophase-separated Ni3Nb as an automobile exhaust catalyst.

PubMed

Tanabe, Toyokazu; Imai, Tsubasa; Tokunaga, Tomoharu; Arai, Shigeo; Yamamoto, Yuta; Ueda, Shigenori; Ramesh, Gubbala V; Nagao, Satoshi; Hirata, Hirohito; Matsumoto, Shin-Ichi; Fujita, Takeshi; Abe, Hideki

2017-05-01

Catalytic remediation of automobile exhaust has relied on precious metals (PMs) including platinum (Pt). Herein, we report that an intermetallic phase of Ni and niobium (Nb) ( i.e. , Ni 3 Nb) exhibits a significantly higher activity than that of Pt for the remediation of the most toxic gas in exhaust ( i.e. , nitrogen monoxide (NO)) in the presence of carbon monoxide (CO). When subjected to the exhaust-remediation atmosphere, Ni 3 Nb spontaneously evolves into a catalytically active nanophase-separated structure consisting of filamentous Ni networks (thickness < 10 nm) that are incorporated in a niobium oxide matrix ( i.e. , NbO x ( x < 5/2)). The exposure of the filamentous Ni promotes NO dissociation, CO oxidation and N 2 generation, and the NbO x matrix absorbs excessive nitrogen adatoms to retain the active Ni 0 sites at the metal/oxide interface. Furthermore, the NbO x matrix immobilizes the filamentous Ni at elevated temperatures to produce long-term and stable catalytic performance over hundreds of hours.

Separation of Ni and Co by D2EHPA in the Presence of Citrate Ion

NASA Astrophysics Data System (ADS)

Nadimi, Hamed; Haghshenas Fatmehsari, Davoud; Firoozi, Sadegh

2017-10-01

Recycling processes for the recovery of metallic content from the electronic wastes are environmentally friendly and economical. This paper reports a method for the recovery and separation of Ni and Co from the sulfate solution by the use of D2EHPA. In this regard, the influence of citrate ion, as a carboxylate ligand, was examined in the separation conditions of Ni and Co via D2EHPA (a poor selective extractant for Ni and Co separation). It was found that the Δ {pH}_{0.5}^{Ni-Co} (the difference between pH values corresponding to 50 pct extraction of metallic ion) increases to 1.5 at the citrate concentration of 0.05 M; this Δ {pH}_{0.5}^{Ni-Co} value is much higher than that obtained in the absence of citrate ion (0.1). Fourier Transform Infrared Spectroscopy (FT-IR) indicated that the citrate ion is co-absorbed during the metallic ions absorption by D2EHPA meaning that the metal-organic complexes contain Co/Ni and citrate ion. Also, the stoichiometric coefficients of the Ni and Co extraction reaction were proposed by applying the slope analysis method.

Computational Screening of MOFs for Acetylene Separation

PubMed Central

Nemati Vesali Azar, Ayda; Keskin, Seda

2018-01-01

Efficient separation of acetylene (C2H2) from CO2 and CH4 is important to meet the requirement of high-purity acetylene in various industrial applications. Metal organic frameworks (MOFs) are great candidates for adsorption-based C2H2/CO2 and C2H2/CH4 separations due to their unique properties such as wide range of pore sizes and tunable chemistries. Experimental studies on the limited number of MOFs revealed that MOFs offer remarkable C2H2/CO2 and C2H2/CH4 selectivities based on single-component adsorption data. We performed the first large-scale molecular simulation study to investigate separation performances of 174 different MOF structures for C2H2/CO2 and C2H2/CH4 mixtures. Using the results of molecular simulations, several adsorbent performance evaluation metrics, such as selectivity, working capacity, adsorbent performance score, sorbent selection parameter, and regenerability were computed for each MOF. Based on these metrics, the best adsorbent candidates were identified for both separations. Results showed that the top three most promising MOF adsorbents exhibit C2H2/CO2 selectivities of 49, 47, 24 and C2H2/CH4 selectivities of 824, 684, 638 at 1 bar, 298 K and these are the highest C2H2 selectivities reported to date in the literature. Structure-performance analysis revealed that the best MOF adsorbents have pore sizes between 4 and 11 Å, surface areas in the range of 600–1,200 m2/g and porosities between 0.4 and 0.6 for selective separation of C2H2 from CO2 and CH4. These results will guide the future studies for the design of new MOFs with high C2H2 separation potentials. PMID:29536004

[Extraction of 10-Deacetyl Baccatin by Supercritical CO2 from Taxus yunnanensis Branches and Leaves].

PubMed

Tang, Yang-qin; Li, Hai-chi; Huang, Wen-jie; Xiong, Yan; Ge, Fa-huan

2015-04-01

To study the supercritical CO2 fluids extraction (SFE) method to extract the components from Taxus yunnanensis. Medicinal meterials were extracted by supercritical CO2, and then purified by industrial chromatography. Using the extraction yield of 10-DAB as the index,single factor test was carried out to investigate the effect of co-solvent, extraction time, extraction pressure, extraction temperature, pressure and temperature of separation kettle I. Then orthogonal experiment was used to optimize the best extraction condition. The suitable extraction condition was as follows: the ratio of co-solvent (80% ethanol) amount and the madicinal materials was 3: 1, Separation kettle I pressure was 14 MPa, separation kettle I temperature was 40 °C, extraction pressure was 25 MPa, extraction temperature was 60 T and extraction time was 90 min. The extract was separated by industrial chromatographic and then crystallized. The supercritical CO2 extraction and purification process of 10-DAB were simple and feasible.

A strain-controlled C2N monolayer membrane for gas separation in PEMFC application

NASA Astrophysics Data System (ADS)

Deng, Shengwei; Hu, Hui; Zhuang, Guilin; Zhong, Xing; Wang, Jianguo

2018-05-01

Ultrathin membranes with controllable pore sizes have great potential to realize high-selectivity gas separation at low energy cost, especially for those mixtures with narrow size distributions. Using a combination of van der Waals-corrected density functional theory (DFT) calculations and molecular dynamics (MD) simulation, we examine the separation ability of biaxial stretched monolayer C2N nanosheets which is applied to the O2 separation from CO/CO2/O2 mixtures in the cathode of proton exchange membrane fuel cells (PEMFC). The DFT calculations show that the diffusion energy barrier for molecules passing through the membrane followed by CO, CO2 and O2 in descending order, and an overall decrease of energy barriers due to the widen the pore size is observed with the increase of applied strains. Furthermore, MD results show that the nanosheet can effectively purify O2 from CO2 and CO with a strain from 8% to 10%. It confirms that the selectivity is determined by the electronic structure related interaction in addition to the kinetic diameter of individual molecules. The O2 permeability is improved progressively with further increase of strain, and small amount of CO2 begins to permeate through the nanosheet at relatively large strain, while the excellent CO isolation is not compromised until the theoretical maximum strain.

Metal-Organic Framework Photosensitized TiO2 Co-catalyst: A Facile Strategy to Achieve a High Efficiency Photocatalytic System.

PubMed

Xie, Ming-Hua; Shao, Rong; Xi, Xin-Guo; Hou, Gui-Hua; Guan, Rong-Feng; Dong, Peng-Yu; Zhang, Qin-Fang; Yang, Xiu-Li

2017-03-17

A 3D metal-organic framework (ADA-Cd=[Cd 2 L 2 (DMF) 2 ]⋅3 H 2 O where H 2 L is (2E,2'E)-3,3'-(anthracene-9,10-diyl)diacrylic acid) constructed from diacrylate substituted anthracene, sharing structural characteristics with some frequently employed anthraquinone-type dye sensitizers, was introduced as an effective sensitizer for anatase TiO 2 to achieve enhanced visible light photocatalytic performance. A facile mechanical mixing procedure was adopted to prepare the co-catalyst denoted as ADA-Cd/TiO 2 , which showed enhanced photodegradation ability, as well as sustainability, towards several dyes under visible light irradiation. Mechanistic studies revealed that ADA-Cd acted as the antenna to harvest visible light energy, generating excited electrons, which were injected to the conduction band (CB) of TiO 2 , facilitating the separation efficiency of charge carriers. As suggested by the results of control experiments, combined with the corresponding redox potential of possible oxidative species, . O 2 - , generated from the oxygen of ambient air at the CB of TiO 2 was believed to play a dominant role over . OH and h + . UV/Vis and photoluminescence technologies were adopted to monitor the generation of . O 2 - and . OH, respectively. This work presents a facile strategy to achieve a visible light photocatalyst with enhanced catalytic activity and sustainability; the simplicity, efficiency, and stability of this strategy may provide a promising way to achieve environmental remediation. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Probe Into the Influence of Crosslinking on CO2 Permeation of Membranes

PubMed Central

Li, Jinghui; Chen, Zhuo; Umar, Ahmad; Liu, Yang; Shang, Ying; Zhang, Xiaokai; Wang, Yao

2017-01-01

Crosslinking is an effective way to fabricate high-selective CO2 separation membranes because of its unique crosslinking framework. Thus, it is essentially significant to study the influence of crosslinking degree on the permeation selectivities of CO2. Herein, we report a successful and facile synthesis of a series of polyethylene oxide (PEO)-based diblock copolymers (BCP) incorporated with an unique UV-crosslinkable chalcone unit using Reversible Addition-Fragmentation Chain Transfer Polymerization (RAFT) process. The membranes of as-prepared BCPs show superior carbon dioxide (CO2) separation properties as compared to nitrogen (N2) after UV-crosslinking. Importantly, the influence of different proportions of crosslinked chalcone on CO2 selectivities was systematically investigated, which revealed that CO2 selectivities increased obviously with the enhancement of chalcone fractions within a certain limit. Further, the CO2 selectivities of block copolymer with the best block proportion was studied by varying the crosslinking time which confirmed that the high crosslinking degree exhibited a better CO2/N2 (αCO2/N2) selectivities. A possible mechanism model revealing that the crosslinking degree played a key role in the gas separation process was also proposed. PMID:28051190

Probe Into the Influence of Crosslinking on CO2 Permeation of Membranes

NASA Astrophysics Data System (ADS)

Li, Jinghui; Chen, Zhuo; Umar, Ahmad; Liu, Yang; Shang, Ying; Zhang, Xiaokai; Wang, Yao

2017-01-01

Crosslinking is an effective way to fabricate high-selective CO2 separation membranes because of its unique crosslinking framework. Thus, it is essentially significant to study the influence of crosslinking degree on the permeation selectivities of CO2. Herein, we report a successful and facile synthesis of a series of polyethylene oxide (PEO)-based diblock copolymers (BCP) incorporated with an unique UV-crosslinkable chalcone unit using Reversible Addition-Fragmentation Chain Transfer Polymerization (RAFT) process. The membranes of as-prepared BCPs show superior carbon dioxide (CO2) separation properties as compared to nitrogen (N2) after UV-crosslinking. Importantly, the influence of different proportions of crosslinked chalcone on CO2 selectivities was systematically investigated, which revealed that CO2 selectivities increased obviously with the enhancement of chalcone fractions within a certain limit. Further, the CO2 selectivities of block copolymer with the best block proportion was studied by varying the crosslinking time which confirmed that the high crosslinking degree exhibited a better CO2/N2 (αCO2/N2) selectivities. A possible mechanism model revealing that the crosslinking degree played a key role in the gas separation process was also proposed.

Potential flue gas impurities in carbon dioxide streams separated from coal-fired power plants.

PubMed

Lee, Joo-Youp; Keener, Tim C; Yang, Y Jeffery

2009-06-01

For geological sequestration of carbon dioxide (CO2) separated from pulverized coal combustion flue gas, it is necessary to adequately evaluate the potential impacts of flue gas impurities on groundwater aquifers in the case of the CO2 leakage from its storage sites. This study estimated the flue gas impurities to be included in the CO2 stream separated from a CO2 control unit for a different combination of air pollution control devices and different flue gas compositions. Specifically, the levels of acid gases and mercury vapor were estimated for the monoethanolamine (MEA)-based absorption process on the basis of published performance parameters of existing systems. Among the flue gas constituents considered, sulfur dioxide (SO2) is known to have the most adverse impact on MEA absorption. When a flue gas contains 3000 parts per million by volume (ppmv) SO2 and a wet flue gas desulfurization system achieves its 95% removal, approximately 2400 parts per million by weight (ppmw) SO2 could be included in the separated CO2 stream. In addition, the estimated concentration level was reduced to as low as 135 ppmw for the SO2 of less than 10 ppmv in the flue gas entering the MEA unit. Furthermore, heat-stable salt formation could further reduce the SO2 concentration below 40 ppmw in the separated CO2 stream. In this study, it is realized that the formation rates of heat-stable salts in MEA solution are not readily available in the literature and are critical to estimating the levels and compositions of flue gas impurities in sequestered CO2 streams. In addition to SO2, mercury, and other impurities in separated CO2 streams could vary depending on pollutant removal at the power plants and impose potential impacts on groundwater. Such a variation and related process control in the upstream management of carbon separation have implications for groundwater protection at carbon sequestration sites and warrant necessary considerations in overall sequestration planning, engineering, and management.

Integration of Bromine and Cyanogen Bromide Generators for the Continuous-Flow Synthesis of Cyclic Guanidines.

PubMed

Glotz, Gabriel; Lebl, René; Dallinger, Doris; Kappe, C Oliver

2017-10-23

A continuous-flow process for the in situ on-demand generation of cyanogen bromide (BrCN) from bromine and potassium cyanide that makes use of membrane-separation technology is described. In order to circumvent the handling, storage, and transportation of elemental bromine, a continuous bromine generator using bromate-bromide synproportionation can optionally be attached upstream. Monitoring and quantification of BrCN generation was enabled through the implementation of in-line FTIR technology. With the Br 2 and BrCN generators connected in series, 0.2 mmol BrCN per minute was produced, which corresponds to a 0.8 m solution of BrCN in dichloromethane. The modular Br 2 /BrCN generator was employed for the synthesis of a diverse set of biologically relevant five- and six-membered cyclic amidines and guanidines. The set-up can either be operated in a fully integrated continuous format or, where reactive crystallization is beneficial, in semi-batch mode. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Metal-Organic Framework (MOF) Compounds: Photocatalysts for Redox Reactions and Solar Fuel Production.

PubMed

Dhakshinamoorthy, Amarajothi; Asiri, Abdullah M; García, Hermenegildo

2016-04-25

Metal-organic frameworks (MOFs) are crystalline porous materials formed from bi- or multipodal organic linkers and transition-metal nodes. Some MOFs have high structural stability, combined with large flexibility in design and post-synthetic modification. MOFs can be photoresponsive through light absorption by the organic linker or the metal oxide nodes. Photoexcitation of the light absorbing units in MOFs often generates a ligand-to-metal charge-separation state that can result in photocatalytic activity. In this Review we discuss the advantages and uniqueness that MOFs offer in photocatalysis. We present the best practices to determine photocatalytic activity in MOFs and for the deposition of co-catalysts. In particular we give examples showing the photocatalytic activity of MOFs in H2 evolution, CO2 reduction, photooxygenation, and photoreduction. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

A novel Zn-based heterocycle metal-organic framework for high C2H2/C2H4, CO2/CH4 and CO2/N2 separations

NASA Astrophysics Data System (ADS)

Zhang, Ling; Jiang, Ke; Yang, Yu; Cui, Yuanjing; Chen, Banglin; Qian, Guodong

2017-11-01

Efficient separation of the small gas molecules especially the hydrocarbons is essential to social economy. The microporous metal-organic frameworks (MOFs) are taking precedence in this respect by virtue of their irreplaceable advantages. Herein, the new organic linker 5-(5-carboxypyridin-3-yl)isophthalic acid simplified as H3L-N has been excavated to construct successfully the novel Zn-based heterocycle metal-organic framework ZnL·(DMF)1.5·(H2O)6.0 (ZJU-197, ZJU = Zhejiang University, DMF = N,N-dimethylformamide). ZJU-197 has been structurally characterized and explored in details for gas separation. It is commendable that the activated ZJU-197a has exhibited excellent C2H2/C2H4, CO2/CH4 and CO2/N2 separations simultaneously with IAST selectivity of 137.8, 53.0 and 514.1 respectively at ambient conditions.

Numerical solution of Boltzmann tranport equation for TEA CO 2 laser having nitrogen-lean gas mixtures to predict laser characteristics and gas lifetime

NASA Astrophysics Data System (ADS)

Kumar, Manoj; Khare, Jai; Nath, A. K.

2007-02-01

Selective laser isotope separation by TEA CO 2 laser often needs short tail-free pulses. Using laser mixtures having very little nitrogen almost tail free laser pulses can be generated. The laser pulse characteristics and its gas lifetime is an important issue for long-term laser operation. Boltzmann transport equation is therefore solved numerically for TEA CO 2 laser gas mixtures having very little nitrogen to predict electron energy distribution function (EEDF). The distribution function is used to calculate various excitation and dissociation rate of CO 2 to predict laser pulse characteristics and laser gas lifetime, respectively. Laser rate equations have been solved with the calculated excitation rates for numerically evaluated discharge current and voltage profiles to calculate laser pulse shape. The calculated laser pulse shape and duration are in good agreement with the measured laser characteristics. The gas lifetime is estimated by integrating the equation governing the dissociation of CO 2. An experimental study of gas lifetime was carried out using quadrapole mass analyzer for such mixtures to estimate the O 2 being produced due to dissociation of CO 2 in the pulse discharge. The theoretically calculated O 2 concentration in the laser gas mixture matches with experimentally observed value. In the present TEA CO 2 laser system, for stable discharge the O 2 concentration should be below 0.2%.

Hybrid air revitalization system for a closed ecosystem

NASA Technical Reports Server (NTRS)

Lee, M. G.; Brown, Mariann F.

1990-01-01

An air-revitalization concept is presented with experimental results to assess the practicality and applicability of the proposed system to extended-duration manned missions. The Hybrid Air Revitalization System (HARS) uses plants in a habitat to remove metabolic CO2 and moisture and produce oxygen and food. CO2 and O2 partial pressures, temperature, and humidity are regulated by means of electrochemical CO2 and O2 chemical separators and a moisture condenser separator. A cell-test facility is described in which the electrochemical CO2 removal processes are investigated with and without using H2. Performance is optimized by using 25-30 percent Teflon in the gas-diffusion-type electrode, employing a thin electrolyte matrix, operating at higher temperatures and lower dew points. The HARS concept is found to be a feasible approach to the electrochemical separation of CO2 and O2.

Effect of amine structure on CO2 capture by polymeric membranes.

PubMed

Taniguchi, Ikuo; Kinugasa, Kae; Toyoda, Mariko; Minezaki, Koki

2017-01-01

Poly(amidoamine)s (PAMAMs) incorporated into a cross-linked poly(ethylene glycol) exhibited excellent CO 2 separation properties over H 2 . However, the CO 2 permeability should be increased for practical applications. Monoethanolamine (MEA) used as a CO 2 determining agent in the current CO 2 capture technology at demonstration scale was readily immobilized in poly(vinyl alcohol) (PVA) matrix by solvent casting of aqueous mixture of PVA and the amine. The resulting polymeric membranes can be self-standing with the thickness above 3 μm and the amine fraction less than 80 wt%. The gas permeation properties were examined at 40 °C and under 80% relative humidity. The CO 2 separation performance increased with increase of the amine content in the polymeric membranes. When the amine fraction was 80 wt%, the CO 2 permeability coefficient of MEA containing membrane was 604 barrer with CO 2 selectivity of 58.5 over H 2 , which was much higher than the PAMAM membrane (83.7 barrer and 51.8, respectively) under the same operation conditions. On the other hand, ethylamine (EA) was also incorporated into PVA matrix to form a thin membrane. However, the resulting polymeric membranes exhibited slight CO 2 -selective gas permeation properties. The hydroxyl group of MEA was crucial for high CO 2 separation performance.

Effect of amine structure on CO2 capture by polymeric membranes

PubMed Central

Taniguchi, Ikuo; Kinugasa, Kae; Toyoda, Mariko; Minezaki, Koki

2017-01-01

Abstract Poly(amidoamine)s (PAMAMs) incorporated into a cross-linked poly(ethylene glycol) exhibited excellent CO2 separation properties over H2. However, the CO2 permeability should be increased for practical applications. Monoethanolamine (MEA) used as a CO2 determining agent in the current CO2 capture technology at demonstration scale was readily immobilized in poly(vinyl alcohol) (PVA) matrix by solvent casting of aqueous mixture of PVA and the amine. The resulting polymeric membranes can be self-standing with the thickness above 3 μm and the amine fraction less than 80 wt%. The gas permeation properties were examined at 40 °C and under 80% relative humidity. The CO2 separation performance increased with increase of the amine content in the polymeric membranes. When the amine fraction was 80 wt%, the CO2 permeability coefficient of MEA containing membrane was 604 barrer with CO2 selectivity of 58.5 over H2, which was much higher than the PAMAM membrane (83.7 barrer and 51.8, respectively) under the same operation conditions. On the other hand, ethylamine (EA) was also incorporated into PVA matrix to form a thin membrane. However, the resulting polymeric membranes exhibited slight CO2-selective gas permeation properties. The hydroxyl group of MEA was crucial for high CO2 separation performance. PMID:29383045

Poly(ionic liquid)/Ionic Liquid Ion-Gels with High "Free" Ionic Liquid Content: Platform Membrane Materials for CO2/Light Gas Separations.

PubMed

Cowan, Matthew G; Gin, Douglas L; Noble, Richard D

2016-04-19

The recycling or sequestration of carbon dioxide (CO2) from the waste gas of fossil-fuel power plants is widely acknowledged as one of the most realistic strategies for delaying or avoiding the severest environmental, economic, political, and social consequences that will result from global climate change and ocean acidification. For context, in 2013 coal and natural gas power plants accounted for roughly 31% of total U.S. CO2 emissions. Recycling or sequestering this CO2 would reduce U.S. emissions by ca. 1800 million metric tons-easily meeting the U.S.'s currently stated CO2 reduction targets of ca. 17% relative to 2005 levels by 2020. This situation is similar for many developed and developing nations, many of which officially target a 20% reduction relative to 1990 baseline levels by 2020. To make CO2 recycling or sequestration processes technologically and economically viable, the CO2 must first be separated from the rest of the waste gas mixture-which is comprised mostly of nitrogen gas and water (ca. 85%). Of the many potential separation technologies available, membrane technology is particularly attractive due to its low energy operating cost, low maintenance, smaller equipment footprint, and relatively facile retrofit integration with existing power plant designs. From a techno-economic standpoint, the separation of CO2 from flue gas requires membranes that can process extremely high amounts of CO2 over a short time period, a property defined as the membrane "permeance". In contrast, the membrane's CO2/N2 selectivity has only a minor effect on the overall cost of some separation processes once a threshold permeability selectivity of ca. 20 is reached. Given the above criteria, the critical properties when developing membrane materials for postcombustion CO2 separation are CO2 permeability (i.e., the rate of CO2 transport normalized to the material thickness), a reasonable CO2/N2 selectivity (≥20), and the ability to be processed into defect-free thin-films (ca. 100-nm-thick active layer). Traditional polymeric membrane materials are limited by a trade-off between permeability and selectivity empirically described by the "Robeson upper bound"-placing the desired membrane properties beyond reach. Therefore, the investigation of advanced and composite materials that can overcome the limitations of traditional polymeric materials is the focus of significant academic and industrial research. In particular, there has been substantial work on ionic-liquid (IL)-based materials due to their gas transport properties. This review provides an overview of our collaborative work on developing poly(ionic liquid)/ionic liquid (PIL/IL) ion-gel membrane technology. We detail developmental work on the preparation of PIL/IL composites and describe how this chemical technology was adapted to allow the roll-to-roll processing and preparation of membranes with defect-free active layers ca. 100 nm thick, CO2 permeances of over 6000 GPU, and CO2/N2 selectivity of ≥20-properties with the potential to reduce the cost of CO2 removal from coal-fired power plant flue gas to ca. $15 per ton of CO2 captured. Additionally, we examine the materials developments that have produced advanced PIL/IL composite membranes. These advancements include cross-linked PIL/IL blends, step-growth PIL/IL networks with facilitated transport groups, and PIL/IL composites with microporous additives for CO2/CH4 separations.

Adsorptive separation of CO 2 in sulfur-doped nanoporous carbons: Selectivity and breakthrough simulation

DOE PAGES

Saha, Dipendu; Orkoulas, Gerassimos; Chen, Jihua; ...

2017-03-01

In this research, we have synthesized two sulfur functionalized nanoporous carbons by post-synthesis modifications with sulfur bearing activating agents that simultaneously enhanced the surface area and introduced sulfur functionalities on the carbon surface. The Brunauer–Emmett–Teller (BET) surface areas of these materials were 2865 and 837 m 2/g with total sulfur contents of 8.2 and 12.9 %, respectively. The sulfur-functionalized carbons were characterized with pore textural properties, X-ray photoelectron spectroscopy (XPS), thermogravimetric analysis (TGA) and electron microscopy (SEM and TEM). In both the carbons, CO 2 adsorption isotherms and kinetics were measured in three different temperatures of 298, 288 and 278more » K and pressures up to 760 torr. The gravimetric CO 2 uptake followed the trend with BET surface area but the surface area-based uptake was reversed and it followed the trend of sulfur content. The heat of adsorption of CO 2 in low uptake was 60-65 kJ/mol, which is the highest for CO 2 adsorption in porous carbons. In order to investigate the adsorptive separation of CO 2, N 2 and CH 4 adsorption isotherms were also measured at 298 K and 760 torr. The selectivity of separation for CO 2/N 2 and CO 2/CH 4 was calculated based on the Ideal Adsorbed Solution Theory (IAST) and all the results demonstrated the high CO 2 selectivity for the carbon with higher sulfur content. The adsorption isotherms were combined with mass balances to calculate the breakthrough behavior of the binary mixtures of CO 2/N 2 and CO 2/CH 4. The simulation results demonstrated that the dimensionless breakthrough time is a decreasing function of the mole fraction of CO 2 in the feed stream. The overall results suggest that the sulfurfunctionalized carbons can be employed as potential adsorbents for CO 2 separation.« less

Properties and Performance Attributes of Novel Co-extruded Polyolefin Battery Separator Materials. Part 2; Electrical Properties

NASA Technical Reports Server (NTRS)

Baldwin, Richard S.

2013-01-01

As NASA prepares for its next era of manned spaceflight missions, advanced energy storage technologies are being developed and evaluated to address and enhance future mission needs and technical requirements. Cell-level components for advanced lithium-ion batteries possessing higher energy, more reliable performance and enhanced, inherent safety characteristics have been under development within the NASA infrastructure. A key component for safe and reliable cell performance is the cell separator, which separates the two energetic electrodes and functions to inhibit the occurrence of an internal short circuit but preserves an ionic current. Recently, a new generation of co-extruded separator films has been developed by ExxonMobil Chemical and introduced into their battery separator product portfolio. Several grades of this new separator material were evaluated with respect to dynamic mechanical properties and safety-related performance attributes, and the results of these evaluations were previously reported in "Part 1: Mechanical Properties" of this publication. This current paper presents safety-related performance results for these novel materials obtained by employing a complementary experimental methodology, which involved the analysis of separator impedance characteristics as a function of temperature. The experimental results from this study are discussed with respect to potential cell safety enhancement for future aerospace as well as for terrestrial energy storage needs, and they are compared with pertinent mechanical properties of these materials, as well as with current state-of-the practice separator materials.

Membraneless laminar flow cell for electrocatalytic CO2 reduction with liquid product separation

NASA Astrophysics Data System (ADS)

Monroe, Morgan M.; Lobaccaro, Peter; Lum, Yanwei; Ager, Joel W.

2017-04-01

The production of liquid fuel products via electrochemical reduction of CO2 is a potential path to produce sustainable fuels. However, to be practical, a separation strategy is required to isolate the fuel-containing electrolyte produced at the cathode from the anode and also prevent the oxidation products (i.e. O2) from reaching the cathode. Ion-conducting membranes have been applied in CO2 reduction reactors to achieve this separation, but they represent an efficiency loss and can be permeable to some product species. An alternative membraneless approach is developed here to maintain product separation through the use of a laminar flow cell. Computational modelling shows that near-unity separation efficiencies are possible at current densities achievable now with metal cathodes via optimization of the spacing between the electrodes and the electrolyte flow rate. Laminar flow reactor prototypes were fabricated with a range of channel widths by 3D printing. CO2 reduction to formic acid on Sn electrodes was used as the liquid product forming reaction, and the separation efficiency for the dissolved product was evaluated with high performance liquid chromatography. Trends in product separation efficiency with channel width and flow rate were in qualitative agreement with the model, but the separation efficiency was lower, with a maximum value of 90% achieved.

Pentiptycene-Based Polyurethane with Enhanced Mechanical Properties and CO2-Plasticization Resistance for Thin Film Gas Separation Membranes.

PubMed

Pournaghshband Isfahani, Ali; Sadeghi, Morteza; Wakimoto, Kazuki; Shrestha, Binod Babu; Bagheri, Rouhollah; Sivaniah, Easan; Ghalei, Behnam

2018-05-23

The development of thin film composite (TFC) membranes offers an opportunity to achieve the permeability/selectivity requirements for optimum CO 2 separation performance. However, the durability and performance of thin film gas separation membranes are mostly challenged by weak mechanical properties and high CO 2 plasticization. Here, we designed new polyurethane (PU) structures with bulky aromatic chain extenders that afford preferred mechanical properties for ultra-thin-film formation. An improvement of about 1500% in Young's modulus and 600% in hardness was observed for pentiptycene-based PUs compared to the typical PU membranes. Single (CO 2 , H 2 , CH 4 , and N 2 ) and mixed (CO 2 /N 2 and CO 2 /CH 4 ) gas permeability tests were performed on the PU membranes. The resulting TFC membranes showed a high CO 2 permeance up to 1400 GPU (10 -6 cm 3 (STP) cm -2 s -1 cmHg -1 ) and the CO 2 /N 2 and CO 2 /H 2 selectivities of about 22 and 2.1, respectively. The enhanced mechanical properties of pentiptycene-based PUs result in high-performance thin membranes with the similar selectivity of the bulk polymer. The thin film membranes prepared from pentiptycene-based PUs also showed a twofold enhanced plasticization resistance compared to non-pentiptycene-containing PU membranes.

A detailed study of Au-Ni bimetal synthesized by the phase separation mechanism for the cathode of low-temperature solid oxide fuel cells

NASA Astrophysics Data System (ADS)

Yang, Tao; Rodrigues de Almeida, Carlos Manuel; Ramasamy, Devaraj; Almeida Loureiro, Francisco José

2014-12-01

A facile co-reduction and annealing synthesis route of nanospheric particles of Au-Ni bimetal with adjustable composition was developed. In a typical synthesis, a direct co-reduction of HAuCl4.4H2O and NiCl2 in aqueous solution was performed with the assistance of reductive NaBH4 and an anionic surfactant sodium dodecyl sulfate (SDS) functioned as the structure-directing agent. Ultrasonic mixing was used at the same time to control the size of the particles. The morphology, microstructure and the state of the surface atoms were analyzed in detail. These nanospheres showed enhanced electrocatalytic activity towards oxygen reduction reaction than that of pure Au nanoparticles, demonstrated in the low temperature SOFC as cathode. The maximum power density generated is 810 mW cm-2 at 550 °C. This is a promising route of taking advantages the Phase Separation Mechanism to greatly reduce the use of noble metals in the ORR field without sacrificing the electrocatalytic activity.

Treatment of low level radioactive liquid waste containing appreciable concentration of TBP degraded products.

PubMed

Valsala, T P; Sonavane, M S; Kore, S G; Sonar, N L; De, Vaishali; Raghavendra, Y; Chattopadyaya, S; Dani, U; Kulkarni, Y; Changrani, R D

2011-11-30

The acidic and alkaline low level radioactive liquid waste (LLW) generated during the concentration of high level radioactive liquid waste (HLW) prior to vitrification and ion exchange treatment of intermediate level radioactive liquid waste (ILW), respectively are decontaminated by chemical co-precipitation before discharge to the environment. LLW stream generated from the ion exchange treatment of ILW contained high concentrations of carbonates, tributyl phosphate (TBP) degraded products and problematic radio nuclides like (106)Ru and (99)Tc. Presence of TBP degraded products was interfering with the co-precipitation process. In view of this a modified chemical treatment scheme was formulated for the treatment of this waste stream. By mixing the acidic LLW and alkaline LLW, the carbonates in the alkaline LLW were destroyed and the TBP degraded products got separated as a layer at the top of the vessel. By making use of the modified co-precipitation process the effluent stream (1-2 μCi/L) became dischargeable to the environment after appropriate dilution. Based on the lab scale studies about 250 m(3) of LLW was treated in the plant. The higher activity of the TBP degraded products separated was due to short lived (90)Y isotope. The cement waste product prepared using the TBP degraded product was having good chemical durability and compressive strength. Copyright © 2011 Elsevier B.V. All rights reserved.

Secondary Vortex Structures in Vortex Generator Induced Flow

NASA Astrophysics Data System (ADS)

Velte, Clara; Okulov, Valery; Hansen, Martin

2010-11-01

Passive rectangular vane actuators can induce a longitudinal vortex that redistributes the momentum in the boundary layer to control the flow. Recent experiments [1] as well as previous studies [2] have shown that a secondary vortex of opposite sign is generated along with the primary one, supposedly from local separation of the boundary layer due to the primary vortex. 2D flow visualizations of a vortex in the vicinity of a boundary support this hypothesis [3]. These secondary vortices are studied for various configurations -- single generator, counter- and co-rotating cascades. The objective is to study their removal through cancelation in cascades using Stereoscopic Particle Image Velocimetry and flow visualization.[4pt] [1] Velte, Hansen and Okulov, J. Fluid Mech. 619, 2009.[0pt] [2] Zhang, Int. J. Heat Fluid Flow 21 2000.[0pt] [3] Harris, Miller and Williamson, APS abstract 2009.

Phase separation of bio-oil produced by co-pyrolysis of corn cobs and polypropylene

NASA Astrophysics Data System (ADS)

Supramono, D.; Julianto; Haqqyana; Setiadi, H.; Nasikin, M.

2017-11-01

In co-pyrolysis of biomass-plastics, bio-oil produced contains both oxygenated and non-oxygenated compounds. High oxygen composition is responsible for instability and low heating value of bio-oil and high acid content for corrosiveness. Aims of the present work are to evaluate possibilities of achieving phase separation between oxygenated and non-oxygenated compounds in bio-oil using a proposed stirred tank reactor and to achieve synergistic effects on bio-oil yield and non-oxygenated compound layer yield. Separation of bio-oil into two layers, i.e. that containing oxygenated compounds (polar phase) and non-oxygenated compounds (non-polar phase) is important to obtain pure non-polar phase ready for the next processing of hydrogenation and used directly as bio-fuel. There has been no research work on co-pyrolysis of biomass-plastic considering possibility of phase separation of bio-oil. The present work is proposing a stirred tank reactor for co-pyrolysis with nitrogen injection, which is capable of tailoring co-pyrolysis conditions leading to low viscosity and viscosity asymmetry, which induce phase separation between polar phase and non-polar phase. The proposed reactor is capable of generating synergistic effect on bio-oil and non-polar yields as the composition of PP in feed is more than 25% weight in which non-polar layers contain only alkanes, alkenes, cycloalkanes and cycloalkenes.

Process for analyzing CO[sub 2] in air and in water

DOEpatents

Atwater, J.E.; Akse, J.R.; DeHart, J.

1999-06-08

The process of this invention comprises providing a membrane for separating CO[sub 2] into a first CO[sub 2] sample phase and a second CO[sub 2] analyte phase. CO[sub 2] is then transported through the membrane thereby separating the CO[sub 2] with the membrane into a first CO[sub 2] sample phase and a second CO[sub 2] analyte liquid phase including an ionized, conductive, dissociated CO[sub 2] species. Next, the concentration of the ionized, conductive, dissociated CO[sub 2] species in the second CO[sub 2] analyte liquid phase is chemically amplified using a water-soluble chemical reagent which reversibly reacts with undissociated CO[sub 2] to produce conductivity changes therein corresponding to fluctuations in the partial pressure of CO[sub 2] in the first CO[sub 2] sample phase. Finally, the chemically amplified, ionized, conductive, dissociated CO[sub 2] species is introduced to a conductivity measuring instrument. Conductivity changes in the chemically amplified, ionized, conductive, dissociated CO[sub 2] species are detected using the conductivity measuring instrument. 43 figs.

Process for analyzing CO.sub.2 in air and in water

DOEpatents

Atwater, James E.; Akse, James R.; DeHart, Jeffrey

1999-01-01

The process of this invention comprises providing a membrane for separating CO.sub.2 into a first CO.sub.2 sample phase and a second CO.sub.2 analyte phase. CO.sub.2 is then transported through the membrane thereby separating the CO.sub.2 with the membrane into a first CO.sub.2 sample phase and a second CO.sub.2 analyte liquid phase including an ionized, conductive, dissociated CO.sub.2 species. Next, the concentration of the ionized, conductive, dissociated CO.sub.2 species in the second CO.sub.2 analyte liquid phase is chemically amplified using a water-soluble chemical reagent which reversibly reacts with undissociated CO.sub.2 to produce conductivity changes therein corresponding to fluctuations in the partial pressure of CO.sub.2 in the first CO.sub.2 sample phase. Finally, the chemically amplified, ionized, conductive, dissociated CO.sub.2 species is introduced to a conductivity measuring instrument. Conductivity changes in the chemically amplified, ionized, conductive, dissociated CO.sub.2 species are detected using the conductivity measuring instrument.

Process for analyzing CO{sub 2} in seawater

DOEpatents

Atwater, J.E.; Akse, J.R.; DeHart, J.

1997-07-01

The process of this invention comprises providing a membrane for separating CO{sub 2} into a first CO{sub 2} sample phase and a second CO{sub 2} analyte phase. CO{sub 2} is then transported through the membrane thereby separating the CO{sub 2} with the membrane into a first CO{sub 2} sample phase and a second CO{sub 2} analyte liquid phase including an ionized, conductive, dissociated CO{sub 2} species. Next, the concentration of the ionized, conductive, dissociated CO{sub 2} species in the second CO{sub 2} analyte liquid phase is chemically amplified using a water-soluble chemical reagent which reversibly reacts with undissociated CO{sub 2} to produce conductivity changes therein corresponding to fluctuations in the partial pressure of CO{sub 2} in the first CO{sub 2} sample phase. Finally, the chemically amplified, ionized, conductive, dissociated CO{sub 2} species is introduced to a conductivity measuring instrument. Conductivity changes in the chemically amplified, ionized, conductive, dissociated CO{sub 2} species are detected using the conductivity measuring instrument. 43 figs.

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

Hong, Tao; Chatterjee, Sabornie; Mahurin, Shannon M.

Amidoxime-functionalized polydimethylsiloxane (AO-PDMSPNB) membranes with various amidoxime compositions were synthesized via ring-opening metathesis polymerization followed by post-polymerization modification. Compared to other previously reported PDMS-based membranes, the amidoxime-functionalized membranes show enhanced CO 2 permeability and CO 2/N 2 selectivity. The overall gas separation performance (CO 2 permeability 6800 Barrer; CO 2/N 2 selectivity 19) of the highest performing membrane exceeds the Robeson upper bound line, and the excellent permeability of the copolymer itself provides great potential for real world applications where huge volumes of gases are separated. This study details how tuning the CO 2-philicity within rubbery polymer matrices influences gasmore » transport properties. Key parameters for tuning gas transport properties are discussed, and the experimental results show good consistency with theoretical calculations. Finally, this study provides a roadmap to enhancing gas separation performance in rubbery polymers by tuning gas solubility selectivity.« less

40 CFR 98.443 - Calculating CO2 geologic sequestration.

Code of Federal Regulations, 2011 CFR

2011-07-01

... each gas-liquid separator for which flow is measured using a mass flow meter, you must calculate...) For each gas-liquid separator for which flow is measured using a volumetric flow meter, you must...) To aggregate production data, you must sum the mass of all of the CO2 separated at each gas-liquid...

Preparation And Evaluation Techniques of Porous Materials and Mixed Matrix Membranes for Targeted CO2 Separation Applications

NASA Astrophysics Data System (ADS)

Tessema, Tsemre Dingel Mesfin

The use of porous sorbents for physisorptive capture of CO2 from gas mixtures has been deemed attractive due to the low energy penalty associated with recycling of such materials. Porous organic polymers (POPs) have emerged as promising candidates with potential in the treatment of pre- and post- fuel combustion processes to separate CO2 from gas mixtures. Concurrently, significant advances have been made in establishing calculation methods that evaluate the practicality of porous sorbents for targeted gas separation applications. However, these methods rely on single gas adsorption isotherms without accounting for the dynamic gas mixtures encountered in real-life applications. To this end, the design and application of a dynamic gas mixture breakthrough apparatus to assess the CO2 separation performance of a new class of heteroatom (N and O) doped porous carbons derived from a Pyrazole precursor from flue gas mixtures is presented. Here in, two new benzimidazole linked polymers (BILPs) have been designed and synthesized. These polymers display high surface while their imidazole functionality and microporous nature resulted in high CO2 uptakes and isosteric heat of adsorption (Qst). BILP-30 displayed very good selectivity for CO2 in flue gas while BILP-31 was superior in CO2 separation from landfill gas mixtures at 298 K and 1 bar. Additionally, a new POP incorporating a highly conjugated pyrene core into a polymer framework linked by azo-bonds is presented. Azo-Py displays a nanofibrous morphology induced by the pi-pi stacking of the electron rich pyrene core. Due to its high surface area and microporous nature, Azo-Py displays impressive CO2 uptakes at 298 K and 1 bar. Evaluation of the S value for CO2 separation of Azo-Py revealed competitive values for flue gas and landfill gas at 298 K and 1 bar. Finally, a highly cross-linked benzimidazole linked polymer, BILP-4, was successfully incorporated into MatrimidRTM polymer to form a series of new mixed matrix membranes. The surface functionality of BILP-4 was exploited to enhance the interaction with MatrimidRTM polymer matrix to produce robust MMMs which displayed significantly improved CO2 gas permeabilities and ideal selectivities for CO 2/N2.

Supercritical fluid extraction and separation of uranium from other actinides.

PubMed

Quach, Donna L; Mincher, Bruce J; Wai, Chien M

2014-06-15

The feasibility of separating U from nitric acid solutions of mixed actinides using tri-n-butylphosphate (TBP)-modified supercritical fluid carbon dioxide (sc-CO2) was investigated. The actinides U, Np, Pu, and Am were extracted into sc-CO2 modified with TBP from a range of nitric acid concentrations, in the absence of, or in the presence of, a number of traditional reducing and/or complexing agents to demonstrate the separation of these metals from U under sc-CO2 conditions. The separation of U from Pu using sc-CO2 was successful at nitric acid concentrations of less than 3M in the presence of acetohydroxamic acid (AHA) or oxalic acid (OA) to mitigate Pu extraction, and the separation of U from Np was successful at nitric acid concentrations of less than 1M in the presence of AHA, OA, or sodium nitrite to mitigate Np extraction. Americium was not well extracted under any condition studied. Copyright © 2014 Elsevier B.V. All rights reserved.

Zeolitic Imidazolate Framework-8 Membrane for H2/CO2 Separation: Experimental and Modeling

NASA Astrophysics Data System (ADS)

Lai, L. S.; Yeong, Y. F.; Lau, K. K.; Azmi, M. S.; Chew, T. L.

2018-03-01

In this work, ZIF-8 membrane synthesized through solvent evaporation secondary seeded growth was tested for single gas permeation and binary gases separation of H2 and CO2. Subsequently, a modified mathematical modeling combining the effects of membrane and support layers was applied to represent the gas transport properties of ZIF-8 membrane. Results showed that, the membrane has exhibited H2/CO2 ideal selectivity of 5.83 and separation factor of 3.28 at 100 kPa and 303 K. Besides, the experimental results were fitted well with the simulated results by demonstrating means absolute error (MAE) values ranged from 1.13 % to 3.88 % for single gas permeation and 10.81 % to 21.22 % for binary gases separation. Based on the simulated data, most of the H2 and CO2 gas molecules have transported through the molecular pores of membrane layer, which was up to 70 %. Thus, the gas transport of the gases is mainly dominated by adsorption and diffusion across the membrane.

Anisotropic Metal Deposition on TiO2 Particles by Electric-Field-Induced Charge Separation.

PubMed

Tiewcharoen, Supakit; Warakulwit, Chompunuch; Lapeyre, Veronique; Garrigue, Patrick; Fourier, Lucas; Elissalde, Catherine; Buffière, Sonia; Legros, Philippe; Gayot, Marion; Limtrakul, Jumras; Kuhn, Alexander

2017-09-11

Deposition of metals on TiO 2 semiconductor particles (M-TiO 2 ) results in hybrid Janus objects combining the properties of both materials. One of the techniques proposed to generate Janus particles is bipolar electrochemistry (BPE). The concept can be applied in a straightforward way for the site-selective modification of conducting particles, but is much less obvious to use for semiconductors. Herein we report the bulk synthesis of anisotropic M-TiO 2 particles based on the synergy of BPE and photochemistry, allowing the intrinsic limitations, when they are used separately, to be overcome. When applying electric fields during irradiation, electrons and holes can be efficiently separated, thus breaking the symmetry of particles by modifying them selectively and in a wireless way on one side with either gold or platinum. Such hybrid materials are an important first step towards high-performance designer catalyst particles, for example for photosplitting of water. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Fabrication of COF-MOF Composite Membranes and Their Highly Selective Separation of H2/CO2.

PubMed

Fu, Jingru; Das, Saikat; Xing, Guolong; Ben, Teng; Valtchev, Valentin; Qiu, Shilun

2016-06-22

The search for new types of membrane materials has been of continuous interest in both academia and industry, given their importance in a plethora of applications, particularly for energy-efficient separation technology. In this contribution, we demonstrate for the first time that a metal-organic framework (MOF) can be grown on the covalent-organic framework (COF) membrane to fabricate COF-MOF composite membranes. The resultant COF-MOF composite membranes demonstrate higher separation selectivity of H2/CO2 gas mixtures than the individual COF and MOF membranes. A sound proof for the synergy between two porous materials is the fact that the COF-MOF composite membranes surpass the Robeson upper bound of polymer membranes for mixture separation of a H2/CO2 gas pair and are among the best gas separation MOF membranes reported thus far.

Radiolytic formation of the carbon dioxide radical anion in acetonitrile revealed by transient IR spectroscopy

DOE PAGES

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

Radiolytic formation of the carbon dioxide radical anion in acetonitrile revealed by transient IR spectroscopy

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

Ethene/ethane and propene/propane separation via the olefin and paraffin selective metal-organic framework adsorbents CPO-27 and ZIF-8.

PubMed

Böhme, Ulrike; Barth, Benjamin; Paula, Carolin; Kuhnt, Andreas; Schwieger, Wilhelm; Mundstock, Alexander; Caro, Jürgen; Hartmann, Martin

2013-07-09

Two types of metal-organic frameworks (MOFs) have been synthesized and evaluated in the separation of C2 and C3 olefins and paraffins. Whereas Co2(dhtp) (=Co-CPO-27 = Co-MOF-74) and Mg2(dhtp) show an adsorption selectivity for the olefins ethene and propene over the paraffins ethane and propane, the zeolitic imidazolate framework ZIF-8 behaves in the opposite way and preferentially adsorbs the alkane. Consequently, in breakthrough experiments, the olefins or paraffins, respectively, can be separated.

Membrane thinning for efficient CO2 capture

PubMed Central

Selyanchyn, Roman; Fujikawa, Shigenori

2017-01-01

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

Pressure Swing Absorption Device and Process for Separating CO{sub 2} from Shifted Syngas and its Capture for Subsequent Storage

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

Sirkar, Kamalesh; Jie, Xingming; Chau, John

Using the ionic liquid (IL) 1-butyl-3-methylimidazolium dicyanamide ([bmim][DCA]) as the absorbent on the shell side of a membrane module containing either a porous hydrophobized ceramic tubule or porous hydrophobized polyether ether ketone (PEEK) hollow fiber membranes, studies for CO{sub 2} removal from hot simulated pre-combustion shifted syngas were carried out by a novel pressure swing membrane absorption (PSMAB) process. Helium was used as a surrogate for H{sub 2} in a simulated shifted syngas with CO{sub 2} around 40% (dry gas basis). In this cyclic separation process, the membrane module was used to achieve non-dispersive gas absorption from a high-pressure feedmore » gas (689-1724 kPag; 100-250 psig) at temperatures between 25-1000C into a stationary absorbent liquid on the module shell side during a certain part of the cycle followed by among other cycle steps controlled desorption of the absorbed gases from the liquid in the rest of the cycle. Two product streams were obtained, one He-rich and the other CO{sub 2}-rich. Addition of polyamidoamine (PAMAM) dendrimer of generation 0 to IL [bmim][DCA] improved the system performance at higher temperatures. The solubilities of CO{sub 2} and He were determined in the ionic liquid with or without the dendrimer in solution as well as in the presence or absence of moisture; polyethylene glycol (PEG) 400 was also studied as a replacement for the IL. The solubility selectivity of the ionic liquid containing the dendrimer for CO{sub 2} over helium was considerably larger than that for the pure ionic liquid. The solubility of CO{sub 2} and CO{sub 2}-He solubility selectivity of PEG 400 and a solution of the dendrimer in PEG 400 were higher than the corresponding ones in the IL, [bmim][DCA]. A mathematical model was developed to describe the PSMAB process; a numerical solution of the governing equations described successfully the observed performance of the PSMAB process for the pure ionic liquid-based system.« less

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

PubMed

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

2015-07-22

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

Development and characterization of polyethersulfone/TiO2 mixed matrix membranes for CO2/CH4 separation

NASA Astrophysics Data System (ADS)

Galaleldin, S.; Mannan, H. A.; Mukhtar, H.

2017-12-01

In this study, mixed matrix membranes comprised of polyethersulfone as the bulk polymer phase and titanium dioxide (TiO2) nanoparticles as the inorganic discontinuous phase were prepared for CO2/CH4 separation. Membranes were synthesized at filler loading of 0, 5, 10 and 15 wt % via dry phase inversion method. Morphology, chemical bonding and thermal characteristics of membranes were scrutinized utilizing different techniques, namely: Field Emission Scanning Electron Microscopy (FESEM), Fourier Transform InfraRed (FTIR) spectra and Thermogravimetric analysis (TGA) respectively. Membranes gas separation performance was evaluated for CO2 and CH4 gases at 4 bar feed pressure. The highest separation performance was achieved by mixed matrix membrane (MMM) at 5 % loading of TiO2.

Inertial extraction system

DOEpatents

Balepin, Vladimir; Castrogiovanni, Anthony; Girlea, Florin; Robertson, Andrew; Sforza, Pasquale

2016-03-15

Disclosed herein are supersonic separation systems that can be used for the removal of CO.sub.2 from a mixed gas stream. Also disclosed are methods for the separation and subsequent collection of solidified CO.sub.2 from a gas stream.

Ionic liquid-based materials: a platform to design engineered CO2 separation membranes.

PubMed

Tomé, Liliana C; Marrucho, Isabel M

2016-05-21

During the past decade, significant advances in ionic liquid-based materials for the development of CO2 separation membranes have been accomplished. This review presents a perspective on different strategies that use ionic liquid-based materials as a unique tuneable platform to design task-specific advanced materials for CO2 separation membranes. Based on compilation and analysis of the data hitherto reported, we provide a judicious assessment of the CO2 separation efficiency of different membranes, and highlight breakthroughs and key challenges in this field. In particular, configurations such as supported ionic liquid membranes, polymer/ionic liquid composite membranes, gelled ionic liquid membranes and poly(ionic liquid)-based membranes are detailed, discussed and evaluated in terms of their efficiency, which is attributed to their chemical and structural features. Finally, an integrated perspective on technology, economy and sustainability is provided.

Natural separation of the acyl-CoA ligase reaction results in a non-adenylating enzyme.

PubMed

Wang, Nan; Rudolf, Jeffrey D; Dong, Liao-Bin; Osipiuk, Jerzy; Hatzos-Skintges, Catherine; Endres, Michael; Chang, Chin-Yuan; Babnigg, Gyorgy; Joachimiak, Andrzej; Phillips, George N; Shen, Ben

2018-06-04

Acyl-coenzyme A (CoA) ligases catalyze the activation of carboxylic acids via a two-step reaction of adenylation followed by thioesterification. Here, we report the discovery of a non-adenylating acyl-CoA ligase PtmA2 and the functional separation of an acyl-CoA ligase reaction. Both PtmA1 and PtmA2, two acyl-CoA ligases from the biosynthetic pathway of platensimycin and platencin, are necessary for the two steps of CoA activation. Gene inactivation of ptmA1 and ptmA2 resulted in the accumulation of free acid and adenylate intermediates, respectively. Enzymatic and structural characterization of PtmA2 confirmed its ability to only catalyze thioesterification. Structural characterization of PtmA2 revealed it binds both free acid and adenylate substrates and undergoes the established mechanism of domain alternation. Finally, site-directed mutagenesis restored both the adenylation and complete CoA activation reactions. This study challenges the currently accepted paradigm of adenylating enzymes and inspires future investigations on functionally separated acyl-CoA ligases and their ramifications in biology.

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

PubMed

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

2017-10-04

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

Impact of CO2-solvent separators on the degradation of benzyl-2,3-dihydroxypiperidine-1-carboxylate during preparative supercritical fluid chromatographic (SFC) purification.

PubMed

Asokan, Kathiravan; Naidu, Harshavardhan; Madam, Ratalababu; Shaikh, Khaja Mohiuddin; Reddy, Manjunath; Kumar, Hemantha; Shirude, Pravin S; Rajendran, Muruganantham; Sarabu, Ramakanth; Wu, Dauh-Rurng; Bajpai, Lakshmikant; Zhang, Yingru

2017-12-29

During a preparative separation of the cis enantiomeric pair of benzyl-2,3-dihydroxypiperidine-1-carboxylate using supercritical-fluid chromatography (SFC) with methanol modifier, significant degradation of the products in the collected fractions was observed when a Waters SFC-350 ® (Milford, MA, USA) was used, but same was not observed when a Waters SFC-80q ® (Milford, MA, USA) was used. Through a systematic investigation, we discovered that the compound degraded over time under an acidic condition created by the formation of methyl carbonic acid from methanol and CO 2. The extent of the product degradation was dependent on the time and the concentration of CO 2 remained in the product fraction, which was governed by the efficiency of CO 2 -methanol separation during the fraction collection. Hence, we demonstrated that the different designs of CO 2 -solvent separator (high pressurized cyclone in Waters SFC-350 ® and low-pressurized vortexing separator in Waters SFC-80q ®® ) had a significant impact on the degradation of an acid-sensitive compound. The acidity caused by CO 2 in methanol was supported by diminished degradation after a nitrogen purging or after neutralizing the collected fractions with a base. Three different solutions to overcome the degradation problem of the acid sensitive compounds using SFC-350 ® with the high pressurized separator were investigated and demonstrated. The degraded products were isolated as four enantiomers and their relative stereochemistry were established based on 2D NMR data along with the plausible mechanism of degradation. Copyright © 2017 Elsevier B.V. All rights reserved.

Evaluation of a Liquid Amine System for Spacecraft Carbon Dioxide Control

NASA Technical Reports Server (NTRS)

Breaux, D. K.; Friedel, P.; Hwang, K. C.; Probert, G.; Ruder, J. M.; Sawamura, L.

1974-01-01

The analytical and experimental studies are described which were directed toward the acquisition of basic information on utilizing a liquid amine sorbent for in use in a CO2 removal system for manned spacecraft. Liquid amine systems are successfully used on submarines for control of CO2 generated by the crew, but liquid amines were not previously considered for spacecraft applications due to lack of development of satisfactory rotary phase separators. Developments in this area now make consideration of liquid amines practical for spacecraft system CO2 removal. The following major tasks were performed to evaluate liquid amine systems for spacecraft: (1) characterization, through testing, of the basic physical and thermodynamic properties of the amine solution; (2) determination of the dynamic characteristics of a cocurrent flow absorber; and (3) evaluation, synthesis, and selection of a liquid amine system concept oriented toward low power requirements. A low weight, low power system concept was developed. Numerical and graphical data are accompanied by pertinent observations.

Beyond Crystal Engineering: Significant Enhancement of C2H2/CO2 Separation by Constructing Composite Material.

PubMed

Wu, Hui Qiong; Yan, Chang Sheng; Luo, Feng; Krishna, Rajamani

2018-04-02

Different from the established crystal engineering method for enhancing gas-separation performance, we demonstrate herein a distinct approach. In contrast to the pristine MOF (metal-organic framework) material, the C 2 H 2 /CO 2 separation ability for the resultant Ag NPs (nanoparticle)@Fe 2 O 3 @MOF composite material, estimated from breakthrough calculations, is greatly enhanced by 2 times, and further magnified up to 3 times under visible light irradiation.

Membraneless laminar flow cell for electrocatalytic CO 2 reduction with liquid product separation

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

Monroe, Morgan M.; Lobaccaro, Peter; Lum, Yanwei

The production of liquid fuel products via electrochemical reduction of CO 2 is a potential path to produce sustainable fuels. However, to be practical, a separation strategy is required to isolate the fuel-containing electrolyte produced at the cathode from the anode and also prevent the oxidation products (i.e. O 2) from reaching the cathode. Ion-conducting membranes have been applied in CO 2 reduction reactors to achieve this separation, but they represent an efficiency loss and can be permeable to some product species. An alternative membraneless approach is developed here to maintain product separation through the use of a laminar flowmore » cell. Computational modelling shows that near-unity separation efficiencies are possible at current densities achievable now with metal cathodes via optimization of the spacing between the electrodes and the electrolyte flow rate. Laminar flow reactor prototypes were fabricated with a range of channel widths by 3D printing. CO 2 reduction to formic acid on Sn electrodes was used as the liquid product forming reaction, and the separation efficiency for the dissolved product was evaluated with high performance liquid chromatography. Trends in product separation efficiency with channel width and flow rate were in qualitative agreement with the model, but the separation efficiency was lower, with a maximum value of 90% achieved.« less

Membraneless laminar flow cell for electrocatalytic CO 2 reduction with liquid product separation

DOE PAGES

Monroe, Morgan M.; Lobaccaro, Peter; Lum, Yanwei; ...

2017-03-16

The production of liquid fuel products via electrochemical reduction of CO 2 is a potential path to produce sustainable fuels. However, to be practical, a separation strategy is required to isolate the fuel-containing electrolyte produced at the cathode from the anode and also prevent the oxidation products (i.e. O 2) from reaching the cathode. Ion-conducting membranes have been applied in CO 2 reduction reactors to achieve this separation, but they represent an efficiency loss and can be permeable to some product species. An alternative membraneless approach is developed here to maintain product separation through the use of a laminar flowmore » cell. Computational modelling shows that near-unity separation efficiencies are possible at current densities achievable now with metal cathodes via optimization of the spacing between the electrodes and the electrolyte flow rate. Laminar flow reactor prototypes were fabricated with a range of channel widths by 3D printing. CO 2 reduction to formic acid on Sn electrodes was used as the liquid product forming reaction, and the separation efficiency for the dissolved product was evaluated with high performance liquid chromatography. Trends in product separation efficiency with channel width and flow rate were in qualitative agreement with the model, but the separation efficiency was lower, with a maximum value of 90% achieved.« less

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

PubMed

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

2015-02-01

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

Highly efficient photocatalytic H2 evolution using TiO2 nanoparticles integrated with electrocatalytic metal phosphides as cocatalysts

NASA Astrophysics Data System (ADS)

Song, Rui; Zhou, Wu; Luo, Bing; Jing, Dengwei

2017-09-01

In this work, electrocatalysts like the metal phosphides Ni2P, NiCoP, and FeP, can serve as cocatalysts of TiO2 to form efficient composite photocatalysts for hydrogen generation from an aqueous methanol solution. On comparing Ni2P, NiCoP, and FeP and optimizing their proportions, the NiCoP(1 wt%)/TiO2 composite was found to exhibit the highest activity toward photocatalytic H2 production (1.54 μmol h-1 mg-1), which is about thirteen times that of the naked TiO2 nanoparticles. Mott-Schottky (MS) analysis indicated that the large upward shift or band bending of the Fermi energy level (EF) in metal phosphides was responsible for the enhanced activity of the composites. The steady-state photoluminescence (PL) spectra and photocurrent transient response further confirmed that the enhanced photoinduced charge transfer and band separation after TiO2 was integrated with the metal phosphides. Thus, these electrocatalysts were shown to be efficient cocatalysts that can replace noble metals as low-cost photocatalytic H2 production.

Highly porous CO 2 hydrate generation aided by silica nanoparticles for potential secure storage of CO 2 and desalination

DOE PAGES

Kim, Ijung; Nole, Michael; Jang, Sunghyun; ...

2017-01-31

Here in this paper, we report a new way of storing CO 2 in a highly porous hydrate structure, stabilized by silica nanoparticles (NPs). Such a porous CO 2 hydrate structure was generated either by cooling down NP-stabilized CO 2-in-seawater foams, or by gently mixing CO 2 and seawater that contains silica NPs under CO 2 hydrate-generating conditions. With the highly porous structure, enhanced desalination was also achievable when the partial meltdown of CO 2 hydrate was allowed.

Highly porous CO 2 hydrate generation aided by silica nanoparticles for potential secure storage of CO 2 and desalination

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

Kim, Ijung; Nole, Michael; Jang, Sunghyun

Here in this paper, we report a new way of storing CO 2 in a highly porous hydrate structure, stabilized by silica nanoparticles (NPs). Such a porous CO 2 hydrate structure was generated either by cooling down NP-stabilized CO 2-in-seawater foams, or by gently mixing CO 2 and seawater that contains silica NPs under CO 2 hydrate-generating conditions. With the highly porous structure, enhanced desalination was also achievable when the partial meltdown of CO 2 hydrate was allowed.

Improving CO2 permeation and separation performance of CO2-philic polymer membrane by blending CO2 absorbents

NASA Astrophysics Data System (ADS)

Cheng, Jun; Hu, Leiqing; Li, Yannan; Liu, Jianzhong; Zhou, Junhu; Cen, Kefa

2017-07-01

To research effects of CO2 absorption capacity and type of CO2 absorbent on the CO2 separation and free-volume properties of facilitated transport membranes, two types of CO2 absorbents, namely monoethanolamine (MEA) and ionic liquids (ILs:[P66614][Triz] and [P66614][2-Op]), were adopted. The CO2 absorption capacities of MEA, [P66614][Triz] and [P66614][2-Op] were about 0.561 mol CO2 per mol, 0.95 mol CO2 per mol and 1.60 mol CO2 per mol, respectively. All mean free-volume hole radiuses of membranes decreased after blending CO2 absorbents. After polymer membrane blended with two ILs, number of free-volume hole increased, resulting in modest increase of the fractional free volume. Both CO2 permeability and selectivity increased after blending MEA and ILs. The increasing range of CO2 permeability corresponded with CO2 absorption capacity of CO2 absorbents, and membrane blending with [P66614][2-Op] showed the highest CO2 permeability of 672.1 Barrers at 25 °C. Pebax/PEGDME membrane blending with MEA obtained the highest CO2/H2 and CO2/CH4 selectivity at 17.8 and 20.5, respectively.

Gas adsorption/separation properties of metal directed self-assembly of two coordination polymers with 5-nitroisophthalate

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

Arıcı, Mürsel; Yeşilel, Okan Zafer, E-mail: yesilel@ogu.edu.tr; Keskin, Seda

2014-02-15

Two new coordination polymers, namely, [Co(µ-nip)(µ-bpe)]{sub n} (1) and [Zn(µ-nip)(µ-bpe)]{sub n} (2) (nip: 5-nitroisophthalate, bpe: 1,2-bis(4-pyridyl)ethane) were hydrothermally synthesized and structurally characterized by single crystal X-ray diffraction, IR spectroscopy, elemental analysis and thermal analysis. Moreover, atomically detailed simulation studies of complex 2 for CO{sub 2}/CH{sub 4} adsorption and separation were performed. Complex 1 consists of two dimensional (2D) (4,4) grid networks with the point symbol of 4{sup 4}.6{sup 2}. Complex 2 exhibits a 3-fold interpenetrating 3D framework with 6{sup 5}.8-dmp topology. Thermal properties of the complexes showed that both complexes were stable over 320 °C. Simulation studies demonstrated that complexmore » 2 can separate CO{sub 2} from CH{sub 4} at low pressures at 273 K. - Graphical abstract: In this study, two new coordination polymers, namely, [Co(µ-nip)(µ-bpe)]{sub n} (1) and [Zn(µ-nip)(µ-bpe)]{sub n} (2) (nip: 5-nitroisophthalate, bpe: 1,2-bis(4-pyridyl)ethane) were hydrothermally synthesized and structurally characterized by single crystal X-ray diffraction, IR spectroscopy, elemental analysis and thermal analysis. Moreover, atomically detailed simulation studies of complex 2 for CO{sub 2}/CH{sub 4} adsorption and separation were performed. Complex 1 consists of two dimensional (2D) (4,4) grid networks with the point symbol of 4{sup 4}.6{sup 2}. Complex 2 exhibits a 3-fold interpenetrating 3D framework with 6{sup 5}.8-dmp topology. Simulation studies demonstrated that complex 2 can separate CO{sub 2} from CH{sub 4} at low pressures at 273 K. Display Omitted - Highlights: • Two new coordination polymers with 5-nitroisophthalate and 1,2-bis(4-pyridyl)ethane. • Atomically detailed simulation studies of the complexes. • Complex 2 can be proposed as molecular sieve to separate CO{sub 2} from CH{sub 4} at low pressures.« less

Carbon Molecular Sieve Membrane as a True One Box Unit for Large Scale Hydrogen Production

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

Liu, Paul

2012-05-01

IGCC coal-fired power plants show promise for environmentally-benign power generation. In these plants coal is gasified to syngas then processed in a water gas-shift (WGS) reactor to maximize the hydrogen/CO{sub 2} content. The gas stream can then be separated into a hydrogen rich stream for power generation and/or further purified for sale as a chemical and a CO{sub 2} rich stream for the purpose of carbon capture and storage (CCS). Today, the separation is accomplished using conventional absorption/desorption processes with post CO{sub 2} compression. However, significant process complexity and energy penalties accrue with this approach, accounting for ~20% of themore » capital cost and ~27% parasitic energy consumption. Ideally, a one-box process is preferred in which the syngas is fed directly to the WGS reactor without gas pre-treatment, converting the CO to hydrogen in the presence of H{sub 2}S and other impurities and delivering a clean hydrogen product for power generation or other uses. The development of such a process is the primary goal of this project. Our proposed "one-box" process includes a catalytic membrane reactor (MR) that makes use of a hydrogen-selective, carbon molecular sieve (CMS) membrane, and a sulfur-tolerant Co/Mo/Al{sub 2}O{sub 3} catalyst. The membrane reactor's behavior has been investigated with a bench top unit for different experimental conditions and compared with the modeling results. The model is used to further investigate the design features of the proposed process. CO conversion >99% and hydrogen recovery >90% are feasible under the operating pressures available from IGCC. More importantly, the CMS membrane has demonstrated excellent selectivity for hydrogen over H{sub 2}S (>100), and shown no flux loss in the presence of a synthetic "tar"-like material, i.e., naphthalene. In summary, the proposed "one-box" process has been successfully demonstrated with the bench-top reactor. In parallel we have successfully designed and fabricated a full-scale CMS membrane and module for the proposed application. This full-scale membrane element is a 3" diameter with 30"L, composed of ~85 single CMS membrane tubes. The membrane tubes and bundles have demonstrated satisfactory thermal, hydrothermal, thermal cycling and chemical stabilities under an environment simulating the temperature, pressure and contaminant levels encountered in our proposed process. More importantly, the membrane module packed with the CMS bundle was tested for over 30 pressure cycles between ambient pressure and >300 -600 psi at 200 to 300°C without mechanical degradation. Finally, internal baffles have been designed and installed to improve flow distribution within the module, which delivered 90% separation efficiency in comparison with the efficiency achieved with single membrane tubes. In summary, the full-scale CMS membrane element and module have been successfully developed and tested satisfactorily for our proposed one-box application; a test quantity of elements/modules have been fabricated for field testing. Multiple field tests have been performed under this project at National Carbon Capture Center (NCCC). The separation efficiency and performance stability of our full-scale membrane elements have been verified in testing conducted for times ranging from 100 to >250 hours of continuous exposure to coal/biomass gasifier off-gas for hydrogen enrichment with no gas pre-treatment for contaminants removal. In particular, "tar-like" contaminants were effectively rejected by the membrane with no evidence of fouling. In addition, testing was conducted using a hybrid membrane system, i.e., the CMS membrane in conjunction with the palladium membrane, to demonstrate that 99+% H{sub 2} purity and a high degree of CO{sub 2} capture could be achieved. In summary, the stability and performance of the full-scale hydrogen selective CMS membrane/module has been verified in multiple field tests in the presence of coal/biomass gasifier off-gas under this project. A promising process scheme has been developed for power generation and/or hydrogen coproduction with CCS based upon our proposed "one-box" process. Our preliminary economic analysis indicates about 10% reduction in the required electricity selling price and ~40% cost reduction in CCS on per ton CO{sub 2} can be achieved in comparison with the base case involving conventional WGS with a two-stage Selexsol® for CCS. Long term field tests (e.g., >1,000 hrs) with the incorporation of the catalyst for the WGS membrane reactor and more in-depth analysis of the process scheme are recommended for the future study.« less

pH neutralization of the by-product sludge waste water generated from waste concrete recycling process using the carbon mineralization

NASA Astrophysics Data System (ADS)

Ji, Sangwoo; Shin, Hee-young; Bang, Jun Hwan; Ahn, Ji-Whan

2017-04-01

About 44 Mt/year of waste concrete is generated in South Korea. More than 95% of this waste concrete is recycled. In the process of regenerating and recycling pulmonary concrete, sludge mixed with fine powder generated during repeated pulverization process and water used for washing the surface and water used for impurity separation occurs. In this way, the solid matter contained in the sludge as a by-product is about 40% of the waste concrete that was input. Due to the cement component embedded in the concrete, the sludge supernatant is very strong alkaline (pH about 12). And it is necessary to neutralization for comply with environmental standards. In this study, carbon mineralization method was applied as a method to neutralize the pH of highly alkaline waste water to under pH 8.5, which is the water quality standard of discharged water. CO2 gas (purity 99%, flow rate 10ml/min.) was injected and reacted with the waste water (Ca concentration about 750mg/L) from which solid matter was removed. As a result of the experiment, the pH converged to about 6.5 within 50 minutes of reaction. The precipitate showed high whiteness. XRD and SEM analysis showed that it was high purity CaCO3. For the application to industry, it is needed further study using lower concentration CO2 gas (about 14%) which generated from power plant.

Pinholes and Nano-oxide Specular Layers in Spin Valves

NASA Astrophysics Data System (ADS)

Fry, R. A.; Egelhoff, W. F., Jr.; McMichael, R. D.; Chen, P. J.; Powell, C. J.; Beach, G.; Berkowitz, A. E.

2001-03-01

Recently, nano-oxide layers (NOL) in giant magnetoresistance (GMR) spin valves have attracted interest as a method of achieving increased GMR associated with specular reflection at Co/oxide interfaces. The NOL must be thin enough so that strong magnetic coupling across it exists; otherwise, the films separated by NOL could switch separately. We have investigated the structure NiO/2.5 nm Co/2.5 nm Cu/2 nm Co/NOL/2 nm Co/10 nm IrMn. The bottom Co is pinned by NiO more strongly than the top Co is pinned by IrMn; thus the top Co film can be switched to observe GMR loops. With no NOL, the GMR loop obtained by switching the 4 nm top Co film is shifted 300 Oe by the exchange bias of IrMn. Using CoO as a NOL, at thickness of 1 nm there is a sudden drop from 300 Oe to <10 Oe. It appears that pinhole coupling at CoO<1 nm forces the two Co films to switch together, but at CoO 1 nm the pinholes close up and the Co films switch separately. Such observations constitute a new approach to the study of pinholes, and we use it to investigate several oxides and metal spacer layers.

Membranes, methods of making membranes, and methods of separating gases using membranes

DOEpatents

Ho, W. S. Winston

2012-10-02

Membranes, methods of making membranes, and methods of separating gases using membranes are provided. The membranes can include at least one hydrophilic polymer, at least one cross-linking agent, at least one base, and at least one amino compound. The methods of separating gases using membranes can include contacting a gas stream containing at least one of CO.sub.2, H.sub.2S, and HCl with one side of a nonporous and at least one of CO.sub.2, H.sub.2S, and HCl selectively permeable membrane such that at least one of CO.sub.2, H.sub.2S, and HCl is selectively transported through the membrane.

The inevitable journey to being

PubMed Central

Russell, Michael J.; Nitschke, Wolfgang; Branscomb, Elbert

2013-01-01

Life is evolutionarily the most complex of the emergent symmetry-breaking, macroscopically organized dynamic structures in the Universe. Members of this cascading series of disequilibria-converting systems, or engines in Cottrell's terminology, become ever more complicated—more chemical and less physical—as each engine extracts, exploits and generates ever lower grades of energy and resources in the service of entropy generation. Each one of these engines emerges spontaneously from order created by a particular mother engine or engines, as the disequilibrated potential daughter is driven beyond a critical point. Exothermic serpentinization of ocean crust is life's mother engine. It drives alkaline hydrothermal convection and thereby the spontaneous production of precipitated submarine hydrothermal mounds. Here, the two chemical disequilibria directly causative in the emergence of life spontaneously arose across the mineral precipitate membranes separating the acidulous, nitrate-bearing CO2-rich, Hadean sea from the alkaline and CH4/H2-rich serpentinization-generated effluents. Essential redox gradients—involving hydrothermal CH4 and H2 as electron donors, CO2 and nitrate, nitrite, and ferric iron from the ambient ocean as acceptors—were imposed which functioned as the original ‘carbon-fixing engine’. At the same time, a post-critical-point (milli)voltage pH potential (proton concentration gradient) drove the condensation of orthophosphate to produce a high energy currency: ‘the pyrophosphatase engine’. PMID:23754808

The inevitable journey to being.

PubMed

Russell, Michael J; Nitschke, Wolfgang; Branscomb, Elbert

2013-07-19

Life is evolutionarily the most complex of the emergent symmetry-breaking, macroscopically organized dynamic structures in the Universe. Members of this cascading series of disequilibria-converting systems, or engines in Cottrell's terminology, become ever more complicated-more chemical and less physical-as each engine extracts, exploits and generates ever lower grades of energy and resources in the service of entropy generation. Each one of these engines emerges spontaneously from order created by a particular mother engine or engines, as the disequilibrated potential daughter is driven beyond a critical point. Exothermic serpentinization of ocean crust is life's mother engine. It drives alkaline hydrothermal convection and thereby the spontaneous production of precipitated submarine hydrothermal mounds. Here, the two chemical disequilibria directly causative in the emergence of life spontaneously arose across the mineral precipitate membranes separating the acidulous, nitrate-bearing CO2-rich, Hadean sea from the alkaline and CH4/H2-rich serpentinization-generated effluents. Essential redox gradients-involving hydrothermal CH4 and H2 as electron donors, CO2 and nitrate, nitrite, and ferric iron from the ambient ocean as acceptors-were imposed which functioned as the original 'carbon-fixing engine'. At the same time, a post-critical-point (milli)voltage pH potential (proton concentration gradient) drove the condensation of orthophosphate to produce a high energy currency: 'the pyrophosphatase engine'.

Influence of * OH adsorbates on the potentiodynamics of the CO 2 generation during the electro-oxidation of ethanol

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

Yang, Guangxing; Namin, Lida M.; Aaron Deskins, N.

Direct ethanol fuel cells (DEFCs) are a promising technology for the generation of electricity via the direct conversion of ethanol into CO2, showing higher thermodynamic efficiency and volumetric energy density than hydrogen fuel cells. However, implementation of DEFCs is hampered by the low CO2 selectivity during the ethanol oxidation reaction (EOR). Comprehensive understanding of the electro-kinetics and reaction pathways of CO2 generation via CC bond-breaking is not only a fundamental question for electro-catalysis, but also a key technological challenge since practical implementation of DEFC technology is contingent on its ability to selectively oxidize ethanol into CO2 to achieve exceptional energymore » density through 12-electron transfer reaction. Here, we present comprehensive in situ potentiodynamics studies of CO2 generation during the EOR on Pt, Pt/SnO2 and Pt/Rh/SnO2 catalysts using a house-made electrochemical cell equipped with a CO2 microelectrode. Highly sensitive CO2 measurements enable the real time detection of the partial pressure of CO2 during linear sweep voltammetry measurements, through which electro-kinetics details of CO2 generation can be obtained. In situ CO2 measurements provide the mechanistic understanding of potentiodynamics of the EOR, particularly the influence of *OH adsorbates on CO2 generation rate and selectivity. Density functional theory (DFT) simulations of Pt, Pt/SnO2, and Pt/Rh/SnO2 surfaces clarify reaction details over these catalysts. Our results show that at low potentials, inadequate *OH adsorbates impair the removal of reaction intermediates, and thus Pt/Rh/SnO2 exhibited the best performance toward CO2 generation, while at high potentials, Rh sites were overwhelmingly occupied (poisoned) by *OH adsorbates, and thus Pt/SnO2 exhibited the best performance toward CO2 generation.« less

Influence of *OH adsorbates on the potentiodynamics of the CO 2 generation during the electro-oxidation of ethanol

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

Yang, Guangxing; Namin, Lida M.; Aaron Deskins, N.

Direct ethanol fuel cells (DEFCs) are a promising technology for the generation of electricity via the direct conversion of ethanol into CO 2, showing higher thermodynamic efficiency and volumetric energy density than hydrogen fuel cells. However, implementation of DEFCs is hampered by the low CO 2 selectivity during the ethanol oxidation reaction (EOR). Comprehensive understanding of the electro-kinetics and reaction pathways of CO 2 generation via CC bond-breaking is not only a fundamental question for electro-catalysis, but also a key technological challenge since practical implementation of DEFC technology is contingent on its ability to selectively oxidize ethanol into CO 2more » to achieve exceptional energy density through 12-electron transfer reaction. Here, we present comprehensive in situ potentiodynamics studies of CO 2 generation during the EOR on Pt, Pt/SnO 2 and Pt/Rh/SnO 2 catalysts using a house-made electrochemical cell equipped with a CO 2 microelectrode. Highly sensitive CO 2 measurements enable the real time detection of the partial pressure of CO 2 during linear sweep voltammetry measurements, through which electro-kinetics details of CO 2 generation can be obtained. In situ CO 2 measurements provide the mechanistic understanding of potentiodynamics of the EOR, particularly the influence of *OH adsorbates on CO 2 generation rate and selectivity. Density functional theory (DFT) simulations of Pt, Pt/SnO 2, and Pt/Rh/SnO 2 surfaces clarify reaction details over these catalysts. Our results show that at low potentials, inadequate *OH adsorbates impair the removal of reaction intermediates, and thus Pt/Rh/SnO 2 exhibited the best performance toward CO 2 generation, while at high potentials, Rh sites were overwhelmingly occupied (poisoned) by *OH adsorbates, and thus Pt/SnO 2 exhibited the best performance toward CO 2 generation.« less

Mixed matrix membranes with fast and selective transport pathways for efficient CO2 separation

NASA Astrophysics Data System (ADS)

Hou, Jinpeng; Li, Xueqin; Guo, Ruili; Zhang, Jianshu; Wang, Zhongming

2018-03-01

To improve CO2 separation performance, porous carbon nanosheets (PCNs) were used as a filler into a Pebax MH 1657 (Pebax) matrix, fabricating mixed matrix membranes (MMMs). The PCNs exhibited a preferential horizontal orientation within the Pebax matrix because of the extremely large 2D plane and nanoscale thickness of the matrix. Therefore, the micropores of the PCNs provided fast CO2 transport pathways, which led to increased CO2 permeability. The reduced pore size of the PCNs was a consequence of the overlapping of PCNs and the polymer chains penetrating into the pores of the PCNs. The reduction in the pore size of the PCNs improved the CO2/gas selectivity. As a result, the CO2 permeability and CO2/CH4 selectivity of the Pebax membrane with 10 wt% PCNs-loading (Pebax-PCNs-10) were 520 barrer and 51, respectively, for CO2/CH4 mixed-gas. The CO2 permeability and CO2/N2 selectivity of the Pebax-PCNs-10 membrane were 614 barrer and 61, respectively, for CO2/N2 mixed-gas.

Expression of calcification and metabolism-related genes in response to elevated pCO2 and temperature in the reef-building coral Acropora millepora.

PubMed

Rocker, Melissa M; Noonan, Sam; Humphrey, Craig; Moya, Aurelie; Willis, Bette L; Bay, Line K

2015-12-01

Declining health of scleractinian corals in response to deteriorating environmental conditions is widely acknowledged, however links between physiological and functional genomic responses of corals are less well understood. Here we explore growth and the expression of 20 target genes with putative roles in metabolism and calcification in the branching coral, Acropora millepora, in two separate experiments: 1) elevated pCO2 (464, 822, 1187 and 1638 μatm) and ambient temperature (27°C), and 2) elevated pCO2 (490 and 822 μatm) and temperature (28 and 31 °C). After 14 days of exposure to elevated pCO2 and ambient temperatures, no evidence of differential expression of either calcification or metabolism genes was detected between control and elevated pCO2 treatments. After 37 days of exposure to control and elevated pCO2, Ubiquinol-Cytochrome-C Reductase Subunit 2 gene (QCR2; a gene involved in complex III of the electron chain transport within the mitochondria and critical for generation of ATP) was significantly down-regulated in the elevated pCO2 treatment in both ambient and elevated temperature treatments. Overall, the general absence of a strong response to elevated pCO2 and temperature by the other 19 targeted calcification and metabolism genes suggests that corals may not be affected by these stressors on longer time scales (37 days). These results also highlight the potential for QCR2 to act as a biomarker of coral genomic responses to changing environments. Copyright © 2015 Elsevier B.V. All rights reserved.

Inhibiting polysulfides diffusion of lithium-sulfur batteries using an acetylene black-CoS2 modified separator: Mechanism research and performance improvement

NASA Astrophysics Data System (ADS)

Zeng, Pan; Huang, Liwu; Zhang, Xinling; Han, Yamiao; Chen, Yungui

2018-01-01

Lithium-sulfur (Li-S) batteries are considered as one of the most promising chemistries in secondary energy storage field owing to their high energy density. However, the poor electrochemical performance mainly associated with the polysulfides shuttle has greatly hampered their practical application. Herein, a simple acetylene black (AB)-CoS2 coated separator is first designed to suppress the migration of polysulfides. The AB-CoS2 modified separator can not only efficiently capture the polysulfides by forming strong chemical bonding but also guarantee the rapid lithium ions diffusion. Moreover, the AB-CoS2 coating could serve as an upper current collector to accelerate electron transport for reinforcing the utilization of sulfur and ensuring the reactivation of the trapped active material. Consequently, the Li-S cell using AB-CoS2 modified separator shows a long-term cycling stability with an extremely low decay rate (0.09% per cycle) up to 450 cycles at a high rate of 2 C (3350 mA g-1). It also exhibits excellent rate capabilities, which maintains a capacity of 475 mAh g-1 even at 4.0 C rate.

Sustained phase separation and spin glass in Co-doped K x Fe 2 - y Se 2 single crystals

DOE PAGES

Ryu, Hyejin; Wang, Kefeng; Opacic, M.; ...

2015-11-19

We describe Co substitution effects in K xFe 2-y-zCo zSe 2 (0.06 ≤ z ≤ 1.73) single crystal alloys. By 3.5% of Co doping superconductivity is suppressed whereas phase separation of semiconducting K 2Fe 4Se 5 and superconducting/metallic K xFe 2Se 2 is still present. We show that the arrangement and distribution of superconducting phase (stripe phase) is connected with the arrangement of K, Fe and Co atoms. Semiconducting spin glass is found in proximity to superconducting state, persisting for large Co concentrations. At high Co concentrations ferromagnetic metallic state emerges above the spin glass. This is coincident withmore » changes of the unit cell, arrangement and connectivity of stripe conducting phase.« less

Properties and Performance Attributes of Novel Co-Extruded Polyolefin Battery Separator Materials. Part 1; Mechanical Properties

NASA Technical Reports Server (NTRS)

Baldwin, Richard S.; Guzik, Monica; Skierski, Michael

2011-01-01

As NASA prepares for its next era of manned spaceflight missions, advanced energy storage technologies are being developed and evaluated to address future mission needs and technical requirements and to provide new mission-enabling technologies. Cell-level components for advanced lithium-ion batteries possessing higher energy, more reliable performance and enhanced, inherent safety characteristics are actively under development within the NASA infrastructure. A key component for safe and reliable cell performance is the cell separator, which separates the two energetic electrodes and functions to prevent the occurrence of an internal short-circuit while enabling ionic transport. Recently, a new generation of co-extruded separator films has been developed by ExxonMobil Chemical and introduced into their battery separator product portfolio. Several grades of this new separator material have been evaluated with respect to dynamic mechanical properties and safety-related performance attributes. This paper presents the results of these evaluations in comparison to a current state-ofthe-practice separator material. The results are discussed with respect to potential opportunities to enhance the inherent safety characteristics and reliability of future, advanced lithium-ion cell chemistries.

Novel Application of Carbonate Fuel Cell for Capturing Carbon Dioxide from Flue Gas Streams

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

Jolly, Stephen; Ghezel-Ayagh, Hossein; Willman, Carl

To address concerns about climate change resulting from emission of CO2 by coal-fueled power plants, FuelCell Energy, Inc. has developed the Combined Electric Power and Carbon-dioxide Separation (CEPACS) system concept. The CEPACS system utilizes Electrochemical Membrane (ECM) technology derived from the Company’s Direct FuelCell® products. The system separates the CO2 from the flue gas of other plants and produces electric power using a supplementary fuel. FCE is currently evaluating the use of ECM to cost effectively separate CO2 from the flue gas of Pulverized Coal (PC) power plants under a U.S. Department of Energy contract. The overarching objective of themore » project is to verify that the ECM can achieve at least 90% CO2 capture from the flue gas with no more than 35% increase in the cost of electricity. The project activities include: 1) laboratory scale operational and performance tests of a membrane assembly, 2) performance tests of the membrane to evaluate the effects of impurities present in the coal plant flue gas, in collaboration with Pacific Northwest National Laboratory, 3) techno-economic analysis for an ECM-based CO2 capture system applied to a 550 MW existing PC plant, in partnership with URS Corporation, and 4) bench scale (11.7 m2 area) testing of an ECM-based CO2 separation and purification system.« less

Mechanistic insights into porous graphene membranes for helium separation and hydrogen purification

NASA Astrophysics Data System (ADS)

Wei, Shuxian; Zhou, Sainan; Wu, Zhonghua; Wang, Maohuai; Wang, Zhaojie; Guo, Wenyue; Lu, Xiaoqing

2018-05-01

Porous graphene (PG) and nitrogen-substituted PG monolayers of 3N-PG and 6N-PG were designed as effective membranes for the separation of He and H2 over Ne, Ar, N2, CO, and CH4 by using density functional theory. Results showed that PG and 3N-PG exhibited suitable pore sizes and relatively high stabilities for He and H2 separation. PG and 3N-PG membranes also presented excellent He and H2 selectivities over Ne, Ar, N2, CO and CH4 at a wide temperature range. 6N-PG membrane exerted unexceptionable permeances of the studied gases, especially He and H2, which could remarkably improve the separation efficiency of He and H2. Analyses on the most stable adsorption configurations and maximum adsorption energies indicated weak Van der Waals interactions between the gases and the three PG-based membranes. Microscopic permeation process analyses based on the minimum energy pathway, energy profiles, and electron density isosurfaces elucidated the remarkable selectivities of He over Ne/CO/N2/Ar/CH4 and H2 over CO/N2/CH4 and the high permeances of He and H2 passing through the three PG-based membranes. This work not only highlighted the potential use of the three PG-based membranes for He separation and H2 purification but also provided a superior alternative strategy to design and screen membrane materials for gas separation.

Oxidant enhancement in martian dust devils and storms: storm electric fields and electron dissociative attachment.

PubMed

Delory, Gregory T; Farrell, William M; Atreya, Sushil K; Renno, Nilton O; Wong, Ah-San; Cummer, Steven A; Sentman, Davis D; Marshall, John R; Rafkin, Scot C R; Catling, David C

2006-06-01

Laboratory studies, numerical simulations, and desert field tests indicate that aeolian dust transport can generate atmospheric electricity via contact electrification or "triboelectricity." In convective structures such as dust devils and dust storms, grain stratification leads to macroscopic charge separations and gives rise to an overall electric dipole moment in the aeolian feature, similar in nature to the dipolar electric field generated in terrestrial thunderstorms. Previous numerical simulations indicate that these storm electric fields on Mars can approach the ambient breakdown field strength of approximately 25 kV/m. In terrestrial dust phenomena, potentials ranging from approximately 20 to 160 kV/m have been directly measured. The large electrostatic fields predicted in martian dust devils and storms can energize electrons in the low pressure martian atmosphere to values exceeding the electron dissociative attachment energy of both CO2 and H2O, which results in the formation of the new chemical products CO/O- and OH/H-, respectively. Using a collisional plasma physics model, we present calculations of the CO/O- and OH/H- reaction and production rates. We demonstrate that these rates vary geometrically with the ambient electric field, with substantial production of dissociative products when fields approach the breakdown value of approximately 25 kV/m. The dissociation of H2O into OH/H- provides a key ingredient for the generation of oxidants; thus electrically charged dust may significantly impact the habitability of Mars.

Predictive framework for shape-selective separations in three-dimensional zeolites and metal-organic frameworks.

PubMed

First, Eric L; Gounaris, Chrysanthos E; Floudas, Christodoulos A

2013-05-07

With the growing number of zeolites and metal-organic frameworks (MOFs) available, computational methods are needed to screen databases of structures to identify those most suitable for applications of interest. We have developed novel methods based on mathematical optimization to predict the shape selectivity of zeolites and MOFs in three dimensions by considering the energy costs of transport through possible pathways. Our approach is applied to databases of over 1800 microporous materials including zeolites, MOFs, zeolitic imidazolate frameworks, and hypothetical MOFs. New materials are identified for applications in gas separations (CO2/N2, CO2/CH4, and CO2/H2), air separation (O2/N2), and chemicals (propane/propylene, ethane/ethylene, styrene/ethylbenzene, and xylenes).

Enhanced charge separation of rutile TiO2 nanorods by trapping holes and transferring electrons for efficient cocatalyst-free photocatalytic conversion of CO2 to fuels.

PubMed

Wu, Jing; Lu, Hongwei; Zhang, Xuliang; Raziq, Fazal; Qu, Yang; Jing, Liqiang

2016-04-11

Modification with chloride and phosphate anions, and coupling with carbon nanotubes could effectively trap holes and transfer the electrons of rutile nanorods, respectively, so as to greatly promote photogenerated charge separation, leading to an obviously-improved cocatalyst-free photocatalytic conversion of CO2 to CH4 and CO, along with the positive effects of constructed phosphate bridges.

Mitochondrial Ubiquinone Homologues, Superoxide Radical Generation, and Longevity in Different Mammalian Species*

PubMed Central

Lass, Achim; Agarwal, Sanjiv; Sohal, Rajindar S.

2010-01-01

Rates of mitochondrial superoxide anion radical ( O2·¯) generation are known to be inversely correlated with the maximum life span potential of different mammalian species. The objective of this study was to understand the possible mechanism(s) underlying such variations in the rate of O2·¯ generation. The hypothesis that the relative amounts of the ubiquinones or coenzyme Q (CoQ) homologues, CoQ9 and CoQ10, are related with the rate of O2·¯ generation was tested. A comparison of nine different mammalian species, namely mouse, rat, guinea pig, rabbit, pig, goat, sheep, cow, and horse, which vary from 3.5 to 46 years in their maximum longevity, indicated that the rate of O2·¯ generation in cardiac submitochondrial particles (SMPs) was directly related to the relative amount of CoQ9 and inversely related to the amount of CoQ10, extractable from their cardiac mitochondria. To directly test the relationship between CoQ homologues and the rate of O2·¯ generation, rat heart SMPs, naturally containing mainly CoQ9 and cow heart SMPs, with high natural CoQ10 content, were chosen for depletion/reconstitution experiments. Repeated extractions of rat heart SMPs with pentane exponentially depleted both CoQ homologues while the corresponding rates of O2·¯ generation and oxygen consumption were lowered linearly. Reconstitution of both rat and cow heart SMPs with different amounts of CoQ9 or CoQ10 caused an initial increase in the rates of O2·¯ generation, followed by a plateau at high concentrations. Within the physiological range of CoQ concentrations, there were no differences in the rates of O2·¯ generation between SMPs reconstituted with CoQ9 or CoQ10. Only at concentrations that were considerably higher than the physiological level, the SMPs reconstituted with CoQ9 exhibited higher rates of O2·¯ generation than those obtained with CoQ10. These in vitro findings do not support the hypothesis that differences in the distribution of CoQ homologues are responsible for the variations in the rates of mitochondrial O2·¯ generation in different mammalian species. PMID:9235911

Stable Isotope Quantitative N-Glycan Analysis by Liquid Separation Techniques and Mass Spectrometry.

PubMed

Mittermayr, Stefan; Albrecht, Simone; Váradi, Csaba; Millán-Martín, Silvia; Bones, Jonathan

2017-01-01

Liquid phase separation analysis and subsequent quantitation remains a challenging task for protein-derived oligosaccharides due to their inherent structural complexity and diversity. Incomplete resolution or co-detection of multiple glycan species complicates peak area-based quantitation and associated statistical analysis when optical detection methods are used. The approach outlined herein describes the utilization of stable isotope variants of commonly used fluorescent tags that allow for mass-based glycan identification and relative quantitation following separation by liquid chromatography (LC) or capillary electrophoresis (CE). Comparability assessment of glycoprotein-derived oligosaccharides is performed by derivatization with commercially available isotope variants of 2-aminobenzoic acid or aniline and analysis by LC- and CE-mass spectrometry. Quantitative information is attained from the extracted ion chromatogram/electropherogram ratios generated from the light and heavy isotope clusters.

Ion-Gated Gas Separation through Porous Graphene

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

Tian, Ziqi; Mahurin, Shannon M.; Dai, Sheng

Porous graphene holds great promise as an atom-thin, high-permeance membrane for gas separation, but to precisely control the pore size at three to five angstroms proves challenging. Here we propose an ion-gated graphene membrane comprising a monolayer of ionic liquid coated porous graphene to dynamically modulate the pore size to achieve selective gas separation. This approach enables the otherwise non-selective large pores on the order of 1 nm in size to be selective for gases whose diameters range from three to four angstroms. We show from molecular dynamics simulations that CO 2, N 2 and CH 4 all can permeatemore » through a 1-nm pore in graphene without any selectivity. But when a monolayer of [emim][BF 4] is deposited on the porous graphene, CO 2 has much higher permeance than the other two gases. We find that the anion dynamically modulates the pore size by hovering above the pore and provides affinity for CO 2 while the larger cation (which cannot go through the pore) holds the anion in place via electrostatic attraction. This composite membrane is especially promising for CO 2/CH 4 separation, with a CO 2/CH 4 selectivity of about 42 and CO 2 permeance ~105 GPU (gas permeation unit). We further demonstrate that selectivity and permeance can be tuned by the anion size. The present work points toward a promising direction of using the atom-thin ionic-liquid/porous-graphene hybrid membrane for high-permeance, selective gas separation that allows a greater flexibility in substrate pore size control.« less

Ion-Gated Gas Separation through Porous Graphene

DOE PAGES

Tian, Ziqi; Mahurin, Shannon M.; Dai, Sheng; ...

2017-02-10

Porous graphene holds great promise as an atom-thin, high-permeance membrane for gas separation, but to precisely control the pore size at three to five angstroms proves challenging. Here we propose an ion-gated graphene membrane comprising a monolayer of ionic liquid coated porous graphene to dynamically modulate the pore size to achieve selective gas separation. This approach enables the otherwise non-selective large pores on the order of 1 nm in size to be selective for gases whose diameters range from three to four angstroms. We show from molecular dynamics simulations that CO 2, N 2 and CH 4 all can permeatemore » through a 1-nm pore in graphene without any selectivity. But when a monolayer of [emim][BF 4] is deposited on the porous graphene, CO 2 has much higher permeance than the other two gases. We find that the anion dynamically modulates the pore size by hovering above the pore and provides affinity for CO 2 while the larger cation (which cannot go through the pore) holds the anion in place via electrostatic attraction. This composite membrane is especially promising for CO 2/CH 4 separation, with a CO 2/CH 4 selectivity of about 42 and CO 2 permeance ~105 GPU (gas permeation unit). We further demonstrate that selectivity and permeance can be tuned by the anion size. The present work points toward a promising direction of using the atom-thin ionic-liquid/porous-graphene hybrid membrane for high-permeance, selective gas separation that allows a greater flexibility in substrate pore size control.« less

Spinel type CoFe oxide porous nanosheets as magnetic adsorbents with fast removal ability and facile separation.

PubMed

Ge, X; Gu, C D; Wang, X L; Tu, J P

2015-09-15

Adsorption is often time consuming due to slow diffusion kinetic. Sizing he adsorbent down might help to accelerate adsorption. For CoFe spinel oxide, a magnetically separable adsorbent, the preparation of nanosheets faces many challenges including phase separation, grain growth and difficulty in preparing two-dimensional materials. In this work, we prepared porous CoFe oxide nanosheet with chemical formula of Co2.698Fe0.302O4 through topochemical transformation of a CoFe precursor, which has a layered double hydroxide (LDH) analogue structure and a large interlayer spacing. The LDH precursor was synthesized from a cheap deep eutectic solvent (DES) system. The calcined Co2.698Fe0.302O4 has small grain size (10-20nm), nanosheet morphology, and porous structure, which contribute to a large specific surface area of 79.5m(2)g(-1). The Co2.698Fe0.302O4 nanosheets show fast removal ability and good adsorption capacity for both organic waste (305mgg(-1) in 5min for Congo red) and toxic heavy metal ion (5.27mgg(-1) in 30min for Cr (VI)). Furthermore, the Co2.698Fe0.302O4 can be separated magnetically. Considering the precursor can be prepared through a fast, simple, surfactant-free and high-yield synthetic strategy, this work should have practical significance in fabricating adsorbents. Copyright © 2015 Elsevier Inc. All rights reserved.

The oxycoal process with cryogenic oxygen supply.

PubMed

Kather, Alfons; Scheffknecht, Günter

2009-09-01

Due to its large reserves, coal is expected to continue to play an important role in the future. However, specific and absolute CO2 emissions are among the highest when burning coal for power generation. Therefore, the capture of CO2 from power plants may contribute significantly in reducing global CO2 emissions. This review deals with the oxyfuel process, where pure oxygen is used for burning coal, resulting in a flue gas with high CO2 concentrations. After further conditioning, the highly concentrated CO2 is compressed and transported in the liquid state to, for example, geological storages. The enormous oxygen demand is generated in an air-separation unit by a cryogenic process, which is the only available state-of-the-art technology. The generation of oxygen and the purification and liquefaction of the CO2-enriched flue gas consumes significant auxiliary power. Therefore, the overall net efficiency is expected to be lowered by 8 to 12 percentage points, corresponding to a 21 to 36% increase in fuel consumption. Oxygen combustion is associated with higher temperatures compared with conventional air combustion. Both the fuel properties as well as limitations of steam and metal temperatures of the various heat exchanger sections of the steam generator require a moderation of the temperatures during combustion and in the subsequent heat-transfer sections. This is done by means of flue gas recirculation. The interdependencies among fuel properties, the amount and the temperature of the recycled flue gas, and the resulting oxygen concentration in the combustion atmosphere are investigated. Expected effects of the modified flue gas composition in comparison with the air-fired case are studied theoretically and experimentally. The different atmosphere resulting from oxygen-fired combustion gives rise to various questions related to firing, in particular, with regard to the combustion mechanism, pollutant reduction, the risk of corrosion, and the properties of the fly ash or the deposits that form. In particular, detailed nitrogen and sulphur chemistry was investigated by combustion tests in a laboratory-scale facility. Oxidant staging, in order to reduce NO formation, turned out to work with similar effectiveness as for conventional air combustion. With regard to sulphur, a considerable increase in the SO2 concentration was found, as expected. However, the H2S concentration in the combustion atmosphere increased as well. Further results were achieved with a pilot-scale test facility, where acid dew points were measured and deposition probes were exposed to the combustion environment. Besides CO2 and water vapour, the flue gas contains impurities like sulphur species, nitrogen oxides, argon, nitrogen, and oxygen. The CO2 liquefaction is strongly affected by these impurities in terms of the auxiliary power requirement and the CO2 capture rate. Furthermore, the impurity of the liquefied CO2 is affected as well. Since the requirements on the liquid CO2 with regard to geological storage or enhanced oil recovery are currently undefined, the effects of possible flue gas treatment and the design of the liquefaction plant are studied over a wide range.

The oxycoal process with cryogenic oxygen supply

NASA Astrophysics Data System (ADS)

Kather, Alfons; Scheffknecht, Günter

2009-09-01

Due to its large reserves, coal is expected to continue to play an important role in the future. However, specific and absolute CO2 emissions are among the highest when burning coal for power generation. Therefore, the capture of CO2 from power plants may contribute significantly in reducing global CO2 emissions. This review deals with the oxyfuel process, where pure oxygen is used for burning coal, resulting in a flue gas with high CO2 concentrations. After further conditioning, the highly concentrated CO2 is compressed and transported in the liquid state to, for example, geological storages. The enormous oxygen demand is generated in an air-separation unit by a cryogenic process, which is the only available state-of-the-art technology. The generation of oxygen and the purification and liquefaction of the CO2-enriched flue gas consumes significant auxiliary power. Therefore, the overall net efficiency is expected to be lowered by 8 to 12 percentage points, corresponding to a 21 to 36% increase in fuel consumption. Oxygen combustion is associated with higher temperatures compared with conventional air combustion. Both the fuel properties as well as limitations of steam and metal temperatures of the various heat exchanger sections of the steam generator require a moderation of the temperatures during combustion and in the subsequent heat-transfer sections. This is done by means of flue gas recirculation. The interdependencies among fuel properties, the amount and the temperature of the recycled flue gas, and the resulting oxygen concentration in the combustion atmosphere are investigated. Expected effects of the modified flue gas composition in comparison with the air-fired case are studied theoretically and experimentally. The different atmosphere resulting from oxygen-fired combustion gives rise to various questions related to firing, in particular, with regard to the combustion mechanism, pollutant reduction, the risk of corrosion, and the properties of the fly ash or the deposits that form. In particular, detailed nitrogen and sulphur chemistry was investigated by combustion tests in a laboratory-scale facility. Oxidant staging, in order to reduce NO formation, turned out to work with similar effectiveness as for conventional air combustion. With regard to sulphur, a considerable increase in the SO2 concentration was found, as expected. However, the H2S concentration in the combustion atmosphere increased as well. Further results were achieved with a pilot-scale test facility, where acid dew points were measured and deposition probes were exposed to the combustion environment. Besides CO2 and water vapour, the flue gas contains impurities like sulphur species, nitrogen oxides, argon, nitrogen, and oxygen. The CO2 liquefaction is strongly affected by these impurities in terms of the auxiliary power requirement and the CO2 capture rate. Furthermore, the impurity of the liquefied CO2 is affected as well. Since the requirements on the liquid CO2 with regard to geological storage or enhanced oil recovery are currently undefined, the effects of possible flue gas treatment and the design of the liquefaction plant are studied over a wide range.

A lignocellulosic ethanol strategy via nonenzymatic sugar production: process synthesis and analysis.

PubMed

Han, Jeehoon; Luterbacher, Jeremy S; Alonso, David Martin; Dumesic, James A; Maravelias, Christos T

2015-04-01

The work develops a strategy for the production of ethanol from lignocellulosic biomass. In this strategy, the cellulose and hemicellulose fractions are simultaneously converted to sugars using a γ-valerolactone (GVL) solvent containing a dilute acid catalyst. To effectively recover GVL for reuse as solvent and biomass-derived lignin for heat and power generation, separation subsystems, including a novel CO2-based extraction for the separation of sugars from GVL, lignin and humins have been designed. The sugars are co-fermented by yeast to produce ethanol. Furthermore, heat integration to reduce utility requirements is performed. It is shown that this strategy leads to high ethanol yields and the total energy requirements could be satisfied by burning the lignin. The integrated strategy using corn stover feedstock leads to a minimum selling price of $5 per gallon of gasoline equivalent, which suggests that it is a promising alternative to current biofuels production approaches. Copyright © 2015 Elsevier Ltd. All rights reserved.

Dynamic adsorption of CO2/N2 on cation-exchanged chabazite SSZ-13: A breakthrough analysis

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

Bower, Jamey K.; Barpaga, Dushyant; Prodinger, Sebastian

2018-04-17

Alkali exchanged SSZ-13 adsorbents were investigated for their applicability in separating N2 from CO2 in flue gas streams using a dynamic breakthrough method. In contrast to IAST calculations based on equilibrium isotherms, K+ exchanged SSZ-13 was found to yield the best N2 productivity under dynamic conditions where diffusion properties play a significant role. This was attributed to the selective, partial blockage of access to the CHA cavities enhancing the separation potential in a 15/85 CO2/N2 binary gas mixture.

Dynamic Adsorption of CO 2 /N 2 on Cation-Exchanged Chabazite SSZ-13: A Breakthrough Analysis

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

Bower, Jamey K.; Barpaga, Dushyant; Prodinger, Sebastian

2018-03-30

Alkali exchanged SSZ-13 adsorbents were investigated for their applicability in separating N2 from CO 2 in flue gas streams using a dynamic breakthrough method. In contrast to IAST calculations based on equilibrium isotherms, K+ exchanged SSZ-13 was found to yield the best N2 productivity under dynamic conditions where diffusion properties play a significant role. This was attributed to the selective, partial blockage of access to the CHA cavities enhancing the separation potential in a 15/85 CO2/N2 binary gas mixture.

CONCEPTUAL DESIGN AND ECONOMICS OF THE ADVANCED CO2 HYBRID POWER CYCLE

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

A. Nehrozoglu

2004-12-01

Research has been conducted under United States Department of Energy Contract DEFC26-02NT41621 to analyze the feasibility of a new type of coal-fired plant for electric power generation. This new type of plant, called the Advanced CO{sub 2} Hybrid Power Plant, offers the promise of efficiencies nearing 36 percent, while concentrating CO{sub 2} for 100% sequestration. Other pollutants, such as SO{sub 2} and NOx, are sequestered along with the CO{sub 2} yielding a zero emissions coal plant. The CO{sub 2} Hybrid is a gas turbine-steam turbine combined cycle plant that uses CO{sub 2} as its working fluid to facilitate carbon sequestration. The key components of the plant are a cryogenic air separation unit (ASU), a pressurized circulating fluidized bed gasifier, a CO{sub 2} powered gas turbine, a circulating fluidized bed boiler, and a super-critical pressure steam turbine. The gasifier generates a syngas that fuels the gas turbine and a char residue that, together with coal, fuels a CFB boiler to power the supercritical pressure steam turbine. Both the gasifier and the CFB boiler use a mix of ASU oxygen and recycled boiler flue gas as their oxidant. The resulting CFB boiler flue gas is essentially a mixture of oxygen, carbon dioxide and water. Cooling the CFB flue gas to 80 deg. F condenses most of the moisture and leaves a CO{sub 2} rich stream containing 3%v oxygen. Approximately 30% of this flue gas stream is further cooled, dried, and compressed for pipeline transport to the sequestration site (the small amount of oxygen in this stream is released and recycled to the system when the CO{sub 2} is condensed after final compression and cooling). The remaining 70% of the flue gas stream is mixed with oxygen from the ASU and is ducted to the gas turbine compressor inlet. As a result, the gas turbine compresses a mixture of carbon dioxide (ca. 64%v) and oxygen (ca. 32.5%v) rather than air. This carbon dioxide rich mixture then becomes the gas turbine working fluid and also becomes the oxidant in the gasification and combustion processes. As a result, the plant provides CO{sub 2} for sequestration without the performance and economic penalties associated with water gas shifting and separating CO{sub 2} from gas streams containing nitrogen. The cost estimate of the reference plant (the Foster Wheeler combustion hybrid) was based on a detailed prior study of a nominal 300 MWe demonstration plant with a 6F turbine. Therefore, the reference plant capital costs were found to be 30% higher than an estimate for a 425 MW fully commercial IGCC with an H class turbine (1438more » $/kW vs. 1111 $$/kW). Consequently, the capital cost of the CO{sub 2} hybrid plant was found to be 25% higher than that of the IGCC with pre-combustion CO{sub 2} removal (1892 $$/kW vs. 1510 $/kW), and the levelized cost of electricity (COE) was found to be 20% higher (7.53 c/kWh vs. 6.26 c/kWh). Although the final costs for the CO{sub 2} hybrid are higher, the study confirms that the relative change in cost (or mitigation cost) will be lower. The conceptual design of the plant and its performance and cost, including losses due to CO{sub 2} sequestration, is reported. Comparison with other proposed power plant CO{sub 2} removal techniques reported by a December 2000 EPRI report is shown. This project supports the DOE research objective of development of concepts for the capture and storage of CO{sub 2}.« less

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

PubMed

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

2015-08-04

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

In vitro differentiation of neural cells from human adipose tissue derived stromal cells.

PubMed

Dave, Shruti D; Patel, Chetan N; Vanikar, Aruna V; Trivedi, Hargovind L

2018-01-01

Stem cells, including neural stem cells (NSCs), are endowed with self-renewal capability and hence hold great opportunity for the institution of replacement/protective therapy. We propose a method for in vitro generation of stromal cells from human adipose tissue and their differentiation into neural cells. Ten grams of donor adipose tissue was surgically resected from the abdominal wall of the human donor after the participants' informed consents. The resected adipose tissue was minced and incubated for 1 hour in the presence of an enzyme (collagenase-type I) at 37 0 C followed by its centrifugation. After centrifugation, the supernatant and pellets were separated and cultured in a medium for proliferation at 37 0 C with 5% CO2 for 9-10 days in separate tissue culture dishes for generation of mesenchymal stromal cells (MSC). At the end of the culture, MSC were harvested and analyzed. The harvested MSC were subjected for further culture for their differentiation into neural cells for 5-7 days using differentiation medium mainly comprising of neurobasal medium. At the end of the procedure, culture cells were isolated and studied for expression of transcriptional factor proteins: orthodenticle homolog-2 (OTX-2), beta-III-tubulin (β3-Tubulin), glial-fibrillary acid protein (GFAP) and synaptophysin-β2. In total, 50 neural cells-lines were generated. In vitro generated MSC differentiated neural cells' mean quantum was 5.4 ± 6.9 ml with the mean cell count being, 5.27 ± 2.65 × 10 3/ μl. All of them showed the presence of OTX-2, β3-Tubulin, GFAP, synaptophysin-β2. Neural cells can be differentiated in vitro from MSC safely and effectively. In vitro generated neural cells represent a potential therapy for recovery from spinal cord injuries and neurodegenerative disease.

Space station molecular sieve development

NASA Technical Reports Server (NTRS)

Chang, C.; Rousseau, J.

1986-01-01

An essential function of a space environmental control system is the removal of carbon dioxide (CO2) from the atmosphere to control the partial pressure of this gas at levels lower than 3 mm Hg. The use of regenerable solid adsorbents for this purpose was demonstrated effectively during the Skylab mission. Earlier sorbent systems used zeolite molecular sieves. The carbon molecular sieve is a hydrophobic adsorbent with excellent potential for space station application. Although carbon molecular sieves were synthesized and investigated, these sieves were designed to simulate the sieving properties of 5A zeolite and for O2/N2 separation. This program was designed to develop hydrophobic carbon molecular sieves for CO2 removal from a space station crew environment. It is a first phase effort involved in sorbent material development and in demonstrating the utility of such a material for CO2 removal on space stations. The sieve must incorporate the following requirements: it must be hydrophobic; it must have high dynamic capacity for carbon dioxide at the low partial pressure of the space station atmosphere; and it must be chemiclly stable and will not generate contaminants.

Experimental study on CO2 frosting and clogging in a brazed plate heat exchanger for natural gas liquefaction process

NASA Astrophysics Data System (ADS)

Wu, Jitan; He, Tianbiao; Ju, Yonglin

2018-04-01

The plate-fin heat exchanger (PFHE), which has been widely used in natural gas liquefaction (LNG) industry at present, has some disadvantages such as being sensitive to the impurities in the feed gas, such as water, CO2 and H2S. Compared with the PFHE, the brazed plate heat exchanger (BPHE), which has been applied in some boil off gas (BOG) recycling LNG plants of small to middle size, has simpler inherent structure and higher impurity tolerance. In this study the BPHE is suggested to replace the PFHE to simplify or even omit the massive CO2 purification equipment for the LNG process. A set of experimental apparatus is designed and constructed to investigate the influence of the CO2 concentration of the natural gas on solid precipitation inside a typical BPHE meanly by considering the flow resistance throughout the LNG process. The results show that the maximum allowable CO2 concentration of the natural gas liquefied in the BPHE is two orders of magnitude higher than that in the PFHE under the same condition. In addition, the solid-liquid separation for the CO2 impurity is studied and the reasonable separating temperature is obtained. The solid CO2 should be separated below 135 K under the pressure of 3 MPa.

Waste Water for Power Generation via Energy Efficient Selective Silica Separations

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

Nenoff, Tina M.; Brady, Patrick Vane; Sasan, Koroush

Silica is ubiquitous in produced and industrial waters, and plays a major disruptive role in water recycle. Herein we have investigated the use of mixed oxides for the removal of silica from these waters, and their incorporation into a low cost and low energy water purification process. High selectivity hydrotalcite (HTC, (Mg 6Al 2(OH) 16(CO 3)•4H 2O)), is combined in series with high surface area active alumina (AA, (Al 2O 3)) as the dissolved silica removal media. Batch test results indicated that combined HTC/AA is a more effective method for removing silica from industrial cooling tower wasters (CTW) than usingmore » HTC or AA separately. The silica uptake via ion exchange on the mixed oxides was confirmed by Fourier transform infrared (FTIR), and Energy dispersive spectroscopy (EDS). Furthermore, HTC/AA effectively removes silica from CTW even in the presence of large concentrations of competing anions, such as Cl -, NO 3 - HCO 3 -, CO 3 2- and SO 4 2-. Similar to batch tests, Single Path Flow Through (SPFT) tests with sequential HTC/AA column filtration has very high silica removal too. Technoeconomic Analysis (TEA) was simultaneously performed for cost comparisons to existing silica removal technologies.« less

Investigation of Cross-Linked and Additive Containing Polymer Materials for Membranes with Improved Performance in Pervaporation and Gas Separation

PubMed Central

Hunger, Katharina; Schmeling, Nadine; Jeazet, Harold B. Tanh; Janiak, Christoph; Staudt, Claudia; Kleinermanns, Karl

2012-01-01

Pervaporation and gas separation performances of polymer membranes can be improved by crosslinking or addition of metal-organic frameworks (MOFs). Crosslinked copolyimide membranes show higher plasticization resistance and no significant loss in selectivity compared to non-crosslinked membranes when exposed to mixtures of CO2/CH4 or toluene/cyclohexane. Covalently crosslinked membranes reveal better separation performances than ionically crosslinked systems. Covalent interlacing with 3-hydroxypropyldimethylmaleimide as photocrosslinker can be investigated in situ in solution as well as in films, using transient UV/Vis and FTIR spectroscopy. The photocrosslinking yield can be determined from the FTIR-spectra. It is restricted by the stiffness of the copolyimide backbone, which inhibits the photoreaction due to spatial separation of the crosslinker side chains. Mixed-matrix membranes (MMMs) with MOFs as additives (fillers) have increased permeabilities and often also selectivities compared to the pure polymer. Incorporation of MOFs into polysulfone and Matrimid® polymers for MMMs gives defect-free membranes with performances similar to the best polymer membranes for gas mixtures, such as O2/N2 H2/CH4, CO2/CH4, H2/CO2, CH4/N2 and CO2/N2 (preferentially permeating gas is named first). The MOF porosity, its particle size and content in the MMM are factors to influence the permeability and the separation performance of the membranes. PMID:24958427

Optical Breath Gas Sensor for Extravehicular Activity Application

NASA Technical Reports Server (NTRS)

Wood, William R.; Casias, Miguel E.; Vakhtin, Andrei B.; Pilgrim, Jeffrey S.; Chullen, Cinda; Falconi, Eric A.; McMillin, Summer

2013-01-01

The function of the infrared gas transducer used during extravehicular activity in the current space suit is to measure and report the concentration of carbon dioxide (CO2) in the ventilation loop. The next generation portable life support system (PLSS) requires next generation CO2 sensing technology with performance beyond that presently in use on the Space Shuttle/International Space Station extravehicular mobility unit (EMU). Accommodation within space suits demands that optical sensors meet stringent size, weight, and power requirements. A laser diode spectrometer based on wavelength modulation spectroscopy is being developed for this purpose by Vista Photonics, Inc. Two prototype devices were delivered to NASA Johnson Space Center (JSC) in September 2011. The sensors incorporate a laser diode-based CO2 channel that also includes an incidental water vapor (humidity) measurement and a separate oxygen channel using a vertical cavity surface emitting laser. Both prototypes are controlled digitally with a field-programmable gate array/microcontroller architecture. The present development extends and upgrades the earlier hardware to the Advanced PLSS 2.0 test article being constructed and tested at JSC. Various improvements to the electronics and gas sampling are being advanced by this project. The combination of low power electronics with the performance of a long wavelength laser spectrometer enables multi-gas sensors with significantly increased performance over that presently offered in the EMU.

Ultrahigh vacuum and high-pressure coadsorption of CO and H2 on Pd(111): A combined SFG, TDS, and LEED study

NASA Astrophysics Data System (ADS)

Morkel, Matthias; Rupprechter, Günther; Freund, Hans-Joachim

2003-11-01

Sum frequency generation (SFG) vibrational spectroscopy was carried out in conjunction with thermal desorption spectroscopy, low-energy electron diffraction, and Auger electron spectroscopy to examine the coadsorption of CO and H2 on Pd(111). Sequential dosing as well as various CO/H2 mixtures was utilized to study intermolecular interactions between CO and H2. Preadsorbed CO effectively prevented the dissociative adsorption of hydrogen for CO coverages ⩾0.33 ML. While preadsorbed hydrogen was able to hinder CO adsorption at low temperature (100 K), hydrogen was replaced from the surface by CO at 150 K. When 1:1 mixtures of CO/H2 were used at 100 K, hydrogen selectively hindered CO adsorption on on-top sites, while above ˜125 K no blocking of CO adsorption was observed. The observations are explained in terms of mutual site blocking, of a CO-H phase separation, and of a CO-assisted hydrogen dissolution in the Pd bulk. The temperature-dependent site blocking effect of hydrogen is attributed to the ability (inability) of surface hydrogen to diffuse into the Pd bulk above (below) ˜125 K. Nonlinear optical SFG spectroscopy allowed us to study these effects not only in ultrahigh vacuum but also in a high-pressure environment. Using an SFG-compatible ultrahigh vacuum-high-pressure cell, spectra of 1:10 CO/H2 mixtures were acquired up to 55 mbar and 550 K, with simultaneous gas chromatographic and mass spectrometric gas phase analysis. Under reaction conditions, CO coverages ⩾0.5 ML were observed which strongly limit H2 adsorption and thus may be partly responsible for the low CO hydrogenation rate. The high-pressure and high-temperature SFG spectra also showed indications of a reversible surface roughening or a highly dynamic (not perfectly ordered) CO adsorbate phase. Implications of the observed adsorbate structures on catalytic CO hydrogenation on supported Pd nanoparticles are discussed.

Co- and contra-directional vertical coupling between ferromagnetic layers with grating for short-wavelength spin wave generation

NASA Astrophysics Data System (ADS)

Graczyk, Piotr; Zelent, Mateusz; Krawczyk, Maciej

2018-05-01

The possibility to generate short spin waves (SWs) is of great interest in the field of magnonics nowadays. We present an effective and technically affordable way of conversion of long SWs, which may be generated by conventional microwave antenna, to the short, sub-micrometer waves. It is achieved by grating-assisted resonant dynamic dipolar interaction between two ferromagnetic layers separated by some distance. We analyze criteria for the optimal conversion giving a semi-analytical approach for the coupling coefficient. We show by the numerical calculations the efficient energy transfer between layers which may be either of co-directional or contra-directional type. Such a system may operate either as a short spin wave generator or a frequency filter, moving forward possible application of magnonics.

Synthesis of FeCo magnetic nanoalloys and investigation of heating properties for magnetic fluid hyperthermia

NASA Astrophysics Data System (ADS)

Çelik, Özer; Fırat, Tezer

2018-06-01

In this study, size controlled FeCo colloidal magnetic nanoalloys in the range of 11.5-37.2 nm were synthesized by surfactant assistant ball milling method. Magnetic separation technique was performed subsequent to synthesis process so as to obtain magnetic nanoalloy fluid with narrow size distribution. Particle distribution was determined by transmission electron microscope (TEM) while X-ray diffraction (XRD) measurements verified FeCo alloy formation as BCC structure. Vibrating sample magnetometer (VSM) method was used to investigate magnetic properties of nanoalloys. Maximum saturation magnetization and maximum coercivity were obtained as 172 Am2/kg for nanoparticles with the mean size of 37.2 nm and 19.4 mT for nanoparticles with the mean size of 13.3 nm, respectively. The heating ability of FeCo magnetic nanoalloys was determined through calorimetrical measurements for magnetic fluid hyperthermia (MFH) applications. Heat generation mechanisms were investigated by using linear response theory and Stoner-Wohlfarth (S-W) model. Specific absorption rate (SAR) values were obtained in the range of 2-15 W/g for magnetic field frequency of 171 kHz and magnetic field strength in between 6 and 14 mT.

Comparison through a LCA evaluation analysis of food waste disposal options from the perspective of global warming and resource recovery.

PubMed

Kim, Mi-Hyung; Kim, Jung-Wk

2010-09-01

This study evaluated feed manufacturing including dry feeding and wet feeding, composting, and landfilling for food waste disposal options from the perspective of global warming and resource recovery. The method of the expanded system boundaries was employed in order to compare different by-products. The whole stages of disposal involved in the systems such as separate discharge, collection, transportation, treatment, and final disposal, were included in the system boundary and evaluated. The Global Warming Potential generated from 1tonne of food wastes for each disposal system was analyzed by the life cycle assessment method. The results showed that 200kg of CO(2)-eq could be produced from dry feeding process, 61kg of CO(2)-eq from wet feeding process, 123kg of CO(2)-eq from composting process, and 1010kg of CO(2)-eq from landfilling. Feed manufacturing and composting, the common treatment methods currently employed, have been known to be environment friendlier than other methods. However, this study shows that they can negatively affect the environment if their by-products are not appropriately utilized as intended. Copyright 2010 Elsevier B.V. All rights reserved.

A visible-light-driven core-shell like Ag2S@Ag2CO3 composite photocatalyst with high performance in pollutants degradation.

PubMed

Yu, Changlin; Wei, Longfu; Zhou, Wanqin; Dionysiou, Dionysios D; Zhu, Lihua; Shu, Qing; Liu, Hong

2016-08-01

A series of Ag2S-Ag2CO3 (4%, 8%, 16%, 32% and 40% Ag2S), Ag2CO3@Ag2S (32%Ag2S) and Ag2S@Ag2CO3 (32%Ag2S) composite photocatalysts were fabricated by coprecipitation or successive precipitation reaction. The obtained catalysts were analyzed by N2 physical adsorption, powder X-ray diffraction, scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy, Raman spectroscopy, UV-vis diffuse reflectance spectroscopy and photocurrent test. Under visible light irradiation, the influences of Ag2S content and core-shell property on photocatalytic activity and stability were evaluated in studies focused on the degradation of methyl orange (MO) dye, phenol, and bisphenol A. Results showed that excellent photocatalytic performance was obtained over Ag2S/Ag2CO3 composite photocatalysts with respect to Ag2S and Ag2CO3. With optimal content of Ag2S (32 wt%), the Ag2S-Ag2CO3 showed the highest photocatalytic degradation efficiency. Moreover, the structured property of Ag2S/Ag2CO3 greatly influenced the activity. Compared with Ag2S-Ag2CO3 and Ag2CO3@Ag2S, core-shell like Ag2S@Ag2CO3 demonstrated the highest activity and stability. The main reason for the boosting of photocatalytic performance was due to the formation of Ag2S/Ag2CO3 well contacted interface and unique electron structures. Ag2S/Ag2CO3 interface could significantly increase the separation efficiency of the photo-generated electrons (e(-)) and holes (h(+)), and production of OH radicals. More importantly, the low solubility of Ag2S shell could effectively protect the core of Ag2CO3, which further guarantees the stability of Ag2CO3. Copyright © 2016 Elsevier Ltd. All rights reserved.

Composites of ionic liquid and amine-modified SAPO 34 improve CO2 separation of CO2-selective polymer membranes

NASA Astrophysics Data System (ADS)

Hu, Leiqing; Cheng, Jun; Li, Yannan; Liu, Jianzhong; Zhang, Li; Zhou, Junhu; Cen, Kefa

2017-07-01

Mixed matrix membranes with ionic liquids and molecular sieve particles had high CO2 permeabilities, but CO2 separation from small gas molecules such as H2 was dissatisfied because of bad interfacial interaction between ionic liquid and molecular sieve particles. To solve that, amine groups were introduced to modify surface of molecular sieve particles before loading with ionic liquid. SAPO 34 was adopted as the original filler, and four mixed matrix membranes with different fillers were prepared on the outer surface of ceramic hollow fibers. Both surface voids and hard agglomerations disappeared, and the surface became smooth after SAPO 34 was modified by amine groups and ionic liquid [P66614][2-Op]. Mixed matrix membranes with composites of amine-modified SAPO 34 and ionic liquid exhibited excellent CO2 permeability (408.9 Barrers) and CO2/H2 selectivity (22.1).

Arterial pressure-based cardiac output monitoring: a multicenter validation of the third-generation software in septic patients.

PubMed

De Backer, Daniel; Marx, Gernot; Tan, Andrew; Junker, Christopher; Van Nuffelen, Marc; Hüter, Lars; Ching, Willy; Michard, Frédéric; Vincent, Jean-Louis

2011-02-01

Second-generation FloTrac software has been shown to reliably measure cardiac output (CO) in cardiac surgical patients. However, concerns have been raised regarding its accuracy in vasoplegic states. The aim of the present multicenter study was to investigate the accuracy of the third-generation software in patients with sepsis, particularly when total systemic vascular resistance (TSVR) is low. Fifty-eight septic patients were included in this prospective observational study in four university-affiliated ICUs. Reference CO was measured by bolus pulmonary thermodilution (iCO) using 3-5 cold saline boluses. Simultaneously, CO was computed from the arterial pressure curve recorded on a computer using the second-generation (CO(G2)) and third-generation (CO(G3)) FloTrac software. CO was also measured by semi-continuous pulmonary thermodilution (CCO). A total of 401 simultaneous measurements of iCO, CO(G2), CO(G3), and CCO were recorded. The mean (95%CI) biases between CO(G2) and iCO, CO(G3) and iCO, and CCO and iCO were -10 (-15 to -5)% [-0.8 (-1.1 to -0.4) L/min], 0 (-4 to 4)% [0 (-0.3 to 0.3) L/min], and 9 (6-13)% [0.7 (0.5-1.0) L/min], respectively. The percentage errors were 29 (20-37)% for CO(G2), 30 (24-37)% for CO(G3), and 28 (22-34)% for CCO. The difference between iCO and CO(G2) was significantly correlated with TSVR (r(2) = 0.37, p < 0.0001). A very weak (r(2) = 0.05) relationship was also observed for the difference between iCO and CO(G3). In patients with sepsis, the third-generation FloTrac software is more accurate, as precise, and less influenced by TSVR than the second-generation software.

Synthesis and photocatalytic CO2 reduction performance of Cu2O/Coal-based carbon nanoparticle composites

NASA Astrophysics Data System (ADS)

Dedong, Zhang; Maimaiti, Halidan; Awati, Abuduheiremu; Yisilamu, Gunisakezi; Fengchang, Sun; Ming, Wei

2018-05-01

The photocatalytic reduction of CO2 into hydrocarbons provides a promising approach to overcome the challenges of environmental crisis and energy shortage. Here we fabricated a cuprous oxide (Cu2O) based composite photocatalyst consisting of Cu2O/carbon nanoparticles (CNPs). To prepare the CNPs, coal samples from Wucaiwan, Xinjiang, China, were first treated with HNO3, followed by hydrogen peroxide (H2O2) oxidation to strip nanocrystalline carbon from coal. After linking with oxygen-containing group such as hydroxyl, coal-based CNPs with sp2 carbon structure and multilayer graphene lattice structure were synthesized. Subsequently, the CNPs were loaded onto the surface of Cu2O nanoparticles prepared by in-situ reduction of copper chloride (CuCl2·2H2O). The physical properties and chemical structure of the Cu2O/CNPs as well as photocatalytic activity of CO2/H2O reduction into CH3OH were measured. The results demonstrate that the Cu2O/CNPs are composed of spherical particles with diameter of 50 nm and mesoporous structure, which are suitable for CO2 adsorption. Under illumination of visible light, electron-hole pairs are generated in Cu2O. Thanks to the CNPs, the fast recombination of electron-hole pairs is suppressed. The energy gradient formed on the surface of Cu2O/CNPs facilitates the efficient separation of electron-hole pairs for CO2 reduction and H2O oxidation, leading to enhanced photocatalytic activity.

A Critical Assessment of Microbiological Biogas to Biomethane Upgrading Systems.

PubMed

Rittmann, Simon K-M R

2015-01-01

Microbiological biogas upgrading could become a promising technology for production of methane (CH(4)). This is, storage of irregular generated electricity results in a need to store electricity generated at peak times for use at non-peak times, which could be achieved in an intermediate step by electrolysis of water to molecular hydrogen (H(2)). Microbiological biogas upgrading can be performed by contacting carbon dioxide (CO(2)), H(2) and hydrogenotrophic methanogenic Archaea either in situ in an anaerobic digester, or ex situ in a separate bioreactor. In situ microbiological biogas upgrading is indicated to require thorough bioprocess development, because only low volumetric CH(4) production rates and low CH(4) fermentation offgas content have been achieved. Higher volumetric production rates are shown for the ex situ microbiological biogas upgrading compared to in situ microbiological biogas upgrading. However, the ex situ microbiological biogas upgrading currently suffers from H(2) gas liquid mass transfer limitation, which results in low volumetric CH(4) productivity compared to pure H(2)/CO(2) conversion to CH(4). If waste gas utilization from biological and industrial sources can be shown without reduction in volumetric CH(4) productivity, as well as if the aim of a single stage conversion to a CH(4) fermentation offgas content exceeding 95 vol% can be demonstrated, ex situ microbiological biogas upgrading with pure or enrichment cultures of methanogens could become a promising future technology for almost CO(2)-neutral biomethane production.

A Moisture-Stable 3D Microporous CoII -Metal-Organic Framework with Potential for Highly Selective CO2 Separation under Ambient Conditions.

PubMed

Chand, Santanu; Pal, Arun; Das, Madhab C

2018-04-17

Selective adsorption and separation of CO 2 from flue gas and landfill gas mixtures have drawn great attention in industry. Porous MOF materials are promising alternatives to achieve such separations; however, the stability in the presence of moisture must be taken into consideration. Herein, we have constructed a microporous metal-organic framework (MOF) {[Co(OBA)(L) 0.5 ]⋅S} n (IITKGP-8), by employing a V-shaped organic linker with an azo-functionalized N,N' spacer forming a 3D network with mab topology and 1D rhombus-shaped channels along the crystallographic 'b' axis with a void volume of 34.2 %. The activated MOF reveals a moderate CO 2 uptake capacity of 55.4 and 26.5 cm 3  g -1 at 273 and 295 K/1 bar, respectively, whereas it takes up a significantly lower amount of CH 4 and N 2 under similar conditions and thus exhibits its potential for highly selective sorption of CO 2 with excellent IAST selectivity of CO 2 /N 2 (106 at 273 K and 43.7 at 295 K) and CO 2 /CH 4 (17.7 at 273 K and 17.1 at 295 K) under 1 bar. More importantly, this MOF exhibits excellent moisture stability as assessed through PXRD experiments coupled with surface area analysis. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Insertion Mutation of the Form I cbbL Gene Encoding Ribulose Bisphosphate Carboxylase/Oxygenase (RuBisCO) in Thiobacillus neapolitanus Results in Expression of Form II RuBisCO, Loss of Carboxysomes, and an Increased CO2 Requirement for Growth

PubMed Central

Baker, Stefanie H.; Jin, Songmu; Aldrich, Henry C.; Howard, Gary T.; Shively, Jessup M.

1998-01-01

It has been previously established that Thiobacillus neapolitanus fixes CO2 by using a form I ribulose bisphosphate carboxylase/oxygenase (RuBisCO), that much of the enzyme is sequestered into carboxysomes, and that the genes for the enzyme, cbbL and cbbS, are part of a putative carboxysome operon. In the present study, cbbL and cbbS were cloned and sequenced. Analysis of RNA showed that cbbL and cbbS are cotranscribed on a message approximately 2,000 nucleotides in size. The insertion of a kanamycin resistance cartridge into cbbL resulted in a premature termination of transcription; a polar mutant was generated. The mutant is able to fix CO2, but requires a CO2 supplement for growth. Separation of cellular proteins from both the wild type and the mutant on sucrose gradients and subsequent analysis of the RuBisCO activity in the collected fractions showed that the mutant assimilates CO2 by using a form II RuBisCO. This was confirmed by immunoblot analysis using antibodies raised against form I and form II RuBisCOs. The mutant does not possess carboxysomes. Smaller, empty inclusions are present, but biochemical analysis indicates that if they are carboxysome related, they are not functional, i.e., do not contain RuBisCO. Northern analysis showed that some of the shell components of the carboxysome are produced, which may explain the presence of these inclusions in the mutant. PMID:9696760

Diagnostic examination of thermally abused high-power lithium-ion cells

NASA Astrophysics Data System (ADS)

Abraham, D. P.; Roth, E. P.; Kostecki, R.; McCarthy, K.; MacLaren, S.; Doughty, D. H.

The inherent thermal instability of lithium-ion cells is a significant impediment to their widespread commercialization for hybrid-electric vehicle applications. Cells containing conventional organic electrolyte-based chemistries are prone to thermal runaway at temperatures around 180 °C. We conducted accelerating rate calorimetry measurements on high-power 18650-type lithium-ion cells in an effort to decipher the sequence of events leading to thermal runaway. In addition, electrode and separator samples harvested from a cell that was heated to 150 °C then air-quenched to room temperature were examined by microscopy, spectroscopy, and diffraction techniques. Self-heating of the cell began at 84 °C. The gases generated in the cell included CO 2 and CO, and smaller quantities of H 2, C 2H 4, CH 4, and C 2H 6. The main changes on cell heating to 150 °C were observed on the anode surface, which was covered by a thick layer of surface deposits that included LiF and inorganic and organo-phosphate compounds. The sources of gas generation and the mechanisms leading to the formation of compounds observed on the electrode surfaces are discussed.

CO2 Acquisition Membrane (CAM)

NASA Technical Reports Server (NTRS)

Mason, Larry W.; Way, J. Douglas; Vlasse, Marcus

2003-01-01

The objective of CAM is to develop, test, and analyze thin film membrane materials for separation and purification of carbon dioxide (CO2) from mixtures of gases, such as those found in the Martian atmosphere. The membranes are targeted toward In Situ Resource Utilization (ISRU) applications that will operate in extraterrestrial environments and support future unmanned and human space missions. A primary application is the Sabatier Electrolysis process that uses Mars atmosphere CO2 as raw material for producing water, oxygen, and methane for rocket fuel and habitat support. Other applications include use as an inlet filter to collect and concentrate Mars atmospheric argon and nitrogen gases for habitat pressurization, and to remove CO2 from breathing gases in Closed Environment Life Support Systems (CELSS). CAM membrane materials include crystalline faujasite (FAU) zeolite and rubbery polymers such as silicone rubber (PDMS) that have been shown in the literature and via molecular simulation to favor adsorption and permeation of CO2 over nitrogen and argon. Pure gas permeation tests using commercial PDMS membranes have shown that both CO2 permeance and the separation factor relative to other gases increase as the temperature decreases, and low (Delta)P(Sub CO2) favors higher separation factors. The ideal CO2/N2 separation factor increases from 7.5 to 17.5 as temperature decreases from 22 C to -30 C. For gas mixtures containing CO2, N2, and Ar, plasticization decreased the separation factors from 4.5 to 6 over the same temperature range. We currently synthesize and test our own Na(+) FAU zeolite membranes using standard formulations and secondary growth methods on porous alumina. Preliminary tests with a Na(+) FAU membrane at 22 C show a He/SF6 ideal separation factor of 62, exceeding the Knudsen diffusion selectivity by an order of magnitude. This shows that the membrane is relatively free from large defects and associated non-selective (viscous flow) transport mechanisms. The Membrane Test Facility (MTF) has been developed to measure membrane permeance over a wide range of temperature and pressure. The facility uses two volume compartments separated by the membrane that are instrumented to measure temperature, delta pressure across the membrane, and gas composition. A thermal shroud supports and encloses the membrane, and provides temperature control. Methods were developed to determine membrane permeance using the first order decay of the pressure difference between the sealed compartments, using the total pressure for pure gases, and partial pressure of each species in gas mixtures. The technique provides an end-to-end measurement of gas permeance that includes concentration polarization effects. Experiments have shown that in addition to membrane permeance properties, the geometry and design of associated structures play an important role in how membrane systems will function on Mars.

The right place for the right job in the photovoltaic life cycle.

PubMed

Kawajiri, Kotaro; Genchi, Yutaka

2012-07-03

The potential for photovoltaic power generation (PV) to reduce primary energy consumption (PEC) and CO(2) emissions depends on the physical locations of each stage of its life cycle. When stages are optimally located, CO(2) emissions are reduced nearly ten times as much as when each stage is located in the country having the largest current market share. The usage stage contributes the most to reducing CO(2) emissions and PEC, and total CO(2) emissions actually increase when PV is installed in countries having small CO(2) emissions from electricity generation. Global maps of CO(2) reduction potential indicate that Botswana and Gobi in Mongolia are the optimal locations to install PV due to favorable conditions for PV power generation and high CO(2) emissions from current electricity generation. However, the small electricity demand in those countries limits the contribution to global CO(2) reduction. The type of PVs has a small but significant effect on life cycle PEC and CO(2) emissions.

Pig slurry acidification and separation techniques affect soil N and C turnover and N2O emissions from solid, liquid and biochar fractions.

PubMed

Gómez-Muñoz, B; Case, S D C; Jensen, L S

2016-03-01

The combined effects of pig slurry acidification, subsequent separation techniques and biochar production from the solid fraction on N mineralisation and N2O and CO2 emissions in soil were investigated in an incubation experiment. Acidification of pig slurry increased N availability from the separated solid fractions in soil, but did not affect N2O and CO2 emissions. However acidification reduced soil N and C turnover from the liquid fraction. The use of more advanced separation techniques (flocculation and drainage > decanting centrifuge > screw press) increased N mineralisation from acidified solid fractions, but also increased N2O and CO2 emissions in soil amended with the liquid fraction. Finally, the biochar production from the solid fraction of pig slurry resulted in a very recalcitrant material, which reduced N and C mineralisation in soil compared to the raw solid fractions. Copyright © 2015 Elsevier Ltd. All rights reserved.

Enhancing visible light photocatalytic and photocharge separation of (BiO){sub 2}CO{sub 3} plate via dramatic I{sup −} ions doping effect

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

Liang, Lei; Cao, Jing; Anhui Collaborative Innovation Center of Advanced Functional Composite, Huaibei, 235000, Anhui

Highlights: • Novel I-(BiO){sub 2}CO{sub 3} was prepared by a facile chemical precipitation method. • I{sup −} ions impurity level located on the top of valence band of (BiO){sub 2}CO{sub 3}. • I{sup −} ions doping largely improved photocatalytic activity of I-(BiO){sub 2}CO{sub 3}. • I-(BiO){sub 2}CO{sub 3} displayed excellent photocharge separation efficiency. - Abstract: Novel I{sup −} ions doped (BiO){sub 2}CO{sub 3} (I-(BiO){sub 2}CO{sub 3}) photocatalysts were successfully synthesized via a facile chemical precipitation method. Under visible light (λ > 400 nm), I-(BiO){sub 2}CO{sub 3} displayed much higher activity for rhodamine B and dichlorophenol degradation than the undoped (BiO){submore » 2}CO{sub 3}. The pseudo-first-order rate constant k{sub app} of RhB degradation over 15.0% I-(BiO){sub 2}CO{sub 3} was 0.54 h{sup −1}, which is 11.3 times higher than that of (BiO){sub 2}CO{sub 3}. The doped I{sup −} ions formed an impurity level on the top of valence band of (BiO){sub 2}CO{sub 3} and induced much more visible light to be absorbed. The enhanced photocurrent and surface photovoltage properties were detected, which strongly ensures the efficient separation of electrons and holes in I-(BiO){sub 2}CO{sub 3} system under visible light. It provides a facile way to improve the photocatalytic activity of the wide-band-gap (BiO){sub 2}CO{sub 3} via intense doping effect of I{sup −} ions.« less

Design Principles of Perovskites for Thermochemical Oxygen Separation.

PubMed

Ezbiri, Miriam; Allen, Kyle M; Gàlvez, Maria E; Michalsky, Ronald; Steinfeld, Aldo

2015-06-08

Separation and concentration of O2 from gas mixtures is central to several sustainable energy technologies, such as solar-driven synthesis of liquid hydrocarbon fuels from CO2 , H2 O, and concentrated sunlight. We introduce a rationale for designing metal oxide redox materials for oxygen separation through "thermochemical pumping" of O2 against a pO2 gradient with low-grade process heat. Electronic structure calculations show that the activity of O vacancies in metal oxides pinpoints the ideal oxygen exchange capacity of perovskites. Thermogravimetric analysis and high-temperature X-ray diffraction for SrCoO3-δ , BaCoO3-δ and BaMnO3-δ perovskites and Ag2 O and Cu2 O references confirm the predicted performance of SrCoO3-δ , which surpasses the performance of state-of-the-art Cu2 O at these conditions with an oxygen exchange capacity of 44 mmol O 2 mol SrCoO 3-δ(-1) exchanged at 12.1 μmol O 2 min(-1)  g(-1) at 600-900 K. The redox trends are understood due to lattice expansion and electronic charge transfer. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Evolving together: the biology of symbiosis, part 2

PubMed Central

2000-01-01

Symbiotic trade-offs dominate the world of biology and medicine in colonist-host relationships and between separate, mutually dependent organisms of different species. Infectious and parasitic diseases can be better understood by exploring the dynamic continuum between pathogenicity and mutualism, between antagonism and cooperation—the sliding scale along which microorganisms can move in a moment's notice with a single nucleotide substitution. Organisms practicing piracy or pastoralism may be close genetic relatives. Mergers occur not only between cells but also between genomes; viruses co-opt host genes and in turn insert themselves into host genomes. Separate organisms, from ants to fungi to plants, establish symbiotic ties with each other that bind over deep time, generating much of the diversity we see in nature. PMID:16389348

Ultrathin Composite Polymeric Membranes for CO2 /N2 Separation with Minimum Thickness and High CO2 Permeance.

PubMed

Benito, Javier; Sánchez-Laínez, Javier; Zornoza, Beatriz; Martín, Santiago; Carta, Mariolino; Malpass-Evans, Richard; Téllez, Carlos; McKeown, Neil B; Coronas, Joaquín; Gascón, Ignacio

2017-10-23

The use of ultrathin films as selective layers in composite membranes offers significant advantages in gas separation for increasing productivity while reducing the membrane size and energy costs. In this contribution, composite membranes have been obtained by the successive deposition of approximately 1 nm thick monolayers of a polymer of intrinsic microporosity (PIM) on top of dense membranes of the ultra-permeable poly[1-(trimethylsilyl)-1-propyne] (PTMSP). The ultrathin PIM films (30 nm in thickness) demonstrate CO 2 permeance up to seven times higher than dense PIM membranes using only 0.04 % of the mass of PIM without a significant decrease in CO 2 /N 2 selectivity. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Solid Solution Photocatalyst with Spontaneous Polarization Exhibiting Low Recombination Toward Efficient CO2 Photoreduction.

PubMed

Zhou, Peng; Wang, Xin; Yan, Shicheng; Zou, Zhigang

2016-08-23

Decreasing the recombination of photogenerated carriers is a major challenge for efficiently converting solar energy into chemical energy by photocatalysis. Here, we have demonstrated that growth of a polar GaN:ZnO solid solution single crystal along its polarization axis is beneficial to efficient separation of photogenerated carriers, owing to the periodic potential barriers and wells generated from the periodically positive and negative atom arrangements in crystal structure. Local charge imbalance caused by replacing Ga(3+) with Zn(2+) leads to a polarization vector in the {0 0 0 1} planes of GaN:ZnO solid solution, thus forming a 1 D electron transport path along [2 1‾  1‾  0] in the {0 0 0 1} planes of GaN:ZnO solid solution to decrease recombination. Shorting the hole-transport distance by synthesizing porous nanoplates can further decrease recombination under the polarization field and improve the performance of polar photocatalyst in photoreduction of CO2 into CH4 . © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Engineering Sedimentary Geothermal Resources for Large-Scale Dispatchable Renewable Electricity

NASA Astrophysics Data System (ADS)

Bielicki, Jeffrey; Buscheck, Thomas; Chen, Mingjie; Sun, Yunwei; Hao, Yue; Saar, Martin; Randolph, Jimmy

2014-05-01

Mitigating climate change requires substantial penetration of renewable energy and economically viable options for CO2 capture and storage (CCS). We present an approach using CO2 and N2 in sedimentary basin geothermal resources that (1) generates baseload and dispatchable power, (2) efficiently stores large amounts of energy, and (3) enables seasonal storage of solar energy, all which (5) increase the value of CO2 and render CCS commercially viable. Unlike the variability of solar and wind resources, geothermal heat is a constant source of renewable energy. Using CO2 as a supplemental geothermal working fluid, in addition to brine, reduces the parasitic load necessary to recirculate fluids. Adding N2 is beneficial because it is cheaper, will not react with materials and subsurface formations, and enables bulk energy storage. The high coefficients of thermal expansion of CO2 and N2 (a) augment reservoir pressure, (b) generate artesian flow at the production wells, and (c) produce self-convecting thermosiphons that directly convert reservoir heat to mechanical energy for fluid recirculation. Stored pressure drives fluid production and responds faster than conventional brine-based geothermal systems. Our design uses concentric rings of horizontal wells to create a hydraulic divide that stores supplemental fluids and pressure. Production and injection wells are controlled to schedule power delivery and time-shift the parasitic power necessary to separate N2 from air and compress it for injection. The parasitic load can be scheduled during minimum power demand or when there is excess electricity from wind or solar. Net power output can nearly equal gross power output during peak demand, and energy storage is almost 100% efficient because it is achieved by the time-shift. Further, per-well production rates can take advantage of the large productivity of horizontal wells, with greater leveraging of well costs, which often constitute a major portion of capital costs for geothermal power systems.

Measurement of black carbon emissions from in-use diesel-electric passenger locomotives in California

NASA Astrophysics Data System (ADS)

Tang, N. W.; Kirchstetter, T.; Martien, P. T.; Apte, J.

2015-12-01

Black carbon (BC) emission factors were measured for a California commuter rail line fleet of diesel-electric passenger locomotives (Caltrain). The emission factors are based on BC and carbon dioxide (CO2) concentrations in the exhaust plumes of passing locomotives, which were measured from pedestrian overpasses using portable analyzers. Each of the 29 locomotives in the fleet was sampled on 4-20 separate occasions at different locations to characterize different driving modes. The average emission factor expressed as g BC emitted per kg diesel consumed was 0.87 ± 0.66 g kg-1 (±1 standard deviation, n = 362 samples). BC emission factors tended to be higher for accelerating locomotives traveling at higher speeds with engines in higher notch settings. Higher fuel-based BC emission factors (g kg-1) were measured for locomotives equipped with separate "head-end" power generators (SEP-HEPs), which power the passenger cars, while higher time-based emission factors (g h-1) were measured for locomotives without SEP-HEPs, whose engines are continuously operated at high speeds to provide both head-end and propulsion power. PM10 emission factors, estimated assuming a BC/PM10 emission ratio of 0.6 and a typical power output-to-fuel consumption ratio, were generally in line with the Environmental Protection Agency's locomotive exhaust emission standards. Per passenger mile, diesel-electric locomotives in this study emit only 20% of the CO2 emitted by typical gasoline-powered light-duty vehicles (i.e., cars). However, the reduction in carbon footprint (expressed in terms of CO2 equivalents) due to CO2 emissions avoidance from a passenger commuting by train rather than car is appreciably offset by the locomotive's higher BC emissions.

Measurement of black carbon emissions from in-use diesel-electric passenger locomotives in California

NASA Astrophysics Data System (ADS)

Tang, Nicholas W.; Apte, Joshua S.; Martien, Philip T.; Kirchstetter, Thomas W.

2015-08-01

Black carbon (BC) emission factors were measured for a California commuter rail line fleet of diesel-electric passenger locomotives (Caltrain). The emission factors are based on BC and carbon dioxide (CO2) concentrations in the exhaust plumes of passing locomotives, which were measured from pedestrian overpasses using portable analyzers. Each of the 29 locomotives in the fleet was sampled on 4-20 separate occasions at different locations to characterize different driving modes. The average emission factor expressed as g BC emitted per kg diesel consumed was 0.87 ± 0.66 g kg-1 (±1 standard deviation, n = 362 samples). BC emission factors tended to be higher for accelerating locomotives traveling at higher speeds with engines in higher notch settings. Higher fuel-based BC emission factors (g kg-1) were measured for locomotives equipped with separate ;head-end; power generators (SEP-HEPs), which power the passenger cars, while higher time-based emission factors (g h-1) were measured for locomotives without SEP-HEPs, whose engines are continuously operated at high speeds to provide both head-end and propulsion power. PM10 emission factors, estimated assuming a BC/PM10 emission ratio of 0.6 and a typical power output-to-fuel consumption ratio, were generally in line with the Environmental Protection Agency's locomotive exhaust emission standards. Per passenger mile, diesel-electric locomotives in this study emit only 20% of the CO2 emitted by typical gasoline-powered light-duty vehicles (i.e., cars). However, the reduction in carbon footprint (expressed in terms of CO2 equivalents) due to CO2 emissions avoidance from a passenger commuting by train rather than car is appreciably offset by the locomotive's higher BC emissions.

Potential Flue Gas Impurities in Carbon Dioxide Streams Separated from Coal-fired Power Plants

EPA Science Inventory

For geological sequestration of CO₂ separated from pulverized coal combustion flue gas, it is necessary to adequately evaluate the potential impacts of flue gas impurities on groundwater aquifers in the case of the CO₂ leakage from its storage sites. This s...

Highly selective separation of carbon dioxide from nitrogen and methane by nitrile/glycol-difunctionalized ionic liquids in supported ionic liquid membranes (SILMs).

PubMed

Hojniak, Sandra D; Silverwood, Ian P; Khan, Asim Laeeq; Vankelecom, Ivo F J; Dehaen, Wim; Kazarian, Sergei G; Binnemans, Koen

2014-07-03

Novel difunctionalized ionic liquids (ILs) containing a triethylene glycol monomethyl ether chain and a nitrile group on a pyrrolidinium or imidazolium cation have been synthesized and incorporated into supported ionic liquid membranes (SILMs). These ILs exhibit ca. 2.3 times higher CO2/N2 and CO2/CH4 gas separation selectivities than analogous ILs functionalized only with a glycol chain. Although the glycol moiety ensures room temperature liquidity of the pyrrolidinium and imidazolium ILs, the two classes of ILs benefit from the presence of a nitrile group in different ways. The difunctionalized pyrrolidinium ILs exhibit an increase in CO2 permeance, whereas the permeances of the contaminant gases rise negligibly, resulting in high gas separation selectivities. In the imidazolium ILs, the presence of a nitrile group does not always increase the CO2 permeance nor does it increase the CO2 solubility, as showed in situ by the ATR-FTIR spectroscopic method. High selectivity of these ILs is caused by the considerably reduced permeances of N2 and CH4, most likely due to the ability of the -CN group to reject the nonpolar contaminant gases. Apart from the CO2 solubility, IL-CO2 interactions and IL swelling were studied with the in situ ATR-FTIR spectroscopy. Different strengths of the IL-CO2 interactions were found to be the major difference between the two classes of ILs. The difunctionalized ILs interacted stronger with CO2 than the glycol-functionalized ILs, as manifested in the smaller bandwidths of the bending mode band of CO2 for the latter.

Greenhouse gas and ammonia emissions from production of compost bedding on a dairy farm.

PubMed

Fillingham, M A; VanderZaag, A C; Burtt, S; Baldé, H; Ngwabie, N M; Smith, W; Hakami, A; Wagner-Riddle, C; Bittman, S; MacDonald, D

2017-12-01

Recent developments in composting technology enable dairy farms to produce their own bedding from composted manure. This management practice alters the fate of carbon and nitrogen; however, there is little data available documenting how gaseous emissions are impacted. This study measured in-situ emissions of methane (CH 4 ), carbon dioxide (CO 2 ), nitrous oxide (N 2 O), and ammonia (NH 3 ) from an on-farm solid-liquid separation system followed by continuously-turned plug-flow composting over three seasons. Emissions were measured separately from the continuously-turned compost phase, and the compost-storage phase prior to the compost being used for cattle bedding. Active composting had low emissions of N 2 O and CH 4 with most carbon being emitted as CO 2 -C and most N emitted as NH 3 -N. Compost storage had higher CH 4 and N 2 O emissions than the active phase, while NH 3 was emitted at a lower rate, and CO 2 was similar. Overall, combining both the active composting and storage phases, the mean total emissions were 3.9×10 -2 gCH 4 kg -1 raw manure (RM), 11.3gCO 2 kg -1 RM, 2.5×10 -4 g N 2 O kg -1 RM, and 0.13g NH 3 kg -1 RM. Emissions with solid-separation and composting were compared to calculated emissions for a traditional (unseparated) liquid manure storage tank. The total greenhouse gas emissions (CH 4 +N 2 O) from solid separation, composting, compost storage, and separated liquid storage were reduced substantially on a CO 2 -equivalent basis compared to traditional liquid storage. Solid-liquid separation and well-managed composting could mitigate overall greenhouse gas emissions; however, an environmental trade off was that NH 3 was emitted at higher rates from the continuously turned composter than reported values for traditional storage. Crown Copyright © 2017. Published by Elsevier Ltd. All rights reserved.

The high squareness Sm-Co magnet having Hcb=10.6 kOe at 150°C

NASA Astrophysics Data System (ADS)

Machida, Hiroaki; Fujiwara, Teruhiko; Kamada, Risako; Morimoto, Yuji; Takezawa, Masaaki

2017-05-01

The relationship between magnetic properties and magnetic domain structures of Sm(Fe, Cu, Zr, Co)7.5 magnet was investigated. The developed Sm-Co magnet, which is conducted homogenization heat treatment at ingot state, high temperature short time sintering and long time solid solution heat treatment showed the maximum energy product, [BH]m of 34.0 MGOe and the coercivity, Hcb of 11.3 kOe at 20°C respectively. Moreover, Hcb of 10.6 kOe at 150°C was achieved. Heat treated ingot has clear 1-7 phase in mother phase from optical microscope observation. Kerr effect microscope with magnetic field applied was used to investigate magnetic domain structure. Reverse magnetic domains were generated evenly but generation of them from inside grain were not observed. Cell structure was observed by scanning transmission electron microscope and composition analysis was conducted by energy dispersive X-ray spectroscopy. Cell size was approximately 150 ˜ 300 nm, Fe and Cu were clearly separated and concentrated to 2-17 phase and 1-5 phase respectively. Moreover, Cu concentration went up to 40 at% in 1-5 phase. That means the gap of domain wall energy between 1-5 phase and 2-17 phase was increased due to microstructure control by conducting heat treatment for compositional homogeneity.

Gradient enhanced-fluidity liquid hydrophilic interaction chromatography of ribonucleic acid nucleosides and nucleotides: A "green" technique.

PubMed

Beilke, Michael C; Beres, Martin J; Olesik, Susan V

2016-03-04

A "green" hydrophilic interaction liquid chromatography (HILIC) technique for separating the components of mixtures with a broad range of polarities is illustrated using enhanced-fluidity liquid mobile phases. Enhanced-fluidity liquid chromatography (EFLC) involves the addition of liquid CO2 to conventional liquid mobile phases. Decreased mobile phase viscosity and increased analyte diffusivity results when a liquefied gas is dissolved in common liquid mobile phases. The impact of CO2 addition to a methanol:water (MeOH:H2O) mobile phase was studied to optimize HILIC gradient conditions. For the first time a fast separation of 16 ribonucleic acid (RNA) nucleosides/nucleotides was achieved (16min) with greater than 1.3 resolution for all analyte pairs. By using a gradient, the analysis time was reduced by over 100% compared to similar separations conducted under isocratic conditions. The optimal separation using MeOH:H2O:CO2 mobile phases was compared to MeOH:H2O and acetonitrile:water (ACN:H2O) mobile phases. Based on chromatographic performance parameters (efficiency, resolution and speed of analysis) and an assessment of the environmental impact of the mobile phase mixtures, MeOH:H2O:CO2 mixtures are preferred over ACN:H2O or MeOH:H2O mobile phases for the separation of mixtures of RNA nucleosides and nucleotides. Copyright © 2016 Elsevier B.V. All rights reserved.

Ionic Liquid Confined in Mesoporous Polymer Membrane with Improved Stability for CO2/N2 Separation

PubMed Central

Tan, Ming; Lu, Jingting; Zhang, Yang; Jiang, Heqing

2017-01-01

Supported ionic liquid membranes (SILMs) have a promising prospect of application in flue gas separation, owing to its high permeability and selectivity of CO2. However, existing SILMs have the disadvantage of poor stability due to the loss of ionic liquid from the large pores of the macroporous support. In this study, a novel SILM with high stability was developed by confining ionic liquid in a mesoporous polymer membrane. First, a mesoporous polymer membrane derived from a soluble, low-molecular-weight phenolic resin precursor was deposited on a porous Al2O3 support, and then 1-ethyl-3-methylimidazolium tetrafluoroborate ([emim][BF4]) was immobilized inside mesopores of phenolic resin, forming the SILM under vacuum. Effects of trans-membrane pressure difference on the SILM separation performance were investigated by measuring the permeances of CO2 and N2. The SILM exhibits a high ideal CO2/N2 selectivity of 40, and an actual selectivity of approximately 25 in a mixed gas (50% CO2 and 50% N2) at a trans-membrane pressure difference of 2.5 bar. Compared to [emim][BF4] supported by polyethersulfone membrane with a pore size of around 0.45 μm, the [emim][BF4] confined in a mesoporous polymer membrane exhibits an improved stability, and its separation performance remained stable for 40 h under a trans-membrane pressure difference of 1.5 bar in a mixed gas before the measurement was intentionally stopped. PMID:28961187

Mercury and trace element distribution in density separates of a South African Highveld (#4) coal: Implications for mercury reduction and preparation of export coal

USGS Publications Warehouse

Kolker, Allan; Senior, Connie L.; van Alphen, Chris; Koenig, Alan E.; Geboy, Nicholas J.

2017-01-01

Eight density separates of Permian Highveld (#4) coal were investigated for partitioning of Hg and trace elements. The separates include float fractions obtained in heavy media having densities of 1.4, 1.5, 1.6, 1.7, 1.8, 1.9, and 2.0 g/cm3, and the sink fraction for 2.0 g/cm3. Bulk analysis of the separates shows strong (R2 ≥ 0.80) positive correlations between pyritic sulfur and mercury, and between ash yield and both pyritic sulfur and mercury. Laser ablation (LA) ICP-MS analysis of individual pyrite grains in the separates confirms association of Hg and As with pyrite as indicated by bulk analysis. Other elements detected in pyrite by LA-ICP-MS include Mn, Co, Ni, Tl, and Pb. Results for the separates allow prediction of Hg, trace elements, and ash yields expected in specific South African coal products. These range from 0.06 ppm Hg and an ash yield of 11.5% ash for the export fraction to 0.47 ppm Hg and an ash yield of 60.9% for the discard (stone) fraction (dry basis). Results show pronounced differences expected between coal used for domestic power generation and coal which is exported.

Pictures of Processes: Automated Graph Rewriting for Monoidal Categories and Applications to Quantum Computing

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.

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

DOE PAGES

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

2016-12-21

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

Carboxydobrachium pacificum gen. nov., sp. nov., a new anaerobic, thermophilic, CO-utilizing marine bacterium from Okinawa Trough.

PubMed

Sokolova, T G; González, J M; Kostrikina, N A; Chernyh, N A; Tourova, T P; Kato, C; Bonch-Osmolovskaya, E A; Robb, F T

2001-01-01

A new anaerobic, thermophilic, CO-utilizing marine bacterium, strain JMT, was isolated from a submarine hot vent in Okinawa Trough. Cells of strain JMT were non-motile thin straight rods, sometimes branching, with a cell wall of the Gram-positive type, surrounded with an S-layer. Chains of three to five cells were often observed. The isolate grew chemolithotrophically on CO, producing equimolar quantities of H2 and CO2 (according to the equation CO+H2O-->CO2+H2) and organotrophically on peptone, yeast extract, starch, cellobiose, glucose, galactose, fructose and pyruvate, producing H2, acetate and CO2. Growth was observed from 50 to 80 degrees C with an optimum at 70 degrees C. The optimum pH was 6.8-7.1. The optimum concentration of sea salts in the medium was 20.5-25.5 g l(-1). The generation time under optimal conditions was 7.1 h. The DNA G+C content was 33 mol %. Growth of isolate JMT was not inhibited by penicillin, but ampicillin, streptomycin, kanamycin and neomycin completely inhibited growth. The results of 16S rDNA sequence analysis revealed that strain JMT belongs to the Thermoanaerobacter phylogenetic group within the Bacillus-Clostridium subphylum of Gram-positive bacteria but represents a separate branch of this group. On the basis of morphological and physiological features and phylogenetic data, this isolate should be assigned to a new genus, for which the name Carboxydobrachium is proposed. The type species is Carboxydobrachium pacificum; the type strain is JMT (= DSM 12653T).

Water, air, Earth and cosmic radiation.

PubMed

Bassez, Marie-Paule

2015-06-01

In the context of the origin of life, rocks are considered mainly for catalysis and adsorption-desorption processes. Here it is shown how some rocks evolve in energy and might induce synthesis of molecules of biological interest. Radioactive rocks are a source of thermal energy and water radiolysis producing molecular hydrogen, H2. Mafic and ultramafic rocks evolve in water and dissolved carbon dioxide releasing thermal energy and H2. Peridotites and basalts contain ferromagnesian minerals which transform through exothermic reactions with the generation of heat. These reactions might be triggered by any heating process such as radioactive decay, hydrothermal and subduction zones or post-shock of meteorite impacts. H2 might then be generated from endothermic hydrolyses of the ferromagnesian minerals olivine and pyroxene. In both cases of mafic and radioactive rocks, production of CO might occur through high temperature hydrogenation of CO2. CO, instead of CO2, was proven to be necessary in experiments synthesizing biological-type macromolecules with a gaseous mixture of CO, N2 and H2O. In the geological context, N2 is present in the environment, and the activation source might arise from cosmic radiation and/or radionuclides. Ferromagnesian and radioactive rocks might consequently be a starting point of an hydrothermal chemical evolution towards the abiotic formation of biological molecules. The two usually separate worlds of rocks and life are shown to be connected through molecular and thermodynamic chemical evolution. This concept has been proposed earlier by the author (Bassez J Phys: Condens Matter 15:L353-L361, 2003, 2008a, 2008b; Bassez Orig Life Evol Biosph 39(3-4):223-225, 2009; Bassez et al. 2011; Bassez et al. Orig Life Evol Biosph 42(4):307-316, 2012, Bassez 2013) without thermodynamic details. This concept leads to signatures of prebiotic chemistry such as radionuclides and also iron and magnesium carbonates associated with serpentine and/or talc, which were discussed at the 2014 European Astrobiology Network Association conference on Signatures of Life.

Optical Breath Gas Sensor for Extravehicular Activity Application

NASA Technical Reports Server (NTRS)

Wood, William R.; Casias, Miguel E.; Vakhtin, Andrei B.; Pilgrim, Jeffrey S> ; Chullen, Cinda; Falconi, Eric A.

2012-01-01

The function of the infrared gas transducer used during extravehicular activity (EVA) in the current space suit is to measure and report the concentration of carbon dioxide (CO2) in the ventilation loop. The next generation Portable Life Support System (PLSS) requires next generation CO2 sensing technology with performance beyond that presently in use on the Shuttle/International Space Station extravehicular mobility unit (EMU). Accommodation within space suits demands that optical sensors meet stringent size, weight, and power requirements. A laser diode (LD) spectrometer based on wavelength modulation spectroscopy (WMS) is being developed for this purpose by Vista Photonics, Inc. Two prototype devices were delivered to NASA Johnson Space Center (JSC) in September 2011. The sensors incorporate a laser diode based CO2 channel that also includes an incidental water vapor (humidity) measurement and a separate oxygen (O2) channel using a vertical cavity surface emitting laser (VCSEL). Both prototypes are controlled digitally with a field-programmable gate array (FPGA)/microcontroller architecture. Based on the results of the initial instrument development, further prototype development and testing of instruments leveraging the lessons learned were desired. The present development extends and upgrades the earlier hardware to the Advanced PLSS 2.0 test article being constructed and tested at JSC. Various improvements to the electronics and gas sampling are being advanced by this project. The combination of low power electronics with the performance of a long wavelength laser spectrometer enables multi-gas sensors with significantly increased performance over that presently offered in the EMU. .

Nanophase-separated Ni3Nb as an automobile exhaust catalyst† †Electronic supplementary information (ESI) available: Demonstration procedure, experimental and characterization details. See DOI: 10.1039/c6sc05473k Click here for additional data file. Click here for additional data file.

PubMed Central

Tanabe, Toyokazu; Imai, Tsubasa; Tokunaga, Tomoharu; Arai, Shigeo; Yamamoto, Yuta; Ueda, Shigenori; Ramesh, Gubbala V.; Nagao, Satoshi; Hirata, Hirohito; Matsumoto, Shin-ichi

2017-01-01

Catalytic remediation of automobile exhaust has relied on precious metals (PMs) including platinum (Pt). Herein, we report that an intermetallic phase of Ni and niobium (Nb) (i.e., Ni3Nb) exhibits a significantly higher activity than that of Pt for the remediation of the most toxic gas in exhaust (i.e., nitrogen monoxide (NO)) in the presence of carbon monoxide (CO). When subjected to the exhaust-remediation atmosphere, Ni3Nb spontaneously evolves into a catalytically active nanophase-separated structure consisting of filamentous Ni networks (thickness < 10 nm) that are incorporated in a niobium oxide matrix (i.e., NbOx (x < 5/2)). The exposure of the filamentous Ni promotes NO dissociation, CO oxidation and N2 generation, and the NbOx matrix absorbs excessive nitrogen adatoms to retain the active Ni0 sites at the metal/oxide interface. Furthermore, the NbOx matrix immobilizes the filamentous Ni at elevated temperatures to produce long-term and stable catalytic performance over hundreds of hours. PMID:28507707

Separate hydrolysis and co-fermentation for improved xylose utilization in integrated ethanol production from wheat meal and wheat straw

PubMed Central

2012-01-01

Background The commercialization of second-generation bioethanol has not been realized due to several factors, including poor biomass utilization and high production cost. It is generally accepted that the most important parameters in reducing the production cost are the ethanol yield and the ethanol concentration in the fermentation broth. Agricultural residues contain large amounts of hemicellulose, and the utilization of xylose is thus a plausible way to improve the concentration and yield of ethanol during fermentation. Most naturally occurring ethanol-fermenting microorganisms do not utilize xylose, but a genetically modified yeast strain, TMB3400, has the ability to co-ferment glucose and xylose. However, the xylose uptake rate is only enhanced when the glucose concentration is low. Results Separate hydrolysis and co-fermentation of steam-pretreated wheat straw (SPWS) combined with wheat-starch hydrolysate feed was performed in two separate processes. The average yield of ethanol and the xylose consumption reached 86% and 69%, respectively, when the hydrolysate of the enzymatically hydrolyzed (18.5% WIS) unwashed SPWS solid fraction and wheat-starch hydrolysate were fed to the fermentor after 1 h of fermentation of the SPWS liquid fraction. In the other configuration, fermentation of the SPWS hydrolysate (7.0% WIS), resulted in an average ethanol yield of 93% from fermentation based on glucose and xylose and complete xylose consumption when wheat-starch hydrolysate was included in the feed. Increased initial cell density in the fermentation (from 5 to 20 g/L) did not increase the ethanol yield, but improved and accelerated xylose consumption in both cases. Conclusions Higher ethanol yield has been achieved in co-fermentation of xylose and glucose in SPWS hydrolysate when wheat-starch hydrolysate was used as feed, then in co-fermentation of the liquid fraction of SPWS fed with the mixed hydrolysates. Integration of first-generation and second-generation processes also increases the ethanol concentration, resulting in a reduction in the cost of the distillation step, thus improving the process economics. PMID:22410131

Carbon nanotubes-modified graphitic carbon nitride photocatalysts with synergistic effect of nickel(II) sulfide and molybdenum(II) disulfide co-catalysts for more efficient H2 evolution.

PubMed

Zhang, Yun-Xiao; Li, Kui; Yu, Yu-Xiang; Zhang, Wei-De

2018-09-15

This work reports effective photocatalysts which are composed of carbon nitride (CN), carbon nanotubes (CNTs), MoS 2 and NiS, for hydrogen evolution aiming at energy crises and environmental pollutions. The morphologies and optical properties of the photocatalysts were carefully characterized and their photocatalytic performance towards water reduction was studied afterwards. MoS 2 and NiS exhibit a significant synergistic effect working as co-catalysts. Compared to MoS 2 /CN nanohybrid, carbon nanotubes and NiS improved the absorption of visible light and the separation of charge carriers effectively. NiS-MoS 2 /CNTs/CN catalyst exhibits high performance for H 2 evolution and the optimized rate is 309.9 μmol·h -1 ·g -1 with no noble metals under visible light irradiation. The study demonstrates a non-noble metal photocatalyst system for effective generation of hydrogen with low cost. Copyright © 2018 Elsevier Inc. All rights reserved.

New understanding on separation of Mn and Fe from ferruginous manganese ores by the magnetic reduction roasting process

NASA Astrophysics Data System (ADS)

Liu, Bingbing; Zhang, Yuanbo; Wang, Juan; Wang, Jia; Su, Zijian; Li, Guanghui; Jiang, Tao

2018-06-01

Magnetic reduction roasting followed by magnetic separation process is reported as a simple route to realize separation of Mn and Fe from ferruginous manganese ores (Fe-Mn ores). However, the separation and recovery of Mn and Fe oxides are not very effective. This work clarified the underlying reason for the poor separation and also proposed some suggestions for the magnetic reduction process. In this work, the effect of temperature on the magnetic reduction roasting - magnetic separation of Fe-Mn ore was investigated firstly. Then the reduction behaviors of MnO2-Fe2O3 system and MnO2-Fe2O3-10 wt.%SiO2 system under 10 vol.% CO-90 vol.% CO2 at 600-1000 °C were investigated by XRD, XPS, SEM-EDS, VSM, DSC and thermodynamics analyses. Reduction and separation tests showed that higher reduction temperature was beneficial to the recovery of iron while it's not in favor of the recovery of manganese when the temperature was over 800 °C. The formation of composite oxide MnxFe3-xO4 with strong magnetism between the interface of the MnO2 and Fe2O3 particles leaded to the poor separation of iron and manganese. In addition, the formation mechanism of MnxFe3-xO4 from MnO2 and Fe2O3 as well as the interface reaction reduced under 10 vol.% CO was discussed in this study. Finally, some suggestions were recommended for the magnetic reduction roasting for utilizing the Fe-Mn ores effectively.

Selective, tunable O 2 binding in cobalt(II)–triazolate/pyrazolate metal–organic frameworks

DOE PAGES

Xiao, Dianne J.; Gonzalez, Miguel I.; Darago, Lucy E.; ...

2016-05-16

Here, the air-free reaction of CoCl 2 with 1,3,5-tri(1H- 1,2,3-triazol-5-yl)benzene (H 3BTTri) in N,N-dimethylformamide (DMF) and methanol leads to the formation of Co- BTTri (Co 3[(Co 4Cl) 3(BTTri) 8] 2·DMF), a sodalite-type metal-organic framework. Desolvation of this material generates coordinatively unsaturated low-spin cobalt(II) centers that exhibit a strong preference for binding O 2 over N 2, with isosteric heats of adsorption (Q st) of -34(1) and -12(1) kJ/ mol, respectively. The low-spin (S = 1/2) electronic configuration of the metal centers in the desolvated framework is supported by structural, magnetic susceptibility, and computational studies. A single-crystal X-ray structure determination revealsmore » that O 2 binds end-on to each framework cobalt center in a 1:1 ratio with a Co-O 2 bond distance of 1.973(6) Å. Replacement of one of the triazolate linkers with a more electron-donating pyrazolate group leads to the isostructural framework Co-BDTriP (Co 3[(Co 4Cl) 3(BDTriP) 8] 2·DMF; H 3BDTriP = 5,5'-(5-(1H-pyrazol-4-yl)-1,3-phenylene)bis(1H-1,2,3-triazole)), which demonstrates markedly higher yet still fully reversible O 2 affinities (Q st = -47(1) kJ/mol at low loadings). Electronic structure calculations suggest that the O 2 adducts in Co-BTTri are best described as cobalt(II)-dioxygen species with partial electron transfer, while the stronger binding sites in Co-BDTriP form cobalt(III)-superoxo moieties. The stability, selectivity, and high O 2 adsorption capacity of these materials render them promising new adsorbents for air separation processes.« less

Two-Stage Separation of V(IV) and Al(III) by Crystallization and Solvent Extraction from Aluminum-Rich Sulfuric Acid Leaching Solution of Stone Coal

NASA Astrophysics Data System (ADS)

Shi, Qihua; Zhang, Yimin; Liu, Tao; Huang, Jing; Liu, Hong

2017-10-01

To improve separation of V(IV) and Al(III) from aluminum-rich sulfuric acid leaching solution of stone coal, the two-stage separation by crystallization and solvent extraction methods have been developed. A co-extraction coefficient ( k) was put forward to evaluate comprehensively co-extraction extent in different solutions. In the crystallization stage, 68.2% of aluminum can be removed from the solution. In the solvent extraction stage, vanadium was selectively extracted using di-2-ethylhexyl phosphoric acid/tri-n-butyl phosphate from the crystalline mother solution, followed by H2SO4 stripped efficiently. A V2O5 product with purity of 98.39% and only 0.10% Al was obtained after oxidation, precipitation, and calcination. Compared with vanadium extraction from solution without crystallization, the counter-current extraction stage of vanadium can be decreased from 6 to 3 and co-extraction coefficient ( k) decreased from 2.51 to 0.58 with two-stage separation. It is suggested that the aluminum removal by crystallization can evidently weaken the influence of aluminum co-extraction on vanadium extraction and improve the selectivity of solvent extraction for vanadium.

A generic analysis of energy use and solvent selection for CO2 separation from post-combustion flue gases

USGS Publications Warehouse

Lu, Y.; Chen, S.; Rostam-Abadi, M.

2008-01-01

A thermodynamic calculation was performed to determine the theoretical minimum energy used to separate CO2 from a coal combustion flue gas in a typical adsorption-desorption system. Under ideal conditions, the minimum energy required to separate CO2 from post-combustion flue gas and produce pure CO2 at 1 atmospheric pressure was only about 1183 kJ/kg CO2. This amount could double with the addition of the driving forces of mass and heat transfer and the adverse impacts of absorption heat release on adsorption capacity. Thermodynamic analyses were also performed for the aqueous amine-based absorption process. Two CO2 reaction mechanisms, the carbamate formation reaction with primary/secondary amines and the CO2 hydration reaction with tertiary amines, were included in the absorption reaction. The reaction heat, sensible heat, and stripping heat were all important to the total heat requirement. The heat use of an ideal tertiary amine amounted to 2786 kJ/kg, compared to 3211 kJ/kg for an ideal primary amine. The heat usage of an ideal amine was about 20% lower than that of commercially available amines. Optimizing the absorption process configuration could further reduce energy use. This is an abstract of a paper presented at the 2008 AIChE Spring National Meeting (New Orleans, LA 4/6-10/2008).

Suitability Evaluation of Multipoint Simultaneous CO2 Sampling Wireless Sensors for Livestock Buildings

PubMed Central

Calvet, Salvador; Campelo, José Carlos; Estellés, Fernando; Perles, Angel; Mercado, Ricardo; Serrano, Juan José

2014-01-01

The environment in livestock buildings must be controlled to ensure the health and welfare of both workers and animals, as well as to restrict the emission of pollutants to the atmosphere. Among the pollutants generated inside these premises, carbon dioxide (CO2) is of great interest in terms of animal welfare and ventilation control. The use of inexpensive sensors means that complete systems can be designed with a number of sensors located around the building. This paper describes a study of the suitability of multipoint simultaneous CO2 sensors operating in a wireless sensor network, which was found to operate satisfactorily under laboratory conditions and was found to be the best alternative for these applications. The sensors showed a highly linear response to CO2 concentrations, ranging from 500 to 5000 ppm. However, individual sensor response was found to differ, which made it necessary to calibrate each one separately. Sensor precision ranged between 80 and 110 ppm CO2, and sensor response to register a 95% change in concentration was estimated at around 5 min. These features mean this type of sensor network can be used to monitor animal welfare and also for environmental control in poorly ventilated livestock premises. According to the tests conducted in this study, a temporal drift may occur and therefore a regular calibration of sensors would be needed. PMID:24932867

Evaluating source separation of plastic waste using conjoint analysis.

PubMed

Nakatani, Jun; Aramaki, Toshiya; Hanaki, Keisuke

2008-11-01

Using conjoint analysis, we estimated the willingness to pay (WTP) of households for source separation of plastic waste and the improvement of related environmental impacts, the residents' loss of life expectancy (LLE), the landfill capacity, and the CO2 emissions. Unreliable respondents were identified and removed from the sample based on their answers to follow-up questions. It was found that the utility associated with reducing LLE and with the landfill capacity were both well expressed by logarithmic functions, but that residents were indifferent to the level of CO2 emissions even though they approved of CO2 reduction. In addition, residents derived utility from the act of separating plastic waste, irrespective of its environmental impacts; that is, they were willing to practice the separation of plastic waste at home in anticipation of its "invisible effects", such as the improvement of citizens' attitudes toward solid waste issues.

40 CFR 1065.550 - Gas analyzer range validation and drift validation.

Code of Federal Regulations, 2012 CFR

2012-07-01

... a dry sample measured with a CLD and the removed water is corrected based on measured CO2, CO, THC... may not validate the concentration subcomponents (e.g., THC and CH4 for NMHC) separately. For example, for NMHC measurements, perform drift validation on NMHC; do not validate THC and CH4 separately. (2...

40 CFR 1065.550 - Gas analyzer range verification and drift verification.

Code of Federal Regulations, 2014 CFR

2014-07-01

... with a CLD and the removed water is corrected based on measured CO2, CO, THC, and NOX concentrations... concentration subcomponents (e.g., THC and CH4 for NMHC) separately. For example, for NMHC measurements, perform drift verification on NMHC; do not verify THC and CH4 separately. (2) Drift verification requires two...

40 CFR 1065.550 - Gas analyzer range validation and drift validation.

Code of Federal Regulations, 2013 CFR

2013-07-01

... a dry sample measured with a CLD and the removed water is corrected based on measured CO2, CO, THC... may not validate the concentration subcomponents (e.g., THC and CH4 for NMHC) separately. For example, for NMHC measurements, perform drift validation on NMHC; do not validate THC and CH4 separately. (2...

Study on O2 generation and CO2 absorption capability of four co-cultured salad plants in an enclosed system

NASA Astrophysics Data System (ADS)

Guo, Shuangsheng; Ai, Weidang; Tang, Yongkang; Cheng, Quanyong; Shen, Yunze; Qin, Lifeng; Ma, Jialu; Zhu, Jingtao; Ren, Jin

2014-06-01

The ability to generate O2 and absorb CO2 of several co-cultured vegetable plants in an enclosed system was studied to provide theoretical reference for the future man-plant integrated tests. Four kinds of salad plants (Lactuca sativa L. var. Dasusheng, Lactuca sativa L. var. Youmaicai, Gynura bicolor and Cichorium endivia L.) were grown in the CELSS Integration Test Platform (CITP). The environmental factors including O2 and CO2 concentration were continuously monitored on-line and the plant biomass was measured at the end of the test. The changing rules of O2 and CO2 concentration in the system were basically understood and it was found that the O2 generated by the plants could satisfy the respiratory needs of 1.75 persons by calculation. It was also found that the plants could absorb the CO2 breathed out by 2 persons when the light intensity was raised to 550 mmol m-2 s-1 PPF. The results showed that the co-cultured plants hold good compatibility and excellent O2-generating and CO2-absorbing capability. They could also supply some fresh edible vegetable for a 2-person crew.

Application of activated carbon modified by acetic acid in adsorption and separation of CO2 and CH4

NASA Astrophysics Data System (ADS)

Song, Xue; Wang, Li'ao; Zeng, Yunmin; Zhan, Xinyuan; Gong, Jian; Li, Tong

2018-03-01

Compared with the methods to modify the activated carbons by alkalis for gas adsorption, fewer studies of that by organic acids have been reported. The acid modified activated carbons are usually utilized to treat wastewater, whereas the application in the separation of CO2/CH4 has less been studied. In this study, acetic acid was used to modify activated carbon. N2 adsorption/desorption isotherms and FT-IR were adopted to describe the properties of the samples. According to the adsorption data of pure gas component at 298 K, the gas adsorbed amount and the selectivity on the modified samples were larger than that on the raw sample. Besides, the adsorbed amount of CO2 and the selectivity on 15H-AC in the adsorption breakthrough experiments showed better performance. The results confirm that the method to modify the activated carbons with acetic acid is feasible to improve the adsorption capacity and the separation effect of CO2/CH4.

Interfacial properties of black phosphorus/transition metal carbide van der Waals heterostructures

NASA Astrophysics Data System (ADS)

Yuan, Hao; Li, Zhenyu

2018-06-01

Owing to its outstanding electronic properties, black phosphorus (BP) is considered as a promising material for next-generation optoelectronic devices. In this work, devices based on BP/MXene (Zr n+1C n T2, T = O, F, OH, n = 1, 2) van der Waals (vdW) heterostructures are designed via first-principles calculations. Zr n+1C n T2 compositions with appropriate work functions lead to the formation of Ohmic contact with BP in the vertical direction. Low Schottky barriers are found along the lateral direction in BP/Zr2CF2, BP/Zr2CO2H2, BP/Zr3C2F2, and BP/Zr3C2O2H2 bilayers, and BP/Zr3C2O2 even exhibits Ohmic contact behavior. BP/Zr2CO2 is a semiconducting heterostructure with type-II band alignment, which facilitates the separation of electron-hole pairs. The band structure of BP/Zr2CO2 can be effectively tuned via a perpendicular electric field, and BP is predicted to undergo a transition from donor to acceptor at a 0.4 V/Å electric field. The versatile electronic properties of the BP/MXene heterostructures examined in this work highlight their promising potential for applications in electronics.

Molecular simulations for adsorption and separation of natural gas in IRMOF-1 and Cu-BTC metal-organic frameworks.

PubMed

Martín-Calvo, Ana; García-Pérez, Elena; Manuel Castillo, Juan; Calero, Sofia

2008-12-21

We use Monte Carlo simulations to study the adsorption and separation of the natural gas components in IRMOF-1 and Cu-BTC metal-organic frameworks. We computed the adsorption isotherms of pure components, binary, and five-component mixtures analyzing the siting of the molecules in the structure for the different loadings. The bulk compositions studied for the mixtures were 50 : 50 and 90 : 10 for CH4-CO2, 90 : 10 for N2-CO2, and 95 : 2.0 : 1.5 : 1.0 : 0.5 for the CH4-C2H6-N2-CO2-C3H8 mixture. We choose this composition because it is similar to an average sample of natural gas. Our simulations show that CO2 is preferentially adsorbed over propane, ethane, methane and N2 in the complete pressure range under study. Longer alkanes are favored over shorter alkanes and the lowest adsorption corresponds to N2. Though IRMOF-1 has a significantly higher adsorption capacity than Cu-BTC, the adsorption selectivity of CO2 over CH4 and N2 is found to be higher in the latter, proving that the separation efficiency is largely affected by the shape, the atomic composition and the type of linkers of the structure.

Contributions of past and present human generations to committed warming caused by carbon dioxide.

PubMed

Friedlingstein, Pierre; Solomon, Susan

2005-08-02

We developed a highly simplified approach to estimate the contributions of the past and present human generations to the increase of atmospheric CO(2) and associated global average temperature increases. For each human generation of adopted 25-year length, we use simplified emission test cases to estimate the committed warming passed to successive children, grandchildren, and later generations. We estimate that the last and the current generation contributed approximately two thirds of the present-day CO(2)-induced warming. Because of the long time scale required for removal of CO(2) from the atmosphere as well as the time delays characteristic of physical responses of the climate system, global mean temperatures are expected to increase by several tenths of a degree for at least the next 20 years even if CO(2) emissions were immediately cut to zero; that is, there is a commitment to additional CO(2)-induced warming even in the absence of emissions. If the rate of increase of CO(2) emissions were to continue up to 2025 and then were cut to zero, a temperature increase of approximately 1.3 degrees C compared to preindustrial conditions would still occur in 2100, whereas a constant-CO(2)-emissions scenario after 2025 would more than double the 2100 warming. These calculations illustrate the manner in which each generation inherits substantial climate change caused by CO(2) emissions that occurred previously, particularly those of their parents, and shows that current CO(2) emissions will contribute significantly to the climate change of future generations.

Integrated System Design for Air Revitalization in Next Generation Crewed Spacecraft

NASA Technical Reports Server (NTRS)

Mulloth, Lila; Perry, Jay; LeVan, Douglas

2004-01-01

The capabilities of NASA's existing environmental control and life support (ECLS) system designs are inadequate for future human space initiatives that involve long-duration space voyages and interplanetary missions. This paper discusses the concept of an integrated system of CO2 removal and trace contaminant control units that utilizes novel gas separation and purification techniques and optimized thermal and mechanical design, for future spacecraft. The integration process will enhance the overall life and economics of the existing systems by eliminating multiple mechanical devices with moving parts.

Conversion of raw carbonaceous fuels

DOEpatents

Cooper, John F [Oakland, CA

2007-08-07

Three configurations for an electrochemical cell are utilized to generate electric power from the reaction of oxygen or air with porous plates or particulates of carbon, arranged such that waste heat from the electrochemical cells is allowed to flow upwards through a storage chamber or port containing raw carbonaceous fuel. These configurations allow combining the separate processes of devolatilization, pyrolysis and electrochemical conversion of carbon to electric power into a single unit process, fed with raw fuel and exhausting high BTU gases, electric power, and substantially pure CO.sub.2 during operation.

CO{sub 2} adsorption-based separation by metal organic framework (Cu-BTC) versus zeolite (13X)

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

Zhijian Liang; Marc Marshall; Alan L. Chaffee

2009-05-15

The potential for the metal organic framework (MOF) Cu-BTC to selectively adsorb and separate CO{sub 2} is considered. Isotherms for CO{sub 2}, CH{sub 4}, and N{sub 2} were measured from 0 to 15 bar and at temperatures between 25 and 105{sup o}C. The isotherms suggest a much higher working capacity (x4) for CO{sub 2} adsorption on Cu-BTC relative to the benchmark zeolite 13X over the same pressure range. Higher CO{sub 2}/N{sub 2} and CO{sub 2}/CH{sub 4} selectivities in the higher pressure range (1-15 bar) and with lower heats of adsorption were also demonstrated. Cu-BTC was observed to be stable inmore » O{sub 2} at 25{sup o}C, but its crystallinity was reduced in humid environments. The CO{sub 2} adsorption capacity was progressively reduced upon cyclic exposure to water vapor at low relative humidity (<30%), but leveled out at 75% of its original value after several water adsorption/desorption cycles. 27 refs., 1 fig.« less

Lithium recycling and cathode material regeneration from acid leach liquor of spent lithium-ion battery via facile co-extraction and co-precipitation processes.

PubMed

Yang, Yue; Xu, Shengming; He, Yinghe

2017-06-01

A novel process for extracting transition metals, recovering lithium and regenerating cathode materials based on facile co-extraction and co-precipitation processes has been developed. 100% manganese, 99% cobalt and 85% nickel are co-extracted and separated from lithium by D2EHPA in kerosene. Then, Li is recovered from the raffinate as Li 2 CO 3 with the purity of 99.2% by precipitation method. Finally, organic load phase is stripped with 0.5M H 2 SO 4 , and the cathode material LiNi 1/3 Co 1/3 Mn 1/3 O 2 is directly regenerated from stripping liquor without separating metal individually by co-precipitation method. The regenerative cathode material LiNi 1/3 Co 1/3 Mn 1/3 O 2 is miro spherical morphology without any impurities, which can meet with LiNi 1/3 Co 1/3 Mn 1/3 O 2 production standard of China and exhibits good electrochemical performance. Moreover, a waste battery management model is introduced to guarantee the material supply for spent battery recycling. Copyright © 2017 Elsevier Ltd. All rights reserved.

Bio-inspired cofacial Fe porphyrin dimers for efficient electrocatalytic CO2 to CO conversion: Overpotential tuning by substituents at the porphyrin rings

PubMed Central

Zahran, Zaki N.; Mohamed, Eman A.; Naruta, Yoshinori

2016-01-01

Efficient reduction of CO2 into useful carbon resources particularly CO is an essential reaction for developing alternate sources of fuels and for reducing the greenhouse effect of CO2. The binuclear Ni, Fe−containing carbon monoxide dehydrogenase (CODHs) efficiently catalyzes the reduction of CO2 to CO. The location of Ni and Fe at proper positions allows their cooperation for CO2 to CO conversion through a push−pull mechanism. Bio−inspired from CODHs, we used several cofacial porphyrin dimers with different substituents as suitable ligands for holding two Fe ions with suitable Fe−Fe separation distance to efficiently and selectively promote CO2 to CO conversion with high turnover frequencies, TOFs. The substituents on the porphyrin rings greatly affect the catalysis process. By introducing electron-withdrawing/-donating groups, e.g. electron-withdrawing perfluorophenyl, at all meso positions of the porphyrin rings, the catalysis overpotential, η was minimized by ≈0.3 V compared to that obtained by introducing electron-donating mesityl groups. The Fe porphyrin dimers among reported catalysts are the most efficient ones for CO2 to CO conversion. Control experiments indicate that the high performance of the current CO2 to CO conversion catalysts is due to the presence of binuclear Fe centers at suitable Fe−Fe separation distance. PMID:27087483

Bio-inspired cofacial Fe porphyrin dimers for efficient electrocatalytic CO2 to CO conversion: Overpotential tuning by substituents at the porphyrin rings.

PubMed

Zahran, Zaki N; Mohamed, Eman A; Naruta, Yoshinori

2016-04-18

Efficient reduction of CO2 into useful carbon resources particularly CO is an essential reaction for developing alternate sources of fuels and for reducing the greenhouse effect of CO2. The binuclear Ni, Fe-containing carbon monoxide dehydrogenase (CODHs) efficiently catalyzes the reduction of CO2 to CO. The location of Ni and Fe at proper positions allows their cooperation for CO2 to CO conversion through a push-pull mechanism. Bio-inspired from CODHs, we used several cofacial porphyrin dimers with different substituents as suitable ligands for holding two Fe ions with suitable Fe-Fe separation distance to efficiently and selectively promote CO2 to CO conversion with high turnover frequencies, TOFs. The substituents on the porphyrin rings greatly affect the catalysis process. By introducing electron-withdrawing/-donating groups, e.g. electron-withdrawing perfluorophenyl, at all meso positions of the porphyrin rings, the catalysis overpotential, η was minimized by ≈0.3 V compared to that obtained by introducing electron-donating mesityl groups. The Fe porphyrin dimers among reported catalysts are the most efficient ones for CO2 to CO conversion. Control experiments indicate that the high performance of the current CO2 to CO conversion catalysts is due to the presence of binuclear Fe centers at suitable Fe-Fe separation distance.

Bio-inspired cofacial Fe porphyrin dimers for efficient electrocatalytic CO2 to CO conversion: Overpotential tuning by substituents at the porphyrin rings

NASA Astrophysics Data System (ADS)

Zahran, Zaki N.; Mohamed, Eman A.; Naruta, Yoshinori

2016-04-01

Efficient reduction of CO2 into useful carbon resources particularly CO is an essential reaction for developing alternate sources of fuels and for reducing the greenhouse effect of CO2. The binuclear Ni, Fe-containing carbon monoxide dehydrogenase (CODHs) efficiently catalyzes the reduction of CO2 to CO. The location of Ni and Fe at proper positions allows their cooperation for CO2 to CO conversion through a push-pull mechanism. Bio-inspired from CODHs, we used several cofacial porphyrin dimers with different substituents as suitable ligands for holding two Fe ions with suitable Fe-Fe separation distance to efficiently and selectively promote CO2 to CO conversion with high turnover frequencies, TOFs. The substituents on the porphyrin rings greatly affect the catalysis process. By introducing electron-withdrawing/-donating groups, e.g. electron-withdrawing perfluorophenyl, at all meso positions of the porphyrin rings, the catalysis overpotential, η was minimized by ≈0.3 V compared to that obtained by introducing electron-donating mesityl groups. The Fe porphyrin dimers among reported catalysts are the most efficient ones for CO2 to CO conversion. Control experiments indicate that the high performance of the current CO2 to CO conversion catalysts is due to the presence of binuclear Fe centers at suitable Fe-Fe separation distance.

Development of vinylic and acetylenic functionalized structures based on high permeable glassy polymers as membrane materials for gas mixtures separation

NASA Astrophysics Data System (ADS)

Roizard, D.; Kiryukhina, Y.; Masalev, A.; Khotimskiy, V.; Teplyakov, V.; Barth, D.

2013-03-01

There are several challenging separation problems in industries which can be solved with the help of membrane technologies. It is the case for instance of the purification of gas energy carriers (i.e. H2, CH4) from CO2 as well as the CO2 recovery from flue gas. Glassy polymers containing trimethylsilyl residues like poly(1-trimethylsilyl-1-propyne) [PTMSP] and polyvinyltrimethylsilane [PVTMS] are known to exhibit good membrane properties for gas separation. This paper reports two ways of improving their performances based on the controlled introduction of selective groups - alkyl imidazomium salts (C4I) and polyethyleneglycol (M-PEG)- able to enhance CO2 selectivity. CO2 Isotherm sorption data and permeability measurements have shown that the membrane performances could be significantly improved when C4I and M-PEG were introduced as residues covalently bounded to the main polymer chain. Moreover the introduced bromine reactive centres could also be used to induce chemical crosslinking giving rise to more resistant and stable membranes to organic vapours. With the C4I groups, the CO2 sorption could be enhanced by a factor 4.4.

Carbon dioxide (hydrogen sulfide) membrane separations and WGS membrane reactor modeling for fuel cells

NASA Astrophysics Data System (ADS)

Huang, Jin

Acid-gas removal is of great importance in many environmental or energy-related processes. Compared to current commercial technologies, membrane-based CO2 and H2S capture has the advantages of low energy consumption, low weight and space requirement, simplicity of installation/operation, and high process flexibility. However, the large-scale application of the membrane separation technology is limited by the relatively low transport properties. In this study, CO2 (H2S)-selective polymeric membranes with high permeability and high selectivity have been studied based on the facilitated transport mechanism. The membrane showed facilitated effect for both CO2 and H2S. A CO2 permeability of above 2000 Barrers, a CO2/H2 selectivity of greater than 40, and a CO2/N2 selectivity of greater than 200 at 100--150°C were observed. As a result of higher reaction rate and smaller diffusing compound, the H2S permeability and H2S/H2 selectivity were about three times higher than those properties for CO2. The novel CO2-selective membrane has been applied to capture CO 2 from flue gas and natural gas. In the CO2 capture experiments from a gas mixture with N2 and H2, a permeate CO 2 dry concentration of greater than 98% was obtained by using steam as the sweep gas. In CO2/CH4 separation, decent CO 2 transport properties were obtained with a feed pressure up to 500 psia. With the thin-film composite membrane structure, significant increase on the CO2 flux was achieved with the decrease of the selective layer thickness. With the continuous removal of CO2, CO2-selective water-gas-shift (WGS) membrane reactor is a promising approach to enhance CO conversion and increase the purity of H2 at process pressure under relatively low temperature. The simultaneous reaction and transport process in the countercurrent WGS membrane reactor was simulated by using a one-dimensional non-isothermal model. The modeling results show that a CO concentration of less than 10 ppm and a H2 recovery of greater than 97% are achievable from reforming syngases. In an experimental study, the reversible WGS was shifted forward by removing CO2 so that the CO concentration was significantly decreased to less than 10 ppm. The modeling results agreed well with the experimental data.

Immobilization of R-ω-transaminase on MnO2 nanorods for catalyzing the conversion of (R)-1-phenylethylamine.

PubMed

Sun, Jian; Cui, Wen-Hui; Du, Kun; Gao, Qian; Du, Mengmeng; Ji, Peijun; Feng, Wei

2017-03-10

R-ɷ-transaminases transfer an amino group from an amino donor (e.g. (R)-1-phenylethylamine) onto an amino acceptor (e.g. pyruvate), resulting a co-product (e.g. d-alanine). This work intends to immobilize R-ɷ-Transaminase on MnO 2 nanorods to achieve multienzyme catalysis. R-ɷ-Transaminase (RTA) and d-amino acid oxidase (DAAO) have been fused to an elastin-like polypeptide (ELP) separately through genetic engineering of the enzymes. ELP-RTA and ELP-DAAO have been separately immobilized on polydopamine-coated MnO 2 nanorods. When the two immobilized enzymes were used together in one pot, the transformation of (R)-1-phenylethylamine was catalyzed by the immobilized ELP-RTA, and the co-product d-alanine was converted back to pyruvate under the catalysis of the immobilized ELP-DAAO, achieving the recycling of pyruvate in situ. Thus pyruvate was maintained at a low concentration in order to reduce its negative effect. On the other hand, the generated H 2 O 2 of ELP-DAAO was decomposed by the MnO 2 nanorods, and the evolved oxygen oxidized the reduced cofactors of ELP-DAAO. Forming the circles of hydrogen peroxide→oxygen→hydrogen peroxide accelerated the deamination reaction. The highly efficient conversion of the co-product d-alanine back to pyruvate accelerated the forming of the pyruvate→d-alanine→pyruvate cycle between the two immobilized enzymes. The coordination of the pyruvate→d-alanine→pyruvate and hydrogen peroxide→oxygen→hydrogen peroxide cycles accelerated the transformation of (R)-1-phenylethylamine. As a result, As a result, the immobilized enzymes achieved a conversion of 98±1.8% in comparison to 69.6±1.2% by free enzymes. Copyright © 2017 Elsevier B.V. All rights reserved.

Design Principles of Perovskites for Thermochemical Oxygen Separation

PubMed Central

Ezbiri, Miriam; Allen, Kyle M.; Gàlvez, Maria E.; Steinfeld, Aldo

2015-01-01

Abstract Separation and concentration of O2 from gas mixtures is central to several sustainable energy technologies, such as solar‐driven synthesis of liquid hydrocarbon fuels from CO2, H2O, and concentrated sunlight. We introduce a rationale for designing metal oxide redox materials for oxygen separation through “thermochemical pumping” of O2 against a pO2 gradient with low‐grade process heat. Electronic structure calculations show that the activity of O vacancies in metal oxides pinpoints the ideal oxygen exchange capacity of perovskites. Thermogravimetric analysis and high‐temperature X‐ray diffraction for SrCoO3−δ, BaCoO3−δ and BaMnO3−δ perovskites and Ag2O and Cu2O references confirm the predicted performance of SrCoO3−δ, which surpasses the performance of state‐of‐the‐art Cu2O at these conditions with an oxygen exchange capacity of 44 mmol O 2 mol SrCoO 3−δ −1 exchanged at 12.1 μmol O 2 min−1 g−1 at 600–900 K. The redox trends are understood due to lattice expansion and electronic charge transfer. PMID:25925955

Preparation and Characterization of Facilitated Transport Membranes Composed of Chitosan-Styrene and Chitosan-Acrylonitrile Copolymers Modified by Methylimidazolium Based Ionic Liquids for CO2 Separation from CH4 and N2

PubMed Central

Otvagina, Ksenia V.; Mochalova, Alla E.; Sazanova, Tatyana S.; Petukhov, Anton N.; Moskvichev, Alexandr A.; Vorotyntsev, Andrey V.; Afonso, Carlos A. M.; Vorotyntsev, Ilya V.

2016-01-01

CO2 separation was found to be facilitated by transport membranes based on novel chitosan (CS)–poly(styrene) (PS) and chitosan (CS)–poly(acrylonitrile) (PAN) copolymer matrices doped with methylimidazolium based ionic liquids: [bmim][BF4], [bmim][PF6], and [bmim][Tf2N] (IL). CS plays the role of biodegradable film former and selectivity promoter. Copolymers were prepared implementing the latest achievements in radical copolymerization with chosen monomers, which enabled the achievement of outstanding mechanical strength values for the CS-based membranes (75–104 MPa for CS-PAN and 69–75 MPa for CS-PS). Ionic liquid (IL) doping affected the surface and mechanical properties of the membranes as well as the gas separation properties. The highest CO2 permeability 400 Barrers belongs to CS-b-PS/[bmim][BF4]. The highest selectivity α (CO2/N2) = 15.5 was achieved for CS-b-PAN/[bmim][BF4]. The operational temperature of the membranes is under 220 °C. PMID:27294964

CEC with new monolithic stationary phase based on a fluorinated monomer, trifluoroethyl methacrylate.

PubMed

Yurtsever, Arda; Saraçoğlu, Berna; Tuncel, Ali

2009-02-01

A new, fluorinated monolithic stationary phase for CEC was first synthesized by a single-stage, thermally initiated copolymerization of a fluorinated monomer, 2,2,2-trifluoroethyl methacrylate (TFEM) and ethylene dimethacrylate (EDMA) in the presence of a porogen mixture. In this preparation, 2-acrylamido-2-methyl-1-propanesulfonic acid was used as the charge-bearing monomer. The porogen mixture was prepared by mixing isoamylalcohol and 1,4-butanediol. A clear increase in the electroosmotic mobility was observed with increasing pH. The electroosmotic mobility decreased with increasing ACN concentration. Poly(TFEM-co-EDMA) monolith prepared under optimized polymerization conditions was successfully used in the separation of alkylbenzenes and phenols by CEC. The best chromatographic separation for alkylbenzenes was performed with lower ACN concentrations (i.e. 60% v/v) with respect to the common acrylic-based CEC monoliths. The theoretical plate numbers up to 220 000 plates/m were achieved in the reversed phase separation of phenols. Poly(TFEM-co-EDMA) monolith also allowed the simultaneous separation of aniline and benzoic acid derivatives by a single run and by using a lower ACN concentration in the mobile phase with respect to the similar electrochromatographic separations. A stable retention behaviour in reversed phase separation of alkylbenzenes was obtained with the poly(TFEM-co-EDMA) monolith.

Low cost hydrogen/novel membrane technology for hydrogen separation from synthesis gas

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

Not Available

1986-02-01

To make the coal-to-hydrogen route economically attractive, improvements are being sought in each step of the process: coal gasification, water-carbon monoxide shift reaction, and hydrogen separation. This report addresses the use of membranes in the hydrogen separation step. The separation of hydrogen from synthesis gas is a major cost element in the manufacture of hydrogen from coal. Separation by membranes is an attractive, new, and still largely unexplored approach to the problem. Membrane processes are inherently simple and efficient and often have lower capital and operating costs than conventional processes. In this report current ad future trends in hydrogen productionmore » and use are first summarized. Methods of producing hydrogen from coal are then discussed, with particular emphasis on the Texaco entrained flow gasifier and on current methods of separating hydrogen from this gas stream. The potential for membrane separations in the process is then examined. In particular, the use of membranes for H{sub 2}/CO{sub 2}, H{sub 2}/CO, and H{sub 2}/N{sub 2} separations is discussed. 43 refs., 14 figs., 6 tabs.« less

STRUCTURAL EFFECTS ON THE HIGH TEMPERATURE ADSORPTION OF CO2 ON A SYNTHETIC HYDROTALCITE

EPA Science Inventory

Hydrotalcite-like compounds (HTlcs) are solid sorbents that may potentially be used for high temperature separation and capture of CO₂. The high-temperature adsorption of CO₂ on Mg-Al-CO₃ HTlc is affected by structural changes that take place upo...

Molecular dynamics investigation of separation of hydrogen sulfide from acidic gas mixtures inside metal-doped graphite micropores.

PubMed

Huang, Pei-Hsing

2015-09-21

The separation of poisonous compounds from various process fluids has long been highly intractable, motivating the present study on the dynamic separation of H2S in acidic-gas-mixture-filled micropores. The molecular dynamics approach, coupled with the isothermal-isochoric ensemble, was used to model the molecular interactions and adsorption of H2S/CO2/CO/H2O mixtures inside metal-doped graphite slits. Due to the difference in the adsorption characteristics between the two distinct adsorbent materials, the metal dopant in the graphitic micropores leads to competitive adsorption, i.e. the Au and graphite walls compete to capture free adsorbates. The effects of competitive adsorption, coupled with changes in the gas temperature, concentration, constituent ratio and slit width on the constituent separation of mixtures were systematically studied. The molecule-wall binding energies calculated in this work (those of H2S, H2O and CO on Au walls and those of H2O, CO and CO2 on graphite walls) show good agreement with those obtained using density functional theory (DFT) and experimental results. The z-directional self-diffusivities (Dz) for adsorbates inside the slit ranged from 10(-9) to 10(-7) m(2) s(-1) as the temperature was increased from 10 to 500 K. The values are comparable with those for a typical microporous fluid (10(-8)-10(-9) m(2) s(-1) in a condensed phase and 10(-6)-10(-7) m(2) s(-1) in the gaseous state). The formation of H-bonding networks and hydrates of H2S is disadvantageous for the separation of mixtures. The results indicate that H2S can be efficiently separated from acidic gas mixtures onto the Au(111) surface by (i) reducing the mole fraction of H2S and H2O in the mixtures, (ii) raising the gas temperature to the high temperature limit (≥400 K), and (iii) lowering the slit width to below the threshold dimension (≤23.26 Å).

Catalyzed CO.sub.2-transport membrane on high surface area inorganic support

DOEpatents

Liu, Wei

2014-05-06

Disclosed are membranes and methods for making the same, which membranes provide improved permeability, stability, and cost-effective manufacturability, for separating CO.sub.2 from gas streams such as flue gas streams. High CO.sub.2 permeation flux is achieved by immobilizing an ultra-thin, optionally catalyzed fluid layer onto a meso-porous modification layer on a thin, porous inorganic substrate such as a porous metallic substrate. The CO.sub.2-selective liquid fluid blocks non-selective pores, and allows for selective absorption of CO.sub.2 from gas mixtures such as flue gas mixtures and subsequent transport to the permeation side of the membrane. Carbon dioxide permeance levels are in the order of 1.0.times.10.sup.-6 mol/(m.sup.2sPa) or better. Methods for making such membranes allow commercial scale membrane manufacturing at highly cost-effective rates when compared to conventional commercial-scale CO.sub.2 separation processes and equipment for the same and such membranes are operable on an industrial use scale.

40 CFR 98.143 - Calculating GHG emissions.

Code of Federal Regulations, 2012 CFR

2012-07-01

... Fuel Combustion Sources). (2) Calculate and report the process and combustion CO2 emissions separately... Fuel Combustion Sources) the combustion CO2 emissions in the glass furnace according to the applicable... calculate and report the annual process CO2 emissions from each continuous glass melting furnace using the...

40 CFR 98.193 - Calculating GHG emissions.

Code of Federal Regulations, 2012 CFR

2012-07-01

... Stationary Fuel Combustion Sources). (2) Calculate and report process and combustion CO2 emissions separately... Stationary Fuel Combustion Sources) the combustion CO2 emissions from each lime kiln according to the... must calculate and report the annual process CO2 emissions from all lime kilns combined using the...

40 CFR 98.193 - Calculating GHG emissions.

Code of Federal Regulations, 2013 CFR

2013-07-01

... Stationary Fuel Combustion Sources). (2) Calculate and report process and combustion CO2 emissions separately... Stationary Fuel Combustion Sources) the combustion CO2 emissions from each lime kiln according to the... must calculate and report the annual process CO2 emissions from all lime kilns combined using the...

40 CFR 98.143 - Calculating GHG emissions.

Code of Federal Regulations, 2013 CFR

2013-07-01

... Fuel Combustion Sources). (2) Calculate and report the process and combustion CO2 emissions separately... Fuel Combustion Sources) the combustion CO2 emissions in the glass furnace according to the applicable... calculate and report the annual process CO2 emissions from each continuous glass melting furnace using the...

Identification of nodes and internodes of chopped biomass stems by Image analysis

USDA-ARS?s Scientific Manuscript database

Separating the morphological components of biomass leads to better handling, more efficient processing as well as value added product generation, as these components vary in their chemical composition and can be preferentially utilized. Nodes and internodes of biomass stems have distinct chemical co...

Economic and energetic analysis of capturing CO2 from ambient air

PubMed Central

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

2011-01-01

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

Highly Permeable Oligo(ethylene oxide)- co-poly(dimethylsiloxane) Membranes for Carbon Dioxide Separation

DOE PAGES

Hong, Tao; Lai, Sophia C.; Mahurin, Shannon Mark; ...

2017-12-27

Here, a series of cross–linked, freestanding oligo(ethylene oxide)– co–(polydimethylsiloxane–norbornene) membranes with varied composition is synthesized via in situ ring–opening metathesis polymerization. These membranes show remarkably high CO 2 permeabilities (3400 Barrer) and their separation performance approaches the Robeson upper bound. The excellent permeability of these copolymer membranes provides great potential for real–world applications where enormous volumes of gases must be separated. The gas transport properties of these films are found to be directly proportional to oligo(ethylene oxide) content incorporation, which stems from the increased solubility selectivity change within the copolymer matrix. This work provides a systematic study of how gasmore » separation performance in rubbery membranes can be enhanced by tuning the CO 2–philicity of their constituent monomeric subunits.« less

Double heterojunction nanowire photocatalysts for hydrogen generation

NASA Astrophysics Data System (ADS)

Tongying, P.; Vietmeyer, F.; Aleksiuk, D.; Ferraudi, G. J.; Krylova, G.; Kuno, M.

2014-03-01

Charge separation and charge transfer across interfaces are key aspects in the design of efficient photocatalysts for solar energy conversion. In this study, we investigate the hydrogen generating capabilities and underlying photophysics of nanostructured photocatalysts based on CdSe nanowires (NWs). Systems studied include CdSe, CdSe/CdS core/shell nanowires and their Pt nanoparticle-decorated counterparts. Femtosecond transient differential absorption measurements reveal how semiconductor/semiconductor and metal/semiconductor heterojunctions affect the charge separation and hydrogen generation efficiencies of these hybrid photocatalysts. In turn, we unravel the role of surface passivation, charge separation at semiconductor interfaces and charge transfer to metal co-catalysts in determining photocatalytic H2 generation efficiencies. This allows us to rationalize why Pt nanoparticle decorated CdSe/CdS NWs, a double heterojunction system, performs best with H2 generation rates of ~434.29 +/- 27.40 μmol h-1 g-1 under UV/Visible irradiation. In particular, we conclude that the CdS shell of this double heterojunction system serves two purposes. The first is to passivate CdSe NW surface defects, leading to long-lived charges at the CdSe/CdS interface capable of carrying out reduction chemistries. Upon photoexcitation, we also find that CdS selectively injects charges into Pt NPs, enabling simultaneous reduction chemistries at the Pt NP/solvent interface. Pt nanoparticle decorated CdSe/CdS NWs thus enable reduction chemistries at not one, but rather two interfaces, taking advantage of each junction's optimal catalytic activities.Charge separation and charge transfer across interfaces are key aspects in the design of efficient photocatalysts for solar energy conversion. In this study, we investigate the hydrogen generating capabilities and underlying photophysics of nanostructured photocatalysts based on CdSe nanowires (NWs). Systems studied include CdSe, CdSe/CdS core/shell nanowires and their Pt nanoparticle-decorated counterparts. Femtosecond transient differential absorption measurements reveal how semiconductor/semiconductor and metal/semiconductor heterojunctions affect the charge separation and hydrogen generation efficiencies of these hybrid photocatalysts. In turn, we unravel the role of surface passivation, charge separation at semiconductor interfaces and charge transfer to metal co-catalysts in determining photocatalytic H2 generation efficiencies. This allows us to rationalize why Pt nanoparticle decorated CdSe/CdS NWs, a double heterojunction system, performs best with H2 generation rates of ~434.29 +/- 27.40 μmol h-1 g-1 under UV/Visible irradiation. In particular, we conclude that the CdS shell of this double heterojunction system serves two purposes. The first is to passivate CdSe NW surface defects, leading to long-lived charges at the CdSe/CdS interface capable of carrying out reduction chemistries. Upon photoexcitation, we also find that CdS selectively injects charges into Pt NPs, enabling simultaneous reduction chemistries at the Pt NP/solvent interface. Pt nanoparticle decorated CdSe/CdS NWs thus enable reduction chemistries at not one, but rather two interfaces, taking advantage of each junction's optimal catalytic activities. Electronic supplementary information (ESI) available: Details of NW syntheses, processing and characterization. Additional TEM images of CdS, CdSe and CdSe/CdS core/shell NWs. NW concentration and cross section estimates. Details of the Pt NP decoration. Additional TEM images of Pt NP decorated CdS, CdSe and CdSe/CdS core/shell NWs. Size distribution of Pt NPs for CdSe/Pt NP and CdSe/CdS/Pt NP NWs. Xe arc lamp spectrum. Details of H2 generation experiments. Estimated photon absorption rate. Details of TDA measurements. TDA spectra and kinetics of CdS and CdS/Pt NP NWs. Plot illustrating CdSe NW band edge bleach kinetics. Comparison of CdSe band edge bleach kinetics in CdSe/CdS core/shell NWs when excited at λexc = 387 nm and λexc = 560 nm. Comparison of CdSe band edge bleach kinetics in CdSe/Pt NP NWs when excited at λexc = 387 nm and λexc = 560 nm. Bar graph showing H2 generation efficiencies of CdS and CdS/Pt NP NWs. Bleach kinetics of CdSe/CdS/Pt NP NWs at λexc = 387 nm and λexc = 560 nm. Comparison of CdS band edge bleach kinetics in CdS/Pt NP, and CdSe/CdS core/shell NWs when excited at λexc = 387 nm. See DOI: 10.1039/c4nr00298a

Development Trends in Porous Adsorbents for Carbon Capture.

PubMed

Sreenivasulu, Bolisetty; Sreedhar, Inkollu; Suresh, Pathi; Raghavan, Kondapuram Vijaya

2015-11-03

Accumulation of greenhouse gases especially CO2 in the atmosphere leading to global warming with undesirable climate changes has been a serious global concern. Major power generation in the world is from coal based power plants. Carbon capture through pre- and post- combustion technologies with various technical options like adsorption, absorption, membrane separations, and chemical looping combustion with and without oxygen uncoupling have received considerable attention of researchers, environmentalists and the stake holders. Carbon capture from flue gases can be achieved with micro and meso porous adsorbents. This review covers carbonaceous (organic and metal organic frameworks) and noncarbonaceous (inorganic) porous adsorbents for CO2 adsorption at different process conditions and pore sizes. Focus is also given to noncarbonaceous micro and meso porous adsorbents in chemical looping combustion involving insitu CO2 capture at high temperature (>400 °C). Adsorption mechanisms, material characteristics, and synthesis methods are discussed. Attention is given to isosteric heats and characterization techniques. The options to enhance the techno-economic viability of carbon capture techniques by integrating with CO2 utilization to produce industrially important chemicals like ammonia and urea are analyzed. From the reader's perspective, for different classes of materials, each section has been summarized in the form of tables or figures to get a quick glance of the developments.

Apparatus and method for heterodyne-generated two-dimensional detector array using a single element detector

DOEpatents

Strauss, Charlie E.

1997-01-01

Apparatus and method for heterodyne-generated, two-dimensional detector array using a single detector. Synthetic-array heterodyne detection, permits a single-element optical detector to behave as though it were divided into an array of separate heterodyne detector elements. A fifteen-element synthetic array has successfully been experimentally realized on a single-element detector, permitting all of the array elements to be read out continuously and in parallel from one electrical connection. A CO.sub.2 laser and a single-element HgCdTe photodiode are employed. A different heterodyne local oscillator frequency is incident upon the spatially resolvable regions of the detector surface. Thus, different regions are mapped to different heterodyne beat frequencies. One can determine where the photons were incident on the detector surface even though a single electrical connection to the detector is used. This also prevents the destructive interference that occurs when multiple speckles are imaged (similar to spatial diversity), In coherent LIDAR this permits a larger field of view. An acoustooptic modulator generates the local oscillator frequencies and can achieve adequate spatial separation of optical frequencies of the order of a megahertz apart.

Apparatus and method for heterodyne-generated two-dimensional detector array using a single element detector

DOEpatents

Strauss, C.E.

1997-11-18

Apparatus and method are disclosed for heterodyne-generated, two-dimensional detector array using a single detector. Synthetic-array heterodyne detection, permits a single-element optical detector to behave as though it were divided into an array of separate heterodyne detector elements. A fifteen-element synthetic array has successfully been experimentally realized on a single-element detector, permitting all of the array elements to be read out continuously and in parallel from one electrical connection. A CO{sub 2} laser and a single-element HgCdTe photodiode are employed. A different heterodyne local oscillator frequency is incident upon the spatially resolvable regions of the detector surface. Thus, different regions are mapped to different heterodyne beat frequencies. One can determine where the photons were incident on the detector surface even though a single electrical connection to the detector is used. This also prevents the destructive interference that occurs when multiple speckles are imaged (similar to spatial diversity), In coherent LIDAR this permits a larger field of view. An acoustooptic modulator generates the local oscillator frequencies and can achieve adequate spatial separation of optical frequencies of the order of a megahertz apart. 4 figs.

Revealing the relationship between the photocatalytic property and structure characteristic of reduced TiO2 by hydrogen and carbon monoxide treatment.

PubMed

Liu, Yunpeng; Li, Yuhang; Yang, Siyuan; Lin, Yuan; Zuo, Jianliang; Liang, Hong; Peng, Feng

2018-06-04

The hydrogenation (reduction) has been considered as an effective method to improve the photocatalytic activity of TiO2, however, the underlying relationship between structure and photocatalytic performance has still not been adequately unveiled so far. Herein, to obtain insight into the effect of structure on photocatalytic activity, two types of reduced TiO2 were prepared by CO (CO-TiO2) and H2 (H-TiO2), respectively. For H-TiO2, Ti-H bonds and oxygen vacancies are formed on the surface of H-TiO2, resulting in a more disorder surface lattice. However, for CO-TiO2, the more Ti-OH bonds are formed on the surface and the more bulk oxygen vacancies are introduced, the disorder layer of CO-TiO2 is relatively thin owing to the most of surface vacancies repaired by Ti-OH bonds. Under the simulated solar irradiation, the photocatalytic H2 evolution rate of CO-TiO2 reaches 7.17 mmol g-1 h-1, which is 4.14 and 1.50 times those of TiO2 and H-TiO2, respectively. The photocatalytic degradation rate constant of methyl orange on CO-TiO2 is 2.45 and 6.39 times those on H-TiO2 and TiO2. The superior photocatalytic activity of CO-TiO2 is attributed to the effective separation and transfer of the photo-generated electron-hole pairs, due to the synergistic effects of oxygen vacancies and surface Ti-OH bonds. This study reveals the relation between the photocatalytic property and structure, and provides a new method to prepare highly active TiO2 for H2 production and environmental treatment. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Construction of an all-solid-state artificial Z-scheme system consisting of Bi2WO6/Au/CdS nanostructure for photocatalytic CO2 reduction into renewable hydrocarbon fuel.

PubMed

Wang, Meng; Han, Qiutong; Li, Liang; Tang, Lanqin; Li, Haijin; Zhou, Yong; Zou, Zhigang

2017-07-07

An all-solid-state Bi 2 WO 6 /Au/CdS Z-scheme system was constructed for the photocatalytic reduction of CO 2 into methane in the presence of water vapor. This Z-scheme consists of ultrathin Bi 2 WO 6 nanoplates and CdS nanoparticles as photocatalysts, and a Au nanoparticle as a solid electron mediator offering a high speed charge transfer channel and leading to more efficient spatial separation of electron-hole pairs. The photo-generated electrons from the conduction band (CB) of Bi 2 WO 6 transfer to the Au, and then release to the valence band (VB) of CdS to recombine with the holes of CdS. It allows the electrons remaining in the CB of CdS and holes in the VB of Bi 2 WO 6 to possess strong reduction and oxidation powers, respectively, leading the Bi 2 WO 6 /Au/CdS to exhibit high photocatalytic reduction of CO 2 , relative to bare Bi 2 WO 6 , Bi 2 WO 6 /Au, and Bi 2 WO 6 /CdS. The depressed hole density on CdS also enhances the stability of the CdS against photocorrosion.

The role of electric field in enhancing separation of gas molecules (H2S, CO2, H2O) on VIB modified g-C3N4 (0 0 1)

NASA Astrophysics Data System (ADS)

Wang, Fang; Li, Penghui; Wei, Shiqian; Guo, Jiaxing; Dan, Meng; Zhou, Ying

2018-07-01

In this study, the first-principles calculations were performed to investigate the adsorption behaviors of gas molecules H2S, CO2 and H2O on Cr, Mo and W modified g-C3N4 (0 0 1) surface. The results show that H2S, CO2 and H2O are physically adsorbed on the pristine g-C3N4, while the adsorption becomes chemisorbed due to the introduction of transition metals which significantly improve the interfacial electron transfer and narrow the band gap of g-C3N4 (0 0 1). Furthermore, it is found that the adsorption behaviors can be greatly influenced by the applied electric field. The adsorption energy is generally arranged in the order of Eads(H2S) > Eads(H2O) > Eads(CO2), and W/g-C3N4 (0 0 1) exhibits the best separation capability. The study could provide a versatile approach to selectively capture and separate the mixed gases in the catalytic reactions by controlling the applied intensity of electric field.

Extraction of aucubin from seeds of Eucommia ulmoides Oliv. using supercritical carbon dioxide.

PubMed

Li, Hui; Hu, Jiangyu; Ouyang, Hui; Li, Yanan; Shi, Hui; Ma, Chengjin; Zhang, Yongkang

2009-01-01

Supercritical CO2 was used as solvent for the extraction of aucubin from the seeds of Eucommia ulmoides Oliv. The co-solvent composition was tested and extraction conditions were optimized. Results showed that the best co-solvent was a water-ethanol mixture (1 + 3, v/v), and the highest yield was obtained when the extraction was performed under 26 MPa at extraction and separation temperatures of 55 and 30 degrees C for 120 min, using 6 mL co-solvent/g material at a CO2 flow rate of 20 L/h. In a comparison of the supercritical CO2 and Soxhlet extraction methods, the Soxhlet method needed 3 h to extract 10 g material, whereas the supercritical CO2 extraction technique needed only 2 h to extract 100 g material, thus showing a high extraction capability. The supercritical CO2 extraction produced a higher yield, with a lower cost for the extraction. Owing to the advantages of low extraction temperature, high yield, and ease of separating the product from the solvent, supercritical CO2 extraction is likely to be developed into an ideal technique for the extraction of aucubin, a compound with thermal instability, from the seeds of this plant.

Apparatus and method for solid fuel chemical looping combustion

DOEpatents

Siriwardane, Ranjani V; Weber, Justin M

2015-04-14

The disclosure provides an apparatus and method utilizing fuel reactor comprised of a fuel section, an oxygen carrier section, and a porous divider separating the fuel section and the oxygen carrier section. The porous divider allows fluid communication between the fuel section and the oxygen carrier section while preventing the migration of solids of a particular size. Maintaining particle segregation between the oxygen carrier section and the fuel section during solid fuel gasification and combustion processes allows gases generated in either section to participate in necessary reactions while greatly mitigating issues associated with mixture of the oxygen carrier with char or ash products. The apparatus and method may be utilized with an oxygen uncoupling oxygen carrier such as CuO, Mn.sub.3O.sub.4, or Co.sub.3O.sub.4, or utilized with a CO/H.sub.2 reducing oxygen carrier such as Fe.sub.2O.sub.3.

Fossil fuel combined cycle power generation method

DOEpatents

Labinov, Solomon D [Knoxville, TN; Armstrong, Timothy R [Clinton, TN; Judkins, Roddie R [Knoxville, TN

2008-10-21

A method for converting fuel energy to electricity includes the steps of converting a higher molecular weight gas into at least one mixed gas stream of lower average molecular weight including at least a first lower molecular weight gas and a second gas, the first and second gases being different gases, wherein the first lower molecular weight gas comprises H.sub.2 and the second gas comprises CO. The mixed gas is supplied to at least one turbine to produce electricity. The mixed gas stream is divided after the turbine into a first gas stream mainly comprising H.sub.2 and a second gas stream mainly comprising CO. The first and second gas streams are then electrochemically oxidized in separate fuel cells to produce electricity. A nuclear reactor can be used to supply at least a portion of the heat the required for the chemical conversion process.

DNA analysis using an integrated microchip for multiplex PCR amplification and electrophoresis for reference samples.

PubMed

Le Roux, Delphine; Root, Brian E; Reedy, Carmen R; Hickey, Jeffrey A; Scott, Orion N; Bienvenue, Joan M; Landers, James P; Chassagne, Luc; de Mazancourt, Philippe

2014-08-19

A system that automatically performs the PCR amplification and microchip electrophoretic (ME) separation for rapid forensic short tandem repeat (STR) forensic profiling in a single disposable plastic chip is demonstrated. The microchip subassays were optimized to deliver results comparable to conventional benchtop methods. The microchip process was accomplished in sub-90 min compared with >2.5 h for the conventional approach. An infrared laser with a noncontact temperature sensing system was optimized for a 45 min PCR compared with the conventional 90 min amplification time. The separation conditions were optimized using LPA-co-dihexylacrylamide block copolymers specifically designed for microchip separations to achieve accurate DNA size calling in an effective length of 7 cm in a plastic microchip. This effective separation length is less than half of other reports for integrated STR analysis and allows a compact, inexpensive microchip design. This separation quality was maintained when integrated with microchip PCR. Thirty samples were analyzed conventionally and then compared with data generated by the microfluidic chip system. The microfluidic system allele calling was 100% concordant with the conventional process. This study also investigated allelic ladder consistency over time. The PCR-ME genetic profiles were analyzed using binning palettes generated from two sets of allelic ladders run three and six months apart. Using these binning palettes, no allele calling errors were detected in the 30 samples demonstrating that a microfluidic platform can be highly consistent over long periods of time.

CO2-Free Power Generation on an Iron Group Nanoalloy Catalyst via Selective Oxidation of Ethylene Glycol to Oxalic Acid in Alkaline Media

NASA Astrophysics Data System (ADS)

Matsumoto, Takeshi; Sadakiyo, Masaaki; Ooi, Mei Lee; Kitano, Sho; Yamamoto, Tomokazu; Matsumura, Syo; Kato, Kenichi; Takeguchi, Tatsuya; Yamauchi, Miho

2014-07-01

An Fe group ternary nanoalloy (NA) catalyst enabled selective electrocatalysis towards CO2-free power generation from highly deliverable ethylene glycol (EG). A solid-solution-type FeCoNi NA catalyst supported on carbon was prepared by a two-step reduction method. High-resolution electron microscopy techniques identified atomic-level mixing of constituent elements in the nanoalloy. We examined the distribution of oxidised species, including CO2, produced on the FeCoNi nanoalloy catalyst in the EG electrooxidation under alkaline conditions. The FeCoNi nanoalloy catalyst exhibited the highest selectivities toward the formation of C2 products and to oxalic acid, i.e., 99 and 60%, respectively, at 0.4 V vs. the reversible hydrogen electrode (RHE), without CO2 generation. We successfully generated power by a direct EG alkaline fuel cell employing the FeCoNi nanoalloy catalyst and a solid-oxide electrolyte with oxygen reduction ability, i.e., a completely precious-metal-free system.

On the impact of CO{sub 2} emission-trading on power generation emissions

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

Chappin, E.J.L.; Dijkema, G.P.J.

2009-03-15

In Europe one of the main policy instruments to meet the Kyoto reduction targets is CO{sub 2} emission-trading (CET), which was implemented as of January 2005. In this system, companies active in specific sectors must be in the possession of CO{sub 2} emission rights to an amount equal to their CO{sub 2} emission. In Europe, electricity generation accounts for one-third of CO{sub 2} emissions. Since the power generation sector has been liberalized, reregulated and privatized in the last decade, around Europe autonomous companies determine the sectors' CO{sub 2} emission. Short-term they adjust their operation, long-term they decide on (dis) investmentmore » in power generation facilities and technology selection. An agent-based model is presented to elucidate the effect of CET on the decisions of power companies in an oligopolistic market. Simulations over an extensive scenario-space show that there CET does have an impact. A long-term portfolio shift towards less-CO{sub 2} intensive power generation is observed. However, the effect of CET is relatively small and materializes late. The absolute emissions from power generation rise under most scenarios. This corresponds to the dominant character of current capacity expansion planned in the Netherlands (50%) and in Germany (68%), where companies have announced many new coal based power plants. Coal is the most CO{sub 2} intensive option available and it seems surprising that even after the introduction of CET these capacity expansion plans indicate a preference for coal. Apparently in power generation the economic effect of CO{sub 2} emission-trading is not sufficient to outweigh the economic incentives to choose for coal.« less

Cocatalysts in Semiconductor-based Photocatalytic CO2 Reduction: Achievements, Challenges, and Opportunities.

PubMed

Ran, Jingrun; Jaroniec, Mietek; Qiao, Shi-Zhang

2018-02-01

Ever-increasing fossil-fuel combustion along with massive CO 2 emissions has aroused a global energy crisis and climate change. Photocatalytic CO 2 reduction represents a promising strategy for clean, cost-effective, and environmentally friendly conversion of CO 2 into hydrocarbon fuels by utilizing solar energy. This strategy combines the reductive half-reaction of CO 2 conversion with an oxidative half reaction, e.g., H 2 O oxidation, to create a carbon-neutral cycle, presenting a viable solution to global energy and environmental problems. There are three pivotal processes in photocatalytic CO 2 conversion: (i) solar-light absorption, (ii) charge separation/migration, and (iii) catalytic CO 2 reduction and H 2 O oxidation. While significant progress is made in optimizing the first two processes, much less research is conducted toward enhancing the efficiency of the third step, which requires the presence of cocatalysts. In general, cocatalysts play four important roles: (i) boosting charge separation/transfer, (ii) improving the activity and selectivity of CO 2 reduction, (iii) enhancing the stability of photocatalysts, and (iv) suppressing side or back reactions. Herein, for the first time, all the developed CO 2 -reduction cocatalysts for semiconductor-based photocatalytic CO 2 conversion are summarized, and their functions and mechanisms are discussed. Finally, perspectives in this emerging area are provided. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

[Optimization for supercritical CO2 extraction with response surface methodology and component analysis of Sapindus mukorossi oil].

PubMed

Wu, Yan; Xiao, Xin-yu; Ge, Fa-huan

2012-02-01

To study the extraction conditions of Sapindus mukorossi oil by Supercritical CO2 Extraction and identify its components. Optimized SFE-CO2 Extraction by response surface methodology and used GC-MS to analysie Sapindus mukorossi oil compounds. Established the model of an equation for the extraction rate of Sapindus mukorossi oil by Supercritical CO2 Extraction, and the optimal parameters for the Supercritical CO2 Extraction determined by the equation were: the extraction pressure was 30 MPa, temperature was 40 degrees C; The separation I pressure was 14 MPa, temperature was 45 degrees C; The separation II pressure was 6 MPa, temperature was 40 degrees C; The extraction time was 60 min and the extraction rate of Sapindus mukorossi oil of 17.58%. 22 main compounds of Sapindus mukorossi oil extracted by supercritical CO2 were identified by GC-MS, unsaturated fatty acids were 86.59%. This process is reliable, safe and with simple operation, and can be used for the extraction of Sapindus mukorossi oil.

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

PubMed

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

2016-10-20

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

SrNb2O6 nanoplates as efficient photocatalysts for the preferential reduction of CO2 in the presence of H2O.

PubMed

Xie, Shunji; Wang, Yu; Zhang, Qinghong; Deng, Weiping; Wang, Ye

2015-02-25

We successfully synthesized SrNb2O6 with nanoplate morphology by a facile hydrothermal method. The SrNb2O6 nanoplate without any promoters or co-catalysts exhibited promising photocatalytic performance for the preferential reduction of CO2 with H2O vapour to CO and CH4 due to its high electron-hole separation and high CO2 chemisorption abilities.

Fire-Retardant and Thermally Insulating Phenolic-Silica Aerogels.

PubMed

Yu, Zhi-Long; Yang, Ning; Apostolopoulou-Kalkavoura, Varvara; Qin, Bing; Ma, Zhi-Yuan; Xing, Wei-Yi; Qiao, Chan; Bergström, Lennart; Antonietti, Markus; Yu, Shu-Hong

2018-04-16

Energy efficient buildings require materials with a low thermal conductivity and a high fire resistance. Traditional organic insulation materials are limited by their poor fire resistance and inorganic insulation materials are either brittle or display a high thermal conductivity. Herein we report a mechanically resilient organic/inorganic composite aerogel with a thermal conductivity significantly lower than expanded polystyrene and excellent fire resistance. Co-polymerization and nanoscale phase separation of the phenol-formaldehyde-resin (PFR) and silica generate a binary network with domain sizes below 20 nm. The PFR/SiO 2 aerogel can resist a high-temperature flame without disintegration and prevents the temperature on the non-exposed side from increasing above the temperature critical for the collapse of reinforced concrete structures. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Assessing CO2 Mitigation Options Utilizing Detailed Electricity Characteristics and Including Renewable Generation

NASA Astrophysics Data System (ADS)

Bensaida, K.; Alie, Colin; Elkamel, A.; Almansoori, A.

2017-08-01

This paper presents a novel techno-economic optimization model for assessing the effectiveness of CO2 mitigation options for the electricity generation sub-sector that includes renewable energy generation. The optimization problem was formulated as a MINLP model using the GAMS modeling system. The model seeks the minimization of the power generation costs under CO2 emission constraints by dispatching power from low CO2 emission-intensity units. The model considers the detailed operation of the electricity system to effectively assess the performance of GHG mitigation strategies and integrates load balancing, carbon capture and carbon taxes as methods for reducing CO2 emissions. Two case studies are discussed to analyze the benefits and challenges of the CO2 reduction methods in the electricity system. The proposed mitigations options would not only benefit the environment, but they will as well improve the marginal cost of producing energy which represents an advantage for stakeholders.

CO excitation in the Seyfert galaxy NGC 7130

NASA Astrophysics Data System (ADS)

Pozzi, F.; Vallini, L.; Vignali, C.; Talia, M.; Gruppioni, C.; Mingozzi, M.; Massardi, M.; Andreani, P.

2017-09-01

We present a coherent multiband modelling of the carbon monoxide (CO) spectral energy distribution of the local Seyfert galaxy NGC 7130 to assess the impact of the active galactic nucleus (AGN) activity on the molecular gas. We take advantage of all the available data from X-ray to the submillimetre, including ALMA data. The high-resolution (˜0.2 arcsec) ALMA CO(6-5) data constrain the spatial extension of the CO emission down to an ˜70 pc scale. From the analysis of the archival Chandra and NuSTAR data, we infer the presence of a buried, Compton-thick AGN of moderate luminosity, L2-10 keV ˜ 1.6 × 1043 erg s-1. We explore photodissociation and X-ray-dominated-region (PDR and XDR) models to reproduce the CO emission. We find that PDRs can reproduce the CO lines up to J ˜ 6; however, the higher rotational ladder requires the presence of a separate source of excitation. We consider X-ray heating by the AGNs as a source of excitation, and find that it can reproduce the observed CO spectral energy distribution. By adopting a composite PDR+XDR model, we derive molecular cloud properties. Our study clearly indicates the capabilities offered by the current generation of instruments to shed light on the properties of nearby galaxies by adopting state-of-the-art physical modelling.

[Observation of carbon-bear free radicals using far infrared laser magnetic resonance spectroscopy].

PubMed

Huang, Guang-ming; Shi, Li-hua; Cai, Xin; Liu, Yu-yan

2003-06-01

The principle and technical characters of far infrared laser magnetic resonance (FIRLMR) spectrometer built up in China are introduced. A CO2 transversely pumped far infrared laser is adopted. In order to obtain high sensitivity, the sample absorption cell is placed in the FIR laser cavity and separated from laser gain cavity with thin polypropylene film. The spectrometer can be employed to study short lived free radicals. The spectra of many transient free radicals including CCH, CF and CH2 have been detected by the spectrometer. These transients are generated by mixing CH4 with the fluorine atoms produced with microwave discharge.

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

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

Kay, John; Stanislowski, Joshua; Tolbert, Scott

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

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

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

Lin, Jerry Y. S.

2015-01-31

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

Immunogenicity and reactogenicity of the human rotavirus vaccine, RIX4414 oral suspension, when co-administered with routine childhood vaccines in Chinese infants.

PubMed

Li, Rong-Cheng; Huang, Teng; Li, Yanping; Wang, Lao-Hong; Tao, Junhui; Fu, Botao; Si, Guoai; Nong, Yi; Mo, Zhaojun; Liao, XueYan; Luan, Ivy; Tang, Haiwen; Rathi, Niraj; Karkada, Naveen; Han, Htay Htay

2016-03-03

This study evaluated the immunogenicity of the human rotavirus (RV) vaccine (RIX4414) when co-administered with routine childhood vaccines in Chinese infants (NCT01171963). Healthy infants aged 6-16 weeks received 2 doses of either RIX4414 or placebo according to a 0, 1-month schedule. Infants received routine diphtheria-tetanus-acellular pertussis (DTPa) and oral poliovirus (OPV) vaccines either separately from or concomitantly with RIX4414/placebo (separate and co-administration cohorts, respectively). Anti-RV IgA seroconversion rates (one month post-dose-2) and seropositivity rates (at one year of age) were measured using ELISA. Immune responses against the DTPa and OPV antigens were measured one month post-DTPa dose-3 in the co-administration cohort. Solicited local and general symptoms were recorded for 8-days post-vaccination (total cohort). The according-to-protocol immunogenicity population included 511 infants in the separate cohort and 275 in the co-administration cohort. One month post-RIX4414 dose-2, anti-RV IgA seroconversion rates were 74.7% (95% confidence interval [CI]: 68.9-79.9) and 64.2% (95% CI: 55.4-72.3) in the separate and co-administration cohorts; seropositivity rates at one year of age were 71.5% (95% CI: 65.5-77.1) and 50.0% (95% CI: 40.9-59.1), respectively. One month post-DTPa dose-3, all infants in the co-administration cohort were seroprotected against diphtheria and tetanus, and seropositive for pertussis toxoid, pertactin and filamentous haemaglutinin. Two months post-OPV dose-3, seroprotection rates against anti-poliovirus types 1, 2 and 3 were >99% in the co-administration cohort. Reactogenicity profiles were similar in both cohorts. RIX4414 was immunogenic and well-tolerated in Chinese infants and did not appear to interfere with the immunogenicity and reactogenicity of co-administered routine childhood vaccines.

Immunogenicity and reactogenicity of the human rotavirus vaccine, RIX4414 oral suspension, when co-administered with routine childhood vaccines in Chinese infants

PubMed Central

Li, Rong-cheng; Huang, Teng; Li, Yanping; Wang, Lao-Hong; Tao, Junhui; Fu, Botao; Si, Guoai; Nong, Yi; Mo, Zhaojun; Liao, XueYan; Luan, Ivy; Tang, Haiwen; Rathi, Niraj; Karkada, Naveen; Han, Htay Htay

2016-01-01

Abstract This study evaluated the immunogenicity of the human rotavirus (RV) vaccine (RIX4414) when co-administered with routine childhood vaccines in Chinese infants (NCT01171963). Healthy infants aged 6–16 weeks received 2 doses of either RIX4414 or placebo according to a 0, 1-month schedule. Infants received routine diphtheria-tetanus-acellular pertussis (DTPa) and oral poliovirus (OPV) vaccines either separately from or concomitantly with RIX4414/placebo (separate and co-administration cohorts, respectively). Anti-RV IgA seroconversion rates (one month post-dose-2) and seropositivity rates (at one year of age) were measured using ELISA. Immune responses against the DTPa and OPV antigens were measured one month post-DTPa dose-3 in the co-administration cohort. Solicited local and general symptoms were recorded for 8-days post-vaccination (total cohort). The according-to-protocol immunogenicity population included 511 infants in the separate cohort and 275 in the co-administration cohort. One month post-RIX4414 dose-2, anti-RV IgA seroconversion rates were 74.7% (95% confidence interval [CI]: 68.9–79.9) and 64.2% (95% CI: 55.4–72.3) in the separate and co-administration cohorts; seropositivity rates at one year of age were 71.5% (95% CI: 65.5–77.1) and 50.0% (95% CI: 40.9–59.1), respectively. One month post-DTPa dose-3, all infants in the co-administration cohort were seroprotected against diphtheria and tetanus, and seropositive for pertussis toxoid, pertactin and filamentous haemaglutinin. Two months post-OPV dose-3, seroprotection rates against anti-poliovirus types 1, 2 and 3 were >99% in the co-administration cohort. Reactogenicity profiles were similar in both cohorts. RIX4414 was immunogenic and well-tolerated in Chinese infants and did not appear to interfere with the immunogenicity and reactogenicity of co-administered routine childhood vaccines. PMID:27149266

Carbon Capture and Utilization in the Industrial Sector.

PubMed

Psarras, Peter C; Comello, Stephen; Bains, Praveen; Charoensawadpong, Panunya; Reichelstein, Stefan; Wilcox, Jennifer

2017-10-03

The fabrication and manufacturing processes of industrial commodities such as iron, glass, and cement are carbon-intensive, accounting for 23% of global CO 2 emissions. As a climate mitigation strategy, CO 2 capture from flue gases of industrial processes-much like that of the power sector-has not experienced wide adoption given its high associated costs. However, some industrial processes with relatively high CO 2 flue concentration may be viable candidates to cost-competitively supply CO 2 for utilization purposes (e.g., polymer manufacturing, etc.). This work develops a methodology that determines the levelized cost ($/tCO 2 ) of separating, compressing, and transporting carbon dioxide. A top-down model determines the cost of separating and compressing CO 2 across 18 industrial processes. Further, the study calculates the cost of transporting CO 2 via pipeline and tanker truck to appropriately paired sinks using a bottom-up cost model and geo-referencing approach. The results show that truck transportation is generally the low-cost alternative given the relatively small volumes (ca. 100 kt CO 2 /a). We apply our methodology to a regional case study in Pennsylvania, which shows steel and cement manufacturing paired to suitable sinks as having the lowest levelized cost of capture, compression, and transportation.

Fast Abiotic Production of Methane at Temperatures Below 100°C

NASA Astrophysics Data System (ADS)

Etiope, G.; Ionescu, A.

2015-12-01

Fischer-Tropsch Type (FTT) reactions, e.g., the Sabatier synthesis between H2 and CO2, are considered a main source of abiotic methane on Earth and likely on other planets. Several laboratory FTT experiments demonstrated abiotic CH4 production at temperatures above 200°C, by using Fe, Ni or Cr catalysts, simulating hydrothermal conditions in peridotite-hosted systems in mid-ocean ridges. Nevertheless, at least on laboratory experiment time-scale, Fe-Ni-Cr catalysts do not support CH4 generation at T<100°C, such as those of land-based serpentinization systems. We have recently reported rapid production of considerable amounts of CH4 (>800 ppmv in 155 mL bottles after 1 day) via Sabatier reaction at 90, 50 and 25°C, using small concentrations of non-pretreated ruthenium (Ru) equivalent to those occurring in chromitites in continental ultramafic rocks (Etiope & Ionescu, 2014; Geofluids, doi:10.1111/gfl.12106). We have repeated the experiments by using 13C-enriched CO2 and we confirm fast production of CH4at percentage levels. The experiments performed so far show that: 1. considerable amounts of CH4can be produced in dry conditions below 100°C with small quantities of Ru; 2. under the same experimental conditions (<100°C), Fe, Ni and Cr oxides do not produce CH4; 3. low T Sabatier reaction can produce CH4 with a large C isotope fractionation between CO2 and CH4, leading to relatively " light" (13C-depleted) CH4, resembling microbial gas; 4. the CO2-CH4isotope separation decreases over time and by increasing the temperature; 5. minor amounts of C2-C6hydrocarbons are also generated. Our laboratory data are compatible with the isotopic patterns of CH4 naturally occurring in land-based seeps and springs. Our experiments suggest that Ru-enriched chromitites could potentially generate CH4 at low T. Since Ru is reported in Martian meteorites, low T abiotic CH4 production on Mars via Sabatier reaction cannot be excluded (Etiope et al. 2013, Icarus, 224, 276-285).

CO2 Reduction Effect of the Utilization of Waste Heat and Solar Heat in City Gas System

NASA Astrophysics Data System (ADS)

Okamura, Tomohito; Matsuhashi, Ryuji; Yoshida, Yoshikuni; Hasegawa, Hideo; Ishitani, Hisashi

We evaluate total energy consumption and CO2 emissions in the phase of the city gas utilization system from obtaining raw materials to consuming the product. First, we develop a simulation model which calculates CO2 emissions for monthly and hourly demands of electricity, heats for air conditioning and hot-water in a typical hospital. Under the given standard capacity and operating time of CGS, energy consumption in the equipments is calculated in detail considering the partial load efficiency and the control by the temperature of exhaust heat. Then, we explored the optimal size and operation of city gas system that minimizes the life cycle CO2 emissions or total cost. The cost-effectiveness is compared between conventional co-generation, solar heat system, and hybrid co-generation utilizing solar heat. We formulate a problem of mixed integer programming that includes integral parameters that express the state of system devices such as on/off of switches. As a result of optimization, the hybrid co-generation can reduce annual CO2 emissions by forty-three percent compared with the system without co-generation. Sensitivity for the scale of CGS on CO2 reduction and cost is also analyzed.

Thermincola carboxydiphila gen. nov., sp. nov., a novel anaerobic, carboxydotrophic, hydrogenogenic bacterium from a hot spring of the Lake Baikal area.

PubMed

Sokolova, Tatyana G; Kostrikina, Nadezhda A; Chernyh, Nikolai A; Kolganova, Tatjana V; Tourova, Tatjana P; Bonch-Osmolovskaya, Elizaveta A

2005-09-01

A novel anaerobic, thermophilic, alkalitolerant bacterium, strain 2204(T), was isolated from a hot spring of the Baikal Lake region. The cells of strain 2204(T) were straight rods of variable length, Gram-positive with an S-layer, motile with one to two lateral flagella, and often formed aggregates of 3-15 cells. The isolate was shown to be an obligate anaerobe oxidizing CO and producing equimolar quantities of H(2) and CO(2) according to the equation CO+H(2)O-->CO(2)+H(2). No organic substrates were used as energy sources. For lithotrophic growth on CO, 0.2 g acetate or yeast extract l(-1) was required but did not support growth in the absence of CO. Growth was observed in the temperature range 37-68 degrees C, the optimum being 55 degrees C. The pH range for growth was 6.7-9.5, the optimum pH being 8.0. The generation time under optimal conditions was 1.3 h. The DNA G+C content was 45 mol%. Penicillin, erythromycin, streptomycin, rifampicin, vancomycin and tetracycline completely inhibited both growth and CO utilization by strain 2204(T). Thus, isolate 2204(T) was found to be the first known moderately thermophilic and alkalitolerant H(2)-producing anaerobic carboxydotroph. The novel bacterium fell within the cluster of the family Peptococcaceae within the low-G+C-content Gram-positive bacteria, where it formed a separate branch. On the basis of morphological, physiological and phylogenetic features, strain 2204(T) should be assigned to a novel genus and species, for which the name Thermincola carboxydiphila gen. nov., sp. nov. is proposed. The type strain is strain 2204(T) (=DSM 17129(T)=VKM B-2283(T)=JCM 13258(T)).

Remarkable separability of the circulation response to Arctic sea ice loss and greenhouse gas forcing

NASA Astrophysics Data System (ADS)

McCusker, K. E.; Kushner, P. J.; Fyfe, J. C.; Sigmond, M.; Kharin, V. V.; Bitz, C. M.

2017-12-01

Arctic sea ice loss has an important effect on local climate through increases in ocean to atmosphere heat flux and associated feedbacks, and may influence midlatitude climate by changing large-scale circulation that can enhance or counter changes that are due to greenhouse gases. The extent to which climate change in a warming world can be understood as greenhouse gas-induced changes that are modulated by Arctic sea ice loss depends on how additive the responses to the separate influences are. Here we use a novel sea ice nudging methodology in the Canadian Earth System Model, which has a fully coupled ocean, to isolate the effects of Arctic sea ice loss and doubled atmospheric carbon dioxide (CO2) to determine their additivity and sensitivity to mean state. We find that the separate effects of Arctic sea ice loss and doubled CO2 are remarkably additive and relatively insensitive to mean climate state. This separability is evident in several thermodynamic and dynamic fields throughout most of the year, from hemispheric to synoptic scales. The extent to which the regional response to sea ice loss sometimes agrees with and sometimes cancels the response to CO2 is quantified. In this model, Arctic sea ice loss enhances the CO2-induced surface air temperature changes nearly everywhere and zonal wind changes over the Pacific sector, whereas sea ice loss counters CO2-induced sea level pressure changes nearly everywhere over land and zonal wind changes over the Atlantic sector. This separability of the response to Arctic sea ice loss from the response to CO2 doubling gives credence to the body of work in which Arctic sea ice loss is isolated from the forcing that modified it, and might provide a means to better interpret the diverse array of modeling and observational studies of Arctic change and influence.

Surface design with self-heating smart polymers for on-off switchable traps

NASA Astrophysics Data System (ADS)

Techawanitchai, Prapatsorn; Yamamoto, Kazuya; Ebara, Mitsuhiro; Aoyagi, Takao

2011-08-01

We have developed a novel self-heating, temperature-responsive chromatography system for the effective separation of biomolecules. Temperature-responsive poly(N-isopropylacrylamide-co-N-hydroxymethylacrylamide), poly(NIPAAm-co-HMAAm), was covalently grafted onto the surface of magnetite/silica composites as 'on-off' switchable surface traps. The lower critical solution temperature (LCST) of the poly(NIPAAm-co-HMAAm)s was controlled from 35 to 55 °C by varying the HMAAm content. Using the heat generated by magnetic particles in an alternating magnetic field (AMF) we were able to induce the hydrophilic to hydrophobic phase separation of the grafted temperature-responsive polymers. To assess the feasibility of the poly(NIPAAm-co-HMAAm)-grafted magnetite/silica particles as the stationary phase for chromatography, we packed the particles into the glass column of a liquid chromatography system and analyzed the elusion profiles for steroids. The retention time for hydrophobic steroids markedly increased in the AMF, because the hydrophobic interaction was enhanced via self-heating of the grafted magnetite/silica particles, and this effect could be controlled by changing the AMF irradiation time. Turning off the AMF shortened the total analysis time for steroids. The proposed system is useful for separating bioactive compounds because their elution profiles can be easily controlled by an AMF.

Bee venom processes human skin lipids for presentation by CD1a

PubMed Central

Bourgeois, Elvire A.; Subramaniam, Sumithra; Cheng, Tan-Yun; De Jong, Annemieke; Layre, Emilie; Ly, Dalam; Salimi, Maryam; Legaspi, Annaliza; Modlin, Robert L.; Salio, Mariolina; Cerundolo, Vincenzo

2015-01-01

Venoms frequently co-opt host immune responses, so study of their mode of action can provide insight into novel inflammatory pathways. Using bee and wasp venom responses as a model system, we investigated whether venoms contain CD1-presented antigens. Here, we show that venoms activate human T cells via CD1a proteins. Whereas CD1 proteins typically present lipids, chromatographic separation of venoms unexpectedly showed that stimulatory factors partition into protein-containing fractions. This finding was explained by demonstrating that bee venom–derived phospholipase A2 (PLA2) activates T cells through generation of small neoantigens, such as free fatty acids and lysophospholipids, from common phosphodiacylglycerides. Patient studies showed that injected PLA2 generates lysophospholipids within human skin in vivo, and polyclonal T cell responses are dependent on CD1a protein and PLA2. These findings support a previously unknown skin immune response based on T cell recognition of CD1a proteins and lipid neoantigen generated in vivo by phospholipases. The findings have implications for skin barrier sensing by T cells and mechanisms underlying phospholipase-dependent inflammatory skin disease. PMID:25584012

New Technologies for Dealing with CO2 Emission and Carbonate Discharge Control Issues Associated with Energy Production

NASA Astrophysics Data System (ADS)

Tuwati, Abdulwahab

Carbonates and bicarbonates as two water contaminants and CO2 as an air pollutant are the byproducts of a number of fossil fuel based energy production processes. It is well known that the eco-environmental impacts of the carbon based compounds are rather negative. Discharge of co-produced waters containing carbonates and bicarbonates can lead to the significant increase of alkalinity and sodicity and eventual degradation of the quality of soils. In addition, many studies have indicated that huge CO2 emission into the atmosphere can result in disastrous climate changes in the future. Therefore, people are increasingly interested in controlling these carbon compounds. A number of technologies such as ion exchange and electrodialysis have been developed for removal of carbonates and bicarbonates from co-produced waters. However, they are too expensive to be widely used by energy producers, farmers and ranchers. Although many approaches including membrane filtration have been explored for CO2 emission control, their costs are not acceptable to fossil fuel generating companies at all. Therefore, searching cost-effective methods for control of the carbon compounds have attracted many researchers' attentions. New technologies have been developed in this research to overcome the abovementioned challenges. For example, a regenerable solid sorbent (KTi) synthesized with K2CO3 and nanoporous TiO(OH)2 can be used to capture CO2. The CO2 sorption capacity of KTi is about 36 times higher than that of conventional K2CO3. The highest CO2 sorption capacity achieved with KTi is 1.69 mmol-CO2/g-KTi. It should be noted that the theoretical sorption capacity of the KTi can be as high as 3.32 mmol-CO 2/g-KTi. Therefore, the potential and improvement in CO2 sorption capacity with the use of nanoporous TiO(OH)2 is significant. Moreover, nanostructured KTi based CO2 separation (from flue gas) does not need additional high specific-heat capacity and high vaporization-enthalpy H2O. This creates a favorable condition for considerable decrease in energy consumption of CO2 capture in coal-fired power plants. It is expected that all the technologies developed in this research could significantly benefit energy producers, although many works need to be done before they can be commercialized.

Committed CO2 Emissions of China's Coal-fired Power Plants

NASA Astrophysics Data System (ADS)

Suqin, J.

2016-12-01

The extent of global warming is determined by the cumulative effects of CO2 in the atmosphere. Coal-fired power plants, the largest anthropogenic source of CO2 emissions, produce large amount of CO2 emissions during their lifetimes of operation (committed emissions), which thus influence the future carbon emission space under specific targets on mitigating climate change (e.g., the 2 degree warming limit relative to pre-industrial levels). Comprehensive understanding of committed CO2 emissions for coal-fired power generators is urgently needed in mitigating global climate change, especially in China, the largest global CO2emitter. We calculated China's committed CO2 emissions from coal-fired power generators installed during 1993-2013 and evaluated their impact on future emission spaces at the provincial level, by using local specific data on the newly installed capacities. The committed CO2 emissions are calculated as the product of the annual coal consumption from newly installed capacities, emission factors (CO2emissions per unit crude coal consumption) and expected lifetimes. The sensitivities about generators lifetimes and the drivers on provincial committed emissions are also analyzed. Our results show that these relatively recently installed coal-fired power generators will lead to 106 Gt of CO2 emissions over the course of their lifetimes, which is more than three times the global CO2 emissions from fossil fuels in 2010. More than 80% (85 Gt) of their total committed CO2 will be emitted after 2013, which are referred to as the remaining emissions. Due to the uncertainties of generators lifetime, these remaining emissions would increase by 45 Gt if the lifetimes of China's coal-fired power generators were prolonged by 15 years. Furthermore, the remaining emissions are very different among various provinces owing to local developments and policy disparities. Provinces with large amounts of secondary industry and abundant coal reserves have higher committed emissions. The national and provincial CO2 emission mitigation objectives might be greatly restricted by existing and planned power plants in China. The policy implications of our results have also been discussed.

Life-Cycle Evaluation of Domestic Energy Systems

NASA Astrophysics Data System (ADS)

Bando, Shigeru; Hihara, Eiji

Among the growing number of environmental issues, the global warming due to the increasing emission of greenhouse gases, such as carbon dioxide CO2, is the most serious one. In order to reduce CO2 emissions in energy use, it is necessary to reduce primary energy consumption, and to replace energy sources with alternatives that emit less CO2.One option of such ideas is to replace fossil gas for water heating with electricity generated by nuclear power, hydraulic power, and other methods with low CO2 emission. It is also important to use energy efficiently and to reduce waste heat. Co-generation system is one of the applications to be able to use waste heat from a generator as much as possible. The CO2 heat pump water heaters, the polymer electrolyte fuel cells, and the micro gas turbines have high potential for domestic energy systems. In the present study, the life-cycle cost, the life-cycle consumption of primary energy and the life-cycle emission of CO2 of these domestic energy systems are compare. The result shows that the CO2 heat pump water heaters have an ability to reduce CO2 emission by 10%, and the co-generation systems also have another ability to reduce primary energy consumption by 20%.

Evaluation of Mars CO2 Capture and Gas Separation Technologies

NASA Technical Reports Server (NTRS)

Muscatello, Anthony C.; Santiago-Maldonado, Edgardo; Gibson, Tracy; Devor, Robert; Captain, James

2011-01-01

Recent national policy statements have established that the ultimate destination of NASA's human exploration program is Mars. In Situ Resource Utilization (ISRU) is a key technology required to ,enable such missions and it is appropriate to review progress in this area and continue to advance the systems required to produce rocket propellant, oxygen, and other consumables on Mars using the carbon dioxide atmosphere and other potential resources. The Mars Atmospheric Capture and Gas separation project is selecting, developing, and demonstrating techniques to capture and purify Martian atmospheric gases for their utilization for the production of hydrocarbons, oxygen, and water in ISRU systems. Trace gases will be required to be separated from Martian atmospheric gases to provide pure CO2 to processing elements. In addition, other Martian gases, such as nitrogen and argon, occur in concentrations high enough to be useful as buffer gas and should be captured as well. To achieve these goals, highly efficient gas separation processes will be required. These gas separation techniques are also required across various areas within the ISRU project to support various consumable production processes. The development of innovative gas separation techniques will evaluate the current state-of-the-art for the gas separation required, with the objective to demonstrate and develop light-weight, low-power methods for gas separation. Gas separation requirements include, but are not limited to the selective separation of: (1) methane and water from unreacted carbon oxides (C02-CO) and hydrogen typical of a Sabatier-type process, (2) carbon oxides and water from unreacted hydrogen from a Reverse Water-Gas Shift process, (3)/carbon oxides from oxygen from a trash/waste processing reaction, and (4) helium from hydrogen or oxygen from a propellant scavenging process. Potential technologies for the separations include' freezers, selective membranes, selective solvents, polymeric sorbents, zeolites, and new technologies. This paper summarizes the results of an extensive literature review of candidate technologies for the capture and separation of CO2 and other relevant gases. This information will be used to prioritize the technologies to be developed further during this and other ISRU projects.

Supercritical Fluid Extraction and Separation of Uranium from Other Actinides

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

Donna L. Quach; Bruce J. Mincher; Chien M. Wai

2014-06-01

This paper investigates the feasibility of separating uranium from other actinides by using supercritical fluid carbon dioxide (sc-CO2) as a solvent modified with tri-n-butylphosphate (TBP) for the development of an extraction and counter current stripping technique, which would be a more efficient and environmentally benign technology for used nuclear fuel reprocessing compared to traditional solvent extraction. Several actinides (U(VI), Np(VI), Pu(IV), and Am(III)) were extracted in sc-CO2 modified with TBP over a range of nitric acid concentrations and then the actinides were exposed to reducing and complexing agents to suppress their extractability. According to this study, the separation of uraniummore » from plutonium in sc-CO2 modified with TBP was successful at nitric acid concentrations of less than 3 M in the presence of acetohydroxamic acid or oxalic acid, and the separation of uranium from neptunium was successful at nitric acid concentrations of less than 1 M in the presence of acetohydroxamic acid, oxalic acid, or sodium nitrite.« less

An active micro-direct methanol fuel cell with self-circulation of fuel and built-in removal of CO 2 bubbles

NASA Astrophysics Data System (ADS)

Meng, Dennis Desheng; Kim, C. J.

As an alternative or supplement to small batteries, the much-anticipated micro-direct methanol fuel cell (μDMFC) faces several key technical issues such as methanol crossover, reactant delivery, and byproduct release. This paper addresses two of the issues, removal of CO 2 bubbles and delivery of methanol fuel, in a non-prohibitive way for system miniaturization. A recently reported bubble-driven pumping mechanism is applied to develop active μDMFCs free of an ancillary pump or a gas separator. The intrinsically generated CO 2 bubbles in the anodic microchannels are used to pump and circulate the liquid fuel before being promptly removed as a part of the pumping mechanism. Without a discrete liquid pump or gas separator, the widely known packaging penalty incurred within many micro-fuel-cell systems can be alleviated so that the system's power/energy density does not decrease dramatically as a result of miniaturization. Since the power required for pumping is provided by the byproduct of the fuel cell reaction, the parasitic power loss due to an external pump is also eliminated. The fuel circulation is visually confirmed, and the effectiveness for fuel cell applications is verified during continuous operation of a μDMFC for over 70 min with 1.2 mL of 2 M methanol. The same device was shown to operate for only 5 min if the pumping mechanism is disabled by blocking the gas venting membrane. Methanol consumption while utilizing the reported self-circulation mechanism is estimated to be 46%. Different from common pump-free fuel delivery approaches, the reported mechanism delivers the fuel actively and is independent of gravity.

Predictive model for CO2 generation and decay in building envelopes

NASA Astrophysics Data System (ADS)

Aglan, Heshmat A.

2003-01-01

Understanding carbon dioxide generation and decay patterns in buildings with high occupancy levels is useful to identify their indoor air quality, air change rates, percent fresh air makeup, occupancy pattern, and how a variable air volume system to off-set undesirable CO2 level can be modulated. A mathematical model governing the generation and decay of CO2 in building envelopes with forced ventilation due to high occupancy is developed. The model has been verified experimentally in a newly constructed energy efficient healthy house. It was shown that the model accurately predicts the CO2 concentration at any time during the generation and decay processes.

"Twin copper source" growth of metal-organic framework membrane: Cu(3)(BTC)(2) with high permeability and selectivity for recycling H(2).

PubMed

Guo, Hailing; Zhu, Guangshan; Hewitt, Ian J; Qiu, Shilun

2009-02-11

In this communication, the copper net supported Cu(3)(BTC)(2) membranes have been successfully synthesized by means of a "twin copper source" technique. Separation studies on gaseous mixtures (H(2)/CO(2), H(2)/CH(4), and H(2)/N(2)) using the membrane revealed that the membrane possesses high permeability and selectivity for H(2) over CO(2), N(2), and CH(4). Compared with the conventional zeolite membranes, the copper net supported Cu(3)(BTC)(2) membrane exhibited high permeation flux in gas separation. Such highly efficient copper net supported Cu(3)(BTC)(2) membranes could be used to separate, recycle, and reuse H(2) exhausted from steam reforming natural gas.

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

Transition-metal oxides with triangular lattices: generation of new magnetic and electronic properties.

PubMed

Maignan, A; Kobayashi, W; Hébert, S; Martinet, G; Pelloquin, D; Bellido, N; Simon, Ch

2008-10-06

The search for multifunctional materials as multiferroics to be applied in microelectronic or for new, chemically stable and nontoxic, thermoelectric materials to recover waste heat is showing a common interest in the oxides whose structures contain a triangular network of transition-metal cations. To illustrate this point, two ternary systems, Ba-Co-O and Ca-Co-O, have been chosen. It is shown that new phases with a complex triangular structure can be discovered, for instance, by introduction of Ga (3+) into the Ba-Co-O system to stabilize Ba 6Ga 2Co 11O 26 and Ba 2GaCo 8O 14, which both belong to a large family of compounds with formula [Ba(Co,Ga)O 3-delta] n [BaCo 8O 11]. In the latter, both sublattices contain triangular networks derived from the hexagonal perovskite and the spinel structure. Among the hexagonal perovskite, the Ca 3Co 2O 6 crystals give clear evidence where the coupling of charges and spins is at the origin of a magnetocapacitance effect. In particular, the ferrimagnetic to ferromagnetic transition, with a one-third plateau on the M( H) curve characteristic of triangular magnetism, is accompanied by a peak in the dielectric constant. A second class of cobaltites is the focus of much interest. Their 2D structure, containing CoO 2 planes isostructural to a CdI 2 slice that are stacked in an incommensurate way with rock salt type layers, is referred to misfit cobaltite. The 2D triangular network of edge-shared CoO 6 octahedra is believed to be responsible for large values of the Seebeck coefficient and low electrical resistivity. A clear relationship between the structuresincommensurability ratiosand the electronic properties is evidenced, showing that the charge carrier concentration can be tuned via the control of the ionic radius of the cations in the separating layers.

Stereoselectivity in catalytic reactions: CO oxidation on Pd(100) by rotationally aligned O2 molecules

NASA Astrophysics Data System (ADS)

Vattuone, L.; Gerbi, A.; Savio, L.; Cappelletti, D.; Pirani, F.; Rocca, M.

2010-05-01

We report on stereodynamical effects in heterogeneous catalytic reactions as measured by molecular beam-surface experiments. Specifically for CO oxidation on Pd(100) we find that the rotational alignment of the incoming O2 at low (Θ = 0.04 ML) and at intermediate (ΘCO = 0.17 ML) CO pre-coverage, causes a higher reactivity of molecules in high and in low helicity states, respectively (corresponding to helicoptering and cartwheeling motion of O2). In first approximation, at low CO pre-coverage the difference in reactivity is determined by the different location of the O atoms generated in the dissociation process by the different parent molecules, while at intermediate CO pre-coverage the reactivity is influenced also by the different ability of cartwheeling and helicoptering O2 to penetrate through the CO adlayer. In accord with this the total amount of CO2 produced is always largest for helicopters which generate supersurface O atoms at least in the low CO pre-coverage limit. A deeper inspection of the data indicates, however, that the dynamics is more complex, two different pathways being present for the reaction with O generated by helicopters and one for O generated by cartwheels. Moreover, cartwheels generated oxygen influences the reactivity of subsequently arriving helicopters.

Hydrogen production by reforming of liquid hydrocarbons in a membrane reactor for portable power generation-Experimental studies

NASA Astrophysics Data System (ADS)

Damle, Ashok S.

One of the most promising technologies for lightweight, compact, portable power generation is proton exchange membrane (PEM) fuel cells. PEM fuel cells, however, require a source of pure hydrogen. Steam reforming of hydrocarbons in an integrated membrane reactor has potential to provide pure hydrogen in a compact system. Continuous separation of product hydrogen from the reforming gas mixture is expected to increase the yield of hydrogen significantly as predicted by model simulations. In the laboratory-scale experimental studies reported here steam reforming of liquid hydrocarbon fuels, butane, methanol and Clearlite ® was conducted to produce pure hydrogen in a single step membrane reformer using commercially available Pd-Ag foil membranes and reforming/WGS catalysts. All of the experimental results demonstrated increase in hydrocarbon conversion due to hydrogen separation when compared with the hydrocarbon conversion without any hydrogen separation. Increase in hydrogen recovery was also shown to result in corresponding increase in hydrocarbon conversion in these studies demonstrating the basic concept. The experiments also provided insight into the effect of individual variables such as pressure, temperature, gas space velocity, and steam to carbon ratio. Steam reforming of butane was found to be limited by reaction kinetics for the experimental conditions used: catalysts used, average gas space velocity, and the reactor characteristics of surface area to volume ratio. Steam reforming of methanol in the presence of only WGS catalyst on the other hand indicated that the membrane reactor performance was limited by membrane permeation, especially at lower temperatures and lower feed pressures due to slower reconstitution of CO and H 2 into methane thus maintaining high hydrogen partial pressures in the reacting gas mixture. The limited amount of data collected with steam reforming of Clearlite ® indicated very good match between theoretical predictions and experimental results indicating that the underlying assumption of the simple model of conversion of hydrocarbons to CO and H 2 followed by equilibrium reconstitution to methane appears to be reasonable one.

[Experimental investigation of laser plasma soft X-ray source with gas target].

PubMed

Ni, Qi-liang; Gong, Yan; Lin, Jing-quan; Chen, Bo; Cao, Jian-lin

2003-02-01

This paper describes a debris-free laser plasma soft X-ray source with a gas target, which has high operating frequency and can produce strong soft X-ray radiation. The valve of this light source is drived by a piezoelectrical ceramic whose operating frequency is up to 400 Hz. In comparison with laser plasma soft X-ray sources using metal target, the light source is debris-free. And it has higher operating frequency than gas target soft X-ray sources whose nozzle is controlled by a solenoid valve. A channel electron multiplier (CEM) operating in analog mode is used to detect the soft X-ray generated by the laser plasma source, and the CEM's output is fed to to a charge-sensitive preamplifier for further amplification purpose. Output charges from the CEM are proportional to the amplitude of the preamplifier's output voltage. Spectra of CO2, Xe and Kr at 8-14 nm wavelength which can be used for soft X-ray projection lithography are measured. The spectrum for CO2 consists of separate spectral lines originate mainly from the transitions in Li-like and Be-like ions. The Xe spectrum originating mainly from 4d-5f, 4d-4f, 4d-6p and 4d-5p transitions in multiply charged xenon ions. The spectrum for Kr consists of separate spectral lines and continuous broad spectra originating mainly from the transitions in Cu-, Ni-, Co- and Fe-like ions.

Report on all ARRA Funded Technical Work

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

None, None

2013-10-05

The main focus of this American Recovery and Reinvestment Act of 2009 (ARRA) funded project was to design an energy efficient carbon capture and storage (CCS) process using the Recipients membrane system for H{sub 2} separation and CO{sub 2} capture. In the ARRA-funded project, the Recipient accelerated development and scale-up of ongoing hydrogen membrane technology research and development (R&D). Specifically, this project focused on accelerating the current R&D work scope of the base program-funded project, involving lab scale tests, detail design of a 250 lb/day H{sub 2} process development unit (PDU), and scale-up of membrane tube and coating manufacturing. Thismore » project scope included the site selection and a Front End Engineering Design (FEED) study of a nominally 4 to 10 ton-per-day (TPD) Pre-Commercial Module (PCM) hydrogen separation membrane system. Process models and techno-economic analysis were updated to include studies on integration of this technology into an Integrated Gasification Combined Cycle (IGCC) power generation system with CCS.« less

Control of low-speed turbulent separated flow over a backward-facing ramp. Ph.D. Thesis - Old Dominion Univ.

NASA Technical Reports Server (NTRS)

Lin, John C.

1992-01-01

The relative performance and flow phenomena associated with several devices for controlling turbulent separated flow were investigated at low speeds. Relative performance of the devices was examined for flow over a curved, backward-facing ramp in a wind tunnel, and the flow phenomena were examined in a water tunnel using dye-flow visualization. Surface static pressure measurements and oil-flow visualization results from the wind tunnel tests indicated that transverse grooves, longitudinal grooves, submerged vortex generators, vortex generator jets (VGJ's), Viets' fluidic flappers, elongated arches at positive angle of attack, and large-eddy breakup devices (LEBU's) at positive angle of attack placed near the baseline separation location reduce flow separation and increase pressure recovery. Spanwise cylinders reduce flow separation but decrease pressure recovery downstream. Riblets, passive porous surfaces, swept grooves, Helmholtz resonators, and arches and LEBU's with angle of attack less than or = 0 degrees had no significant effect in reducing the extent of the separation region. Wall-cooling computations indicated that separation delay on a partially-cooled ramp is nearly the same as on a fully-cooled ramp, while minimizing the frictional drag increase associated with the wall cooling process. Dry-flow visualization tests in the water tunnel indicated that wishbone vortex generators in the forward orientation shed horseshoe vortices; wishbone vortex generators oriented in the reverse direction and doublet vortex generators shed streamwise counterrotating vortices; a spanewise cylinder located near the wall and LEBU's at angle of attack = -10 degrees produced eddies or transverse vortices which rotated with the same sign as the mean vorticity in a turbulent boundary layer; and the most effective VGJ's produced streamwise co-rotating vortices. Comparative wind-tunnel test results indicated that transferring momentum from the outer region of a turbulent boundary layer through the action of embedded streamwise vortices is more effective than by transverse vortices for the separation control application studied herein.

Novel, Ceramic Membrane System For Hydrogen Separation

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

Elangovan, S.

2012-12-31

Separation of hydrogen from coal gas represents one of the most promising ways to produce alternative sources of fuel. Ceramatec, teamed with CoorsTek and Sandia National Laboratories has developed materials technology for a pressure driven, high temperature proton-electron mixed conducting membrane system to remove hydrogen from the syngas. This system separates high purity hydrogen and isolates high pressure CO{sub 2} as the retentate, which is amenable to low cost capture and transport to storage sites. The team demonstrated a highly efficient, pressure-driven hydrogen separation membrane to generate high purity hydrogen from syngas using a novel ceramic-ceramic composite membrane. Recognizing themore » benefits and limitations of present membrane systems, the all-ceramic system has been developed to address the key technical challenges related to materials performance under actual operating conditions, while retaining the advantages of thermal and process compatibility offered by the ceramic membranes. The feasibility of the concept has already been demonstrated at Ceramatec. This project developed advanced materials composition for potential integration with water gas shift rectors to maximize the hydrogenproduction.« less

40 CFR 98.183 - Calculating GHG emissions.

Code of Federal Regulations, 2012 CFR

2012-07-01

... Stationary Fuel Combustion Sources). (2) Calculate and report process and combustion CO2 emissions separately... calculate and report the annual process CO2 emissions from each smelting furnace using the procedure in... § 98.33(b)(4)(ii) or (b)(4)(iii), you must calculate and report combined process and combustion CO2...

40 CFR 98.183 - Calculating GHG emissions.

Code of Federal Regulations, 2013 CFR

2013-07-01

... Stationary Fuel Combustion Sources). (2) Calculate and report process and combustion CO2 emissions separately... calculate and report the annual process CO2 emissions from each smelting furnace using the procedure in... § 98.33(b)(4)(ii) or (b)(4)(iii), you must calculate and report combined process and combustion CO2...

40 CFR 98.183 - Calculating GHG emissions.

Code of Federal Regulations, 2011 CFR

2011-07-01

... Stationary Fuel Combustion Sources). (2) Calculate and report process and combustion CO2 emissions separately... calculate and report the annual process CO2 emissions from each smelting furnace using the procedure in... § 98.33(b)(4)(ii) or (b)(4)(iii), you must calculate and report combined process and combustion CO2...

40 CFR 98.183 - Calculating GHG emissions.

Code of Federal Regulations, 2014 CFR

2014-07-01

... Stationary Fuel Combustion Sources). (2) Calculate and report process and combustion CO2 emissions separately... calculate and report the annual process CO2 emissions from each smelting furnace using the procedure in... § 98.33(b)(4)(ii) or (b)(4)(iii), you must calculate and report combined process and combustion CO2...

Advanced air revitalization for optimized crew and plant environments

NASA Technical Reports Server (NTRS)

Lee, M. G.; Grigger, David J.; Brown, Mariann F.

1991-01-01

The Hybrid Air Revitalization System (HARS) closed ecosystem concept presented encompasses electrochemical CO2 and O2 separators, in conjunction with a mechanical condenser/separator for maintaining CO2, O2, and humidity levels in crew and plant habitats at optimal conditions. HARS requires no expendables, and allows flexible process control on the bases of electrochemical cell current, temperature, and airflow rate variations. HARS capacity can be easily increased through the incorporation of additional chemical cells. Detailed system flowcharts are provided.

Fabrication of zeolitic imidazolate framework-8-methacrylate monolith composite capillary columns for fast gas chromatographic separation of small molecules.

PubMed

Yusuf, Kareem; Badjah-Hadj-Ahmed, Ahmed Yacine; Aqel, Ahmad; ALOthman, Zeid Abdullah

2015-08-07

A composite zeolitic imidazolate framework-8 (ZIF-8) with a butyl methacrylate-co-ethylene dimethacrylate (BuMA-co-EDMA) monolithic capillary column (33.5cm long×250μm i.d.) was fabricated to enhance the separation efficiency of methacrylate monoliths toward small molecules using conventional low-pressure gas chromatography in comparison with a neat butyl methacrylate-co-ethylene dimethacrylate (BuMA-co-EDMA) monolithic capillary column (33.5cm long×250μm i.d.). The addition of 10mgmL(-1) ZIF-8 micro-particles increased the BET surface area of BuMA-co-EDMA by 3.4-fold. A fast separation of five linear alkanes in 36s with high resolution (Rs≥1.3) was performed using temperature program. Isothermal separation of the same sample also showed a high efficiency (3315platesm(-1) for octane) at 0.89min. Moreover, the column was able to separate skeletal isomers, such as iso-octane/octane and 2-methyl octane/nonane. In addition, an iso-butane/iso-butylene gas mixture was separated at ambient temperature. Comparison with an open tubular TR-5MS column (30m long×250μm i.d.) revealed the superiority of the composite column in separating the five-membered linear alkane mixture with 4-5 times increase in efficiency and a total separation time of 0.89min instead of 4.67min. A paint thinner sample was fully separated using the composite column in 2.43min with a good resolution (Rs≥0.89). The perfect combination between the polymeric monolith, with its high permeability, and ZIF-8, with its high surface area and flexible 0.34nm pore openings, led to the fast separation of small molecules with high efficiency and opened a new horizon in GC applications. Copyright © 2015 Elsevier B.V. All rights reserved.

Extreme diel dissolved oxygen and carbon cycles in shallow vegetated lakes.

PubMed

Andersen, Mikkel R; Kragh, Theis; Sand-Jensen, Kaj

2017-09-13

A common perception in limnology is that shallow lakes are homogeneously mixed owing to their small water volume. However, this perception is largely gained by downscaling knowledge from large lakes to their smaller counterparts. Here we show that shallow vegetated lakes (less than 0.6 m), in fact, undergo recurring daytime stratification and nocturnal mixing accompanied by extreme chemical variations during summer. Dense submerged vegetation effectively attenuates light and turbulence generating separation between warm surface waters and much colder bottom waters. Photosynthesis in surface waters produces oxygen accumulation and CO 2 depletion, whereas respiration in dark bottom waters causes anoxia and CO 2 accumulation. High daytime pH in surface waters promotes precipitation of CaCO 3 which is re-dissolved in bottom waters. Nocturnal convective mixing re-introduces oxygen into bottom waters for aerobic respiration and regenerated inorganic carbon into surface waters, which supports intense photosynthesis. Our results reconfigure the basic understanding of local environmental gradients in shallow lakes, one of the most abundant freshwater habitats globally. © 2017 The Author(s).

Low cost hydrogen/novel membrane technology for hydrogen separation from synthesis gas. Task 1, Literature survey

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

Not Available

1986-02-01

To make the coal-to-hydrogen route economically attractive, improvements are being sought in each step of the process: coal gasification, water-carbon monoxide shift reaction, and hydrogen separation. This report addresses the use of membranes in the hydrogen separation step. The separation of hydrogen from synthesis gas is a major cost element in the manufacture of hydrogen from coal. Separation by membranes is an attractive, new, and still largely unexplored approach to the problem. Membrane processes are inherently simple and efficient and often have lower capital and operating costs than conventional processes. In this report current ad future trends in hydrogen productionmore » and use are first summarized. Methods of producing hydrogen from coal are then discussed, with particular emphasis on the Texaco entrained flow gasifier and on current methods of separating hydrogen from this gas stream. The potential for membrane separations in the process is then examined. In particular, the use of membranes for H{sub 2}/CO{sub 2}, H{sub 2}/CO, and H{sub 2}/N{sub 2} separations is discussed. 43 refs., 14 figs., 6 tabs.« less

Millivolt-scale DC shifts in the human scalp EEG: evidence for a nonneuronal generator.

PubMed

Voipio, Juha; Tallgren, Pekka; Heinonen, Erkki; Vanhatalo, Sampsa; Kaila, Kai

2003-04-01

Slow shifts in the human scalp-recorded EEG, including those related to changes in brain CO(2) levels, have been generally assumed to result from changes in the level of tonic excitation of apical dendrites of cortical pyramidal neurons. We readdressed this issue using DC-EEG shifts elicited in healthy adult subjects by hypo- or hypercapnia. A 3-min period of hyperventilation resulted in a prompt negative shift with a rate of up to 10 microV/s at the vertex (Cz) and an extremely steep dependence (up to 100 microV/mmHg) on the end-tidal Pco(2). This shift had a maximum of up to -2 mV at Cz versus the temporal derivations (T3/T4). Hyperventilation-like breathing of 5% CO(2)-95% O(2), which does not lead to a significant hypocapnia, resulted in a near-complete block of the negative DC shift at Cz. Hypoventilation, or breathing 5% CO(2) in air at normal respiratory rate, induced a positive shift. The high amplitude of the voltage gradients on the scalp induced by hyperventilation is not consistent with a neuronal origin. Instead, the present data suggest that they are generated by extracortical volume currents driven by a Pco(2)-dependent potential difference across epithelia separating the cerebrospinal fluid and blood. Since changes in respiratory patterns and, hence, in the level of brain Pco(2), are likely to occur under a number of experimental conditions in which slow EEG responses have been reported (e.g., attention shifts, preparatory states, epileptic seizures, and hypoxic episodes), the present results call for a thorough reexamination of the mechanisms underlying scalp-recorded DC-EEG responses.

Membranes for Environmentally Friendly Energy Processes

PubMed Central

He, Xuezhong; Hägg, May-Britt

2012-01-01

Membrane separation systems require no or very little chemicals compared to standard unit operations. They are also easy to scale up, energy efficient, and already widely used in various gas and liquid separation processes. Different types of membranes such as common polymers, microporous organic polymers, fixed-site-carrier membranes, mixed matrix membranes, carbon membranes as well as inorganic membranes have been investigated for CO2 capture/removal and other energy processes in the last two decades. The aim of this work is to review the membrane systems applied in different energy processes, such as post-combustion, pre-combustion, oxyfuel combustion, natural gas sweetening, biogas upgrading, hydrogen production, volatile organic compounds (VOC) recovery and pressure retarded osmosis for power generation. Although different membranes could probably be used in a specific separation process, choosing a suitable membrane material will mainly depend on the membrane permeance and selectivity, process conditions (e.g., operating pressure, temperature) and the impurities in a gas stream (such as SO2, NOx, H2S, etc.). Moreover, process design and the challenges relevant to a membrane system are also being discussed to illustrate the membrane process feasibility for a specific application based on process simulation and economic cost estimation. PMID:24958426

CO2-Free Power Generation on an Iron Group Nanoalloy Catalyst via Selective Oxidation of Ethylene Glycol to Oxalic Acid in Alkaline Media

PubMed Central

Matsumoto, Takeshi; Sadakiyo, Masaaki; Ooi, Mei Lee; Kitano, Sho; Yamamoto, Tomokazu; Matsumura, Syo; Kato, Kenichi; Takeguchi, Tatsuya; Yamauchi, Miho

2014-01-01

An Fe group ternary nanoalloy (NA) catalyst enabled selective electrocatalysis towards CO2-free power generation from highly deliverable ethylene glycol (EG). A solid-solution-type FeCoNi NA catalyst supported on carbon was prepared by a two-step reduction method. High-resolution electron microscopy techniques identified atomic-level mixing of constituent elements in the nanoalloy. We examined the distribution of oxidised species, including CO2, produced on the FeCoNi nanoalloy catalyst in the EG electrooxidation under alkaline conditions. The FeCoNi nanoalloy catalyst exhibited the highest selectivities toward the formation of C2 products and to oxalic acid, i.e., 99 and 60%, respectively, at 0.4 V vs. the reversible hydrogen electrode (RHE), without CO2 generation. We successfully generated power by a direct EG alkaline fuel cell employing the FeCoNi nanoalloy catalyst and a solid-oxide electrolyte with oxygen reduction ability, i.e., a completely precious-metal-free system. PMID:25004118

Integration of heterogeneous molecular networks to unravel gene-regulation in Mycobacterium tuberculosis.

PubMed

van Dam, Jesse C J; Schaap, Peter J; Martins dos Santos, Vitor A P; Suárez-Diez, María

2014-09-26

Different methods have been developed to infer regulatory networks from heterogeneous omics datasets and to construct co-expression networks. Each algorithm produces different networks and efforts have been devoted to automatically integrate them into consensus sets. However each separate set has an intrinsic value that is diluted and partly lost when building a consensus network. Here we present a methodology to generate co-expression networks and, instead of a consensus network, we propose an integration framework where the different networks are kept and analysed with additional tools to efficiently combine the information extracted from each network. We developed a workflow to efficiently analyse information generated by different inference and prediction methods. Our methodology relies on providing the user the means to simultaneously visualise and analyse the coexisting networks generated by different algorithms, heterogeneous datasets, and a suite of analysis tools. As a show case, we have analysed the gene co-expression networks of Mycobacterium tuberculosis generated using over 600 expression experiments. Regarding DNA damage repair, we identified SigC as a key control element, 12 new targets for LexA, an updated LexA binding motif, and a potential mismatch repair system. We expanded the DevR regulon with 27 genes while identifying 9 targets wrongly assigned to this regulon. We discovered 10 new genes linked to zinc uptake and a new regulatory mechanism for ZuR. The use of co-expression networks to perform system level analysis allows the development of custom made methodologies. As show cases we implemented a pipeline to integrate ChIP-seq data and another method to uncover multiple regulatory layers. Our workflow is based on representing the multiple types of information as network representations and presenting these networks in a synchronous framework that allows their simultaneous visualization while keeping specific associations from the different networks. By simultaneously exploring these networks and metadata, we gained insights into regulatory mechanisms in M. tuberculosis that could not be obtained through the separate analysis of each data type.

Identification of Preferential Paths of Fossil Carbon within Water Resource Recovery Facilities via Radiocarbon Analysis.

PubMed

Tseng, Linda Y; Robinson, Alice K; Zhang, Xiaying; Xu, Xiaomei; Southon, John; Hamilton, Andrew J; Sobhani, Reza; Stenstrom, Michael K; Rosso, Diego

2016-11-15

The Intergovernmental Panel on Climate Change (IPCC) reported that all carbon dioxide (CO 2 ) emissions generated by water resource recovery facilities (WRRFs) during treatment are modern, based on available literature. Therefore, such emissions were omitted from IPCC's greenhouse gas (GHG) accounting procedures. However, a fraction of wastewater's carbon is fossil in origin. We hypothesized that since the fossil carbon entering municipal WRRFs is mostly from soaps and detergents as dissolved organic matter, its fate can be selectively determined during the universally applied separation treatment processes. Analyzing radiocarbon at different treatment points within municipal WRRFs, we verified that the fossil content could amount to 28% in primary influent and showed varying distribution leaving different unit operations. We recorded the highest proportion of fossil carbon leaving the secondary treatment as off-gas and as solid sludge (averaged 2.08 kg fossil-CO 2 -emission-potential m -3 wastewater treated). By including fossil CO 2 , total GHG emission in municipal WRRFs increased 13%, and 23% if an on-site energy recovery system exists although much of the postdigestion fossil carbon remained in biosolids rather than in biogas, offering yet another carbon sequestration opportunity during biosolids handling. In comparison, fossil carbon contribution to GHG emission can span from negligible to substantial in different types of industrial WRRFs. With such a considerable impact, CO 2 should be analyzed for each WRRF and not omitted from GHG accounting.

A multiple chamber, semicontinuous, crop carbon dioxide exchange system: design, calibration, and data interpretation

NASA Technical Reports Server (NTRS)

van Iersel, M. W.; Bugbee, B.

2000-01-01

Long-term, whole crop CO2 exchange measurements can be used to study factors affecting crop growth. These factors include daily carbon gain, cumulative carbon gain, and carbon use efficiency, which cannot be determined from short-term measurements. We describe a system that measures semicontinuously crop CO2 exchange in 10 chambers over a period of weeks or months. Exchange of CO2 in every chamber can be measured at 5 min intervals. The system was designed to be placed inside a growth chamber, with additional environmental control provided by the individual gas exchange chambers. The system was calibrated by generating CO2 from NaHCO3 inside the chambers, which indicated that accuracy of the measurements was good (102% and 98% recovery for two separate photosynthesis systems). Since the systems measure net photosynthesis (P-net, positive) and dark respiration(R-dark, negative), the data can be used to estimate gross photosynthesis, daily carbon gain, cumulative carbon gain, and carbon use efficiency. Continuous whole-crop measurements are a valuable tool that complements leaf photosynthesis measurements. Multiple chambers allow for replication and comparison among several environmental or cultural treatments that may affect crop growth. Example data from a 2 week study with petunia (Petunia x hybrida Hort. Vilm.-Andr.) are presented to illustrate some of the capabilities of this system.

Harvesting multiple electron-hole pairs generated through plasmonic excitation of Au nanoparticles.

PubMed

Kim, Youngsoo; Smith, Jeremy G; Jain, Prashant K

2018-05-07

Multi-electron redox reactions, although central to artificial photosynthesis, are kinetically sluggish. Amidst the search for synthetic catalysts for such processes, plasmonic nanoparticles have been found to catalyse multi-electron reduction of CO 2 under visible light. This example motivates the need for a general, insight-driven framework for plasmonic catalysis of such multi-electron chemistry. Here, we elucidate the principles underlying the extraction of multiple redox equivalents from a plasmonic photocatalyst. We measure the kinetics of electron harvesting from a gold nanoparticle photocatalyst as a function of photon flux. Our measurements, supported by theoretical modelling, reveal a regime where two-electron transfer from the excited gold nanoparticle becomes prevalent. Multiple electron harvesting becomes possible under continuous-wave, visible-light excitation of moderate intensity due to strong interband transitions in gold and electron-hole separation accomplished using a hole scavenger. These insights will help expand the utility of plasmonic photocatalysis beyond CO 2 reduction to other challenging multi-electron, multi-proton transformations such as N 2 fixation.

A System Level Mass and Energy Calculation for a Temperature Swing Adsorption Pump used for In-Situ Resource Utilization (ISRU) on Mars

NASA Technical Reports Server (NTRS)

Hasseeb, Hashmatullah; Iannetti, Anthony

2017-01-01

A major component of a Martian In-Situ Resource Utilization (ISRU) system is the CO2 acquisition subsystem. This subsystem must be able to extract and separate CO2 at ambient Martian pressures and then output the gas at high pressures for the chemical reactors to generate fuel and oxygen. The Temperature Swing Adsorption (TSA) Pump is a competitive design that can perform this task using heating and cooling cycles in an enclosed volume. The design of this system is explored and analyzed for an output pressure range of 50 kPa to 500 kPa and an adsorption temperature range of -50 C to 40 C while meeting notional requirements for two mission scenarios. Mass and energy consumption results are presented for 2-stage, 3-stage, and 4-stage systems using the following adsorbents: Grace 544 13X, BASF 13X, Grace 522 5A and VSA 10 LiX.

Direct visualization of phase separation between superconducting and nematic domains in Co-doped CaFe2As2 close to a first-order phase transition

NASA Astrophysics Data System (ADS)

Fente, Antón; Correa-Orellana, Alexandre; Böhmer, Anna E.; Kreyssig, Andreas; Ran, S.; Bud'ko, Sergey L.; Canfield, Paul C.; Mompean, Federico J.; García-Hernández, Mar; Munuera, Carmen; Guillamón, Isabel; Suderow, Hermann

2018-01-01

We show that biaxial strain induces alternating tetragonal superconducting and orthorhombic nematic domains in Co-substituted CaFe2As2 . We use atomic force, magnetic force, and scanning tunneling microscopy to identify the domains and characterize their properties, finding in particular that tetragonal superconducting domains are very elongated, more than several tens of micrometers long and about 30 nm wide; have the same Tc as unstrained samples; and hold vortices in a magnetic field. Thus, biaxial strain produces a phase-separated state, where each phase is equivalent to what is found on either side of the first-order phase transition between antiferromagnetic orthorhombic and superconducting tetragonal phases found in unstrained samples when changing Co concentration. Having such alternating superconducting domains separated by normal conducting domains with sizes of the order of the coherence length opens opportunities to build Josephson junction networks or vortex pinning arrays and suggests that first-order quantum phase transitions lead to nanometric-size phase separation under the influence of strain.

Direct visualization of phase separation between superconducting and nematic domains in Co-doped CaFe 2 As 2 close to a first-order phase transition

DOE PAGES

Fente, Antón; Correa-Orellana, Alexandre; Böhmer, Anna E.; ...

2018-01-09

We show that biaxial strain induces alternating tetragonal superconducting and orthorhombic nematic domains in Co substituted CaFe 2As 2. We use Atomic Force, Magnetic Force and Scanning Tunneling Microscopy (AFM, MFM and STM) to identify the domains and characterize their properties, nding in particular that tetragonal superconducting domains are very elongated, more than several tens of μm long and about 30 nm wide, have the same Tc than unstrained samples and hold vortices in a magnetic eld. Thus, biaxial strain produces a phase separated state, where each phase is equivalent to what is found at either side of the rstmore » order phase transition between antiferromagnetic orthorhombic and superconducting tetragonal phases found in unstrained samples when changing Co concentration. Having such alternating superconducting domains separated by normal conducting domains with sizes of order of the coherence length opens opportunities to build Josephson junction networks or vortex pinning arrays and suggests that first order quantum phase transitions lead to nanometric size phase separation under the influence of strain.« less

Analysis of the role of the particle-wall interaction on the separation efficiencies of field flow fractionation dielectrophoretic devices.

PubMed

Camarda, Massimo; Scalese, Silvia; La Magna, Antonino

2015-07-01

In this paper we have used both analytical models and finite element simulations to analyze the role of the particle-wall dipole interaction in field-flow fractionation dielectrophoretic (FFF-DEP) devices. We identify the existence of "anomalous" regions where the dielectrophoretic response is altered, independently of the complex dielectric permittivity of the particles and suspending medium. In these regions the interaction between the particle and the conductive (isolating) walls induces cohesive (repulsive) forces, independently of the Clausius-Mossotti term. We quantify the impact of such an effect, which can critically decrease the specificity and sensitivity of both continuous- and batch-mode FFF-DEP. We find a scale invariant relation correlating the particles radius (Rp ) and the electrodes width (Wel ), which permits the design of dielectrophoretic schema capable of avoiding the generation of such regions. Specifically, to avoid the generation of the anomalous DEP regions, Wel should be chosen smaller than ∼5.2 Rp . For this reason, interdigitate schema with electrode widths of 14 μm and gaps of 50 μm could improve the separation efficiency of FFF-DEP devices in the case of rare cells separation in blood samples. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Subsurface capture of carbon dioxide

DOEpatents

Blount, Gerald; Siddal, Alvin A.; Falta, Ronald W.

2014-07-22

A process and apparatus of separating CO.sub.2 gas from industrial off-gas source in which the CO.sub.2 containing off-gas is introduced deep within an injection well. The CO.sub.2 gases are dissolved in the, liquid within the injection well while non-CO.sub.2 gases, typically being insoluble in water or brine, are returned to the surface. Once the CO.sub.2 saturated liquid is present within the injection well, the injection well may be used for long-term geologic storage of CO.sub.2 or the CO.sub.2 saturated liquid can be returned to the surface for capturing a purified CO.sub.2 gas.

Simulated moving bed system for CO.sub.2 separation, and method of same

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

Elliott, Jeannine Elizabeth; Copeland, Robert James; Lind, Jeff

A system and method for separating and/or purification of CO.sub.2 gas from a CO.sub.2 feed stream is described. The system and method include a plurality of fixed sorbent beds, adsorption zones and desorption zones, where the sorbent beds are connected via valve and lines to create a simulated moving bed system, where the sorbent beds move from one adsorption position to another adsorption position, and then into one regeneration position to another regeneration position, and optionally back to an adsorption position. The system and method operate by concentration swing adsorption/desorption and by adsorptive/desorptive displacement.

Kinetics study of carbon dioxide absorption reaction into the promoted methyldiethanolamine solution

NASA Astrophysics Data System (ADS)

Sitorus, Yasmikha Tiurlan Susanti; Taurina, Hanna Sucita; Altway, Ali; Rahmawati, Yeni; Nurkhamidah, Siti

2017-05-01

The absorption of carbon dioxide (CO2) is important in the industrial world. In industries, especially petrochemical, oil, and natural gas sectors, separation process of CO2 gas which is a corrosive gas (acid gas) is required. So, the separation process of CO2 gas stream is important, one of the methods used to remove CO2 from the gas stream is reactive absorption process using the promoted methyldiethanolamine (MDEA) solution. Therefore, this study is aimed to obtain the reaction kinetics data of CO2 absorption in MDEA solution using arginine as a promoter. Arginine was chosen because of its amino acid molecule which is reactive, so it can accelerate the reaction rate of MDEA. Moreover, this study also made a comparison between the reactivity of MDEA solution using arginine and MDEA solution using other promoters (glycine and piperazine) for CO2 absorption. The method used is absorption using laboratory scale of Wetted Wall Column (WWC) equipment at 1 atm. This study provides the reaction kinetics data information in order to optimize the separation process of CO2 in the industrialized world. The experimental results show that CO2 absorption rate at 323.15 K without any additon of arginine is 2.33 × 10-7 kmol/sec. By addition of 0.5 and 1 wt% of arginine, the absorption rate becomes 4 × 10-7 kmol/sec (2 times larger) and 6 × 10-7 kmol/sec (3 times larger). These results show that the addition of arginine as a promoter can increase the absorption rate of CO2 in MDEA solution and cover the weaknesses of MDEA solution. Based on the experimental result, the reaction kinetics constant for arginine is 1.91 × 1025 exp (-12296/T) (m3/kmol.s). Although, arginine reaction rate constant is lower than glycine and piperazine.

Carbon dioxide emissions from the electricity sector in major countries: a decomposition analysis.

PubMed

Li, Xiangzheng; Liao, Hua; Du, Yun-Fei; Wang, Ce; Wang, Jin-Wei; Liu, Yanan

2018-03-01

The electric power sector is one of the primary sources of CO 2 emissions. Analyzing the influential factors that result in CO 2 emissions from the power sector would provide valuable information to reduce the world's CO 2 emissions. Herein, we applied the Divisia decomposition method to analyze the influential factors for CO 2 emissions from the power sector from 11 countries, which account for 67% of the world's emissions from 1990 to 2013. We decompose the influential factors for CO 2 emissions into seven areas: the emission coefficient, energy intensity, the share of electricity generation, the share of thermal power generation, electricity intensity, economic activity, and population. The decomposition analysis results show that economic activity, population, and the emission coefficient have positive roles in increasing CO 2 emissions, and their contribution rates are 119, 23.9, and 0.5%, respectively. Energy intensity, electricity intensity, the share of electricity generation, and the share of thermal power generation curb CO 2 emissions and their contribution rates are 17.2, 15.7, 7.7, and 2.8%, respectively. Through decomposition analysis for each country, economic activity and population are the major factors responsible for increasing CO 2 emissions from the power sector. However, the other factors from developed countries can offset the growth in CO 2 emissions due to economic activities.

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

PubMed

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

2017-08-15

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

Long Wavelength Electromagnetic Light Bullets Generated by a 10.6 micron CO2 Ultrashort Pulsed Source

DTIC Science & Technology

2016-11-29

AFRL-AFOSR-VA-TR-2016-0365 Long Wavelength Electromagnetic Light Bullets Generated by a 10.6 micron CO2 Ultrashort Pulsed Source Jerome Moloney...SUBTITLE "Long Wavelength Electromagnetic Light Bullets Generated by a 10.6 micron CO2 Ultrashort Pulsed Source 5a. CONTRACT NUMBER FA9550-15-1-0272 5b...afosr.reports.sgizmo.com/s3/> Subject: Final Report to Dr. Arje Nachman Contract/Grant Title: Long Wavelength Electromagnetic Light Bullets Generated by a 10.6

The feasibility of using molten carbonate corrosion for separating a nuclear surrogate for plutonium oxide from silicon carbide inert matrix

NASA Astrophysics Data System (ADS)

Cheng, Ting; Baney, Ronald H.; Tulenko, James

2010-10-01

Silicon carbide is one of the prime candidates as a matrix material in inert matrix fuels (IMF) being designed to reduce the plutonium inventories. Since complete fission and transmutation is not practical in a single in-core run, it is necessary to separate the non-transmuted actinide materials from the silicon carbide matrix for recycling. In this work, SiC was corroded in sodium carbonate (Na 2CO 3) and potassium carbonate (K 2CO 3), to form water soluble sodium or potassium silicate. Separation of the transuranics was achieved by dissolving the SiC corrosion product in boiling water. Ceria (CeO 2), which was used as a surrogate for plutonium oxide (PuO 2), was not corroded in these molten salt environments. The molten salt depth, which is a distance between the salt/air interface to the upper surface of SiC pellets, significantly affected the rate of corrosion. The corrosion was faster in K 2CO 3 than in Na 2CO 3 molten salt at 1050 °C, when the initial molten salt depths were kept the same for both salts.

Phase Separation Kinetics in Isopycnic Mixtures of H2O/CO2/Ethoxylated Alcohol Surfactants

NASA Technical Reports Server (NTRS)

Lesemann, Markus; Paulaitis, Michael E.; Kaler, Eric W.

1999-01-01

Ternary mixtures of H2O and CO2 with ethoxylated alcohol (C(sub i)E(sub j)) surfactants form three coexisting liquid phases at conditions where two of the phases have equal densities (isopycnic phases). Isopycnic phase behavior has been observed for mixtures containing C8E5, C10E6, and C12E6 surfactants, but not for those mixtures containing either C4E1 or C8E3 surfactants. Pressure-temperature (PT) projections for this three-phase equilibrium were determined for H2O/CO2/C8E5 and H2O/CO2/C10E6 mixtures at temperatures from approximately 25 to 33 C and pressures between 90 and 350 bar. Measurements of the microstructure in H2O/CO2/C12E6 mixtures as a function of temperature (25-31 C), pressure (63.1-90.7 bar), and CO2 composition (0-3.9 wt%) have also been carried out to show that while micellar structure remains essentially un-changed, critical concentration fluctuations increase as the phase boundary and plait point are approached. In this report, we present our first measurements of the kinetics of isopycnic phase separation for ternary mixtures of H2O/CO2/C8E5.

MoS2 Nanosheet-Modified CuInS2 Photocatalyst for Visible-Light-Driven Hydrogen Production from Water.

PubMed

Yuan, Yong-Jun; Chen, Da-Qin; Huang, Yan-Wei; Yu, Zhen-Tao; Zhong, Jia-Song; Chen, Ting-Ting; Tu, Wen-Guang; Guan, Zhong-Jie; Cao, Da-Peng; Zou, Zhi-Gang

2016-05-10

Exploiting photocatalysts respond to visible light is of huge challenge for photocatalytic H2 production. Here, we synthesize a new composite material consisting of few-layer MoS2 nanosheets grown on CuInS2 surface as an efficient photocatalyst for solar H2 generation. The photocatalytic results demonstrate that the 3 wt % MoS2 /CuInS2 photocatalyst exhibits the highest H2 generation rate of 316 μmol h(-1)  g(-1) under visible light irradiation, which is almost 28 times higher than that of CuInS2 . Importantly, the MoS2 /CuInS2 photocatalyst shows a much higher photocatalytic activity than that of Pt-loaded CuInS2 photocatalyst. The enhanced photocatalytic activities of MoS2 /CuInS2 photocatalysts can be attributed to the improved charge separation at the interface of MoS2 and CuInS2, which is demonstrated by the significant enhancement of photocurrent responses in MoS2 /CuInS2 photoelectrodes. This work presents a noble-metal-free photocatalyst that responds to visible light for solar H2 generation. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Hydrogen Purification and Recycling for an Integrated Oxygen Recovery System Architecture

NASA Technical Reports Server (NTRS)

Abney, Morgan B.; Greenwood, Zachary; Wall, Terry; Miller, Lee; Wheeler, Ray

2016-01-01

The United States Atmosphere Revitalization life support system on the International Space Station (ISS) performs several services for the crew including oxygen generation, trace contaminant control, carbon dioxide (CO2) removal, and oxygen recovery. Oxygen recovery is performed using a Sabatier reactor developed by Hamilton Sundstrand, wherein CO2 is reduced with hydrogen in a catalytic reactor to produce methane and water. The water product is purified in the Water Purification Assembly and recycled to the Oxygen Generation Assembly (OGA) to provide O2 to the crew. This architecture results in a theoretical maximum oxygen recovery from CO2 of approximately 54% due to the loss of reactant hydrogen in Sabatier-produced methane that is currently vented outside of ISS. Plasma Methane Pyrolysis technology (PPA), developed by Umpqua Research Company, provides the capability to further close the Atmosphere Revitalization oxygen loop by recovering hydrogen from Sabatier-produced methane. A key aspect of this technology approach is to purify the hydrogen from the PPA product stream which includes acetylene, unreacted methane and byproduct water and carbon monoxide. In 2015, four sub-scale hydrogen separation systems were delivered to NASA for evaluation. These included two electrolysis single-cell hydrogen purification cell stacks developed by Sustainable Innovations, LLC, a sorbent-based hydrogen purification unit using microwave power for sorbent regeneration developed by Umpqua Research Company, and a LaNi4.6Sn0.4 metal hydride produced by Hydrogen Consultants, Inc. Here we report the results of these evaluations, discuss potential architecture options, and propose future work.

Hydrogen Purification and Recycling for an Integrated Oxygen Recovery System Architecture

NASA Technical Reports Server (NTRS)

Abney, Morgan B.; Greenwood, Zachary; Wall, Terry; Nur, Mononita; Wheeler, Richard R., Jr.; Preston, Joshua; Molter, Trent

2016-01-01

The United States Atmosphere Revitalization life support system on the International Space Station (ISS) performs several services for the crew including oxygen generation, trace contaminant control, carbon dioxide (CO2) removal, and oxygen recovery. Oxygen recovery is performed using a Sabatier reactor developed by Hamilton Sundstrand, wherein CO2 is reduced with hydrogen in a catalytic reactor to produce methane and water. The water product is purified in the Water Purification Assembly and recycled to the Oxygen Generation Assembly (OGA) to provide O2 to the crew. This architecture results in a theoretical maximum oxygen recovery from CO2 of approx.54% due to the loss of reactant hydrogen in Sabatier-produced methane that is currently vented outside of ISS. Plasma Pyrolysis Assembly (PPA) technology, developed by Umpqua Research Company, provides the capability to further close the Atmosphere Revitalization oxygen loop by recovering hydrogen from Sabatier-produced methane. A key aspect of this technology approach is the need to purify the hydrogen from the PPA product stream which includes acetylene, unreacted methane and byproduct water and carbon monoxide. In 2015, four sub-scale hydrogen separation systems were delivered to NASA for evaluation. These included two electrolysis single-cell hydrogen purification cell stacks developed by Sustainable Innovations, LLC, a sorbent-based hydrogen purification unit using microwave power for sorbent regeneration developed by Umpqua Research Company, and a LaNi4.6Sn0.4 metal hydride produced by Hydrogen Consultants, Inc. Here we report the results of these evaluations to-date, discuss potential architecture options, and propose future work.

Hydro-geophysical responses to the injection of CO2 in core plugs of Berea sandstone

NASA Astrophysics Data System (ADS)

Song, I.; Park, K. G.

2017-12-01

We have built a laboratory-scale core flooding system to measure the relative permeability of a core sample and the acoustic response to the CO2 saturation degree at in situ condition of pressure and temperature down to a few kilometer depths. The system consisted of an acoustic velocity core holder (AVC model from the Core Laboratories) between upstream where CO2 and H2O were injected separately and downstream where the mixed fluids came out of a core sample. Core samples with 4 cm in diameter and 5 cm in length of Berea sandstone were in turn placed in the core holder for confining and axial pressures. The flooding operations of the multiphase fluids were conducted through the sample at 40ºC in temperature and 8 MPa in backpressure. CO2 and H2O in the physical condition were injected separately into a sample at constant rate with various ratios. The two phases were mixed during flowing through the sample. The mixed fluids out of the sample were separated again by their different densities in a chamber equipped with a level gauge of the interface. From the level change of the water in the separator, we measured the volume of water coming out of the sample for each test with a constant ratio of the injection rates. Then it was possible to calculate the saturation degree of CO2 from the difference between input volume and output volume of water. The differential pressure between upstream and downstream was directly measured to calculate the relative permeability as a function of the CO2 saturation degree. We also conducted ultrasonic measurements using piezoelectric sensors on the end plugs. An electric pulse was given to a sensor on one end of sample, and then ultrasonic waves were recorded from the other end. The various ratios of injection rate of CO2 and H2O into Berea sandstone yielded a range of 0.1-0.7 in CO2 saturation degree. The relative permeability was obtained at the condition of steady-state flow for given stages from the velocity of each phase and the pressure gradient. The arrival time of P-wave became retarded and its amplitude became smaller as the degree of CO2 saturation increases. However no change was observed in S-wave in both characters. According to our results, time-lapse measurements of P-wave signals can be a monitoring tool of the subsurface migration of CO2, thus of detecting even its leakage.

In vivo effect of carbon dioxide laser-skin resurfacing and mechanical abrasion on the skin's microbial flora in an animal model.

PubMed

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.

pH-controlled gas-generating mineralized nanoparticles: a theranostic agent for ultrasound imaging and therapy of cancers.

PubMed

Min, Kyung Hyun; Min, Hyun Su; Lee, Hong Jae; Park, Dong Jin; Yhee, Ji Young; Kim, Kwangmeyung; Kwon, Ick Chan; Jeong, Seo Young; Silvestre, Oscar F; Chen, Xiaoyuan; Hwang, Yu-Shik; Kim, Eun-Cheol; Lee, Sang Cheon

2015-01-27

We report a theranostic nanoparticle that can express ultrasound (US) imaging and simultaneous therapeutic functions for cancer treatment. We developed doxorubicin-loaded calcium carbonate (CaCO3) hybrid nanoparticles (DOX-CaCO3-MNPs) through a block copolymer templated in situ mineralization approach. The nanoparticles exhibited strong echogenic signals at tumoral acid pH by producing carbon dioxide (CO2) bubbles and showed excellent echo persistence. In vivo results demonstrated that the DOX-CaCO3-MNPs generated CO2 bubbles at tumor tissues sufficient for echogenic reflectivity under a US field. In contrast, the DOX-CaCO3-MNPs located in the liver or tumor-free subcutaneous area did not generate the CO2 bubbles necessary for US contrast. The DOX-CaCO3-MNPs could also trigger the DOX release simultaneously with CO2 bubble generation at the acidic tumoral environment. The DOX-CaCO3-MNPs displayed effective antitumor therapeutic activity in tumor-bearing mice. The concept described in this work may serve as a useful guide for development of various theranostic nanoparticles for US imaging and therapy of various cancers.

CO2 Separation and Capture Properties of Porous Carbonaceous Materials from Leather Residues

PubMed Central

Bermúdez, José M.; Dominguez, Pablo Haro; Arenillas, Ana; Cot, Jaume; Weber, Jens; Luque, Rafael

2013-01-01

Carbonaceous porous materials derived from leather skin residues have been found to have excellent CO2 adsorption properties, with interestingly high gas selectivities for CO2 (α > 200 at a gas composition of 15% CO2/85% N2, 273K, 1 bar) and capacities (>2 mmol·g−1 at 273 K). Both CO2 isotherms and the high heat of adsorption pointed to the presence of strong binding sites for CO2 which may be correlated with both: N content in the leather residues and ultrasmall pore sizes. PMID:28788352

Advances and recent trends in heterogeneous photo(electro)-catalysis for solar fuels and chemicals.

PubMed

Highfield, James

2015-04-15

In the context of a future renewable energy system based on hydrogen storage as energy-dense liquid alcohols co-synthesized from recycled CO2, this article reviews advances in photocatalysis and photoelectrocatalysis that exploit solar (photonic) primary energy in relevant endergonic processes, viz., H2 generation by water splitting, bio-oxygenate photoreforming, and artificial photosynthesis (CO2 reduction). Attainment of the efficiency (>10%) mandated for viable techno-economics (USD 2.00-4.00 per kg H2) and implementation on a global scale hinges on the development of photo(electro)catalysts and co-catalysts composed of earth-abundant elements offering visible-light-driven charge separation and surface redox chemistry in high quantum yield, while retaining the chemical and photo-stability typical of titanium dioxide, a ubiquitous oxide semiconductor and performance "benchmark". The dye-sensitized TiO2 solar cell and multi-junction Si are key "voltage-biasing" components in hybrid photovoltaic/photoelectrochemical (PV/PEC) devices that currently lead the field in performance. Prospects and limitations of visible-absorbing particulates, e.g., nanotextured crystalline α-Fe2O3, g-C3N4, and TiO2 sensitized by C/N-based dopants, multilayer composites, and plasmonic metals, are also considered. An interesting trend in water splitting is towards hydrogen peroxide as a solar fuel and value-added green reagent. Fundamental and technical hurdles impeding the advance towards pre-commercial solar fuels demonstration units are considered.

Dental radiography: tooth enamel EPR dose assessment from Rando phantom measurements

NASA Astrophysics Data System (ADS)

Aragno, D.; Fattibene, P.; Onori, S.; Aragno, D.; Fattibene, P.

2000-09-01

Electron paramagnetic resonance dosimetry of tooth enamel is now established as a suitable method for individual dose reconstruction following radiation accidents. The accuracy of the method is limited by some confounding factors, among which is the dose received due to medical x-ray irradiation. In the present paper the EPR response of tooth enamel to endoral examination was experimentally evaluated using an anthropomorphic phantom. The dose to enamel for a single exposure of a typical dental examination performed with a new x-ray generation unit working at 65 kVp gave rise to a CO2- signal of intensity similar to that induced by a dose of about 2 mGy of 60Co. EPR measurements were performed on the entire tooth with no attempt to separate buccal and lingual components. Also the dose to enamel for an orthopantomography exam was estimated. It was derived from TLD measurements as equivalent to 0.2 mGy of 60Co. In view of application to risk assessment analysis, in the present work the value for the ratio of the reference dose at the phantom surface measured with TLD to the dose at the tooth measured with EPR was determined.

Spacecraft nitrogen generation. [liquid hydrazine

NASA Technical Reports Server (NTRS)

Marshall, R. D.; Carlson, J. N.; Powell, J. D.; Kacholia, K. K.

1974-01-01

Two spacecraft nitrogen (N2) generation systems based on the catalytic dissociation of hydrazine (N2H4) were evaluated. In the first system, liquid N2H4 is catalytically dissociated to yield an N2 and hydrogen (H2) gas mixture. Separation of the N2/H2 gas mixture to yield N2 and a supply of H2 is accomplished using a polymer-electrochemical N2/H2 separator. In the second system, the N2/H2 gas mixture is separated in a two-stage palladium/silver (Pd/Ag) N2/H2 separator. The program culminated in the successful design, fabrication, and testing of a N2H4 catalytic dissociator, a polymer-electrochemical N2/H2 separator, and a two-stage Pd/Ag N2/H2 separator. The hardware developed was sized for an N2 delivery rate of 6.81 kg/d (15lb/day). Experimental results demonstrated that both spacecraft N2 generation systems are capable of producing 6.81 kg/d (15lb/day) of 99.9% pure N2 at a pressure greater than or equal to 1035 kN/m(2) (150 psia).

Short run effects of a price on carbon dioxide emissions from U.S. electric generators.

PubMed

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.

Change detection and classification of land cover in multispectral satellite imagery using clustering of sparse approximations (CoSA) over learned feature dictionaries

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

Moody, Daniela I.; Brumby, Steven P.; Rowland, Joel C.

Neuromimetic machine vision and pattern recognition algorithms are of great interest for landscape characterization and change detection in satellite imagery in support of global climate change science and modeling. We present results from an ongoing effort to extend machine vision methods to the environmental sciences, using adaptive sparse signal processing combined with machine learning. A Hebbian learning rule is used to build multispectral, multiresolution dictionaries from regional satellite normalized band difference index data. Land cover labels are automatically generated via our CoSA algorithm: Clustering of Sparse Approximations, using a clustering distance metric that combines spectral and spatial textural characteristics tomore » help separate geologic, vegetative, and hydrologie features. We demonstrate our method on example Worldview-2 satellite images of an Arctic region, and use CoSA labels to detect seasonal surface changes. In conclusion, our results suggest that neuroscience-based models are a promising approach to practical pattern recognition and change detection problems in remote sensing.« less

Change detection and classification of land cover in multispectral satellite imagery using clustering of sparse approximations (CoSA) over learned feature dictionaries

DOE PAGES

Moody, Daniela I.; Brumby, Steven P.; Rowland, Joel C.; ...

2014-10-01

Neuromimetic machine vision and pattern recognition algorithms are of great interest for landscape characterization and change detection in satellite imagery in support of global climate change science and modeling. We present results from an ongoing effort to extend machine vision methods to the environmental sciences, using adaptive sparse signal processing combined with machine learning. A Hebbian learning rule is used to build multispectral, multiresolution dictionaries from regional satellite normalized band difference index data. Land cover labels are automatically generated via our CoSA algorithm: Clustering of Sparse Approximations, using a clustering distance metric that combines spectral and spatial textural characteristics tomore » help separate geologic, vegetative, and hydrologie features. We demonstrate our method on example Worldview-2 satellite images of an Arctic region, and use CoSA labels to detect seasonal surface changes. In conclusion, our results suggest that neuroscience-based models are a promising approach to practical pattern recognition and change detection problems in remote sensing.« less

Interfacial dynamics and solar fuel formation in dye-sensitized photoelectrosynthesis cells.

PubMed

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.

Ionic liquid-impregnated activated carbon for biohydrogen purification in an adsorption unit

NASA Astrophysics Data System (ADS)

Yusuf, N. Y.; Masdar, M. S.; Isahak, W. N. R. W.; Nordin, D.; Husaini, T.; Majlan, E. H.; Rejab, S. A. M.; Chew, C. L.

2017-06-01

Biological methods for hydrogen production (biohydrogen) are known as energy intensive and can be operated at ambient temperature and pressure; however, consecutive productions such as purification and separation processes still remain challenging in the industry. Various techniques are used to purify and separate hydrogen. These techniques include the use of sorbents/solvents, membranes and cryogenic distillation. In this study, carbon dioxide (CO2) was purified and separated from biohydrogen to produce high purity hydrogen gas. CO2 capture was studied using the activated carbon (AC) modified with the ionic liquid (IL) choline chloride as adsorbent. The physical and chemical properties of the adsorbents were characterized through XRD, FTIR, SEM-EDX, TGA, and BET analyses. The effects of IL loading, flow rate, temperature, and gas mixture were also investigated based on the absorption and desorption of CO2. The CO2 level in the biohydrogen composition was analyzed using a CO2 gas analyzer. The SEM image indicated that the IL homogeneously covered the AC surface. High IL dispersion inlet enhanced the capability of the adsorbent to capture CO2 gas. The thermal stability and presence of the functionalized group of ILs on AC were analyzed by TGA and FTIR techniques, respectively. CO2 adsorption experiments were conducted using a 1 L adsorber unit. Hence, adsorption technologies exhibit potential for biohydrogen purification and mainly affected by adsorbent ability and operating parameters. This research presents an improved biohydrogen technique based on adsorption technology with novel adsorbents. Two different types of commercial CO2 adsorbents were used in the experiment. Results show that the IL/AC exhibited properties suitable for CO2 adsorption. The IL/AC sample presented a high CO2 uptake of 30 wt. % IL when treated at 30 °C for 6 h under a flow rate of 1 L/min. The presence of IL increased the selectivity of CO2 removal during the adsorption process. This IL/AC can be regenerated for several times without any significant loss in the performance.

Attraction of subterranean termites (Isoptera) to carbon dioxide.

PubMed

Bernklau, Elisa Jo; Fromm, Erich A; Judd, Timothy M; Bjostad, Louis B

2005-04-01

Subterranean termites, Reticulitermes spp., were attracted to carbon dioxide (CO2) in laboratory and field tests. In behavioral bioassays, Reticulitermes flavipes (Kollar), Reticulitermes tibialis Banks, and Reticulitermes virginicus Banks were attracted to CO2 concentrations between 5 and 50 mmol/mol. In further bioassays, R. tibialis and R. virginicus were attracted to the headspace from polyisocyanurate construction foam that contained 10-12 mmol/mol CO2. In soil bioassays in the laboratory, more termites foraged in chambers containing CO2-generating formulations than in unbaited control chambers. In field tests, stations containing CO2-generating baits attracted R. tibialis away from wooden fence posts at rangeland sites in Colorado. For all of the CO2 formulations tested, termites foraged in significantly more bait stations at treatment fenceposts than in bait stations at the control fenceposts. By the end of the 8-wk study, the number of bait stations located by termites at treatment fenceposts ranged from 40 to 90%. At control fenceposts, termites foraged in only a single station and the one positive station was not located by termites until week 5 of the study. At treatment fenceposts, termites foraged equally in active stations (containing a CO2-generating bait) and passive stations (with no CO2-generating bait), indicating that bait stations may benefit passively from a proximal CO2 source in the soil. CO2 used as an attractant in current baiting systems could improve their effectiveness by allowing earlier exposure of termites to an insecticide.

Separation and/or sequestration apparatus and methods

DOEpatents

Rieke, Peter C; Towne, Silas A; Coffey, Greg W; Appel, Aaron M

2015-02-03

Apparatus for separating CO.sub.2 from an electrolyte solution are provided. Example apparatus can include: a vessel defining an interior volume and configured to house an electrolyte solution; an input conduit in fluid communication with the interior volume; an output conduit in fluid communication with the interior volume; an exhaust conduit in fluid communication with the interior volume; and an anode located within the interior volume. Other example apparatus can include: an elongated vessel having two regions; an input conduit extending outwardly from the one region; an output conduit extending outwardly from the other region; an exhaust conduit in fluid communication with the one region; and an anode located within the one region. Methods for separating CO.sub.2 from an electrolyte solution are provided. Example methods can include: providing a CO.sub.2 rich electrolyte solution to a vessel containing an anode; and distributing hydrogen from the anode to acidify the electrolyte solution.

Fabrication of 6FDA-durene membrane incorporated with zeolite T and aminosilane grafted zeolite T for CO2/CH4 separation

NASA Astrophysics Data System (ADS)

Jusoh, Norwahyu; Fong Yeong, Yin; Keong Lau, Kok; Shariff, Azmi Mohd

2017-08-01

In the present work, zeolite T and aminosilane grafted zeolite T are embedded into 6FDA-durene polyimide phase for the fabrication of mixed matrix membranes (MMMs). FESEM images demonstrated that the improvement of interfacial adhesion between zeolite and polymer phases in MMM loaded with aminosilane grafted zeolite T was not significant as compared to zeolite T/6FDA-durene MMM. From the gas permeation test, CO2/CH4 selectivity up to 26.4 was achieved using MMM containing aminosilane grafted zeolite T, while MMM loaded with ungrafted zeolite T showed CO2/CH4 selectivity of 19.1. In addition, MMM incorporated with aminosilane grafted zeolite T particles successfully lies on Robeson upper bound 2008, which makes it an attractive candidate for CO2/CH4 separation.

Carbon dioxide-selective membranes and their applications in hydrogen processing

NASA Astrophysics Data System (ADS)

Zou, Jian

Fuel cells, which are regarded as a promising energy conversion approach in the 21st century, are now receiving increasing attention worldwide. In most cases, hydrogen is the preferred fuel for fuel cells, especially for proton-exchange membrane fuel cells (PEMFCs). One key issue in the development of PEMFC is how to generate hydrogen from the available hydrocarbon fuels. Most feasible strategies consist of a reforming step followed by the water gas shift (WGS) reaction. The resulting synthesis gas (syngas) still consists of 0.5--1.0% CO, which needs to be reduced to less than 10 ppm to meet the requirement of PEMFCs. Therefore, a further CO clean-up step is usually used to decrease CO concentration. In the present work, new CO2-selective membranes were synthesized and their applications for fuel cell fuel processing and synthesis gas purification were investigated. In order to enhance CO2 transport across membranes, the synthesized membranes contained both mobile and fixed site carriers in crosslinked poly(vinyl alcohol). The effects of crosslinking, membrane composition, feed pressure, water content, and temperature on transport properties were investigated. The membranes have shown a high permeability and a good CO 2/H2 selectivity and maintained their separation performance up to 170°C. One type of these membranes showed a permeability of 8000 Barrers (1 Barrer = 10-10 cm3 (STP).cm/(cm 2.s.cm.Hg)) and a CO2/H2 selectivity of 290 at 110°C. This membrane had a permeability of 1200 Barrers and a CO 2/H2 selectivity of 33 even at 170°C. The applications of the synthesized membranes were demonstrated in a CO2-removal experiment, in which the CO2 concentration in retentate was decreased from 17% to less than 10 ppm. With such membranes, there are several options to reduce the CO concentration of syngas. One option is to develop a WGS membrane reactor, in which both the low temperature WGS reaction and the CO2-removal take place. Another option is to use a proposed process consisting of a CO2-removal membrane module followed by a conventional low-temperature WGS reactor. A third option is to use methanation after the CO2-removal, one of the most widely used processes for the CO clean-up step. Experimental results showed that CO concentration was reduced to below 10 ppm with all three approaches. In the membrane reactor, a CO concentration of less than 10 ppm and a H 2 concentration of greater than 50% (on the dry basis) were achieved at various flow rates of a simulated autothermal reformate. In the proposed CO2-removal/WGS process, with more than 99.5 % CO2 removed from the synthesis gas, the reversible WGS was shifted forward so that the CO concentration was decreased from 1.2% to less than 10 ppm (dry), which is the requirement for PEMFC. The WGS reactor had a gas hourly space velocity of 7650 h-1 at 150°C and the H2 concentration in the outlet was more than 54.7% (dry). The applications of the synthesized CO2-selective membranes for high-pressure synthesis gas purification were also studied. Synthesis gas is the primary source for hydrogen as well as an intermediate for a broad range of chemicals. The separation of CO2 from synthesis gas is a critical step to obtain high purity hydrogen in many industrial plants, especially refinery plants. We studied the synthesized polymeric CO2 -selective membranes for synthesis gas purification at feed pressures higher than 200 psia and temperatures ranging from 100 to 150°C. The effects of feed pressure, microporous support, temperature, and permeate pressure were investigated using a simulated synthesis gas containing 20% carbon dioxide and 80% hydrogen. The membranes synthesized showed best CO2 permeability and CO2/H2 selectivity at 110°C. At a feed pressure of 220 psia, the CO2 permeability and CO2/H2 selectivity reached 756 Barrers and 42, respectively, whereas at a feed pressure of 440 psia, the CO2 permeability was 391 Barrers and the CO 2/H2 selectivity was about 25.

External CO2 and water supplies for enhancing electrical power generation of air-cathode microbial fuel cells.

PubMed

Ishizaki, So; Fujiki, Itto; Sano, Daisuke; Okabe, Satoshi

2014-10-07

Alkalization on the cathode electrode limits the electrical power generation of air-cathode microbial fuel cells (MFCs), and thus external proton supply to the cathode electrode is essential to enhance the electrical power generation. In this study, the effects of external CO2 and water supplies to the cathode electrode on the electrical power generation were investigated, and then the relative contributions of CO2 and water supplies to the total proton consumption were experimentally evaluated. The CO2 supply decreased the cathode pH and consequently increased the power generation. Carbonate dissolution was the main proton source under ambient air conditions, which provides about 67% of total protons consumed for the cathode reaction. It is also critical to adequately control the water content on the cathode electrode of air-cathode MFCs because the carbonate dissolution was highly dependent on water content. On the basis of these experimental results, the power density was increased by 400% (143.0 ± 3.5 mW/m(2) to 575.0 ± 36.0 mW/m(2)) by supplying a humid gas containing 50% CO2 to the cathode chamber. This study demonstrates that the simultaneous CO2 and water supplies to the cathode electrode were effective to increase the electrical power generation of air-cathode MFCs for the first time.

Carbonic Anhydrase Activity Associated with the Cyanobacterium Synechococcus PCC7942 1

PubMed Central

Badger, Murray R.; Price, G. Dean

1989-01-01

Intact cells and crude homogenates of high (1% CO2) and low dissolved inorganic carbon (Ci) (30-50 microliters per liter of CO2) grown Synechococcus PCC7942 have carbonic anhydrase (CA)-like activity, which enables them to catalyze the exchange of 18O from CO2 to H2O. This activity was studied using a mass spectrometer coupled to a cuvette with a membrane inlet system. Intact high and low Ci cells were found to contain CA activity, separated from the medium by a membrane which is preferentially permeable to CO2. This activity is most apparent in the light, where 18O-labeled CO2 species are being taken up by the cells but the effluxing CO2 has lost most of its label to water. In the dark, low Ci cells catalyze the depletion of the 18O enrichment of CO2 and this activity is inhibited by both ethoxyzolamide and 2-(trifluoromethoxy)carbonyl cyanide. This may occur via a common inhibition of the Ci pump and the Ci pump is proposed as a potential site for the exchange of 18O. CA activity was measurable in homogenates of both cell types but was 5- to 10-fold higher in low Ci cells. This was inhibited by ethoxyzolamide with an I50 of 50 to 100 micromolar in both low and high Ci cells. A large proportion of the internal CA activity appears to be pelletable in nature. This pelletability is increased by the presence of Mg2+ in a manner similar to that of ribulose bisphosphate carboxylase-oxygenase activity and chlorophyll (thylakoids) and may be the result of nonspecific aggregation. Separation of crude homogenates on sucrose gradients is consistent with the notion that CA and ribulose bisphosphate carboxylase-oxygenase activity may be associated with the same pelletable fraction. However, we cannot unequivocally establish that CA is located within the carboxysome. The sucrose gradients show the presence of separate soluble and pelletable CA activity. This may be due to the presence of separate forms of the enzyme or may arise from the same pelletable association which is unstable during extraction. PMID:16666546

Mitochondrial Reactive Oxygen Species Trigger Hypoxia-Induced Transcription

NASA Astrophysics Data System (ADS)

Chandel, N. S.; Maltepe, E.; Goldwasser, E.; Mathieu, C. E.; Simon, M. C.; Schumacker, P. T.

1998-09-01

Transcriptional activation of erythropoietin, glycolytic enzymes, and vascular endothelial growth factor occurs during hypoxia or in response to cobalt chloride (CoCl2) in Hep3B cells. However, neither the mechanism of cellular O2 sensing nor that of cobalt is fully understood. We tested whether mitochondria act as O2 sensors during hypoxia and whether hypoxia and cobalt activate transcription by increasing generation of reactive oxygen species (ROS). Results show (i) wild-type Hep3B cells increase ROS generation during hypoxia (1.5% O2) or CoCl2 incubation, (ii) Hep3B cells depleted of mitochondrial DNA (ρ 0 cells) fail to respire, fail to activate mRNA for erythropoietin, glycolytic enzymes, or vascular endothelial growth factor during hypoxia, and fail to increase ROS generation during hypoxia; (iii) ρ 0 cells increase ROS generation in response to CoCl2 and retain the ability to induce expression of these genes; and (iv) the antioxidants pyrrolidine dithiocarbamate and ebselen abolish transcriptional activation of these genes during hypoxia or CoCl2 in wild-type cells, and abolish the response to CoCl2 in ρ 0 cells. Thus, hypoxia activates transcription via a mitochondria-dependent signaling process involving increased ROS, whereas CoCl2 activates transcription by stimulating ROS generation via a mitochondria-independent mechanism.

Importance of Micropore-Mesopore Interfaces in Carbon Dioxide Capture by Carbon-Based Materials.

PubMed

Durá, Gema; Budarin, Vitaliy L; Castro-Osma, José A; Shuttleworth, Peter S; Quek, Sophie C Z; Clark, James H; North, Michael

2016-08-01

Mesoporous carbonaceous materials (Starbons®) derived from low-value/waste bio-resources separate CO2 from CO2 /N2 mixtures. Compared to Norit activated charcoal (AC), Starbons® have much lower microporosities (8-32 % versus 73 %) yet adsorb up to 65 % more CO2 . The presence of interconnected micropores and mesopores is responsible for the enhanced CO2 adsorption. The Starbons® also showed three-four times higher selectivity for CO2 adsorption rather than N2 adsorption compared to AC. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

An ab initio molecular dynamics study of S0 ketene fragmentation

NASA Astrophysics Data System (ADS)

Forsythe, Kelsey M.; Gray, Stephen K.; Klippenstein, Stephen J.; Hall, Gregory E.

2001-08-01

The dynamical origins of product state distributions in the unimolecular dissociation of S0 ketene, CH2CO (X˜ 1A1)→CH2(ã1A1)+CO, are studied with ab initio molecular dynamics. We focus on rotational distributions associated with ground vibrational state fragments. Trajectories are integrated between an inner, variational transition state (TS) and separated fragments in both the dissociative and associative directions. The average rotational energy in both CO and CH2 fragments decreases during the motion from the TS to separated fragments. However, the CO distribution remains slightly hotter than phase space theory (PST) predictions, whereas that for CH2 ends up significantly colder than PST, in good agreement with experiment. Our calculations do not, however, reproduce the experimentally observed correlations between CH2 and CO rotational states, in which the simultaneous formation of low rotational levels of each fragment is suppressed relative to PST. A limited search for nonstatistical behavior in the strong interaction region also fails to explain this discrepancy.

Radiation Stability of Benzyl Tributyl Ammonium Chloride towards Technetium-99 Extraction - 13016

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

Paviet-Hartmann, Patricia; Horkley, Jared; Campbell, Keri

2013-07-01

A closed nuclear fuel cycle combining new separation technologies along with generation III and generation IV reactors is a promising way to achieve a sustainable energy supply. But it is important to keep in mind that future recycling processes of used nuclear fuel (UNF) must minimize wastes, improve partitioning processes, and integrate waste considerations into processes. New separation processes are being developed worldwide to complement the actual industrialized PUREX process which selectively separates U(VI) and Pu(IV) from the raffinate. As an example, the UREX process has been developed in the United States to co-extract hexavalent uranium (U) and hepta-valent technetiummore » (Tc) by tri-n-butyl phosphate (TBP). Tc-99 is recognized to be one of the most abundant, long-lived radio-toxic isotopes in UNF (half-life, t{sub 1/2} = 2.13 x 10{sup 5} years), and as such, is targeted in UNF separation strategies for isolation and encapsulation in solid waste-forms for final disposal in a nuclear waste repository. Immobilization of Tc-99 by a durable solid waste-form is a challenge, and its fate in new advanced technology processes is of importance. It is essential to be able to quantify and locate 1) its occurrence in any new developed flowsheets, 2) its chemical form in the individual phases of a process, 3) its potential quantitative transfer in any waste streams, and consequently, 4) its quantitative separation for either potential transmutation to Ru-100 or isolation and encapsulation in solid waste-forms for ultimate disposal. In addition, as a result of an U(VI)-Tc(VII) co-extraction in a UREX-based process, Tc(VII) could be found in low level waste (LLW) streams. There is a need for the development of new extraction systems that would selectively extract Tc-99 from LLW streams and concentrate it for feed into high level waste (HLW) for either Tc-99 immobilization in metallic waste-forms (Tc-Zr alloys), and/or borosilicate-based waste glass. Studies have been launched to investigate the suitability of new macro-compounds such as crown-ethers, aza-crown ethers, quaternary ammonium salts, and resorcin-arenes for the selective extraction of Tc-99 from nitric acid solutions. The selectivity of the ligand is important in evaluating potential separation processes and also the radiation stability of the molecule is essential for minimization of waste and radiolysis products. In this paper, we are reporting the extraction of TcO{sub 4}{sup -} by benzyl tributyl ammonium chloride (BTBA). Experimental efforts were focused on determining the best extraction conditions by varying the ligand's matrix conditions and concentration, as well as varying the organic phase composition (i.e. diluent variation). Furthermore, the ligand has been investigated for radiation stability. The ?-irradiation was performed on the neat organic phases containing the ligand at different absorbed doses to a maximum of 200 kGy using an external Co-60 source. Post-irradiation solvent extraction measurements will be discussed. (authors)« less

Analyses of the Integration of Carbon Dioxide Removal Assembly, Compressor, Accumulator and Sabatier Carbon Dioxide Reduction Assembly

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.

System approach to the analysis of an integrated oxy-fuel combustion power plant

NASA Astrophysics Data System (ADS)

Ziębik, Andrzej; Gładysz, Paweł

2014-09-01

Oxy-fuel combustion (OFC) belongs to one of the three commonly known clean coal technologies for power generation sector and other industry sectors responsible for CO2 emissions (e.g., steel or cement production). The OFC capture technology is based on using high-purity oxygen in the combustion process instead of atmospheric air. Therefore flue gases have a high concentration of CO2. Due to the limited adiabatic temperature of combustion some part of CO2 must be recycled to the boiler in order to maintain a proper flame temperature. An integrated oxy-fuel combustion power plant constitutes a system consisting of the following technological modules: boiler, steam cycle, air separation unit, cooling water and water treatment system, flue gas quality control system and CO2 processing unit. Due to the interconnections between technological modules, energy, exergy and ecological analyses require a system approach. The paper present the system approach based on the `input-output' method to the analysis of the: direct energy and material consumption, cumulative energy and exergy consumption, system (local and cumulative) exergy losses, and thermoecological cost. Other measures like cumulative degree of perfection or index of sustainable development are also proposed. The paper presents a complex example of the system analysis (from direct energy consumption to thermoecological cost) of an advanced integrated OFC power plant.

Enzymes involved in branched-chain amino acid metabolism in humans.

PubMed

Adeva-Andany, María M; López-Maside, Laura; Donapetry-García, Cristóbal; Fernández-Fernández, Carlos; Sixto-Leal, Cristina

2017-06-01

Branched-chain amino acids (leucine, isoleucine and valine) are structurally related to branched-chain fatty acids. Leucine is 2-amino-4-methyl-pentanoic acid, isoleucine is 2-amino-3-methyl-pentanoic acid, and valine is 2-amino-3-methyl-butanoic acid. Similar to fatty acid oxidation, leucine and isoleucine produce acetyl-coA. Additionally, leucine generates acetoacetate and isoleucine yields propionyl-coA. Valine oxidation produces propionyl-coA, which is converted into methylmalonyl-coA and succinyl-coA. Branched-chain aminotransferase catalyzes the first reaction in the catabolic pathway of branched-chain amino acids, a reversible transamination that converts branched-chain amino acids into branched-chain ketoacids. Simultaneously, glutamate is converted in 2-ketoglutarate. The branched-chain ketoacid dehydrogenase complex catalyzes the irreversible oxidative decarboxylation of branched-chain ketoacids to produce branched-chain acyl-coA intermediates, which then follow separate catabolic pathways. Human tissue distribution and function of most of the enzymes involved in branched-chain amino acid catabolism is unknown. Congenital deficiencies of the enzymes involved in branched-chain amino acid metabolism are generally rare disorders. Some of them are associated with reduced pyruvate dehydrogenase complex activity and respiratory chain dysfunction that may contribute to their clinical phenotype. The biochemical phenotype is characterized by accumulation of the substrate to the deficient enzyme and its carnitine and/or glycine derivatives. It was established at the beginning of the twentieth century that the plasma level of the branched-chain amino acids is increased in conditions associated with insulin resistance such as obesity and diabetes mellitus. However, the potential clinical relevance of this elevation is uncertain.

Production of Excess CO2 relative to methane in peatlands: a new H2 sink

NASA Astrophysics Data System (ADS)

Wilson, R.; Woodcroft, B. J.; Varner, R. K.; Tyson, G. W.; Tfaily, M. M.; Sebestyen, S.; Saleska, S. R.; Rogers, K.; Rich, V. I.; McFarlane, K. J.; Kostka, J. E.; Kolka, R. K.; Keller, J.; Iversen, C. M.; Hodgkins, S. B.; Hanson, P. J.; Guilderson, T. P.; Griffiths, N.; de La Cruz, F.; Crill, P. M.; Chanton, J.; Bridgham, S. D.; Barlaz, M.

2015-12-01

Methane is generated as the end product of anaerobic organic matter degradation following a series of reaction pathways including fermentation and syntrophy. Along with acetate and CO2, syntrophic reactions generate H2 and are only thermodynamically feasible when coupled to an exothermic reaction that consumes H2. The usual model of organic matter degradation in peatlands has assumed that methanogenesis is that exothermic H2-consuming reaction. If correct, this paradigm should ultimately result in equimolar production of CO2 and methane from the degradation of the model organic compound cellulose: i.e. C6H12O6 à 3CO2 + 3CH4. However, dissolved gas measurement and modeling results from field and incubation experiments spanning peatlands across the northern hemisphere have failed to demonstrate equimolar production of CO2 and methane. Instead, in a flagrant violation of thermodynamics, these studies show a large bias favoring CO2 production over methane generation. In this talk, we will use an array of complementary analytical techniques including FT-IR, cellulose and lignin measurements, 13C-NMR, fluorescence spectroscopy, and ultra-high resolution mass spectrometry to describe organic matter degradation within a peat column and identify the important degradation mechanisms. Hydrogenation was the most common transformation observed in the ultra-high resolution mass spectrometry data. From these results we propose a new mechanism for consuming H2 generated during CO2 production, without concomitant methane formation, consistent with observed high CO2/CH4 ratios. While homoacetogenesis is a known sink for H2 in these systems, this process also consumes CO2 and therefore does not explain the excess CO2 measured in field and incubation samples. Not only does the newly proposed mechanism consume H2 without generating methane, but it also yields enough energy to balance the coupled syntrophic reactions, thereby restoring thermodynamic order. Schematic of organic matter degradation. Solid lines indicate traditional pathways from Conrad (1999), dashed lines indicates new proposed mechanism.

Far-infrared-light shadowgraphy for high extraction efficiency of extreme ultraviolet light from a CO2-laser-generated tin plasma

NASA Astrophysics Data System (ADS)

Matsukuma, Hiraku; Hosoda, Tatsuya; Suzuki, Yosuke; Yogo, Akifumi; Yanagida, Tatsuya; Kodama, Takeshi; Nishimura, Hiroaki

2016-08-01

The two-color, double-pulse method is an efficient scheme to generate extreme ultraviolet light for fabricating the next generation semiconductor microchips. In this method, a Nd:YAG laser pulse is used to expand a several-tens-of-micrometers-scale tin droplet, and a CO2 laser pulse is subsequently directed at the expanded tin vapor after an appropriate delay time. We propose the use of shadowgraphy with a CO2 laser probe-pulse scheme to optimize the CO2 main-drive laser. The distribution of absorption coefficients is derived from the experiment, and the results are converted to a practical absorption rate for the CO2 main-drive laser.

Carbonic anhydrase-facilitated CO2 absorption with polyacrylamide buffering bead capture

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

Dilmore, Robert; Griffith, Craid; Liu, Zhu

2009-07-01

A novel CO2 separation concept is described wherein the enzyme carbonic anhydrase (CA) is used to increase the overall rate Of CO2 absorption after which hydrated CO2 reacts with regenerable amine-bearing polyacrylamide buffering beads (PABB). Following saturation of the material's immobilized tertiary amines, CA-bearing carrier water is separated and recycled to the absorption stage while CO2-loaded material is thermally regenerated. Process application of this concept would involve operation of two or more columns in parallel with thermal regeneration with low-pressure steam taking place after the capacity of a column of amine-bearing polymeric material was exceeded. PABB CO2- bearing capacity wasmore » evaluated by thermogravimetric analysis (TGA) for beads of three acrylamido buffering monomer ingredient concentrations: 0 mol/kg bead, 0.857 mol/kg bead, and 2 mol/kg bead. TGA results demonstrate that CO2- bearing capacity increases with increasing PABB buffering concentration and that up to 78% of the theoretical CO2- bearing capacity was realized in prepared PABB samples (0.857 mol/kg recipe). The highest observed CO2-bearing capacity of PABB was 1.37 mol of CO2 per kg dry bead. TGA was also used to assess the regenerability Of CO2-loaded PABB. Preliminary results suggest that CO2 is partially driven from PABB samples at temperatures as low as 55 degrees C, with complete regeneration occurring at 100 degrees C. Other physical characteristics of PABB are discussed. In addition, the effectiveness of bovine carbonic anhydrase for the catalysis Of CO2 dissolution is evaluated. Potential benefits and drawbacks of the proposed process are discussed. Published by Elsevier Ltd.« less

Phase separations of amorphous CoW films during oxidation and reactions with Si and Al

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

Wang, S.Q.; Mayer, J.W.

1989-03-01

Reactions of thin Co/sub 55/ W/sub 45/ films in contact with Si(100) substrates and aluminum overlayers annealed in vacuum in the temperature ranges of 625--700 /sup 0/C and 500--600 /sup 0/C, respectively, and of thin Co/sub 55/W/sub 45/ films in air from 500 to 600 /sup 0/C were investigated by Rutherford backscattering spectrometry, glancing angle x-ray diffraction, and scanning electron microscope techniques. CoW alloy films were amorphous and have a crystallization temperature of 850 /sup 0/C on SiO/sub 2/ substrates. The compound formed is Co/sub 7/ W/sub 6/. Phase separations were found in all the reactions. A layer of cobaltmore » compounds (CoSi/sub 2/ in Si/CoW, Co/sub 2/ Al/sub 9/ in CoW/Al, and Co/sub 3/ O/sub 4/ in CoW with air) was found to form at the reaction interfaces. In addition, a layer of mainly tungsten compounds (WSi/sub 2/ in Si/CoW, WAl/sub 12/ in CoW/Al, and WO/sub 3/ in CoW with air) was found next to cobalt compound layers, but further away from the reaction interfaces. The reactions started at temperatures comparable to those required for the formation of corresponding tungsten compounds.« less

Two-dimensional TiO2-based nanosheets co-modified by surface-enriched carbon dots and Gd2O3 nanoparticles for efficient visible-light-driven photocatalysis

NASA Astrophysics Data System (ADS)

Lu, Dingze; Fang, Pengfei; Ding, Junqian; Yang, Minchen; Cao, Yufei; Zhou, Yawei; Peng, Kui; Kondamareddy, Kiran Kumar; Liu, Min

2017-02-01

Two-dimensional TiO2-based nanosheets (TNSs) co-modified by surface-enriched carbon dots (CDs) and Gd2O3 nanoparticles: (Gd-C-TNSs), capable of exhibiting visible-light-driven photo catalysis were synthesized using a two-pot hydrothermal route. The samples had a sheet-like structure, thickness of approximately 3.6 nm, large specific surface area of 240-350 cm2/g. The CDs (2-3 nm) and Gd2O3 nanoparticles (1-2 nm) were highly dispersed over the surface of the nanosheets. The co-modification by Gd2O3 nanoparticles and CDs influenced the crystallinity, crystal structure, and surface area of the TNSs, and improved the visible-light absorption. Surface photocurrent and fluorescence spectral studies revealed that the photo-generated charge carrier separation efficiency could be improved by an appropriate amount of modification. A very high efficiency was obtained using 0.5 at% Gd/Ti and 3.0 g/L of CDs. The visible-light-induced photocatalytic activity is enhanced under the isolated Cr(VI) system, isolated Rhodamin B (RhB) system, and the synergism between RhB degradation and Cr(VI) reduction for the Gd-C-TNSs photocatalysts. Initially, the photocatalytic activity gradually increased with an increase in the amount of CDs, and then decreased after attaining a maximum, in the case where 0.5 at% Gd/Ti and 3.0 g/L of CDs were used. The enhancement in the photocatalytic activity was attributed to the synergetic effect of the Gd2O3 nanoparticles, TNSs, and CDs in the Gd-C-TNSs composites. The effect led to a fast separation and slow recombination of photo-induced electron-hole pairs. An alternate mechanism for enhanced visible-light photocatalytic activity was also considered.

High Throughput Strontium Isotope Method for Monitoring Fluid Flow Related to Geological CO2 Storage

NASA Astrophysics Data System (ADS)

Capo, R. C.; Wall, A. J.; Stewart, B. W.; Phan, T. T.; Jain, J. C.; Hakala, J. A.; Guthrie, G. D.

2012-12-01

Natural isotope tracers, such as strontium (Sr), can be a unique and powerful component of a monitoring strategy at a CO2 storage site, facilitating both the quantification of reaction progress for fluid-rock interactions and the tracking of brine migration caused by CO2 injection. Several challenges must be overcome, however, to enable the routine use of isotopic tracers, including the ability to rapidly analyze numerous aqueous samples with potentially complex chemical compositions. In a field situation, it might be necessary to analyze tens of samples over a short period of time to identify subsurface reactions and respond to unexpected fluid movement in the host formation. These conditions require streamlined Sr separation chemistry for samples ranging from pristine groundwaters to those containing high total dissolved solids, followed by rapid measurement of isotope ratios with high analytical precision. We have optimized Sr separation chemistry and MC-ICP-MS methods to provide rapid and precise measurements of isotope ratios in geologic, hydrologic, and environmental samples. These improvements will allow an operator to independently prepare samples for Sr isotope analysis off-site using fast, low cost chemical separation procedures and commercially available components. Existing vacuum-assisted Sr separation procedures were modified by using inexpensive disposable parts to eliminate cross contamination. Experimental results indicate that the modified columns provide excellent separation of Sr from chemically complex samples and that Sr can be effectively isolated from problematic matrix elements (e.g., Ca, Ba, K) associated with oilfield brines and formation waters. The separation procedure is designed for high sample throughput in which batches of 24 samples can be processed in approximately 2 hours, and are ready for Sr isotope measurements by MC-ICP-MS immediately after collection from the columns. Precise Sr isotope results can be achieved by MC-ICP-MS with a throughput of 4 to 5 samples per hour. Our mean measured value of NIST Sr isotope standard SRM 987 is 0.710265 ± 0.000014 (2σ, n = 94). A range of brines and CO2-rich fluids analyzed by this method yielded results within the analytical uncertainty of 87Sr/86Sr ratios previously determined by standard column separation and thermal ionization mass spectrometry. This method provides a fast and effective way to use Sr isotopes for monitoring purposes related to geological CO2 storage.

Facile synthesis of 2D Zn(II) coordination polymer and its crystal structure, selective removal of methylene blue and molecular simulations

NASA Astrophysics Data System (ADS)

Sezer, Güneş Günay; Yeşilel, Okan Zafer; Şahin, Onur; Arslanoğlu, Hasan; Erucar, İlknur

2017-09-01

A new coordination polymer {[Zn(μ3-ppda)(H2O)(μ-bpa)Zn(μ-ppda)(μ-bpa)]·4H2O}n (1) (ppda = 1,4-phenylenediacetate, bpa = 1,2-bis(4-pyridyl)ethane) has been synthesized by microwave-assisted reaction and characterized by elemental analysis, IR spectroscopy, single-crystal and powder X-ray diffractions. The asymmetric unit of 1 consists of two Zn(II) ions, two bpa ligands, two ppda ligands, one coordinated and four non-coordinated water molecules. In 1, ppda2- anions are linked the adjacent Zn(II) centers to generate 1D double-stranded chains. These chains are connected into 2D sheets by the bridging bpa ligands. Atomically detailed modeling was performed to compute single and binary component adsorption isotherms of H2, CO2, CH4 and N2 in complex 1. Results showed that 1 exhibits a high adsorption selectivity towards CO2 due to its high affinity for CO2. Results of this study will be helpful to guide the microwave-assisted reaction of coordination polymers to design promising adsorbents for gas storage and gas separation applications. The luminescent property of 1 and the selective removal of dyes in 1 have been also discussed. Results showed that 1 can be a potential candidate for luminescence applications and can selectively adsorb methylene blue (MB) dye molecules.

Synergy of Siam weed (Chromolaena odorata) and poultry manure for energy generation: Effects of pretreatment methods, modeling and process optimization.

PubMed

Dahunsi, S O; Oranusi, S; Owolabi, J B; Efeovbokhan, V E

2017-02-01

The co-digestion of Chromolaena odorata with poultry manure was evaluated in this study. Two samples of the weed: (A: which was pre-treated with mechanical, chemical and thermal methods) and (B: which was pretreated using mechanical and chemical methods only) were separately digested with poultry manure. Biogas generation started from the 2nd to 4th and 4th to 7th day for samples 'A' and 'B' respectively. The most desired actual biogas yield from samples 'A' and 'B' were 3884.20 and 2544.70 (10 -4 m 3 /kg VS) respectively and the gas composition was 68±2% Methane and 20±2% Carbon dioxide for sample A while it was 62±3% Methane and 22±2% Carbon dioxide for sample B. In all, there was a 38.06% increase in gas generation in 'A' over 'B'. The coefficient of determination (R 2 ) for the Response Surface Methodology (RSM) model (0.9009) was high suggesting high accuracy in the modeling and prediction. The worldwide usage of C. odorata is encouraged. Copyright © 2016 Elsevier Ltd. All rights reserved.

DESIGNING AND OPPORTUNITY FUEL WITH BIOMASS AND TIRE-DERIVED FUEL FOR COFIRING AT WILLOW ISLAND GENERATING STATION AND COFIRING SAWDUST WITH COAL AT ALBRIGHT GENERATING STATION

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

K. Payette; D. Tillman

During the period July 1, 2000-March 31, 2004, Allegheny Energy Supply Co., LLC (Allegheny) conducted an extensive demonstration of woody biomass cofiring at its Willow Island and Albright Generating Stations. This demonstration, cofunded by USDOE and Allegheny, and supported by the Biomass Interest Group (BIG) of EPRI, evaluated the impacts of sawdust cofiring in both cyclone boilers and tangentially-fired pulverized coal boilers. The cofiring in the cyclone boiler--Willow Island Generating Station Unit No.2--evaluated the impacts of sawdust alone, and sawdust blended with tire-derived fuel. The biomass was blended with the coal on its way to the combustion system. The cofiringmore » in the pulverized coal boiler--Albright Generating Station--evaluated the impact of cofiring on emissions of oxides of nitrogen (NO{sub x}) when the sawdust was injected separately into the furnace. The demonstration of woody biomass cofiring involved design, construction, and testing at each site. The results addressed impacts associated with operational issues--capacity, efficiency, and operability--as well as formation and control of airborne emissions such as NO{sub x}, sulfur dioxide (SO{sub 2}2), opacity, and mercury. The results of this extensive program are detailed in this report.« less

A Study on the Optimal Generation Mix Based on Portfolio Theory with Considering the Basic Condition for Power Supply

NASA Astrophysics Data System (ADS)

Kato, Moritoshi; Zhou, Yicheng

This paper presents a novel method to analyze the optimal generation mix based on portfolio theory with considering the basic condition for power supply, which means that electricity generation corresponds with load curve. The optimization of portfolio is integrated with the calculation of a capacity factor of each generation in order to satisfy the basic condition for power supply. Besides, each generation is considered to be an asset, and risks of the generation asset both in its operation period and construction period are considered. Environmental measures are evaluated through restriction of CO2 emissions, which are indicated by CO2 price. Numerical examples show the optimal generation mix according to risks such as the deviation of capacity factor of nuclear power or restriction of CO2 emissions, the possibility of introduction of clean coal technology (IGCC, CCS) or renewable energy, and so on. The results of this work will be possibly applied as setting the target of the generation mix for the future according to prospects of risks of each generation and restrictions of CO2 emissions.

Photoexcitation and ionization in carbon dioxide - Theoretical studies in the separated-channel static-exchange approximation

NASA Technical Reports Server (NTRS)

Padial, N.; Csanak, G.; Mckoy, B. V.; Langhoff, P. W.

1981-01-01

Vertical-electronic static-exchange photoexcitation and ionization cross sections are reported which provide a first approximation to the complete dipole spectrum of CO2. Separated-channel static-exchange calculations of vertical-electronic transition energies and oscillator strengths, and Stieltjes-Chebyshev moment methods were used in the development. Detailed comparisons were made of the static-exchange excitation and ionization spectra with photoabsorption, electron-impact excitation, and quantum-defect estimates of discrete transition energies and intensities, and with partial-channel photoionization cross sections obtained from fluorescence measurements and from tunable-source and (e, 2e) photoelectron spectroscopy. Results show that the separate-channel static-exchange approximation is generally satisfactory in CO2.

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

Sridharan, Kumar; Anderson, Mark

The supercritical CO{sub 2} Brayton cycle is gaining importance for power conversion in the Generation IV fast reactor system because of its high conversion efficiencies. When used in conjunction with a sodium fast reactor, the supercritical CO{sub 2} cycle offers additional safety advantages by eliminating potential sodium-water interactions that may occur in a steam cycle. In power conversion systems for Generation IV fast reactors, supercritical CO{sub 2} temperatures could be in the range of 30°C to 650°C, depending on the specific component in the system. Materials corrosion primarily at high temperatures will be an important issue. Therefore, the corrosion performancemore » limits for materials at various temperatures must be established. The proposed research will have four objectives centered on addressing corrosion issues in a high-temperature supercritical CO{sub 2} environment: Task 1: Evaluation of corrosion performance of candidate alloys in high-purity supercritical CO{sub 2}: The following alloys will be tested: Ferritic-martensitic Steels NF616 and HCM12A, austenitic alloys Incoloy 800H and 347 stainless steel, and two advanced concept alloys, AFA (alumina forming austenitic) steel and MA754. Supercritical CO{sub 2} testing will be performed at 450°C, 550°C, and 650°C at a pressure of 20 MPa, in a test facility that is already in place at the proposing university. High purity CO{sub 2} (99.9998%) will be used for these tests. Task 2: Investigation of the effects of CO, H{sub 2}O, and O{sub 2} impurities in supercritical CO{sub 2} on corrosion: Impurities that will inevitably present in the CO{sub 2} will play a critical role in dictating the extent of corrosion and corrosion mechanisms. These effects must be understood to identify the level of CO{sub 2} chemistry control needed to maintain sufficient levels of purity to manage corrosion. The individual effects of important impurities CO, H{sub 2}O, and O{sub 2} will be investigated by adding them separately to high purity CO{sub 2}. Task 3: Evaluation of surface treatments on the corrosion performance of alloys in supercritical CO{sub 2}: Surface treatments can be very beneficial in improving corrosion resistance. Shot peening and yttrium and aluminum surface treatments will be investigated. Shot peening refines the surface grain sizes and promotes protective Cr-oxide layer formation. Both yttrium and aluminum form highly stable oxide layers (Y{sub 2}O{sub 3} and Al{sub 2}O{sub 3}), which can get incorporated in the growing Fe-oxide layer to form an impervious complex oxide to enhance corrosion resistance. Task 4: Study of flow-assisted corrosion of select alloys in supercritical CO{sub 2} under a selected set of test conditions: To study the effects of flow-assisted corrosion, tests will be conducted in a supercritical CO{sub 2} flow loop. An existing facility used for supercritical water flow studies at the proposing university will be modified for use in this task. The system is capable of flow velocities up to 10 m/s and can operate at temperatures and pressures of up to 650°C and 20 MPa, respectively. All above tasks will be performed in conjunction with detailed materials characterization and analysis using scanning electron microscopy/energy dispersive spectroscopy (SEM-EDS), x-ray diffraction (XRD), Auger electron spectroscopy (AES) techniques, and weight change measurements. Inlet and outlet gas compositions will be monitored using gas chromatography-mass spectrometry (GCMS).« less

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

PubMed

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

2017-11-30

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

Low Temperature Thermodynamic Equilibrium of CO2 Dimer Anion Species in Cryogenic Argon and Krypton Matrices

NASA Astrophysics Data System (ADS)

Goodrich, Michael E.; Moore, David T.

2016-06-01

The separated CO2 dimer anion, (CO2)(CO2-), is observed by FTIR spectroscopy in matrix isolation experiments at 1652 cm-1 upon deposition of high energy argon ions into an argon matrix doped with 0.5% CO2. It has previously been reported by Andrews that upon annealing the matrix to 25K, the separated species converts to an oxalate-like C2O4- species which appears at 1856 cm-1.a We have observed that subsequently holding the matrix at 10K caused the C2O4- species to fully convert back to (CO2)(CO2-). Upon further investigation, we determined that the two species reversibly interconvert between 19K and 23K, suggesting the species are in thermodynamic equilibrium. The associated van't Hoff plot has a linear trend and indicates an endothermic reaction driven by a large increase in entropy. An analogous experiment in a krypton matrix was performed, and the equilibrium was found to occur between 26K and 31K. Interestingly, analysis revealed the reaction in krypton is more endothermic, but has nearly the same entropy value as was observed in the argon experiment. aZhou, M.; Andrews, L.; J. Chem. Phys. 110, 2414 (1999).

Room-Temperature Synthesis of Two-Dimensional Metal–Organic Frameworks with Controllable Size and Functionality for Enhanced CO 2 Sorption

DOE PAGES

Zha, Jie; Zhang, Xueyi

2018-04-17

Here, two-dimensional (2D) metal-organic frameworks (MOFs), as a newly emerged member of 2D materials, have gained extensive attention due to their great potential in gas separation, sensing, and catalysis. However, it is still challenging to synthesize 2D MOFs with controllable size and functionalities using direct and scalable approaches at mild conditions (e.g., room temperature). Herein, we demonstrated onestep, room-temperature synthesis of a series of 2D MOFs based on Cu(II) paddle-wheel units, where the intrinsically anisotropic building blocks led to the anisotropic growth of 2D MOF nanoparticles, and the pillared structure led to high surface areas. The size of 2D MOFsmore » can be adjusted by using a DMF/H 2O mixed solvent. The thinnest particles were around 3 nm, and the highest aspect ratio was up to 200. The functionalization of 2D MOFs was also achieved by selecting ligands with desired functional groups. The gas sorption results revealed that amino and nitro-functionalized 2D MOFs showed higher CO 2 sorption selectivity over CH 4 and N 2, suggesting these materials can be further applied in natural gas sweetening (CO 2/CH 4 separation) and carbon capture from flue gas (CO 2/N 2 separation).« less

Room-Temperature Synthesis of Two-Dimensional Metal–Organic Frameworks with Controllable Size and Functionality for Enhanced CO 2 Sorption

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

Zha, Jie; Zhang, Xueyi

Here, two-dimensional (2D) metal-organic frameworks (MOFs), as a newly emerged member of 2D materials, have gained extensive attention due to their great potential in gas separation, sensing, and catalysis. However, it is still challenging to synthesize 2D MOFs with controllable size and functionalities using direct and scalable approaches at mild conditions (e.g., room temperature). Herein, we demonstrated onestep, room-temperature synthesis of a series of 2D MOFs based on Cu(II) paddle-wheel units, where the intrinsically anisotropic building blocks led to the anisotropic growth of 2D MOF nanoparticles, and the pillared structure led to high surface areas. The size of 2D MOFsmore » can be adjusted by using a DMF/H 2O mixed solvent. The thinnest particles were around 3 nm, and the highest aspect ratio was up to 200. The functionalization of 2D MOFs was also achieved by selecting ligands with desired functional groups. The gas sorption results revealed that amino and nitro-functionalized 2D MOFs showed higher CO 2 sorption selectivity over CH 4 and N 2, suggesting these materials can be further applied in natural gas sweetening (CO 2/CH 4 separation) and carbon capture from flue gas (CO 2/N 2 separation).« less

Fabrication of Heterogeneous-Phase Solid-Solution Promoting Band Structure and Charge Separation for Enhancing Photocatalytic CO2 Reduction: A Case of ZnXCa1-XIn2S4.

PubMed

Zeng, Chao; Huang, Hongwei; Zhang, Tierui; Dong, Fan; Zhang, Yihe; Hu, Yingmo

2017-08-23

Photocatalytic CO 2 reduction into solar fuels illustrates huge charm for simultaneously settling energy and environmental issues. The photoreduction ability of a semiconductor is closely correlated to its conduction band (CB) position. A homogeneous-phase solid-solution with the same crystal system always has a monotonously changed CB position, and the high CB level has to be sacrificed to achieve a benign photoabsorption. Herein, we report the fabrication of heterogeneous-phase solid-solution Zn X Ca 1-X In 2 S 4 between trigonal ZnIn 2 S 4 and cubic CaIn 2 S 4 . The Zn X Ca 1-X In 2 S 4 solid solutions with orderly tuned photoresponsive range from 540 to 640 nm present a more negative CB level and highly enhanced charge-separation efficiency. Profiting from these merits, all of these Zn X Ca 1-X In 2 S 4 solid solutions exhibit remarkably strengthened photocatalytic CO 2 reduction performance under visible light (λ > 420 nm) irradiation. Zn 0.4 Ca 0.6 In 2 S 4 , bearing the most negative CB position and highest charge-separation efficiency, casts the optimal photocatalytic CH 4 and CO evolution rates, which reach 16.7 and 6.8 times higher than that of ZnIn 2 S 4 and 7.2 and 3.9 times higher than that of CaIn 2 S 4 , respectively. To verify the crucial role of the heterogeneous-phase solid solution in promoting the band structure and photocatalytic performance, another heterogeneous-phase solid-solution Zn X Cd 1-X In 2 S 4 has been synthesized. It also displays an upshifted CB level and promoted charge separation. This work may provide a new perspective into the development of an efficient visible-light driven photocatalyst for CO 2 reduction and other photoreduction reactions.

Open-cycle magnetohydrodynamic power plant with CO.sub.2 recycling

DOEpatents

Berry, Gregory F.

1991-01-01

A method of converting the chemical energy of fossil fuel to electrical and mechanical energy with a MHD generator. The fossil fuel is mixed with preheated oxygen and carbon dioxide and a conducting seed of potassium carbonate to form a combustive and electrically conductive mixture which is burned in a combustion chamber. The burned combustion mixture is passed through a MHD generator to generate electrical energy. The burned combustion mixture is passed through a diffuser to restore the mixture approximately to atmospheric pressure, leaving a spent combustion mixture which is used to heat oxygen from an air separation plant and recycled carbon dioxide for combustion in a high temperature oxygen preheater and for heating water/steam for producing superheated steam. Relatively pure carbon dioxide is separated from the spent combustion mixture for further purification or for exhaust, while the remainder of the carbon dioxide is recycled from the spent combustion mixture to a carbon dioxide purification plant for removal of water and any nitrous oxides present, leaving a greater than 98% pure carbon dioxide. A portion of the greater then 98% pure carbon dioxide stream is recovered and the remainder is recycled to combine with the oxygen for preheating and combination with the fossil fuel to form a combustion mixture.

Improving the Photo-Oxidative Performance of Bi2MoO6 by Harnessing the Synergy between Spatial Charge Separation and Rational Co-Catalyst Deposition.

PubMed

Wu, Xuelian; Hart, Judy N; Wen, Xiaoming; Wang, Liang; Du, Yi; Dou, Shi Xue; Ng, Yun Hau; Amal, Rose; Scott, Jason

2018-03-21

It has been reported that photogenerated electrons and holes can be directed toward specific crystal facets of a semiconductor particle, which is believed to arise from the differences in their surface electronic structures, suggesting that different facets can act as either photoreduction or photo-oxidation sites. This study examines the propensity for this effect to occur in faceted, plate-like bismuth molybdate (Bi 2 MoO 6 ), which is a useful photocatalyst for water oxidation. Photoexcited electrons and holes are shown to be spatially separated toward the {100} and {001}/{010} facets of Bi 2 MoO 6 , respectively, by facet-dependent photodeposition of noble metals (Pt, Au, and Ag) and metal oxides (PbO 2 , MnO x , and CoO x ). Theoretical calculations revealed that differences in energy levels between the conduction bands and valence bands of the {100} and {001}/{010} facets can contribute to electrons and holes being drawn to different surfaces of the plate-like Bi 2 MoO 6 . Utilizing this knowledge, the photo-oxidative capability of Bi 2 MoO 6 was improved by adding an efficient water oxidation co-catalyst, CoO x , to the system, whereby the extent of enhancement was shown to be governed by the co-catalyst location. A greater oxygen evolution occurred when CoO x was selectively deposited on the hole-rich {001}/{010} facets of Bi 2 MoO 6 compared to when CoO x was randomly located across all of the facets. The elevated performance exhibited for the selectively loaded CoO x /Bi 2 MoO 6 was ascribed to the greater opportunity for hole trapping by the co-catalyst being accentuated over other potentially detrimental effects, such as the co-catalyst acting as a recombination medium and/or covering reactive sites. The results indicate that harnessing the synergy between the spatial charge separation and the co-catalyst location on the appropriate facets of plate-like Bi 2 MoO 6 can promote its photocatalytic activity.

Geochemical Impacts of CO2 Intrusion into Ground Water due to Carbon Dioxide Release from Geologic Sequestration Projects: Overview of ORD Research

EPA Science Inventory

Abstract: Even with the large physical separation between storage reservoirs and surficial environments, there is concern that CO2 stored in reservoirs may eventually leak back to the surface through abandoned wells or along geological features such as faults. Leakage of CO2 into...

Flue gas adsorption on periodic mesoporous phenylene-silica: a DFT approach.

PubMed

Lourenço, Mirtha A O; Ferreira, Paula; Gomes, José R B

2018-06-20

Periodic mesoporous organosilicas (PMOs) were suggested as potential adsorbents for CO2/CH4 separation because of their large affinities towards CO2 and low interaction with CH4. Herewith, we present a comprehensive computational study on the binding properties of flue gas species with the pore walls of periodic mesoporous phenylene-silica (Ph-PMO) for understanding the possible impact of other gaseous species in the CO2/CH4 separation. The calculations considered three exchange-correlation functionals (PBE, PBE-D2 and M06-2X) based on the density functional theory and the walls of the periodic mesoporous phenylene-silica were modelled within the cluster model approach. The components of the flue gas considered were the diatomic CO, H2, N2, O2 and NO molecules, the triatomic CO2, H2O, H2S and SO2 species, the tetratomic SO3 and NH3 gases and the pentatomic CH4 molecule. The calculated data demonstrate that the presence of H2O, SO2, NH3, H2S and SO3 is a significant threat to CO2 capture by Ph-PMO and suggest that the Ph-PMO material would present high selectivity for CO2 over CH4, CO, H2 or N2 adsorption. The adsorption behaviour of flue gas components in Ph-PMO can be directly related to the experimental proton affinities, basicities or even the polarizabilities of the gaseous molecules.

CO2 microbubble contrast enhancement in x-ray angiography.

PubMed

Kariya, S; Komemushi, A; Nakatani, M; Yoshida, R; Sawada, S; Tanigawa, N

2013-04-01

To demonstrate that carbon dioxide (CO2) microbubble contrast enhancement depicts blood vessels when used for x-ray examinations. Microbubbles were generated by cavitation of physiological saline to which CO2 gas had been added using an ejector-type microbubble generator. The input pressure values for CO2 gas and physiological saline that produced a large quantity of CO2 microbubbles were obtained in a phantom. In an animal study, angiography was performed in three swine using three types of contrast: CO2 microbubbles, conventional CO2 gas, and iodinated contrast medium. For CO2 microbubble contrast enhancement, physiological saline, and CO2 gas were supplied at the input pressures calculated in the phantom experiment. Regions of interest were set in the abdominal aorta, external iliac arteries, and background. The difference in digital values between each artery and the background was calculated. The input pressures obtained in the phantom experiment were 0.16 MPa for physiological saline and 0.5 MPa for CO2 gas, with physiological saline input volume being 8.1 ml/s. Three interventional radiologists all evaluated the depictions of all arteries as "present" in the CO2 microbubble contrast enhancement, conventional CO2 contrast enhancement, and iodinated contrast enhancement performed in three swine. Digital values for all vessels with microbubble CO2 contrast enhancement were higher than background values. In x-ray angiography, blood vessels can be depicted by CO2 microbubble contrast enhancement, in which a large quantity of CO2 microbubbles is generated within blood vessels. Copyright © 2012 The Royal College of Radiologists. Published by Elsevier Ltd. All rights reserved.

Environmentally-friendly oxygen-free roasting/wet magnetic separation technology for in situ recycling cobalt, lithium carbonate and graphite from spent LiCoO2/graphite lithium batteries.

PubMed

Li, Jia; Wang, Guangxu; Xu, Zhenming

2016-01-25

The definite aim of the present paper is to present some novel methods that use oxygen-free roasting and wet magnetic separation to in situ recycle of cobalt, Lithium Carbonate and Graphite from mixed electrode materials. The in situ recycling means to change waste into resources by its own components, which is an idea of "waste+waste→resources." After mechanical scraping the mixed electrode materials enrich powders of LiCoO2 and graphite. The possible reaction between LiCoO2 and graphite was obtained by thermodynamic analysis. The feasibility of the reaction at high temperature was studied with the simultaneous thermogravimetry analysis under standard atmospheric pressure. Then the oxygen-free roasting/wet magnetic separation method was used to transfer the low added value mixed electrode materials to high added value products. The results indicated that, through the serious technologies of oxygen-free roasting and wet magnetic separation, mixture materials consist with LiCoO2 and graphite powders are transferred to the individual products of cobalt, Lithium Carbonate and Graphite. Because there is not any chemical solution added in the process, the cost of treating secondary pollution can be saved. This study provides a theoretical basis for industrial-scale recycling resources from spent LIBs. Copyright © 2015 Elsevier B.V. All rights reserved.

Synthesis Strategies for Ultrastable Zeolite GIS Polymorphs as Sorbents for Selective Separations.

PubMed

Oleksiak, Matthew D; Ghorbanpour, Arian; Conato, Marlon T; McGrail, B Peter; Grabow, Lars C; Motkuri, Radha Kishan; Rimer, Jeffrey D

2016-11-02

Designing zeolites with tunable physicochemical properties can substantially impact their performance in commercial applications, such as adsorption, separations, catalysis, and drug delivery. Zeolite synthesis typically requires an organic structure-directing agent to produce crystals with specific pore topology. Attempts to remove organics from syntheses to achieve commercially viable methods of preparing zeolites often lead to the formation of impurities. Herein, we present organic-free syntheses of two polymorphs of the small-pore zeolite P (GIS), P1 and P2. Using a combination of adsorption measurements and density functional theory calculations, we show that GIS polymorphs are selective adsorbents for H 2 O relative to other light gases (e.g., H 2 , N 2 , CO 2 ). Our findings refute prior theoretical studies postulating that GIS-type zeolites are excellent materials for CO 2 separation/sequestration. We also show that P2 is significantly more thermally stable than P1, which broadens the operating conditions for GIS-type zeolites in commercial applications and opens new avenues for exploring their potential use in processes such as catalysis. © 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Microbial electrochemical separation of CO2 for biogas upgrading.

PubMed

Kokkoli, Argyro; Zhang, Yifeng; Angelidaki, Irini

2018-01-01

Biogas upgrading to natural gas quality has been under focus the recent years for increasing the utilization potential of biogas. Conventional methods for CO 2 removal are expensive and have environmental challenges, such as increased emissions of methane in the atmosphere with serious greenhouse impact. In this study, an innovative microbial electrochemical separation cell (MESC) was developed to in-situ separate and regenerate CO 2 via alkali and acid regeneration. The MESC was tested under different applied voltages, inlet biogas rates and electrolyte concentrations. Pure biomethane was obtained at 1.2V, inlet biogas rate of 0.088mL/h/mL reactor and NaCl concentration of 100mM at a 5-day operation. Meanwhile, the organic matter of the domestic wastewater in the anode was almost completely removed at the end. The study demonstrated a new sustainable way to simultaneously upgrade biogas and treat wastewater which can be used as proof of concept for further investigation. Copyright © 2017 Elsevier Ltd. All rights reserved.

Effects of ZnO Nanoparticle on the Gas Separation Performance of Polyurethane Mixed Matrix Membrane

PubMed Central

Soltani, Banafsheh

2017-01-01

Polyurethane (PU)-ZnO mixed matrix membranes (MMM) were fabricated and characterized for gas separation. A thermogravimetric analysis (TGA), a scanning electron microscope (SEM) test and an atomic-force microscopy (AFM) revealed that the physical properties and thermal stability of the membranes were improved through filler loading. Hydrogen Bonding Index, obtained from the Fourier transform infrared spectroscopy (FTIR), demonstrate that the degree of phase separation in PU-ZnO 0.5 wt % MMM was more than the neat PU, while in PU-ZnO 1.0 wt % MMM, the phase mixing had increased. Compared to the neat membrane, the CO2 permeability of the MMMs increased by 31% for PU-ZnO 0.5 wt % MMM and decreased by 34% for 1.0 wt % ZnO MMM. The CO2/CH4 and CO2/N2 selectivities of PU-ZnO 0.5 wt % were 18.75 and 64.75, respectively. PMID:28800109

Simultaneous separation of copper, cadmium and cobalt from sea-water by co-flotation with octadecylamine and ferric hydroxide as collectors.

PubMed

Cabezon, L M; Caballero, M; Cela, R; Perez-Bustamante, J A

1984-08-01

A method is proposed for the simultaneous quantitative separation of traces ofCu(II), Cd(II) and Co(II) from sea-water samples by means of the co-flotation (adsorbing colloid flotation) technique with ferric hydroxide as co-precipitant and octadecylamine as collector. The experimental parameters have been studied and optimized. The drawbacks arising from the low solubility of octadecylamine and the corresponding sublates in water have been avoided by use of a 6M hydrochloric acid-MIBK-ethanol (1:2:2 v v ) mixture. The results obtained by means of the proposed method have been compared with those given by the usual ammonium pyrrolidine dithiocarbamate/MIBK extraction method.

The artificial leaf.

PubMed

Nocera, Daniel G

2012-05-15

To convert the energy of sunlight into chemical energy, the leaf splits water via the photosynthetic process to produce molecular oxygen and hydrogen, which is in a form of separated protons and electrons. The primary steps of natural photosynthesis involve the absorption of sunlight and its conversion into spatially separated electron-hole pairs. The holes of this wireless current are captured by the oxygen evolving complex (OEC) of photosystem II (PSII) to oxidize water to oxygen. The electrons and protons produced as a byproduct of the OEC reaction are captured by ferrodoxin of photosystem I. With the aid of ferrodoxin-NADP(+) reductase, they are used to produce hydrogen in the form of NADPH. For a synthetic material to realize the solar energy conversion function of the leaf, the light-absorbing material must capture a solar photon to generate a wireless current that is harnessed by catalysts, which drive the four electron/hole fuel-forming water-splitting reaction under benign conditions and under 1 sun (100 mW/cm(2)) illumination. This Account describes the construction of an artificial leaf comprising earth-abundant elements by interfacing a triple junction, amorphous silicon photovoltaic with hydrogen- and oxygen-evolving catalysts made from a ternary alloy (NiMoZn) and a cobalt-phosphate cluster (Co-OEC), respectively. The latter captures the structural and functional attributes of the PSII-OEC. Similar to the PSII-OEC, the Co-OEC self-assembles upon oxidation of an earth-abundant metal ion from 2+ to 3+, may operate in natural water at room temperature, and is self-healing. The Co-OEC also activates H(2)O by a proton-coupled electron transfer mechanism in which the Co-OEC is increased by four hole equivalents akin to the S-state pumping of the Kok cycle of PSII. X-ray absorption spectroscopy studies have established that the Co-OEC is a structural relative of Mn(3)CaO(4)-Mn cubane of the PSII-OEC, where Co replaces Mn and the cubane is extended in a corner-sharing, head-to-tail dimer. The ability to perform the oxygen-evolving reaction in water at neutral or near-neutral conditions has several consequences for the construction of the artificial leaf. The NiMoZn alloy may be used in place of Pt to generate hydrogen. To stabilize silicon in water, its surface is coated with a conducting metal oxide onto which the Co-OEC may be deposited. The net result is that immersing a triple-junction Si wafer coated with NiMoZn and Co-OEC in water and holding it up to sunlight can effect direct solar energy conversion via water splitting. By constructing a simple, stand-alone device composed of earth-abundant materials, the artificial leaf provides a means for an inexpensive and highly distributed solar-to-fuels system that employs low-cost systems engineering and manufacturing. Through this type of system, solar energy can become a viable energy supply to those in the non-legacy world.

Transition from the diamagnetic insulator to ferromagnetic metal in La1-xSrxCoO3

NASA Astrophysics Data System (ADS)

Knížek, Karel; Jirák, Zdeněk; Hejtmánek, Jiří; Novák, Pavel

2010-05-01

We have analyzed, using the theoretical GGA+U calculations, different configurations of spin states (low-spin, LS; intermediate-spin, IS and high-spin, HS Co) and proposed a model that accounts for magnetic and electric transport properties of perovskite cobaltites upon doping by charge carriers. In particular, it appears that the compositional transition from the diamagnetic LS phase of LaCoO3 to the ferromagnetic metallic IS phase in La1-xSrxCoO3 ( x>0.2) involves the same mechanisms as the high-temperature transition in pure LaCoO3. The process occurs gradually via a phase-separated state, where metallic IS domains stabilized through a charge transfer between Co and Co neighbors coexist with the Co poor regions in the LS ground state (or at higher temperatures, in mixed LS/HS state). This phase separation vanishes when doping in La1-xSrxCoO3 reaches x˜0.2, and a uniform IS phase, analogous to that in pure LaCoO3 in the high-temperature limit, is established.

Physical study on Cobalt-Indium Co-doped ZnO nanofilms as hydrophobic surfaces

NASA Astrophysics Data System (ADS)

Mimouni, R.; Mahdhi, N.; Boubaker, K.; Madouri, A.; Amlouk, M.

2016-03-01

The present work reports some physical investigations on (Co,In) codoped zinc oxide nanofilms deposited on glass substrates at 460 °C by the spray pyrolysis technique. The effect of Co and In concentration on the structural, morphological, optical and surface wettability properties have been investigated using X-ray diffraction (XRD) patterns, Raman spectroscopy, SEM, optical measurement, photoluminescence spectroscopy as well as the measurement of hydrophobicity in terms of water contact angle. It is found that all films crystallized in würtzite ZnO phase, with a preferentially orientation towards (002) direction parallel to c-axis. The Raman spectra of the samples exhibit the presence of E2high characteristic mode of würtzite structure with high crystallinity as well as two dominant bands 1LO and 2LO. Also, no additional modes introduced by codopoing have been found. SEM micrographs show the uniform deposition of fine grains on surface films. Thicknesses of films are less than 100 nm. In addition, optical investigations indicate that the band gap narrowing of (Co,In) codoped ZnO thin films is due to the increase in the band tail width. Indeed, PL study indicates that (Co,In) codoped ZnO nanofilms exhibit a large decrease of the UV luminescence, which is assigned to the trapping of photo-generated electrons by both In3+ and Co2+ ions as well as an improvement of charge separation in the ZnO thin films. Finally, the (Co,In) codoping influences the surface wettability property and transform the ZnO character from hydrophilic (θ < 90°) for pure ZnO nanofilm to hydrophobic (θ > 90°) for (Co,In) codoped ZnO ones.

Combining XCO2 Measurements Derived from SCIAMACHY and GOSAT for Potentially Generating Global CO2 Maps with High Spatiotemporal Resolution

PubMed Central

Wang, Tianxing; Shi, Jiancheng; Jing, Yingying; Zhao, Tianjie; Ji, Dabin; Xiong, Chuan

2014-01-01

Global warming induced by atmospheric CO2 has attracted increasing attention of researchers all over the world. Although space-based technology provides the ability to map atmospheric CO2 globally, the number of valid CO2 measurements is generally limited for certain instruments owing to the presence of clouds, which in turn constrain the studies of global CO2 sources and sinks. Thus, it is a potentially promising work to combine the currently available CO2 measurements. In this study, a strategy for fusing SCIAMACHY and GOSAT CO2 measurements is proposed by fully considering the CO2 global bias, averaging kernel, and spatiotemporal variations as well as the CO2 retrieval errors. Based on this method, a global CO2 map with certain UTC time can also be generated by employing the pattern of the CO2 daily cycle reflected by Carbon Tracker (CT) data. The results reveal that relative to GOSAT, the global spatial coverage of the combined CO2 map increased by 41.3% and 47.7% on a daily and monthly scale, respectively, and even higher when compared with that relative to SCIAMACHY. The findings in this paper prove the effectiveness of the combination method in supporting the generation of global full-coverage XCO2 maps with higher temporal and spatial sampling by jointly using these two space-based XCO2 datasets. PMID:25119468

Ultraselective Carbon Molecular Sieve Membranes with Tailored Synergistic Sorption Selective Properties.

PubMed

Zhang, Chen; Koros, William J

2017-09-01

Membrane-based separations can reduce the energy consumption and the CO 2 footprint of large-scale fluid separations, which are traditionally practiced by energy-intensive thermally driven processes. Here, a new type of membrane structure based on nanoporous carbon is reported, which, according to this study, is best referred to as carbon/carbon mixed-matrix (CCMM) membranes. The CCMM membranes are formed by high-temperature (up to 900 °C) pyrolysis of polyimide precursor hollow-fiber membranes. Unprecedentedly high permselectivities are seen in CCMM membranes for CO 2 /CH 4 , N 2 /CH 4 , He/CH 4 , and H 2 /CH 4 separations. Analysis of permeation data suggests that the ultrahigh selectivities result from substantially increased sorption selectivities, which is hypothetically owing to the formation of ultraselective micropores that selectively exclude the bulkier CH 4 molecules. With tunable sorption selectivities, the CCMM membranes outperform flexible polymer membranes and traditional rigid molecular-sieve membranes. The capability to increase sorption selectivities is a powerful tool to leverage diffusion selectivities, and has opened the door to many challenging and economically important fluid separations that require ultrafine differentiation of closely sized molecules. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Native defects in silver orthophosphate and their effects on photocatalytic activity under visible light irradiation

NASA Astrophysics Data System (ADS)

Sulaeman, Uyi; Hermawan, Dadan; Andreas, Roy; Abdullah, Ahmad Zuhairi; Yin, Shu

2018-01-01

Native defects in silver orthophosphate could be generated by simple co-precipitation method under ethanol-aqueous solution using AgNO3 and Na2HPO4.12H2O. AgNO3 ethanol-aqueous solution with the ethanol contents of 0%, 25%, 50%, 75%, 90% and 100% was reacted with Na2HPO4 aqueous solution. The produced catalysts were characterized using XRD, DRS, FE-SEM, BET specific surface area and XPS. The increase of ethanol content in the synthesis process decreased the Ag/P atomic ratio of Ag3PO4. The native defects of silver vacancy might be generated on the surface of Ag3PO4. The activity of Ag3PO4 for Rhodamine B degradation dramatically increased by 5.8 times higher compared to that of the pristine Ag3PO4. The defect states of Ag vacancies enhanced the separation of electron-hole pairs, leading to the improvement of photocatalytic activity.

Combination of supercritical CO2 and vacuum distillation for the fractionation of bergamot oil.

PubMed

Fang, Tao; Goto, Motonobu; Sasaki, Mitsuru; Hirose, Tsutomu

2004-08-11

Supercritical CO2 can be used to separate oxygenated compounds from essential oils. This technique still cannot replace vacuum distillation as an industrial process because of low recoveries and inconsistent results. In the present work, a comparison between the two methods was made in terms of composition, recovery, and color. Vacuum distillation and supercritical CO2 are complementary processes for producing high quality oxygenated compounds with high recovery rates. The former is more suitable for removing monoterpenes at low fraction temperatures (< or =308 K), and the latter is more suitable for separating oxygenated compounds from pigments and waxes. Consequently, the two methods were combined. For supercritical CO2 fractionation, the parameters of pressure, temperature gradient, and the ratio of solvent to feed were investigated for the fractionation of oxygenated compounds with high recoveries (> or =85%) and without other macromolecules, such as pigments and waxes.

Continuous Processing With Mars Gases

NASA Technical Reports Server (NTRS)

Parrish, Clyde; Jennings, Paul

2000-01-01

Current Martian missions call for the production of oxygen for breathing, and fuel and oxygen for propulsion to be produced from atmospheric carbon dioxide (CO2). Adsorption and freezing are the two methods considered for capturing CO2 from the atmosphere. However, the nitrogen (N2) and argon (Ar), which make up less than 5 percent of the atmosphere, cause difficulties with both of these processes by blocking the CO2. This results in the capture process rapidly changing from a pressure driven process to a diffusion controlled process. To increase the CO2 capture rates, some type of mechanical pump is usually proposed to remove the N2 and Ar. The N2 and Ar are useful and have been proposed for blanketing and pressurizing fuel tanks and as buffer gas for breathing air for manned missions. Separation of the Martian gases with the required purity can be accomplished with a combination of membranes. These membrane systems do not require a high feed pressure and provide suitable separation. Therefore, by use of the appropriate membrane combination with the Martian atmosphere supplied by a compressor a continuous Supply Of CO2 for fuel and oxygen production can be supplied. This phase of our program has focused on the selection of the membrane system. Since permeation data for membranes did not exist for Martian atmospheric pressures and temperatures, this information had to be compiled. The general trend as the temperature was lowered was for the membranes to become more selective. In addition, the relative permeation rates between the three gases changed with temperature. The end result was to provide design parameters that could be used to separate CO2 from N2 and Ar. This paper will present the membrane data, provide the design requirements for a compressor, and compare the results with adsorption and freezer methods.

Selectivity trend of gas separation through nanoporous graphene

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

Liu, Hongjun; Chen, Zhongfang; Dai, Sheng

2015-04-15

By means of molecular dynamics (MD) simulations, we demonstrate that porous graphene can efficiently separate gases according to their molecular sizes. The flux sequence from the classical MD simulation is H{sub 2}>CO{sub 2}≫N{sub 2}>Ar>CH{sub 4}, which generally follows the trend in the kinetic diameters. This trend is also confirmed from the fluxes based on the computed free energy barriers for gas permeation using the umbrella sampling method and kinetic theory of gases. Both brute-force MD simulations and free-energy calcualtions lead to the flux trend consistent with experiments. Case studies of two compositions of CO{sub 2}/N{sub 2} mixtures further demonstrate themore » separation capability of nanoporous graphene. - Graphical abstract: Classical molecular dynamics simulations show the flux trend of H{sub 2}>CO{sub 2}≫N{sub 2}>Ar>CH{sub 4} for their permeation through a porous graphene, in excellent agreement with a recent experiment. - Highlights: • Classical MD simulations show the flux trend of H{sub 2}>CO{sub 2}≫N{sub 2}>Ar>CH{sub 4} for their permeation through a porous graphene. • Free energy calculations yield permeation barriers for those gases. • Selectivities for several gas pairs are estimated from the free-energy barriers and the kinetic theory of gases. • The selectivity trend is in excellent agreement with a recent experiment.« less

A dye-sensitized photoelectrochemical tandem cell for light driven hydrogen production from water

DOE PAGES

Sherman, Benjamin D.; Sheridan, Matthew V.; Wee, Kyung -Ryang; ...

2016-12-02

Here, tandem junction photoelectrochemical water-splitting devices, whereby two light absorbing electrodes targeting separate portions of the solar spectrum generate the voltage required to convert water to oxygen and hydrogen, enable much higher possible efficiencies than single absorber systems. We report here on the development of a tandem system consisting of a dye-sensitized photoelectrochemical cell (DSPEC) wired in series with a dye-sensitized solar cell (DSC). The DSPEC photoanode incorporates a tris(bipyridine)ruthenium(II)-type chromophore and molecular ruthenium based water oxidation catalyst. The DSPEC was tested with two more-red absorbing DSC variations, one utilizing N719 dye with an I 3 –/I – redox mediatormore » solution and the other D35 dye with a tris(bipyridine)cobalt ([Co(bpy) 3] 3+/2+) based mediator. The tandem configuration consisting of the DSPEC and D35/[Co(bpy) 3] 3+/2+ based DSC gave the best overall performance and demonstrated the production of H 2 from H 2O with the only energy input from simulated solar illumination.« less

The model of nano-scale copper particle removal from silicon surface in high pressure CO2 + H2O and CO2 + H2O + IPA cleaning solutions.

PubMed

Tan, Xin; Chai, Jiajue; Zhang, Xiaogang; Chen, Jiawei

2011-12-01

This study focuses on the description of the static forces in CO2-H2O and CO2-H2O-IPA cleaning solutions with a separate fluid phase entrapped between nano-scale copper particles and a silicon surface. Calculations demonstrate that increasing the pressure of the cleaning system decreases net adhesion force (NAF) between the particle and silicon. The NAF of a particle for in CO2-H2O-IPA system is less than that in CO2-H2O system, suggesting that the particles enter into bulk layer more easily as the CO2-H2O cleaning system is added IPA.

Inherent variations in CO-H2S-mediated carotid body O2 sensing mediate hypertension and pulmonary edema

PubMed Central

Peng, Ying-Jie; Makarenko, Vladislav V.; Nanduri, Jayasri; Vasavda, Chirag; Raghuraman, Gayatri; Yuan, Guoxiang; Gadalla, Moataz M.; Kumar, Ganesh K.; Snyder, Solomon H.; Prabhakar, Nanduri R.

2014-01-01

Oxygen (O2) sensing by the carotid body and its chemosensory reflex is critical for homeostatic regulation of breathing and blood pressure. Humans and animals exhibit substantial interindividual variation in this chemosensory reflex response, with profound effects on cardiorespiratory functions. However, the underlying mechanisms are not known. Here, we report that inherent variations in carotid body O2 sensing by carbon monoxide (CO)-sensitive hydrogen sulfide (H2S) signaling contribute to reflex variation in three genetically distinct rat strains. Compared with Sprague-Dawley (SD) rats, Brown-Norway (BN) rats exhibit impaired carotid body O2 sensing and develop pulmonary edema as a consequence of poor ventilatory adaptation to hypobaric hypoxia. Spontaneous Hypertensive (SH) rat carotid bodies display inherent hypersensitivity to hypoxia and develop hypertension. BN rat carotid bodies have naturally higher CO and lower H2S levels than SD rat, whereas SH carotid bodies have reduced CO and greater H2S generation. Higher CO levels in BN rats were associated with higher substrate affinity of the enzyme heme oxygenase 2, whereas SH rats present lower substrate affinity and, thus, reduced CO generation. Reducing CO levels in BN rat carotid bodies increased H2S generation, restoring O2 sensing and preventing hypoxia-induced pulmonary edema. Increasing CO levels in SH carotid bodies reduced H2S generation, preventing hypersensitivity to hypoxia and controlling hypertension in SH rats. PMID:24395806

Enhanced selective photocatalytic reduction of CO2 to CH4 over plasmonic Au modified g-C3N4 photocatalyst under UV-vis light irradiation

NASA Astrophysics Data System (ADS)

Li, Hailong; Gao, Yan; Xiong, Zhuo; Liao, Chen; Shih, Kaimin

2018-05-01

A series of Au-g-C3N4 (Au-CN) catalysts were prepared through a NaBH4-reduction method using g-C3N4 (CN) from pyrolysis of urea as precursor. The catalysts' surface area, crystal structure, surface morphology, chemical state, functional group composition and optical properties were characterized by X-ray diffraction, transmission electron microscope, X-ray photoelectron spectroscopy, ultraviolet visible (UV-vis) diffuse reflectance spectra, fourier transform infrared, photoluminescence and transient photocurrent analysis. The carbon dioxide (CO2) photoreduction activities under ultraviolet visible (UV-vis) light irradiation were significantly enhanced when gold (Au) was loaded on the surface of CN. 2Au-CN catalyst with Au to CN mole ratio of 2% showed the best catalytic activity. After 2 h UV-vis light irradiation, the methane (CH4) yield over the 2Au-CN catalyst was 9.1 times higher than that over the pure CN. The CH4 selectivity also greatly improved for the 2Au-CN compared to the CN. The deposited Au nanoparticles facilitated the separation of electron-hole pairs on the CN surface. Moreover, the surface plasmon resonance effect of Au further promoted the generation of hot electrons and visible light absorption. Therefore, Au loading significantly improved CO2 photoreduction performance of CN under UV-vis light irradiation.

Detection of co-eluted peptides using database search methods

PubMed Central

Alves, Gelio; Ogurtsov, Aleksey Y; Kwok, Siwei; Wu, Wells W; Wang, Guanghui; Shen, Rong-Fong; Yu, Yi-Kuo

2008-01-01

Background Current experimental techniques, especially those applying liquid chromatography mass spectrometry, have made high-throughput proteomic studies possible. The increase in throughput however also raises concerns on the accuracy of identification or quantification. Most experimental procedures select in a given MS scan only a few relatively most intense parent ions, each to be fragmented (MS2) separately, and most other minor co-eluted peptides that have similar chromatographic retention times are ignored and their information lost. Results We have computationally investigated the possibility of enhancing the information retrieval during a given LC/MS experiment by selecting the two or three most intense parent ions for simultaneous fragmentation. A set of spectra is created via superimposing a number of MS2 spectra, each can be identified by all search methods tested with high confidence, to mimick the spectra of co-eluted peptides. The generated convoluted spectra were used to evaluate the capability of several database search methods – SEQUEST, Mascot, X!Tandem, OMSSA, and RAId_DbS – in identifying true peptides from superimposed spectra of co-eluted peptides. We show that using these simulated spectra, all the database search methods will gain eventually in the number of true peptides identified by using the compound spectra of co-eluted peptides. Open peer review Reviewed by Vlad Petyuk (nominated by Arcady Mushegian), King Jordan and Shamil Sunyaev. For the full reviews, please go to the Reviewers' comments section. PMID:18597684

A gas trapping method for high-throughput metabolic experiments.

PubMed

Krycer, James R; Diskin, Ciana; Nelson, Marin E; Zeng, Xiao-Yi; Fazakerley, Daniel J; James, David E

2018-01-01

Research into cellular metabolism has become more high-throughput, with typical cell-culture experiments being performed in multiwell plates (microplates). This format presents a challenge when trying to collect gaseous products, such as carbon dioxide (CO2), which requires a sealed environment and a vessel separate from the biological sample. To address this limitation, we developed a gas trapping protocol using perforated plastic lids in sealed cell-culture multiwell plates. We used this trap design to measure CO2 production from glucose and fatty acid metabolism, as well as hydrogen sulfide production from cysteine-treated cells. Our data clearly show that this gas trap can be applied to liquid and solid gas-collection media and can be used to study gaseous product generation by both adherent cells and cells in suspension. Since our gas traps can be adapted to multiwell plates of various sizes, they present a convenient, cost-effective solution that can accommodate the trend toward high-throughput measurements in metabolic research.

Isolation, observation, and computational modeling of proposed intermediates in catalytic proton reductions with the hydrogenase mimic Fe2(CO)6S2C6H4.

PubMed

Wright, Robert J; Zhang, Wei; Yang, Xinzheng; Fasulo, Meg; Tilley, T Don

2012-01-07

Proposed electrocatalytic proton reduction intermediates of hydrogenase mimics were synthesized, observed, and studied computationally. A new mechanism for H(2) generation appears to involve Fe(2)(CO)(6)(1,2-S(2)C(6)H(4)) (3), the dianions {[1,2-S(2)C(6)H(4)][Fe(CO)(3)(μ-CO)Fe(CO)(2)](2-) (3(2-)), the bridging hydride {[1,2-S(2)C(6)H(4)][Fe(CO)(3)(μ-CO)(μ-H)Fe(CO)(2)]}(-), 3H(-)(bridging), and the terminal hydride 3H(-)(term-stag), {[1,2-S(2)C(6)H(4)][HFe(CO)(3)Fe(CO)(3)]}(-), as intermediates. The dimeric sodium derivative of 3(2-), {[Na(2)(THF)(OEt(2))(3)][3(2-)]}(2) (4) was isolated from reaction of Fe(2)(CO)(6)(1,2-S(2)C(6)H(4)) (3) with excess sodium and was characterized by X-ray crystallography. It possesses a bridging CO and an unsymmetrically bridging dithiolate ligand. Complex 4 reacts with 4 equiv. of triflic or benzoic acid (2 equiv. per Fe center) to generate H(2) and 3 in 75% and 60% yields, respectively. Reaction of 4 with 2 equiv. of benzoic acid generated two hydrides in a 1.7 : 1 ratio (by (1)H NMR spectroscopy). Chemical shift calculations on geometry optimized structures of possible hydride isomers strongly suggest that the main product, 3H(-)(bridging), possesses a bridging hydride ligand, while the minor product is a terminal hydride, 3H(-)(term-stag). Computational studies support a catalytic proton reduction mechanism involving a two-electron reduction of 3 that severs an Fe-S bond to generate a dangling thiolate and an electron rich Fe center. The latter iron center is the initial site of protonation, and this event is followed by protonation at the dangling thiolate to give the thiol thiolate [Fe(2)H(CO)(6)(1,2-SHSC(6)H(4))]. This species then undergoes an intramolecular acid-base reaction to form a dihydrogen complex that loses H(2) and regenerates 3.

Magnetically separable Prussian blue analogue Mn₃[Co(CN)₆]₂·nH₂O porous nanocubes as excellent absorbents for heavy metal ions.

PubMed

Hu, Lin; Mei, Ji-Yang; Chen, Qian-Wang; Zhang, Ping; Yan, Nan

2011-10-05

The application of Prussian blue analogue (PBA) Mn(3)[Co(CN)(6)](2)·nH(2)O porous nanocubes as absorbents for heavy metal ions has been demonstrated. The result indicates that Mn(3)[Co(CN)(6)](2)·nH(2)O porous nanocubes with average diameter of 240 nm possess excellent adsorption efficiency for Pb(2+) ions (94.21% at initial Pb(2+) concentration of 10 mg L(-1)). Moreover, Mn(3)[Co(CN)(6)](2)·nH(2)O porous nanocubes can also show high adsorption efficiency on heavy metal ions even in a strong acidic solution due to its chemical stability. Notably, an external magnet could be used to accelerate the separation of Mn(3)[Co(CN)(6)](2)·nH(2)O from the treated solution. It is suggested that the high adsorption efficiency may derive from the large surface area, M(3)(II)[M(III)(CN)(6)](2)·nH(2)O porous framework structure and affinity between polarizable π-electron clouds of the cyanide bridges and heavy metals ions.

Energetic valorization of wood waste: estimation of the reduction in CO2 emissions.

PubMed

Vanneste, J; Van Gerven, T; Vander Putten, E; Van der Bruggen, B; Helsen, L

2011-09-01

This paper investigates the potential CO(2) emission reductions related to a partial switch from fossil fuel-based heat and electricity generation to renewable wood waste-based systems in Flanders. The results show that valorization in large-scale CHP (combined heat and power) systems and co-firing in coal plants have the largest CO(2) reduction per TJ wood waste. However, at current co-firing rates of 10%, the CO(2) reduction per GWh of electricity that can be achieved by co-firing in coal plants is five times lower than the CO(2) reduction per GWh of large-scale CHP. Moreover, analysis of the effect of government support for co-firing of wood waste in coal-fired power plants on the marginal costs of electricity generation plants reveals that the effect of the European Emission Trading Scheme (EU ETS) is effectively counterbalanced. This is due to the fact that biomass integrated gasification combined cycles (BIGCC) are not yet commercially available. An increase of the fraction of coal-based electricity in the total electricity generation from 8 to 10% at the expense of the fraction of gas-based electricity due to the government support for co-firing wood waste, would compensate entirely for the CO(2) reduction by substitution of coal by wood waste. This clearly illustrates the possibility of a 'rebound' effect on the CO(2) reduction due to government support for co-combustion of wood waste in an electricity generation system with large installed capacity of coal- and gas-based power plants, such as the Belgian one. Copyright © 2011 Elsevier B.V. All rights reserved.

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

PubMed

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

2017-11-08

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

Stepwise observation and quantification and mixed matrix membrane separation of CO2 within a hydroxy-decorated porous host† †Electronic supplementary information (ESI) available. CCDC 1504685–1504693. See DOI: 10.1039/c6sc04343g Click here for additional data file. Click here for additional data file.

PubMed Central

Morris, Christopher G.; Jacques, Nicholas M.; Godfrey, Harry G. W.; Mitra, Tamoghna; Fritsch, Detlev; Lu, Zhenzhong; Murray, Claire A.; Potter, Jonathan; Cobb, Tom M.; Yuan, Fajin

2017-01-01

The identification of preferred binding domains within a host structure provides important insights into the function of materials. State-of-the-art reports mostly focus on crystallographic studies of empty and single component guest-loaded host structures to determine the location of guests. However, measurements of material properties (e.g., adsorption and breakthrough of substrates) are usually performed for a wide range of pressure (guest coverage) and/or using multi-component gas mixtures. Here we report the development of a multifunctional gas dosing system for use in X-ray powder diffraction studies on Beamline I11 at Diamond Light Source. This facility is fully automated and enables in situ crystallographic studies of host structures under (i) unlimited target gas loadings and (ii) loading of multi-component gas mixtures. A proof-of-concept study was conducted on a hydroxyl-decorated porous material MFM-300(VIII) under (i) five different CO2 pressures covering the isotherm range and (ii) the loading of equimolar mixtures of CO2/N2. The study has successfully captured the structural dynamics underpinning CO2 uptake as a function of surface coverage. Moreover, MFM-300(VIII) was incorporated in a mixed matrix membrane (MMM) with PIM-1 in order to evaluate the CO2/N2 separation potential of this material. Gas permeation measurements on the MMM show a great improvement over the bare PIM-1 polymer for CO2/N2 separation based on the ideal selectivity. PMID:28507700

Hydrogen separation through tailored dual phase membranes with nominal composition BaCe0.8Eu0.2O3-δ:Ce0.8Y0.2O2-δ at intermediate temperatures

NASA Astrophysics Data System (ADS)

Ivanova, Mariya E.; Escolástico, Sonia; Balaguer, Maria; Palisaitis, Justinas; Sohn, Yoo Jung; Meulenberg, Wilhelm A.; Guillon, Olivier; Mayer, Joachim; Serra, Jose M.

2016-11-01

Hydrogen permeation membranes are a key element in improving the energy conversion efficiency and decreasing the greenhouse gas emissions from energy generation. The scientific community faces the challenge of identifying and optimizing stable and effective ceramic materials for H2 separation membranes at elevated temperature (400-800 °C) for industrial separations and intensified catalytic reactors. As such, composite materials with nominal composition BaCe0.8Eu0.2O3-δ:Ce0.8Y0.2O2-δ revealed unprecedented H2 permeation levels of 0.4 to 0.61 mL·min-1·cm-2 at 700 °C measured on 500 μm-thick-specimen. A detailed structural and phase study revealed single phase perovskite and fluorite starting materials synthesized via the conventional ceramic route. Strong tendency of Eu to migrate from the perovskite to the fluorite phase was observed at sintering temperature, leading to significant Eu depletion of the proton conducing BaCe0.8Eu0.2O3-δ phase. Composite microstructure was examined prior and after a variety of functional tests, including electrical conductivity, H2-permeation and stability in CO2 containing atmospheres at elevated temperatures, revealing stable material without morphological and structural changes, with segregation-free interfaces and no further diffusive effects between the constituting phases. In this context, dual phase material based on BaCe0.8Eu0.2O3-δ:Ce0.8Y0.2O2-δ represents a very promising candidate for H2 separating membrane in energy- and environmentally-related applications.

Improved visible-light photocatalytic activity of TiO2 co-doped with copper and iodine

NASA Astrophysics Data System (ADS)

Dorraj, Masoumeh; Goh, Boon Tong; Sairi, Nor Asrina; Woi, Pei Meng; Basirun, Wan Jefrey

2018-05-01

Cu-I-co-doped TiO2 photocatalysts active to visible light absorption were prepared by hydrothermal method and calcined at various temperatures (350 °C, 450 °C, and 550 °C). The co-doped powders at 350 °C displayed the highest experimental Brunauer-Emmett-Teller surface area and lowest photoluminescence intensity, which demonstrated that a decrease in electron-hole recombination process. The synthesis of co-doped TiO2 was performed at this optimized temperature. In the co-doped sample, the Cu2+ doped TiO2 lattice created a major "red-shift" in the absorption edge due to the presence of the 3d Cu states, whereas the amount of red-shift from the I5+ doping in the TiO2 lattice was minor. Interestingly, the presence of Cu2+ species also boosted the reduction of I5+ ions to the lower multi-valance state I- in the TiO2 lattice by trapping the photogenerated electrons, which resulted in effective separation of the photogenerated charges. The Cu-I-co-doped TiO2 was able to degrade methyl orange dye under visible-light irradiation with improved photocatalytic activity compared with the single metal-doped TiO2 and pure TiO2 because of the strong visible light absorption and effective separation of photogenerated charges caused by the synergistic effects of Cu and I co-dopants.

CO2 Capture Project: An Integrated, Collaborative Technology Development Project For CO2 Separation, Capture And Geologic Sequestration

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

Helen Kerr

2002-01-10

This report (which forms part of the requirements of the Statement of Work Task 0, subtask 0.4) records progress towards defining a detailed Work Plan for the CCP 30 days after contract initiation. It describes the studies planned, workscope development and technology provider bid evaluation status at that time. Business sensitive information is provided separately in Appendix 1. Contract negotiations are on hold pending award of patent waiver status to the CCP.

Pulsed infrared difference frequency generation in CdGeAs.sub.2

DOEpatents

Piltch, Martin S.; Rink, John P.; Tallman, Charles R.

1977-03-08

The disclosure relates to a laser apparatus for generating a line-tunable pulsed infrared difference frequency output. The apparatus comprises a CO.sub.2 laser which produces a first frequency, a CO laser which produces a second frequency and a mixer for combining the output of the CO.sub.2 and CO lasers so as to produce a final output comprising a difference frequency from the first and second frequency outputs.

Pulsed infrared difference frequency generation in CdGeAs/sub 2/

DOEpatents

Piltch, M.S.; Rink, J.P.; Tallman, C.R.

1975-11-26

A laser apparatus for generating a line-tunable pulsed infrared difference frequency output is described. The apparatus comprises a CO/sub 2/ laser which produces a first frequency, a CO laser which produces a second frequency, and a mixer for combining the output of the CO/sub 2/ and CO lasers so as to produce a final output comprising a difference frequency from the first and second frequency outputs.

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

PubMed

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

2017-10-18

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

In-vitro generation of interleukin-10 secreting B-regulatory cells from donor adipose tissue derived mesenchymal stem cells and recipient peripheral blood mononuclear cells for potential cell therapy.

PubMed

Gupte, Kunal S; Vanikar, Aruna V; Trivedi, Hargovind L; Patel, Chetan N; Patel, Jignesh V

2017-02-01

Interleukin-10 secreting B-cells are a major subset of B-regulatory cells (B-regs), commonly recognized as CD19 + /38 hi /24 hi /IL10 + . They carry out immunomodulation by release of specific cytokines and/or cell-to-cell contact. We have generated B-regs in-vitro from donor adipose tissue derived mesenchymal stem cells (AD-MSC) and renal allograft recipient (RAR) peripheral blood mononuclear cells (PBMC) for potential cell therapy. Mononuclear cells separated by density gradient centrifugation from 50 ml anti-coagulated blood of 15-RAR and respective donors were analysed for baseline B-regs using appropriate antibodies. Equal amount (20 × 10 6  cells/ml) of stimulator (irradiated at 7.45 Gy/min for 10 min) and responder (non-irradiated) cells were co-cultured with in-vitro generated AD-MSC (1 × 10 6  cells/ml) in proliferation medium containing lipopolysaccharide from E. coli K12 strain at 37 °C with 5% CO 2 . Cells were harvested on day-7 and analyzed for viability, sterility, quantity, morphology and phenotyping. In-vitro generated B-reg levels were compared with baseline B-regs. In-vitro generated B-reg count increased to 16.75% from baseline count of 3.35%. B-regs can be successfully generated in-vitro from donor AD-MSC and RAR PBMC for potential cell therapy. Copyright © 2017 Chang Gung University. Published by Elsevier B.V. All rights reserved.

Adsorption and separation of binary and ternary mixtures of SO2, CO2 and N2 by ordered carbon nanotube arrays: grand-canonical Monte Carlo simulations.

PubMed

Rahimi, Mahshid; Singh, Jayant K; Müller-Plathe, Florian

2016-02-07

The adsorption and separation behavior of SO2-CO2, SO2-N2 and CO2-N2 binary mixtures in bundles of aligned double-walled carbon nanotubes is investigated using the grand-canonical Monte Carlo (GCMC) method and ideal adsorbed solution theory. Simulations were performed at 303 K with nanotubes of 3 nm inner diameter and various intertube distances. The results showed that the packing with an intertube distance d = 0 has the highest selectivity for SO2-N2 and CO2-N2 binary mixtures. For the SO2-CO2 case, the optimum intertube distance for having the maximum selectivity depends on the applied pressure, so that at p < 0.8 bar d = 0 shows the highest selectivity and at 0.8 bar < p < 2.5 bar, the highest selectivity belongs to d = 0.5 nm. Ideal adsorbed solution theory cannot predict the adsorption of the binary systems containing SO2, especially when d = 0. As the intertube distance is increased, the ideal adsorbed solution theory based predictions become closer to those of GCMC simulations. Only in the case of CO2-N2, ideal adsorbed solution theory is everywhere in good agreement with simulations. In a ternary mixture of all three gases, the behavior of SO2 and CO2 remains similar to that in a SO2-CO2 binary mixture because of the weak interaction between N2 molecules and CNTs.

UV/H2O2 and UV/PDS Treatment of Trimethoprim and Sulfamethoxazole in Synthetic Human Urine: Transformation Products and Toxicity.

PubMed

Zhang, Ruochun; Yang, Yongkui; Huang, Ching-Hua; Li, Na; Liu, Hang; Zhao, Lin; Sun, Peizhe

2016-03-01

Elimination of pharmaceuticals in source-separated human urine is a promising approach to minimize the pharmaceuticals in the environment. Although the degradation kinetics of pharmaceuticals by UV/H2O2 and UV/peroxydisulfate (PDS) processes has been investigated in synthetic fresh and hydrolyzed urine, comprehensive evaluation of the advanced oxidation processes (AOPs), such as product identification and toxicity testing, has not yet been performed. This study identified the transformation products of two commonly used antibiotics, trimethoprim (TMP) and sulfamethoxazole (SMX), by UV/H2O2 and UV/PDS in synthetic urine matrices. The effects of reactive species, including •OH, SO4(•-), CO3(•-), and reactive nitrogen species, on product generation were investigated. Multiple isomeric transformation products of TMP and SMX were observed, especially in the reaction with hydroxyl radical. SO4(•-) and CO3(•-) reacted with pharmaceuticals by electron transfer, thus producing similar major products. The main reactive species deduced on the basis of product generation are in good agreement with kinetic simulation of the advanced oxidation processes. A strain identified as a polyphosphate-accumulating organism was used to investigate the antimicrobial activity of the pharmaceuticals and their products. No antimicrobial property was detected for the transformation products of either TMP or SMX. Acute toxicity employing luminescent bacterium Vibrio qinghaiensis indicated 20-40% higher inhibitory effect of TMP and SMX after treatment. Ecotoxicity was estimated by quantitative structure-activity relationship analysis using ECOSAR.

Photocatalytic generation of hydrogen by core-shell WO3/BiVO4 nanorods with ultimate water splitting efficiency

PubMed Central

Pihosh, Yuriy; Turkevych, Ivan; Mawatari, Kazuma; Uemura, Jin; Kazoe, Yutaka; Kosar, Sonya; Makita, Kikuo; Sugaya, Takeyoshi; Matsui, Takuya; Fujita, Daisuke; Tosa, Masahiro; Kondo, Michio; Kitamori, Takehiko

2015-01-01

Efficient photocatalytic water splitting requires effective generation, separation and transfer of photo-induced charge carriers that can hardly be achieved simultaneously in a single material. Here we show that the effectiveness of each process can be separately maximized in a nanostructured heterojunction with extremely thin absorber layer. We demonstrate this concept on WO3/BiVO4+CoPi core-shell nanostructured photoanode that achieves near theoretical water splitting efficiency. BiVO4 is characterized by a high recombination rate of photogenerated carriers that have much shorter diffusion length than the thickness required for sufficient light absorption. This issue can be resolved by the combination of BiVO4 with more conductive WO3 nanorods in a form of core-shell heterojunction, where the BiVO4 absorber layer is thinner than the carrier diffusion length while it’s optical thickness is reestablished by light trapping in high aspect ratio nanostructures. Our photoanode demonstrates ultimate water splitting photocurrent of 6.72 mA cm−2 under 1 sun illumination at 1.23 VRHE that corresponds to ~90% of the theoretically possible value for BiVO4. We also demonstrate a self-biased operation of the photoanode in tandem with a double-junction GaAs/InGaAsP photovoltaic cell with stable water splitting photocurrent of 6.56 mA cm−2 that corresponds to the solar to hydrogen generation efficiency of 8.1%. PMID:26053164

Photocatalytic generation of hydrogen by core-shell WO3/BiVO4 nanorods with ultimate water splitting efficiency

NASA Astrophysics Data System (ADS)

Pihosh, Yuriy; Turkevych, Ivan; Mawatari, Kazuma; Uemura, Jin; Kazoe, Yutaka; Kosar, Sonya; Makita, Kikuo; Sugaya, Takeyoshi; Matsui, Takuya; Fujita, Daisuke; Tosa, Masahiro; Kondo, Michio; Kitamori, Takehiko

2015-06-01

Efficient photocatalytic water splitting requires effective generation, separation and transfer of photo-induced charge carriers that can hardly be achieved simultaneously in a single material. Here we show that the effectiveness of each process can be separately maximized in a nanostructured heterojunction with extremely thin absorber layer. We demonstrate this concept on WO3/BiVO4+CoPi core-shell nanostructured photoanode that achieves near theoretical water splitting efficiency. BiVO4 is characterized by a high recombination rate of photogenerated carriers that have much shorter diffusion length than the thickness required for sufficient light absorption. This issue can be resolved by the combination of BiVO4 with more conductive WO3 nanorods in a form of core-shell heterojunction, where the BiVO4 absorber layer is thinner than the carrier diffusion length while it’s optical thickness is reestablished by light trapping in high aspect ratio nanostructures. Our photoanode demonstrates ultimate water splitting photocurrent of 6.72 mA cm-2 under 1 sun illumination at 1.23 VRHE that corresponds to ~90% of the theoretically possible value for BiVO4. We also demonstrate a self-biased operation of the photoanode in tandem with a double-junction GaAs/InGaAsP photovoltaic cell with stable water splitting photocurrent of 6.56 mA cm-2 that corresponds to the solar to hydrogen generation efficiency of 8.1%.

Co-Thought and Co-Speech Gestures Are Generated by the Same Action Generation Process

ERIC Educational Resources Information Center

Chu, Mingyuan; Kita, Sotaro

2016-01-01

People spontaneously gesture when they speak (co-speech gestures) and when they solve problems silently (co-thought gestures). In this study, we first explored the relationship between these 2 types of gestures and found that individuals who produced co-thought gestures more frequently also produced co-speech gestures more frequently (Experiments…

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

Mays, Jeff

One-step hydrogen generation, using Sorption Enhanced Reforming (SER) technology, is an innovative means of providing critical energy and environmental improvements to US manufacturing processes. The Gas Technology Institute (GTI) is developing a Compact Hydrogen Generator (CHG) process, based on SER technology, which successfully integrates previously independent process steps, achieves superior energy efficiency by lowering reaction temperatures, and provides pathways to doubling energy productivity with less environmental pollution. GTI’s prior CHG process development efforts have culminated in an operational pilot plant. During the initial pilot testing, GTI identified two operating risks- 1) catalyst coating with calcium aluminate compounds, 2) limited solidsmore » handling of the sorbent. Under this contract GTI evaluated alternative materials (one catalyst and two sorbents) to mitigate both risks. The alternate catalyst met performance targets and did not experience coating with calcium aluminate compounds of any kind. The alternate sorbent materials demonstrated viable operation, with one material enabling a three-fold increase in sorbent flow. The testing also demonstrated operation at 90% of its rated capacity. Lastly, a carbon dioxide co-production study was performed to assess the advantage of the solid phase separation of carbon dioxide- inherent in the CHG process. Approximately 70% lower capital cost is achievable compared to SMR-based hydrogen production with CO2 capture, as well as improved operating costs.« less

Process parameters and morphology in puerarin, phospholipids and their complex microparticles generation by supercritical antisolvent precipitation.

PubMed

Li, Ying; Yang, Da-Jian; Chen, Shi-Lin; Chen, Si-Bao; Chan, Albert Sun-Chi

2008-07-09

The aim of the study was to develop and evaluate a new method for the production of puerarin phospholipids complex (PPC) microparticles. The advanced particle formation method, solution enhanced dispersion by supercritical fluids (SEDS), was used for the preparation of puerarin (Pur), phospholipids (PC) and their complex particles for the first time. Evaluation of the processing variables on PPC particle characteristics was also conducted. The processing variables included temperature, pressure, solution concentration, the flow rate of supercritical carbon dioxide (SC-CO2) and the relative flow rate of drug solution to CO2. The morphology, particle size and size distribution of the particles were determined. Meanwhile Pur and phospholipids were separately prepared by gas antisolvent precipitation (GAS) method and solid characterization of particles by the two supercritical methods was also compared. Pur formed by GAS was more orderly, purer crystal, whereas amorphous Pur particles between 0.5 and 1microm were formed by SEDS. The complex was successfully obtained by SEDS exhibiting amorphous, partially agglomerated spheres comprised of particles sized only about 1microm. SEDS method may be useful for the processing of other pharmaceutical preparations besides phospholipids complex particles. Furthermore adopting a GAS process to recrystallize pharmaceuticals will provide a highly versatile methodology to generate new polymorphs of drugs in addition to conventional techniques.

Beneficial effects of substituting trivalent ions in the B-site of La0.5Sr0.5Mn1-xAxO3 (A = Al, Ga, Sc) on the thermochemical generation of CO and H2 from CO2 and H2O.

PubMed

Dey, Sunita; Naidu, B S; Rao, C N R

2016-02-14

The effect of substitution of Al(3+), Ga(3+) and Sc(3+) ions in the Mn(3+) site of La0.5Sr0.5MnO3 on the thermochemical splitting of CO2 to generate CO has been studied in detail. Both La0.5Sr0.5Mn1-xGaxO3 and La0.5Sr0.5Mn1-xScxO3 give high yields of O2 and generate CO more efficiently than La0.5Sr0.5Mn1-xAlxO3 or the parent La0.5Sr0.5MnO3. Substitution of even 5% Sc(3+) (x = 0.05) results in a remarkable improvement in performance. Thus La0.5Sr0.5Mn0.95Sc0.05O3 produces 417 μmol g(-1) of O2 and 545 μmol g(-1) of CO, respectively, i.e. 2 and 1.7 times more O2 and CO than La0.5Sr0.5MnO3. This manganite also generates H2 satisfactorily by the thermochemical splitting of H2O.

A new metal-organic framework for separation of C2H2/CH4 and CO2/CH4 at room temperature

NASA Astrophysics Data System (ADS)

Duan, Xing; Zhou, You; Lv, Ran; Yu, Ben; Chen, Haodong; Ji, Zhenguo; Cui, Yuanjing; Yang, Yu; Qian, Guodong

2018-04-01

A 3D microporous metal-organic framework with open Cu2+ sites and suitable pore space, [Cu2(L)(H2O)2]·(H2O)4(DMF)8 (ZJU-15, H4L = 5,5‧-(9H-carbazole-2,7-diyl)diisophthalic acid; DMF = N,N-dimethylformamide; ZJU = Zhejiang University), has been constructed and characterized. The activated ZJU-15a has three different types of cages and exhibits BET surface area of 1660 m2 g-1, and can separate gas mixture of C2H2/CH4 and CO2/CH4 at room temperature.

Remarkable separability of circulation response to Arctic sea ice loss and greenhouse gas forcing

NASA Astrophysics Data System (ADS)

McCusker, K. E.; Kushner, P. J.; Fyfe, J. C.; Sigmond, M.; Kharin, V. V.; Bitz, C. M.

2017-08-01

Arctic sea ice loss may influence midlatitude climate by changing large-scale circulation. The extent to which climate change can be understood as greenhouse gas-induced changes that are modulated by this loss depends on how additive the responses to the separate influences are. A novel sea ice nudging methodology in a fully coupled climate model reveals that the separate effects of doubled atmospheric carbon dioxide (CO2) concentrations and associated Arctic sea ice loss are remarkably additive and insensitive to the mean climate state. This separability is evident in several fields throughout most of the year, from hemispheric to synoptic scales. The extent to which the regional response to sea ice loss sometimes agrees with and sometimes cancels the response to CO2 is quantified. The separability of the responses might provide a means to better interpret the diverse array of modeling and observational studies of Arctic change and influence.

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

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

Dongxiao Yang; Zhi Wang; Jixiao Wang

2009-09-15

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

Continuous Processing with Mars Gases

NASA Technical Reports Server (NTRS)

Parrish, Clyde; Jennings, Paul; Delgado, Hugo (Technical Monitor)

2001-01-01

Current Martian missions call for the production of oxygen for breathing, and fuel and oxygen for propulsion to be produced from atmospheric carbon dioxide (CO2). Adsorption and freezing are the two methods considered for capturing CO, from the atmosphere. However, the nitrogen (N2) and argon (Ar), which make up less than 5 percent of the atmosphere, cause difficulties with both of these processes by blocking the CO2, This results in the capture process rapidly changing from a pressure driven process to a diffusion controlled process. To increase the CO, capture rates, some type of mechanical pump is usually proposed to remove the N2 and Ar. The N2 and Ar are useful and have been proposed for blanketing and pressurizing fuel tanks and as buffer gas for breathing air for manned missions. Separation of the Martian gases with the required purity can be accomplished with a combination of membranes. These membrane systems do not require a high feed pressure and provide suitable separation. Therefore, by use of the appropriate membrane combination with the Martian atmosphere supplied by a compressor a continuous supply of CO2 for fuel and oxygen production can be supplied. This phase of our program has focused on the selection of the membrane system. Since permeation data for membranes did not exist for Martian atmospheric pressures and temperatures, this information had to be compiled. The general trend as the temperature was lowered was for the membranes to become more selective. In addition, the relative permeation rates between the three gases changed with temperature. The end result was to provide design parameters that could be used to separate CO2 from N2 and Ar. This paper will present the membrane data, provide the design requirements for a compressor, and compare the results with adsorption and freezer methods.

Highly hydrothermally stable microporous silica membranes for hydrogen separation.

PubMed

Wei, Qi; Wang, Fei; Nie, Zuo-Ren; Song, Chun-Lin; Wang, Yan-Li; Li, Qun-Yan

2008-08-07

Fluorocarbon-modified silica membranes were deposited on gamma-Al2O3/alpha-Al2O3 supports by the sol-gel technique for hydrogen separation. The hydrophobic property, pore structure, gas transport and separation performance, and hydrothermal stability of the modified membranes were investigated. It is observed that the water contact angle increases from 27.2+/-1.5 degrees for the pure silica membranes to 115.0+/-1.2 degrees for the modified ones with a (trifluoropropyl)triethoxysilane (TFPTES)/tetraethyl orthosilicate (TEOS) molar ratio of 0.6. The modified membranes preserve a microporous structure with a micropore volume of 0.14 cm3/g and a pore size of approximately 0.5 nm. A single gas permeation of H2 and CO2 through the modified membranes presents small positive apparent thermal activation energies, indicating a dominant microporous membrane transport. At 200 degrees C, a single H2 permeance of 3.1x10(-6) mol m(-2) s(-1) Pa(-1) and a H2/CO2 permselectivity of 15.2 were obtained after proper correction for the support resistance and the contribution from the defects. In the gas mixture measurement, the H2 permeance and the H2/CO2 separation factor almost remain constant at 200 degrees C with a water vapor pressure of 1.2x10(4) Pa for at least 220 h, indicating that the modified membranes are hydrothermally stable, benefiting from the integrity of the microporous structure due to the fluorocarbon modification.

DESIGNING AN OPPORTUNITY FUEL WITH BIOMASS AND TIRE-DERIVED FUEL FOR COFIRING AT WILLOW ISLAND GENERATING STATION

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

K. Payette; D. Tillman

During the period October 1, 2000 - December 31, 2000, Allegheny Energy Supply Co., LLC (Allegheny) executed a Cooperative Agreement with the National Energy Technology Laboratory to implement a major cofiring demonstration at the Willow Island Generating Station Boiler No.2. Willow Island Boiler No.2 is a cyclone boiler. Allegheny also will demonstrate separate injection cofiring at the Albright Generating Station Boiler No.3, a tangentially fired boiler. The Allegheny team includes Foster Wheeler as its primary subcontractor. Additional subcontractors are Cofiring Alternatives and N.S. Harding and Associates. This report summarizes the activities associated with the Designer Opportunity Fuel program, and demonstrationsmore » at Willow Island and Albright Generating Stations. The second quarter of the project involved completing the designs for each location. Further, geotechnical investigations proceeded at each site. Preparations were made to perform demolition on two small buildings at the Willow Island site. Fuels strategies were initiated for each site. Test planning commenced for each site. A groundbreaking ceremony was held at the Willow Island site on October 18, with Governor C. Underwood being the featured speaker.« less

Preparation Methods of Metal Organic Frameworks and Their Capture of CO2

NASA Astrophysics Data System (ADS)

Zhang, Linjian; Liand, Fangqin; Luo, Liangfei

2018-01-01

The increasingly serious greenhouse effect makes people pay more attention to the capture and storage technology of CO2. Metal organic frameworks (MOFs) have the advantages of high specific surface area, porous structure and controllable structure, and become the research focus of CO2 emission reduction technology in recent years. In this paper, the characteristics, preparation methods and application of MOFs in the field of CO2 adsorption and separation are discussed, especially the application of flue gas environment in power plants.

Organic oxalate as leachant and precipitant for the recovery of valuable metals from spent lithium-ion batteries

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

Sun Liang; Key Laboratory of Resources Chemistry of Nonferrous Metals, Central South University, Ministry of Education of the People's Republic of China; Qiu Keqiang, E-mail: qiuwhs@sohu.com

2012-08-15

Graphical abstract: Display Omitted Highlights: Black-Right-Pointing-Pointer Vacuum pyrolysis as a pretreatment was used to separate cathode material from aluminum foils. Black-Right-Pointing-Pointer Cobalt and lithium can be leached using oxalate while cobalt can be directly precipitated as cobalt oxalate. Black-Right-Pointing-Pointer Cobalt and lithium can be separated efficiently from each other only in the oxalate leaching process. Black-Right-Pointing-Pointer High reaction efficiency of LiCoO{sub 2} was obtained with oxalate. - Abstract: Spent lithium-ion batteries containing lots of strategic resources such as cobalt and lithium are considered as an attractive secondary resource. In this work, an environmentally compatible process based on vacuum pyrolysis, oxalatemore » leaching and precipitation is applied to recover cobalt and lithium from spent lithium-ion batteries. Oxalate is introduced as leaching reagent meanwhile as precipitant which leaches and precipitates cobalt from LiCoO{sub 2} and CoO directly as CoC{sub 2}O{sub 4}{center_dot}2H{sub 2}O with 1.0 M oxalate solution at 80 Degree-Sign C and solid/liquid ratio of 50 g L{sup -1} for 120 min. The reaction efficiency of more than 98% of LiCoO{sub 2} can be achieved and cobalt and lithium can also be separated efficiently during the hydrometallurgical process. The combined process is simple and adequate for the recovery of valuable metals from spent lithium-ion batteries.« less

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

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

Merkel, Tim; Wei, Xiaotong; Firat, Bilgen

2012-03-31

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

Power generation using spinel manganese-cobalt oxide as a cathode catalyst for microbial fuel cell applications.

PubMed

Mahmoud, Mohamed; Gad-Allah, Tarek A; El-Khatib, K M; El-Gohary, Fatma

2011-11-01

This study focused on the use of spinel manganese-cobalt (Mn-Co) oxide, prepared by a solid state reaction, as a cathode catalyst to replace platinum in microbial fuel cells (MFCs) applications. Spinel Mn-Co oxides, with an Mn/Co atomic ratios of 0.5, 1, and 2, were prepared and examined in an air cathode MFCs which was fed with a molasses-laden synthetic wastewater and operated in batch mode. Among the three Mn-Co oxide cathodes and after 300 h of operation, the Mn-Co oxide catalyst with Mn/Co atomic ratio of 2 (MnCo-2) exhibited the highest power generation 113 mW/m2 at cell potential of 279 mV, which were lower than those for the Pt catalyst (148 mW/m2 and 325 mV, respectively). This study indicated that using spinel Mn-Co oxide to replace platinum as a cathodic catalyst enhances power generation, increases contaminant removal, and substantially reduces the cost of MFCs. Copyright © 2011 Elsevier Ltd. All rights reserved.

Enhanced the performance of graphene oxide/polyimide hybrid membrane for CO2 separation by surface modification of graphene oxide using polyethylene glycol

NASA Astrophysics Data System (ADS)

Wu, Li-guang; Yang, Cai-hong; Wang, Ting; Zhang, Xue-yang

2018-05-01

Polyethylene glycol (PEG) with different molecular weights was first used to modify graphene oxide (GO) samples. Subsequently, polyimide (PI) hybrid membranes containing modified-GO were fabricated via in situ polymerization. The separation performance of these hybrid membranes was evaluated using permeation experiments for CO2 and N2 gases. The morphology characterization showed that PEG with suitable molecular weight could be successfully grafted on the GO surface. PEG modification altered the surface properties of GO and introduced defective structures onto GO surface. This caused strong surface polarity and high free volume of membranes containing PEG-modified GO, thereby improving the separation performance of membranes. The addition of PEG-GO with low molecular weight effectively increased gas diffusion through hybrid membranes. The hybrid membranes containing PEG-GO with large molecular weight had high solubility performance for CO2 gas due to the introduction of numerous polar groups into polymeric membranes. With the loading content of modified GO, the CO2 gas permeability of hybrid membranes initially increased but eventually decreased. The optimal content of modified GO in membranes reached 3.0 wt%. When too much PEG added (exceeding 30 g), some impurities formed on GO surface and some aggregates appeared in the resulting hybrid membrane, which depressed the membrane performance.

Highly CO2-Selective Gas Separation Membranes Based on Segmented Copolymers of Poly(Ethylene oxide) Reinforced with Pentiptycene-Containing Polyimide Hard Segments.

PubMed

Luo, Shuangjiang; Stevens, Kevin A; Park, Jae Sung; Moon, Joshua D; Liu, Qiang; Freeman, Benny D; Guo, Ruilan

2016-01-27

Poly(ethylene oxide) (PEO)-containing polymer membranes are attractive for CO2-related gas separations due to their high selectivity toward CO2. However, the development of PEO-rich membranes is frequently challenged by weak mechanical properties and a high crystallization tendency of PEO that hinders gas transport. Here we report a new series of highly CO2-selective, amorphous PEO-containing segmented copolymers prepared from commercial Jeffamine polyetheramines and pentiptycene-based polyimide. The copolymers are much more mechanically robust than the nonpentiptycene containing counterparts due to the molecular reinforcement mechanism of supramolecular chain threading and interlocking interactions induced by the pentiptycene structures, which also effectively suppresses PEO crystallization leading to a completely amorphous structure even at 60% PEO weight content. Membrane transport properties are sensitively affected by both PEO weight content and PEO chain length. A nonlinear correlation between CO2 permeability with PEO weight content was observed due to the competition between solubility and diffusivity contributions, whereby the copolymers change from being size-selective to solubility-selective when PEO content reaches 40%. CO2 selectivities over H2 and N2 increase monotonically with both PEO content and chain length, indicating strong CO2-philicity of the copolymers. The copolymer film with the longest PEO sequence (PEO2000) and highest PEO weight content (60%) showed a measured CO2 pure gas permeability of 39 Barrer, and ideal CO2/H2 and CO2/N2 selectivities of 4.1 and 46, respectively, at 35 °C and 3 atm, making them attractive for hydrogen purification and carbon capture.

Carbon Dioxide Emissions Effects of Grid-Scale Electricity Storage in a Decarbonizing Power System

DOE PAGES

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.

Neural correlates of frog calling: production by two semi-independent generators.

PubMed

Schmidt, R S

1992-09-28

The anterior preoptic nuclei of the isolated brainstem of male, Northern leopard frogs (Rana p. pipiens) were stimulated electrically and neural correlates of mating calling recorded from the rhombencephalic mating calling pattern generator. Lesions of discrete areas of the brainstem showed that the mating calling generator is separable into two generators, the pretrigeminal nucleus and the classical pulmonary respiration generator (which is approximately co-extensive with the motor nuclei IX-X). Each of these still can produce pulses when isolated from the other. Their interaction changes the expiratory phase of breathing into the vocal phase of calling. All stages of intermediates between these phases could be seen. An updated and simplified model of call production and evolution is presented.

Evaluation of relative effects of carbohydrate sources in yeast-fermentation CO2 generators on mosquito surveillance

USDA-ARS?s Scientific Manuscript database

In order to collect mosquitoes in remote locations that do not have access to attractive lures, such as CO2 (i.e., dry ice or compressed gas), a natural method to generate CO2 on-site has been developed. Our research explored alternative sugar sources such as honey, molasses, and granulated sugar u...

Cu2ZnSnS4/MoS2-Reduced Graphene Oxide Heterostructure: Nanoscale Interfacial Contact and Enhanced Photocatalytic Hydrogen Generation.

PubMed

Ha, Enna; Liu, Wei; Wang, Luyang; Man, Ho-Wing; Hu, Liangsheng; Tsang, Shik Chi Edman; Chan, Chris Tsz-Leung; Kwok, Wai-Ming; Lee, Lawrence Yoon Suk; Wong, Kwok-Yin

2017-01-03

Hydrogen generation from water using noble metal-free photocatalysts presents a promising platform for renewable and sustainable energy. Copper-based chalcogenides of earth-abundant elements, especially Cu 2 ZnSnS 4 (CZTS), have recently arisen as a low-cost and environment-friendly material for photovoltaics and photocatalysis. Herein, we report a new heterostructure consisting of CZTS nanoparticles anchored onto a MoS 2 -reduced graphene oxide (rGO) hybrid. Using a facile two-step method, CZTS nanoparticles were in situ grown on the surface of MoS 2 -rGO hybrid, which generated high density of nanoscale interfacial contact between CZTS and MoS 2 -rGO hybrid. The photoexcited electrons of CZTS can be readily transported to MoS 2 through rGO backbone, reducing the electron-hole pair recombination. In photocatalytic hydrogen generation under visible light irradiation, the presence of MoS 2 -rGO hybrids enhanced the hydrogen production rate of CZTS by 320%, which can be attributed to the synergetic effect of increased charge separation by rGO and more catalytically active sites from MoS 2 . Furthermore, this CZTS/MoS 2 -rGO heterostructure showed much higher photocatalytic activity than both Au and Pt nanoparticle-decorated CZTS (Au/CZTS and Pt/CZTS) photocatalysts, indicating the MoS 2 -rGO hybrid is a better co-catalyst for photocatalytic hydrogen generation than the precious metal. The CZTS/MoS 2 -rGO system also demonstrated stable photocatalytic activity for a continuous 20 h reaction.

Cu2ZnSnS4/MoS2-Reduced Graphene Oxide Heterostructure: Nanoscale Interfacial Contact and Enhanced Photocatalytic Hydrogen Generation

NASA Astrophysics Data System (ADS)

Ha, Enna; Liu, Wei; Wang, Luyang; Man, Ho-Wing; Hu, Liangsheng; Tsang, Shik Chi Edman; Chan, Chris Tsz-Leung; Kwok, Wai-Ming; Lee, Lawrence Yoon Suk; Wong, Kwok-Yin

2017-01-01

Hydrogen generation from water using noble metal-free photocatalysts presents a promising platform for renewable and sustainable energy. Copper-based chalcogenides of earth-abundant elements, especially Cu2ZnSnS4 (CZTS), have recently arisen as a low-cost and environment-friendly material for photovoltaics and photocatalysis. Herein, we report a new heterostructure consisting of CZTS nanoparticles anchored onto a MoS2-reduced graphene oxide (rGO) hybrid. Using a facile two-step method, CZTS nanoparticles were in situ grown on the surface of MoS2-rGO hybrid, which generated high density of nanoscale interfacial contact between CZTS and MoS2-rGO hybrid. The photoexcited electrons of CZTS can be readily transported to MoS2 through rGO backbone, reducing the electron-hole pair recombination. In photocatalytic hydrogen generation under visible light irradiation, the presence of MoS2-rGO hybrids enhanced the hydrogen production rate of CZTS by 320%, which can be attributed to the synergetic effect of increased charge separation by rGO and more catalytically active sites from MoS2. Furthermore, this CZTS/MoS2-rGO heterostructure showed much higher photocatalytic activity than both Au and Pt nanoparticle-decorated CZTS (Au/CZTS and Pt/CZTS) photocatalysts, indicating the MoS2-rGO hybrid is a better co-catalyst for photocatalytic hydrogen generation than the precious metal. The CZTS/MoS2-rGO system also demonstrated stable photocatalytic activity for a continuous 20 h reaction.

Cu2ZnSnS4/MoS2-Reduced Graphene Oxide Heterostructure: Nanoscale Interfacial Contact and Enhanced Photocatalytic Hydrogen Generation

PubMed Central

Ha, Enna; Liu, Wei; Wang, Luyang; Man, Ho-Wing; Hu, Liangsheng; Tsang, Shik Chi Edman; Chan, Chris Tsz-Leung; Kwok, Wai-Ming; Lee, Lawrence Yoon Suk; Wong, Kwok-Yin

2017-01-01

Hydrogen generation from water using noble metal-free photocatalysts presents a promising platform for renewable and sustainable energy. Copper-based chalcogenides of earth-abundant elements, especially Cu2ZnSnS4 (CZTS), have recently arisen as a low-cost and environment-friendly material for photovoltaics and photocatalysis. Herein, we report a new heterostructure consisting of CZTS nanoparticles anchored onto a MoS2-reduced graphene oxide (rGO) hybrid. Using a facile two-step method, CZTS nanoparticles were in situ grown on the surface of MoS2-rGO hybrid, which generated high density of nanoscale interfacial contact between CZTS and MoS2-rGO hybrid. The photoexcited electrons of CZTS can be readily transported to MoS2 through rGO backbone, reducing the electron-hole pair recombination. In photocatalytic hydrogen generation under visible light irradiation, the presence of MoS2-rGO hybrids enhanced the hydrogen production rate of CZTS by 320%, which can be attributed to the synergetic effect of increased charge separation by rGO and more catalytically active sites from MoS2. Furthermore, this CZTS/MoS2-rGO heterostructure showed much higher photocatalytic activity than both Au and Pt nanoparticle-decorated CZTS (Au/CZTS and Pt/CZTS) photocatalysts, indicating the MoS2-rGO hybrid is a better co-catalyst for photocatalytic hydrogen generation than the precious metal. The CZTS/MoS2-rGO system also demonstrated stable photocatalytic activity for a continuous 20 h reaction. PMID:28045066

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

Liu, Jian; Canfield, Nathan L.; Liu, Wei

A hydrophobic metal-organic framework (MOF) UiO-66-CH3 is prepared and its solvothermal stability is investigated in comparison to UiO-66. It is confirmed that the MOF stability is enhanced by introduction of the two methyl groups, while the water adsorption is reduced. Given its hydrophobicity and stability, UiO-66-CH3 is proposed as an attractive membrane material for gas separation under moisture conditions. The UiO-66-CH3 membrane is prepared on a 50µm-thin porous Ni support sheet for the first time by use of a secondary growth method. It is found that uniform seed coating on the support is necessary to form a continuous membrane. Inmore » addition to growth time and temperature, presence of a modulator in the growth solution is found to be useful for controlling hydrothermal membrane growth on the seeded support. A dense, inter-grown membrane layer is formed by 24-h growth over a temperature range from 120 oC to 160 oC. The membrane surface comprises 500 nm octahedral crystals, which are supposed to grow out of the original 100 nm spherical seeding crystals. The separation characteristics of resulting membranes are tested with pure CO2, air, CO2/air mixture, and humid CO2/air mixture. CO2 permeance as high as 1.9E-06 mol/m2/s/Pa at 31oC is obtained. Unlike the hydrophilic zeolite membranes, CO2 permeation through this membrane is not blocked by the presence of water vapor in the feed gas. The results suggest that this MOF framework is a promising membrane material worth to be further investigated for separation of CO2 and other small molecules from humid gas mixtures.« less

Separation of Rebaudiana A from Steviol glycoside using a polymeric adsorbent with multi-hydrogen bonding in a non-aqueous system.

PubMed

Ba, Jing; Zhang, Na; Yao, Lijuan; Ma, Ning; Wang, Chunhong

2014-11-15

Rebaudioside A (RA) and stevioside (SS) are the primary effective glycoside components in Stevia Rebaudiana. The RA glycoside is sweeter, and it tastes similarly to sucrose. Because extracts with a high RA content can be used as natural sweeteners for food additives approved by the FAO and FDA, RA should generate high market demand. In this study, an efficient method for separating RA was established based on the synergistic multi-hydrogen bonding interaction between a polymeric adsorbent and the RA glycoside. To overcome the destruction of the hydrophobic affinity required for the selective adsorption of RA, an innovative non-aqueous environment was established for adsorption and separation. To this end, an initial polymeric adsorbent composed of a glycidyl methacrylate and trimethylolpropane trimethacrylate (GMA-co-TMPTMA) copolymer matrix was synthesized, and polyethylene polyamine was employed as a functional reagent designed to react with the epoxy group on GME-co-TMPTMA to form a highly selective macroporous adsorbent. The effects of the different functional reagents and the solvent polarity on the adsorption selectivity for RA and SS, respectively, were investigated. Matching the structure of the polyethylene polyamine and sugar ligand on the glycoside molecule was essential in ensuring that the maximum synergistic interaction between adsorbent and adsorbate would be achieved. Moreover, the hydrogen-bonding force was observed to increase when the polarity of the adsorption solvent decreased. Therefore, among the synthesized macroporous polymeric adsorbents, the GTN4 adsorbent-bonding tetraethylenepentamine functional group provided the best separation in an n-butyl alcohol solution. Under the optimized gradient elution conditions, RA and SS can be effectively separated, and the contents of RA and SS increased from 33.5% and 51.5% in the initial crude extract to 95.4% and 78.2% after separation, respectively. Compared to conventional methods, the adsorption-desorption process is more advanced due to its procedural simplicity, low cost and adaptability for industrial production. Copyright © 2014 Elsevier B.V. All rights reserved.

High-throughput screening of small-molecule adsorption in MOF-74

NASA Astrophysics Data System (ADS)

Thonhauser, T.; Canepa, P.

2014-03-01

Using high-throughput screening coupled with state-of-the-art van der Waals density functional theory, we investigate the adsorption properties of four important molecules, H2, CO2, CH4, and H2O in MOF-74-  with  = Be, Mg, Al, Ca, Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Sr, Zr, Nb, Ru, Rh, Pd, La, W, Os, Ir, and Pt. We show that high-throughput techniques can aid in speeding up the development and refinement of effective materials for hydrogen storage, carbon capture, and gas separation. The exploration of the configurational adsorption space allows us to extract crucial information concerning, for example, the competition of water with CO2 for the adsorption binding sites. We find that only a few noble metals--Rh, Pd, Os, Ir, and Pt--favor the adsorption of CO2 and hence are potential candidates for effective carbon-capture materials. Our findings further reveal significant differences in the binding characteristics of H2, CO2, CH4, and H2O within the MOF structure, indicating that molecular blends can be successfully separated by these nano-porous materials. Supported by DOE DE-FG02-08ER46491.

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

DOEpatents

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

2012-03-06

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