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Title: Separation of CO2 from flue gas using electrochemical cells

Abstract

ABSTRACT Past research with high temperature molten carbonate electrochemical cells has shown that carbon dioxide can be separated from flue gas streams produced by pulverized coal combustion for power generation, However, the presence of trace contaminants, i.e" sulfur dioxide and nitric oxides, will impact the electrolyte within the cell. If a lower temperature cell could be devised that would utilize the benefits of commercially-available, upstream desulfurization and denitrification in the power plant, then this CO2 separation technique can approach more viability in the carbon sequestration area, Recent work has led to the assembly and successful operation of a low temperature electrochemical cell. In the proof-of-concept testing with this cell, an anion exchange membrane was sandwiched between gas-diffusion electrodes consisting of nickel-based anode electrocatalysts on carbon paper. When a potential was applied across the cell and a mixture of oxygen and carbon dioxide was flowed over the wetted electrolyte on the cathode side, a stream of CO2 to O2 was produced on the anode side, suggesting that carbonate/ bicarbonate ions are the CO2 carrier in the membrane. Since a mixture of CO 2 and 02 is produced, the possibility exists to use this stream in oxy-firing of additional fuel. From thismore » research, a novel concept for efficiently producing a carbon dioxide rich effiuent from combustion of a fossil fuel was proposed. Carbon dioxide and oxygen are captured from the flue gas of a fossilfuel combustor by one or more electrochemical cells or cell stacks. The separated stream is then transferred to an oxy-fired combustor which uses the gas stream for ancillary combustion, ultimately resulting in an effluent rich in carbon dioxide, A portion of the resulting flow produced by the oxy-fired combustor may be continuously recycled back into the oxy-fired combustor for temperature control and an optimal carbon dioxide rich effluent.« less

Authors:
; ; ; ; ;
Publication Date:
Research Org.:
National Energy Technology Lab. (NETL), Pittsburgh, PA, and Morgantown, WV (United States). In-house Research
Sponsoring Org.:
USDOE Office of Fossil Energy (FE)
OSTI Identifier:
1010667
Report Number(s):
NETL-TPR2857
Journal ID: ISSN 0016-2361; TRN: US201108%%507
Resource Type:
Journal Article
Resource Relation:
Journal Name: Fuel; Journal Volume: 89; Journal Issue: 6
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; ACID CARBONATES; CARBON; CARBON DIOXIDE; CARBON SEQUESTRATION; COMBUSTION; DENITRIFICATION; DESULFURIZATION; ELECTROCATALYSTS; ELECTROCHEMICAL CELLS; ELECTROLYTES; FLUE GAS; FOSSIL FUELS; NITRIC OXIDE; POWER GENERATION; POWER PLANTS; SULFUR DIOXIDE; TEMPERATURE CONTROL; carbon dioxide sequestration, carbon capture and separation, electrochemical separation

Citation Formats

Pennline, H.W, Granite, E.J., Luebke, D.R, Kitchin, J.R, Landon, J., and Weiland, L.M. Separation of CO2 from flue gas using electrochemical cells. United States: N. p., 2010. Web. doi:10.1016/j.fuel.2009.11.036.
Pennline, H.W, Granite, E.J., Luebke, D.R, Kitchin, J.R, Landon, J., & Weiland, L.M. Separation of CO2 from flue gas using electrochemical cells. United States. doi:10.1016/j.fuel.2009.11.036.
Pennline, H.W, Granite, E.J., Luebke, D.R, Kitchin, J.R, Landon, J., and Weiland, L.M. 2010. "Separation of CO2 from flue gas using electrochemical cells". United States. doi:10.1016/j.fuel.2009.11.036.
@article{osti_1010667,
title = {Separation of CO2 from flue gas using electrochemical cells},
author = {Pennline, H.W and Granite, E.J. and Luebke, D.R and Kitchin, J.R and Landon, J. and Weiland, L.M.},
abstractNote = {ABSTRACT Past research with high temperature molten carbonate electrochemical cells has shown that carbon dioxide can be separated from flue gas streams produced by pulverized coal combustion for power generation, However, the presence of trace contaminants, i.e" sulfur dioxide and nitric oxides, will impact the electrolyte within the cell. If a lower temperature cell could be devised that would utilize the benefits of commercially-available, upstream desulfurization and denitrification in the power plant, then this CO2 separation technique can approach more viability in the carbon sequestration area, Recent work has led to the assembly and successful operation of a low temperature electrochemical cell. In the proof-of-concept testing with this cell, an anion exchange membrane was sandwiched between gas-diffusion electrodes consisting of nickel-based anode electrocatalysts on carbon paper. When a potential was applied across the cell and a mixture of oxygen and carbon dioxide was flowed over the wetted electrolyte on the cathode side, a stream of CO2 to O2 was produced on the anode side, suggesting that carbonate/ bicarbonate ions are the CO2 carrier in the membrane. Since a mixture of CO 2 and 02 is produced, the possibility exists to use this stream in oxy-firing of additional fuel. From this research, a novel concept for efficiently producing a carbon dioxide rich effiuent from combustion of a fossil fuel was proposed. Carbon dioxide and oxygen are captured from the flue gas of a fossilfuel combustor by one or more electrochemical cells or cell stacks. The separated stream is then transferred to an oxy-fired combustor which uses the gas stream for ancillary combustion, ultimately resulting in an effluent rich in carbon dioxide, A portion of the resulting flow produced by the oxy-fired combustor may be continuously recycled back into the oxy-fired combustor for temperature control and an optimal carbon dioxide rich effluent.},
doi = {10.1016/j.fuel.2009.11.036},
journal = {Fuel},
number = 6,
volume = 89,
place = {United States},
year = 2010,
month = 6
}
  • Past research with high temperature molten carbonate electrochemical cells has shown that carbon dioxide can be separated from flue gas streams produced by pulverized coal combustion for power generation. However, the presence of trace contaminants, i.e., sulfur dioxide and nitric oxides, will impact the electrolyte within the cell. If a lower temperature cell could be devised that would utilize the benefits of commercially-available, upstream desulfurization and denitrification in the power plant, then this CO2 separation technique can approach more viability in the carbon sequestration area. Recent work has led to the assembly and successful operation of a low temperature electrochemicalmore » cell. In the proof-of-concept testing with this cell, an anion exchange membrane was sandwiched between gas-diffusion electrodes consisting of nickel-based anode electrocatalysts on carbon paper. When a potential was applied across the cell and a mixture of oxygen and carbon dioxide was flowed over the wetted electrolyte on the cathode side, a stream of CO2 to O2 was produced on the anode side, suggesting that carbonate/ bicarbonate ions are the CO2 carrier in the membrane. Since a mixture of CO2 and O2 is produced, the possibility exists to use this stream in oxy-firing of additional fuel. From this research, a novel concept for efficiently producing a carbon dioxide rich effluent from combustion of a fossil fuel was proposed. Carbon dioxide and oxygen are captured from the flue gas of a fossilfuel combustor by one or more electrochemical cells or cell stacks. The separated stream is then transferred to an oxy-fired combustor which uses the gas stream for ancillary combustion, ultimately resulting in an effluent rich in carbon dioxide. A portion of the resulting flow produced by the oxy-fired combustor may be continuously recycled back into the oxy-fired combustor for temperature control and an optimal carbon dioxide rich effluent« less
  • Results are presented of work done at Argonne National Laboratory to develop a molten-salt-based electrochemical technology for extracting uranium and transuranic elements from spent light water reactor fuel. In this process, the actinide oxides in the spent fuel are reduced using lithium at 650{sup o}C in the presence of molten LiCl, yielding the corresponding actinides and Li{sub 2}O. The actinides are then extracted from the reduction product by means of electrorefining. Associated with the reduction step is an ancillary salt-recovery step designed to electrochemically reduce the Li{sub 2}O concentration of the salt and recover the lithium metal.Experiments were performed atmore » the laboratory scale (50 to 150 g of fuel and 0.5 to 3.5 l of salt) and engineering scale (3.7 to 5.2 kg of fuel and 50 l of salt). Laboratory-scale experiments were designed to obtain information on the fundamental factors affecting process rates. Engineering-scale experiments were conducted to verify that the parameters controlling process scaleup are sufficiently understood, and to test equipment and operating concepts at or near full scale. All indications are that the electrochemical-based process should be workable at practical plant sizes.« less
  • This paper reports on the electroreduction of Hf(IV) in chloraluminate melts of similar compositions and on the electrochemical separation of zirconium from hafnium using low-melting chloraluminate melts. Results indicated that the addition of HfCl/sub 4/ to AlCl/sub 3/-NaCl melts (ranging in composition from 50.3 to 52 mol % AlCl/sub 3/) resulted in a poorly defined voltammetric reduction wave that occurs at potentials somewhat more negative than the reduction of Al/sub 2/Cl/sub 7//sup -/. The cyclic voltammograms exhibit either one or two reoxidation peaks depending on the switching potential, concentration of Hf(IV), and melt acidity. The reoxidation peak at more negativemore » potentials (approx.+0.1V with respect to an Al(III)/Al reference electrode in the melt of the same composition) is observed when the Hf(IV) concentration is small compared to that of Al/sub 2/Cl/sub 7//sup -/. The reoxidation peak at more positive potentials (/sub 0/.2V with respect to the same reference electrode) increases with the Hf(IV) concentration.« less
  • Results are presented of work done at Argonne National Laboratory to develop a molten-salt-based electrochemical technology for extracting uranium and transuranic elements from spent light water reactor fuel. In this process, the actinide oxides in the spent fuel are reduced using lithium at 650 deg. C in the presence of molten LiCl, yielding the corresponding actinides and Li{sub 2}O. The actinides are then extracted from the reduction product by means of electrorefining. Associated with the reduction step is an ancillary salt-recovery step designed to electrochemically reduce the Li{sub 2}O concentration of the salt and recover the lithium metal.Experiments were performedmore » at the laboratory scale (50 to 150 g of fuel and 0.5 to 3.5 l of salt) and engineering scale (3.7 to 5.2 kg of fuel and 50 l of salt). Laboratory-scale experiments were designed to obtain information on the fundamental factors affecting process rates. Engineering-scale experiments were conducted to verify that the parameters controlling process scaleup are sufficiently understood, and to test equipment and operating concepts at or near full scale. All indications are that the electrochemical-based process should be workable at practical plant sizes.« less