Influence of dilute feed and pH on electrochemical reduction of CO2 to CO on Ag in a continuous flow electrolyzer

被引:183
作者
Kim, Byoungsu [1 ,3 ]
Ma, Sichao [2 ,3 ]
Jhong, Huei-Ru Molly [1 ,3 ]
Kenis, Paul J. A. [1 ,3 ]
机构
[1] Univ Illinois, Dept Chem & Biomol Engn, Urbana, IL 61801 USA
[2] Univ Illinois, Dept Chem, Urbana, IL 61801 USA
[3] Kyushu Univ, Int Inst Carbon Neutral Energy Res WPI I2CNER, Fukuoka 812, Japan
基金
美国国家科学基金会;
关键词
Carbon dioxide; Electrochemical reduction; Dilute feed; Carbon monoxide; Electrolyte pH; CARBON-DIOXIDE; ELECTRODES; CONVERSION; PERFORMANCE; CATALYSTS; FORMATE; DESIGN; ACID; CELL;
D O I
10.1016/j.electacta.2015.03.064
中图分类号
O646 [电化学、电解、磁化学];
学科分类号
081704 ;
摘要
Electrochemical conversion of CO2 to useful chemical intermediates may be a promising strategy to help reduce CO2 emissions, while utilizing otherwise wasted excess renewable energy. Here we explore the effect of diluted CO2 streams (10-100% by volume using N-2 as diluting inert gas) on the product selectivity and on the CO/CO2 conversion ratio for the electrochemical reduction of CO2 into CO, specifically using a gas diffusion electrode loaded with Ag catalyst in a continuous flow electrolyzer. When using diluted CO2 feeds for the electrolyzer, we still observed high Faradaic efficiencies for CO (>80%), high conversion ratios (up to 32% per pass), and partial current densities for CO of 29 mA/cm(2) when operating the cell at 3.0 V. Most notably, we observed that the decrease in partial current density for CO was less than 45% when switching from a 100% CO2 feed to a 10% CO2 feed. Also, we studied the effect of pH and the interplay between pH and the diluted CO2 feed. We observed higher levels of CO formation as well as a higher Faradaic efficiency for CO when using an alkaline electrolyte, compared to when using a neutral or acidic electrolyte. However, the effect of CO2 concentration in the feed is more significant than the effect of pH on electrochemical reduction of CO2 to CO. (C) 2015 Elsevier Ltd. All rights reserved.
引用
收藏
页码:271 / 276
页数:6
相关论文
共 36 条
[1]   The Electrochemical Reduction of Carbon Dioxide to Formate/Formic Acid: Engineering and Economic Feasibility [J].
Agarwal, Arun S. ;
Zhai, Yumei ;
Hill, Davion ;
Sridhar, Narasi .
CHEMSUSCHEM, 2011, 4 (09) :1301-1310
[2]   Frontiers, Opportunities, and Challenges in Biochemical and Chemical Catalysis of CO2 Fixation [J].
Appel, Aaron M. ;
Bercaw, John E. ;
Bocarsly, Andrew B. ;
Dobbek, Holger ;
DuBois, Daniel L. ;
Dupuis, Michel ;
Ferry, James G. ;
Fujita, Etsuko ;
Hille, Russ ;
Kenis, Paul J. A. ;
Kerfeld, Cheal A. ;
Morris, Robert H. ;
Peden, Charles H. F. ;
Portis, Archie R. ;
Ragsdale, Stephen W. ;
Rauchfuss, Thomas B. ;
Reek, Joost N. H. ;
Seefeldt, Lance C. ;
Thauer, Rudolf K. ;
Waldrop, Grover L. .
CHEMICAL REVIEWS, 2013, 113 (08) :6621-6658
[3]   Efficient reduction of CO2 in a solid oxide electrolyzer [J].
Bidrawn, F. ;
Kim, G. ;
Corre, G. ;
Irvine, J. T. S. ;
Vohs, J. M. ;
Gorte, R. J. .
ELECTROCHEMICAL AND SOLID STATE LETTERS, 2008, 11 (09) :B167-B170
[4]   Opportunities and prospects in the chemical recycling of carbon dioxide to fuels [J].
Centi, Gabriele ;
Perathoner, Siglinda .
CATALYSIS TODAY, 2009, 148 (3-4) :191-205
[5]   Aqueous CO2 Reduction at Very Low Overpotential on Oxide-Derived Au Nanoparticles [J].
Chen, Yihong ;
Li, Christina W. ;
Kanan, Matthew W. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2012, 134 (49) :19969-19972
[6]   Using a One-Electron Shuttle for the Multielectron Reduction of CO2 to Methanol: Kinetic, Mechanistic, and Structural Insights [J].
Cole, Emily Barton ;
Lakkaraju, Prasad S. ;
Rampulla, David M. ;
Morris, Amanda J. ;
Abelev, Esta ;
Bocarsly, Andrew B. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2010, 132 (33) :11539-11551
[7]   HIGH-RATE GAS-PHASE CO2 REDUCTION TO ETHYLENE AND METHANE USING GAS-DIFFUSION ELECTRODES [J].
COOK, RL ;
MACDUFF, RC ;
SAMMELLS, AF .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1990, 137 (02) :607-608
[8]   Carbon Dioxide Capture: Prospects for New Materials [J].
D'Alessandro, Deanna M. ;
Smit, Berend ;
Long, Jeffrey R. .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2010, 49 (35) :6058-6082
[9]   Design of an electrochemical cell making syngas (CO+H2) from CO2 and H2O reduction at room temperature [J].
Delacourt, Charles ;
Ridgway, Paul L. ;
Kerr, John B. ;
Newman, John .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 2008, 155 (01) :B42-B49
[10]   The Fischer-Tropsch process: 1950-2000 [J].
Dry, ME .
CATALYSIS TODAY, 2002, 71 (3-4) :227-241