Carbon Monoxide Gas Diffusion Electrolysis that Produces Concentrated C2 Products with High Single-Pass Conversion

被引:260
作者
Ripatti, Donald S. [1 ]
Veltman, Thomas R. [1 ]
Kanan, Matthew W. [1 ]
机构
[1] Stanford Univ, Dept Chem, 337 Campus Dr, Stanford, CA 94305 USA
基金
美国国家科学基金会;
关键词
ELECTROCHEMICAL REDUCTION; EXCHANGE MEMBRANE; CO REDUCTION; ELECTROREDUCTION; COPPER; TRANSPORT; CATALYST; CONDUCTIVITY; TEMPERATURE; FUEL;
D O I
10.1016/j.joule.2018.10.007
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Electrochemical CO conversion is critical for the development of alternative fuel and chemical syntheses. To be efficient, electrosynthesis must make concentrated product streams at high rates with modest potentials, but the combination of these features has not been established for CO or the related CO2 electrolysis. Here we investigate CO electrolysis with gas diffusion electrodes (GDEs) supplied by interdigitated flow fields in electrochemical cells with different ion transport properties. By optimizing gas and ion transport, we show that it is possible to simultaneously achieve high current density, high selectivity, and high single-pass conversion at moderate cell potentials. Using a cell with the GDE directly contacting a Nafion membrane, we demonstrate >100 mA cm(-2) CO reduction to C-2 products and direct production of 1.1 M acetate at a cell potential of 2.4 V over 24 hr. Our results reveal critical design features for maximizing the efficiency of C-2 electrosynthesis.
引用
收藏
页码:240 / 256
页数:17
相关论文
共 41 条
[1]   AN EXPERIMENTAL STUDY OF MODE OF OPERATION OF POROUS GAS-DIFFUSION ELECTRODES WITH HYDROGEN FUEL [J].
AUSTIN, LG ;
ALMAULA, S .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1967, 114 (09) :927-&
[2]   Ethanol electro-oxidation reaction using a polycrystalline nickel electrode in alkaline media: Temperature influence and reaction mechanism [J].
Barbosa, A. F. B. ;
Oliveira, V. L. ;
van Drunen, J. ;
Tremiliosi-Filho, G. .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 2015, 746 :31-38
[3]   Electroreduction of CO on Polycrystalline Copper at Low Overpotentials [J].
Bertheussen, Erlend ;
Hogg, Thomas V. ;
Abghoui, Younes ;
Engstfeld, Albert K. ;
Chorkendorff, Ib ;
Stephens, Ifan E. L. .
ACS ENERGY LETTERS, 2018, 3 (03) :634-640
[4]   What Should We Make with CO2 and How Can We Make It? [J].
Bushuyev, Oleksandr S. ;
De Luna, Phil ;
Cao Thang Dinh ;
Tao, Ling ;
Saur, Genevieve ;
van de lagemaat, Jao ;
Kelley, Shana O. ;
Sargent, Edward H. .
JOULE, 2018, 2 (05) :825-832
[5]   Mass transport through a proton exchange membrane (Nafion) in microbial fuel cells [J].
Chae, Kyu Jung ;
Choi, Mijin ;
Ajayi, Folusho F. ;
Park, Wooshin ;
Chang, In Seop ;
Kim, In S. .
ENERGY & FUELS, 2008, 22 (01) :169-176
[6]   CO2 electroreduction to ethylene via hydroxide-mediated copper catalysis at an abrupt interface [J].
Dinh, Cao-Thang ;
Burdyny, Thomas ;
Kibria, Md Golam ;
Seifitokaldani, Ali ;
Gabardo, Christine M. ;
de Arquer, F. Pelayo Garcia ;
Kiani, Amirreza ;
Edwards, Jonathan P. ;
De Luna, Phil ;
Bushuyev, Oleksandr S. ;
Zou, Chengqin ;
Quintero-Bermudez, Rafael ;
Pang, Yuanjie ;
Sinton, David ;
Sargent, Edward H. .
SCIENCE, 2018, 360 (6390) :783-787
[7]   A Direct Grain-Boundary-Activity Correlation for CO Electroreduction on Cu Nanoparticles [J].
Feng, Xiaofeng ;
Jiang, Kaili ;
Fan, Shoushan ;
Kanan, Matthew W. .
ACS CENTRAL SCIENCE, 2016, 2 (03) :169-174
[8]   Supramolecular Porphyrin Cages Assembled at Molecular-Materials Interfaces for Electrocatalytic CO Reduction [J].
Gong, Ming ;
Cao, Zhi ;
Liu, Wei ;
Nichols, Eva M. ;
Smith, Peter T. ;
Derrick, Jeffrey S. ;
Liu, Yi-Sheng ;
Liu, Jinjia ;
Wen, Xiaodong ;
Chang, Christopher J. .
ACS CENTRAL SCIENCE, 2017, 3 (09) :1032-1040
[9]   The Technical and Energetic Challenges of Separating (Photo)Electrochemical Carbon Dioxide Reduction Products [J].
Greenblatt, Jeffery B. ;
Miller, Daniel J. ;
Ager, Joel W. ;
Houle, Frances A. ;
Sharp, Ian D. .
JOULE, 2018, 2 (03) :381-420
[10]   Technical photosynthesis involving CO2 electrolysis and fermentation [J].
Haas, Thomas ;
Krause, Ralf ;
Weber, Rainer ;
Demler, Martin ;
Schmid, Guenter .
NATURE CATALYSIS, 2018, 1 (01) :32-39