Activity and Selectivity Control in CO 2 Electroreduction to Multicarbon Products over CuO x Catalysts via Electrolyte Design
Abstract
The CO2 electroreduction reaction (CO2RR) to chemicals and fuels is of both fundamental and practical significance, since it would lead to a more efficient storage of renewable energy while closing the carbon cycle. Here we report enhanced activity and selectivity for the CO2RR to multicarbon hydrocarbons and alcohols (~69% Faradaic efficiency and -45.5 mA cm–2 partial current density for C2+ at -1.0 V vs RHE) over O2-plasma-activated Cu catalysts via electrolyte design. Increasing the size of the alkali-metal cations in the electrolyte, in combination with the presence of subsurface oxygen species which favor their adsorption, significantly improved C–C coupling on CuOx electrodes. The coexistence of Cs+ and I– induced drastic restructuring of the CuOx surface, the formation of shaped particles containing stable CuI species, and a more favorable stabilization of the reaction intermediates and concomitant high C2+ selectivity. This work, combining both experiment and density functional theory, provides insights into the active sites and reaction mechanism of oxide-derived Cu catalysts for the CO2RR.
- Authors:
-
- Max Planck Society, Berlin (Germany). Fritz-Haber Inst., Dept. of Interface Science; Ruhr-Univ., Bochum (Germany). Dept. of Physics
- Pennsylvania State Univ., University Park, PA (United States). Dept. of Chemical Engineering
- ennsylvania State Univ., University Park, PA (United States). Dept. of Chemical Engineering
- Max Planck Society, Berlin (Germany). Fritz-Haber Inst., Dept. of Interface Science; Ruhr-Univ., Bochum (Germany). Dept. of Physics
- Columbia Univ., New York, NY (United States). Dept. of Chemical Engineering
- Columbia Univ., New York, NY (United States). Dept. of Chemical Engineering; Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Dept.
- Publication Date:
- Research Org.:
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1484885
- Report Number(s):
- BNL-209655-2018-JAAM
Journal ID: ISSN 2155-5435
- Grant/Contract Number:
- SC0012704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Catalysis
- Additional Journal Information:
- Journal Volume: 8; Journal Issue: 11; Journal ID: ISSN 2155-5435
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY
Citation Formats
Gao, Dunfeng, McCrum, Ian T., Deo, Shyam, Choi, Yong-Wook, Scholten, Fabian, Wan, Weiming, Chen, Jingguang G., Janik, Michael J., and Roldan Cuenya, Beatriz. Activity and Selectivity Control in CO 2 Electroreduction to Multicarbon Products over CuO x Catalysts via Electrolyte Design. United States: N. p., 2018.
Web. doi:10.1021/acscatal.8b02587.
Gao, Dunfeng, McCrum, Ian T., Deo, Shyam, Choi, Yong-Wook, Scholten, Fabian, Wan, Weiming, Chen, Jingguang G., Janik, Michael J., & Roldan Cuenya, Beatriz. Activity and Selectivity Control in CO 2 Electroreduction to Multicarbon Products over CuO x Catalysts via Electrolyte Design. United States. https://doi.org/10.1021/acscatal.8b02587
Gao, Dunfeng, McCrum, Ian T., Deo, Shyam, Choi, Yong-Wook, Scholten, Fabian, Wan, Weiming, Chen, Jingguang G., Janik, Michael J., and Roldan Cuenya, Beatriz. Tue .
"Activity and Selectivity Control in CO 2 Electroreduction to Multicarbon Products over CuO x Catalysts via Electrolyte Design". United States. https://doi.org/10.1021/acscatal.8b02587. https://www.osti.gov/servlets/purl/1484885.
@article{osti_1484885,
title = {Activity and Selectivity Control in CO 2 Electroreduction to Multicarbon Products over CuO x Catalysts via Electrolyte Design},
author = {Gao, Dunfeng and McCrum, Ian T. and Deo, Shyam and Choi, Yong-Wook and Scholten, Fabian and Wan, Weiming and Chen, Jingguang G. and Janik, Michael J. and Roldan Cuenya, Beatriz},
abstractNote = {The CO2 electroreduction reaction (CO2RR) to chemicals and fuels is of both fundamental and practical significance, since it would lead to a more efficient storage of renewable energy while closing the carbon cycle. Here we report enhanced activity and selectivity for the CO2RR to multicarbon hydrocarbons and alcohols (~69% Faradaic efficiency and -45.5 mA cm–2 partial current density for C2+ at -1.0 V vs RHE) over O2-plasma-activated Cu catalysts via electrolyte design. Increasing the size of the alkali-metal cations in the electrolyte, in combination with the presence of subsurface oxygen species which favor their adsorption, significantly improved C–C coupling on CuOx electrodes. The coexistence of Cs+ and I– induced drastic restructuring of the CuOx surface, the formation of shaped particles containing stable CuI species, and a more favorable stabilization of the reaction intermediates and concomitant high C2+ selectivity. This work, combining both experiment and density functional theory, provides insights into the active sites and reaction mechanism of oxide-derived Cu catalysts for the CO2RR.},
doi = {10.1021/acscatal.8b02587},
journal = {ACS Catalysis},
number = 11,
volume = 8,
place = {United States},
year = {Tue Sep 11 00:00:00 EDT 2018},
month = {Tue Sep 11 00:00:00 EDT 2018}
}
Web of Science
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