Journal
ACS CATALYSIS
Volume 8, Issue 11, Pages 10012-+Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.8b02587
Keywords
CO2 electroreduction; CuOx catalysts; electrolyte design; cation adsorption; subsurface oxygen
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Funding
- German Federal Ministry of Education and Research (Bundesministerium fur Bildung and Forschung, BMBF) [03SF0523C, 033RCOO4D]
- Cluster of Excellence RESOLV at RUB - Deutsche Forschungsgemeinschaft (DFG) [EXC 1069]
- European Research Council [ERG-725915]
- U.S. National Science Foundation [ACI-1053575, NRT-1449785]
- U.S. Department of Energy [DE-FG02-13ER16381]
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The CO, 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 (similar to 69% Faradaic efficiency and -45.5 mA cm(-2) partial current density for C2+ at -1.0 V vs RHE) over O-2-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.
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