期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 56, 期 38, 页码 11394-11398出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201704613
关键词
CO2 reduction; electrocatalysis; nanostructures; silver
资金
- Bundesministerium fur Bildung und Forschung (BMBF) [03SF0523-CCO2EKAT]
- Cluster of Excellence RESOLV at RUB - Deutsche Forschungsgemeinschaft [EXC 1069]
- European Research Council under grant ERC-OPERANDOCAT [ERC-725915]
- flagship Climate KIC/EnCO2re program as part of the Horizon2020 EU funding instrument
- Carlsberg Foundation [CF15-0165]
- US National Science Foundation [NSF-CHEM 1213182]
- US Department of Energy (DOE) by Argonne National Laboratory (ANL) [DE-AC02-06CH11357]
- MRCAT member institutions
- DOE
- DOE-BES [DE FG02-03ER15476]
- DOE Office of Science Facility, at Brookhaven National Laboratory [DE-SC0012704]
- [NSF-CHE-1534630]
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1213182] Funding Source: National Science Foundation
Efficient, stable catalysts with high selectivity for a single product are essential if electroreduction of CO2 is to become a viable route to the synthesis of industrial feedstocks and fuels. A plasma oxidation pre-treatment of silver foil enhances the number of low-coordinated catalytically active sites, which dramatically lowers the overpotential and increases the activity of CO2 electroreduction to CO. At -0.6 V versus RHE more than 90% Faradaic efficiency towards CO was achieved on a pre-oxidized silver foil. While transmission electron microscopy (TEM) and operando X-ray absorption spectroscopy showed that oxygen species can survive in the bulk of the catalyst during the reaction, quasi in situ X-ray photoelectron spectroscopy showed that the surface is metallic under reaction conditions. DFT calculations reveal that the defect-rich surface of the plasma-oxidized silver foils in the presence of local electric fields drastically decrease the overpotential of CO2 electroreduction.
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