期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 58, 期 19, 页码 6271-6275出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201900781
关键词
carbides; CO2 electroreduction; computational chemistry; insitu X-ray spectroscopy; palladium hydride
资金
- U.S. Department of Energy, Office of Science, Catalysis Program [DE-FG02-13ER16381, 201706250084]
- China Scholarship Council
Electrochemical CO2 reduction reaction (CO2RR) with renewable electricity is a potentially sustainable method to reduce CO2 emissions. Palladium supported on cost-effective transition-metal carbides (TMCs) are studied to reduce the Pd usage and tune the activity and selectivity of the CO2RR to produce synthesis gas, using a combined approach of studying thin films and practical powder catalysts, insitu characterization, and density functional theory (DFT) calculations. Notably, Pd/TaC exhibits higher CO2RR activity, stability and CO Faradaic efficiency than those of commercial Pd/C while significantly reducing the Pd loading. Insitu measurements confirm the transformation of Pd into hydride (PdH) under the CO2RR environment. DFT calculations reveal that the TMC substrates modify the binding energies of key intermediates on supported PdH. This work suggests the prospect of using TMCs as low-cost and stable substrates to support and modify Pd for enhanced CO2RR activity.
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