期刊
NATURE COMMUNICATIONS
卷 11, 期 1, 页码 -出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-020-17499-5
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资金
- Ontario Research Fund Research-Excellence Program
- Natural Sciences and Engineering Research Council (NSERC) of Canada
- CIFAR Bio-Inspired Solar Energy program
- University of Toronto Connaught grant
- U.S. DOE [DE-AC02-06CH11357]
- Canadian Light Source
- NSERC E.W.R Steacie Memorial Fellowship
- Canada Foundation for Innovation
- Ontario Research Fund
- Government of Ontario
- Ontario Research Fund Research Excellence Program
- University of Toronto
Multi-carbon alcohols such as ethanol are valued as fuels in view of their high energy density and ready transport. Unfortunately, the selectivity toward alcohols in CO2/CO electro-reduction is diminished by ethylene production, especially when operating at high current densities (>100 mA cm(-2)). Here we report a metal doping approach to tune the adsorption of hydrogen at the copper surface and thereby promote alcohol production. Using density functional theory calculations, we screen a suite of transition metal dopants and find that incorporating Pd in Cu moderates hydrogen adsorption and assists the hydrogenation of C-2 intermediates, providing a means to favour alcohol production and suppress ethylene. We synthesize a Pd-doped Cu catalyst that achieves a Faradaic efficiency of 40% toward alcohols and a partial current density of 277 mA cm(-2) from CO electroreduction. The activity exceeds that of prior reports by a factor of 2.
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