期刊
NATURE COMMUNICATIONS
卷 11, 期 1, 页码 -出版社
NATURE PORTFOLIO
DOI: 10.1038/s41467-020-20004-7
关键词
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资金
- Natural Gas Innovation Fund
- Natural Sciences and Engineering Research Council (NSERC) of Canada
- Natural Resources Canada - Clean Growth Program
- Ontario Research Fund-Research Excellence program
- Canada Foundation for Innovation
- Government of Ontario
- Ontario Research Fund Research Excellence Program
- University of Toronto
- U.S. DOE [DE-AC02-06CH11357]
- Canadian Light Source
- program of China Scholarships Council [201906745001]
Electroreduction uses renewable energy to upgrade carbon dioxide to value-added chemicals and fuels. Renewable methane synthesized using such a route stands to be readily deployed using existing infrastructure for the distribution and utilization of natural gas. Here we design a suite of ligand-stabilized metal oxide clusters and find that these modulate carbon dioxide reduction pathways on a copper catalyst, enabling thereby a record activity for methane electroproduction. Density functional theory calculations show adsorbed hydrogen donation from clusters to copper active sites for the *CO hydrogenation pathway towards *CHO. We promote this effect via control over cluster size and composition and demonstrate the effect on metal oxides including cobalt(II), molybdenum(VI), tungsten(VI), nickel(II) and palladium(II) oxides. We report a carbon dioxide-to-methane faradaic efficiency of 60% at a partial current density to methane of 135 milliampere per square centimetre. We showcase operation over 18h that retains a faradaic efficiency exceeding 55%.
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