期刊
NATURE CATALYSIS
卷 1, 期 12, 页码 946-951出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/s41929-018-0168-4
关键词
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资金
- Ontario Research Fund Research-Excellence Program
- Natural Sciences and Engineering Research Council (NSERC) of Canada
- University of Toronto Connaught grant
- US DOE [DE-AC02-06CH11357]
- Canadian Light Source
- National Natural Science Foundation of China [21431006]
- Foundation for Innovative Research Groups of the National Natural Science Foundation of China [21521001]
- CIFAR Bio-Inspired Solar Energy program
The electrosynthesis of higher-order alcohols from carbon dioxide and carbon monoxide addresses the need for the long-term storage of renewable electricity; unfortunately, the present-day performance remains below what is needed for practical applications. Here we report a catalyst design strategy that promotes C3 formation via the nanoconfinement of C2 intermediates, and thereby promotes C2:C1 coupling inside a reactive nanocavity. We first employed finite-element method simulations to assess the potential for the retention and binding of C2 intermediates as a function of cavity structure. We then developed a method of synthesizing open Cu nanocavity structures with a tunable geometry via the electroreduction of Cu2O cavities formed through acidic etching. The nanocavities showed a morphology-driven shift in selectivity from C2 to C3 products during the carbon monoxide electroreduction, to reach a propanol Faradaic efficiency of 21 +/- 1% at a conversion rate of 7.8 +/- 0.5 mA cm(-2) at -0.56 V versus a reversible hydrogen electrode.
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