Journal
NATURE CATALYSIS
Volume 2, Issue 12, Pages 1124-1131Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41929-019-0380-x
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Funding
- Ontario Research Fund: Research Excellence programme
- Natural Sciences and Engineering Research Council of Canada
- CIFAR Bio-inspired Solar Energy programme
- University of Toronto Connaught grant
- US Department of Energy [DE-AC02-06CH11357]
- Canadian Light Source
- Natural Sciences and Engineering Research Council
- Banting Postdoctoral Fellowships programme
- Southern Ontario Smart Computing Innovation Platform
- Niagara supercomputer at the SciNet HPC Consortium
- Federal Economic Development Agency of Southern Ontario
- Province of Ontario
- IBM Canada Ltd.
- Ontario Centres of Excellence
- Mitacs
- Canada Foundation for Innovation
- Government of Ontario
- Ontario Research Fund - Research Excellence
- University of Toronto
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The availability of inexpensive industrial CO gas streams motivates efficient electrocatalytic upgrading of CO to higher-value feedstocks such as ethylene. However, the electrosynthesis of ethylene by the CO reduction reaction (CORR) has suffered from low selectivity and energy efficiency. Here we find that the recent strategy of increasing performance through use of highly alkaline electrolyte-which is very effective in CO2RR-fails in CORR and drives the reaction to acetate. We then observe that ethylene selectivity increases when we constrain (decrease) CO availability. Using density functional theory, we show how CO coverage on copper influences the reaction pathways of ethylene versus oxygenate: lower CO coverage stabilizes the ethylene-relevant intermediates whereas higher CO coverage favours oxygenate formation. We then control local CO availability experimentally by tuning the CO concentration and reaction rate; we achieve ethylene Faradaic efficiencies of 72% and a partial current density of >800 mA cm(-2). The overall system provides a half-cell energy efficiency of 44% for ethylene production.
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