Journal
NATURE COMMUNICATIONS
Volume 10, Issue -, Pages -Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-019-13833-8
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Funding
- Suncor Energy
- Ontario Research Fund
- Natural Sciences and Engineering Research Council (NSERC)
- Southern Ontario Smart Computing Innovation Platform (SOSCIP)
- 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
- 15 Ontario academic member institutions
- Canada Foundation for Innovation
- Ontario Research Fund - Research Excellence
- University of Toronto
- U.S. DOE [DE-AC02-06CH11357]
- Canadian Light Source
- Banting Postdoctoral Fellowships program
- NSERC E.W.R Steacie Memorial Fellowship
- Government of Ontario
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Producing liquid fuels such as ethanol from CO2, H2O, and renewable electricity offers a route to store sustainable energy. The search for efficient electrocatalysts for the CO2 reduction reaction relies on tuning the adsorption strength of carbonaceous intermediates. Here, we report a complementary approach in which we utilize hydroxide and oxide doping of a catalyst surface to tune the adsorbed hydrogen on Cu. Density functional theory studies indicate that this doping accelerates water dissociation and changes the hydrogen adsorption energy on Cu. We synthesize and investigate a suite of metal-hydroxide-interface-doped-Cu catalysts, and find that the most efficient, Ce(OH)(x)-doped-Cu, exhibits an ethanol Faradaic efficiency of 43% and a partial current density of 128 mA cm(-2). Mechanistic studies, wherein we combine investigation of hydrogen evolution performance with the results of operando Raman spectroscopy, show that adsorbed hydrogen hydrogenates surface (HCCOH)-H-star, a key intermediate whose fate determines branching to ethanol versus ethylene.
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