Journal
JOULE
Volume 1, Issue 4, Pages 794-805Publisher
CELL PRESS
DOI: 10.1016/j.joule.2017.09.014
Keywords
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Funding
- Ontario Research Fund - Research Excellence Program [RE08-034]
- NSERC [RGPIN-2017-06477]
- CIFAR Bio-Inspired Solar Energy program [FL-000560]
- Director, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, & Biosciences Division, of the U.S. Department of Energy [DE-AC02-05CH11231]
- FWP [CH030201]
- National Basic Research Program of China [2014CB931703]
- Natural Science Foundation of China [51471115, 51571149]
- China Scholarship Council (CSC) [20140625004]
- Canada Graduate Scholarship - Doctoral (CGS-D)
- Natural Sciences and Engineering Research Council of Canada
- National Research Council Canada
- Canadian Institutes of Health Research
- Province of Saskatchewan, Western Economic Diversification Canada
- University of Saskatchewan
- Director, Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231]
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Electrochemical reduction of carbon dioxide (CO2RR) to formate provides an avenue to the synthesis of value-added carbon-based fuels and feedstocks powered using renewable electricity. Here, we hypothesized that the presence of sulfur atoms in the catalyst surface could promote undercoordinated sites, and thereby improve the electrochemical reduction of CO2 to formate. We explored, using density functional theory, how the incorporation of sulfur into tin may favor formate generation. We used atomic layer deposition of SnSx followed by a reduction process to synthesize sulfur-modulated tin (Sn(S)) catalysts. X-ray absorption near-edge structure (XANES) studies reveal higher oxidation states in Sn(S) compared with that of tin in Sn nanoparticles. Sn(S)/Au accelerates CO2RR at geometric current densities of 55 mA cm(-2) at -0.75 V versus reversible hydrogen electrode with a Faradaic efficiency of 93%. Furthermore, Sn(S) catalysts show excellent stability without deactivation (<2% productivity change) following more than 40 hours of operation.
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