期刊
ACS ENERGY LETTERS
卷 6, 期 9, 页码 3252-3260出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.1c01485
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资金
- U.S. Department of Energy, Office of Science, Office of Advanced Scientific Computing Research, Scientific Discovery through Advanced Computing (SciDAC) program
- Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]
- Liquid Sunlight Alliance - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Fuels from Sunlight Hub [DE-SC0021266]
- Knut and Alice Wallenberg foundation [2019.0586]
- College of Chemistry at the University of California, Berkeley [NIH S10OD023532]
This research theoretically studied the role of roughened copper electrodes in the CO2 electroreduction process, revealing a potential mechanism for enhancing selectivity to C2+ products on copper. Design rules were proposed to maximize selectivity based on the findings.
Roughened copper electrodes, including those derived from cuprous oxide, have long been known to exhibit an enhanced Faradaic efficiency to C2+ products during CO2 electroreduction. However, the source of this enhancement has not been rationalized mechanistically. In this work, we present a theoretical study of roughened copper electrodes derived from cuprous oxide, phosphide, nitride, and sulfide. We utilize a carefully benchmarked effective medium theory potential to develop geometric models of the roughened electrodes on an unprecedented scale. Using density functional theory with an implicit electrolyte, we determine applied bias dependent binding energy distributions for critical reaction intermediates. We apply simple thermodynamic models to evaluate the role of surface roughening on selectivity during CO2 electroreduction. We find that the manner of roughening (i.e., starting from oxide, phosphide, sulfide, or nitride) does not significantly affect the binding energy distributions found, and we suggest design rules to maximize selectivity to C2+ products on copper.
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