期刊
ACS APPLIED MATERIALS & INTERFACES
卷 13, 期 12, 页码 14050-14055出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c17668
关键词
electrochemical CO2 reduction; pulsed potential; temperature; ethylene; ethanol
资金
- National Science Foundation (NSF) [CBET-1805400]
- NSF MRSEC program [DMR-1719875]
The study demonstrates the enhancement of ethylene selectivity and achievement of selectivity towards either ethylene or ethanol by using pulsed overpotentials. The improved CO dimerization kinetics on active Cu surface and reduced hydrogen adsorption coverage during pulsed CO2RR are crucial for achieving this goal.
The electrochemical CO2 reduction reaction (CO2RR) can convert widely available CO2 into value-added C-2 products, such as ethylene and ethanol. However, low selectivity toward either compound limits the effectiveness of current CO2RR electrocatalysts. Here, we report the use of pulsed overpotentials to improve the ethylene selectivity to 67% with >75% overall C-2 selectivity on (100)-textured polycrystalline Cu foil. The pulsed CO2RR can be made selective to either ethylene or ethanol by controlling the reaction temperature. We attribute the enhanced C-2 selectivity to the improved CO dimerization kinetics on the active Cu surface on predominately (100)-textured Cu grains with the reduced hydrogen adsorption coverage during the pulsed CO2RR. The ethylene vs ethanol selectivity can be explained by the reducibility of the Cu(I) species during the cathodic potential cycle. Our work demonstrates a simple route to improve the ethylene vs ethanol selectivity and identifies Cu(I) as the species responsible for ethanol production.
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