期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 62, 期 36, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202308782
关键词
CO2 reduction; Electrocatalysis; Electrochemistry; Isotopic Labelling; Tandem Catalysis
Electrochemical CO2 reduction (CO2R) in acidic media with Cu-based catalysts tends to suffer from lowered selectivity towards multicarbon products. Tandem catalysis, using a CO generating catalyst (e.g. Ag) in close proximity to increase *CO coverage on Cu, is impeded in acidic electrolyte. Co-reduction experiments of CO2 and CO mixtures with Cu and CuAg catalysts provide evidence for tandem catalysis in neutral media and its curtailment under acidic conditions. Density functional theory simulations suggest that the presence of H3O+ weakens the *CO binding energy of Cu, preventing effective utilization of tandem-supplied CO. These findings provide insights into the tandem catalysis reaction pathway and important design considerations for effective CO2R in acidic media.
Electrochemical CO2 reduction (CO2R) in acidic media with Cu-based catalysts tends to suffer from lowered selectivity towards multicarbon products. This could in principle be mitigated using tandem catalysis, whereby the *CO coverage on Cu is increased by introducing a CO generating catalyst (e.g. Ag) in close proximity. Although this has seen significant success in neutral/alkaline media, here we report that such a strategy becomes impeded in acidic electrolyte. This was investigated through the co-reduction of (CO2)-C-13/(CO)-C-12 mixtures using a series of Cu and CuAg catalysts. These experiments provide strong evidence for the occurrence of tandem catalysis in neutral media and its curtailment under acidic conditions. Density functional theory simulations suggest that the presence of H3O+ weakens the *CO binding energy of Cu, preventing effective utilization of tandem-supplied CO. Our findings also provide other unanticipated insights into the tandem catalysis reaction pathway and important design considerations for effective CO2R in acidic media.
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