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  • 标题:Selective reduction of CO to acetaldehyde with CuAg electrocatalysts
  • 本地全文:下载
  • 作者:Lei Wang ; Drew C. Higgins ; Yongfei Ji
  • 期刊名称:Proceedings of the National Academy of Sciences
  • 印刷版ISSN:0027-8424
  • 电子版ISSN:1091-6490
  • 出版年度:2020
  • 卷号:117
  • 期号:23
  • 页码:12572-12575
  • DOI:10.1073/pnas.1821683117
  • 出版社:The National Academy of Sciences of the United States of America
  • 摘要:Electrochemical CO reduction can serve as a sequential step in the transformation of CO 2 into multicarbon fuels and chemicals. In this study, we provide insights on how to steer selectivity for CO reduction almost exclusively toward a single multicarbon oxygenate by carefully controlling the catalyst composition and its surrounding reaction conditions. Under alkaline reaction conditions, we demonstrate that planar CuAg electrodes can reduce CO to acetaldehyde with over 50% Faradaic efficiency and over 90% selectivity on a carbon basis at a modest electrode potential of −0.536 V vs. the reversible hydrogen electrode. The Faradaic efficiency to acetaldehyde was further enhanced to 70% by increasing the roughness factor of the CuAg electrode. Density functional theory calculations indicate that Ag ad-atoms on Cu weaken the binding energy of the reduced acetaldehyde intermediate and inhibit its further reduction to ethanol, demonstrating that the improved selectivity to acetaldehyde is due to the electronic effect from Ag incorporation. These findings will aid in the design of catalysts that are able to guide complex reaction networks and achieve high selectivity for the desired product.
  • 关键词:electrocatalysis ; CO 2 reduction ; CO reduction ; bimetallics ; heterogeneous catalysis
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