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Selective reduction of CO to acetaldehyde with CuAg electrocatalysts.
Wang, Lei; Higgins, Drew C; Ji, Yongfei; Morales-Guio, Carlos G; Chan, Karen; Hahn, Christopher; Jaramillo, Thomas F.
Afiliação
  • Wang L; SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, CA 94305.
  • Higgins DC; SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, CA 94305.
  • Ji Y; SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, CA 94025.
  • Morales-Guio CG; Department of Chemical Engineering, McMaster University, Hamilton, ON L8S 4L8, Canada.
  • Chan K; SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, CA 94305.
  • Hahn C; SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, CA 94305.
  • Jaramillo TF; SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, CA 94025.
Proc Natl Acad Sci U S A ; 117(23): 12572-12575, 2020 06 09.
Artigo em Inglês | MEDLINE | ID: mdl-31980521
ABSTRACT
Electrochemical CO reduction can serve as a sequential step in the transformation of CO2 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.
Texto completo: Disponível Coleções: Bases de dados internacionais Base de dados: MEDLINE Idioma: Inglês Revista: Proc Natl Acad Sci U S A Ano de publicação: 2020 Tipo de documento: Artigo

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Texto completo: Disponível Coleções: Bases de dados internacionais Base de dados: MEDLINE Idioma: Inglês Revista: Proc Natl Acad Sci U S A Ano de publicação: 2020 Tipo de documento: Artigo
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