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Oxidation State and Surface Reconstruction of Cu under CO2 Reduction Conditions from In Situ X-ray Characterization.
Lee, Soo Hong; Lin, John C; Farmand, Maryam; Landers, Alan T; Feaster, Jeremy T; Avilés Acosta, Jaime E; Beeman, Jeffrey W; Ye, Yifan; Yano, Junko; Mehta, Apurva; Davis, Ryan C; Jaramillo, Thomas F; Hahn, Christopher; Drisdell, Walter S.
Afiliação
  • Lin JC; Department of Chemical Engineering, Stanford University, Stanford, California 94305, United States.
  • Farmand M; SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States.
  • Feaster JT; SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States.
  • Avilés Acosta JE; Department of Chemistry, Stanford University, Stanford, California 94305, United States.
  • Beeman JW; Department of Chemical Engineering, Stanford University, Stanford, California 94305, United States.
  • Ye Y; SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States.
  • Yano J; SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States.
  • Mehta A; Department of Materials Science and Engineering, Stanford University, Stanford, California 94305, United States.
  • Jaramillo TF; Advanced Light Source, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, California 94720, United States.
  • Hahn C; Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, California 94720, United States.
  • Drisdell WS; Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States.
J Am Chem Soc ; 2020 Dec 31.
Artigo em Inglês | MEDLINE | ID: mdl-33382947
ABSTRACT
The electrochemical CO2 reduction reaction (CO2RR) using Cu-based catalysts holds great potential for producing valuable multi-carbon products from renewable energy. However, the chemical and structural state of Cu catalyst surfaces during the CO2RR remains a matter of debate. Here, we show the structural evolution of the near-surface region of polycrystalline Cu electrodes under in situ conditions through a combination of grazing incidence X-ray absorption spectroscopy (GIXAS) and X-ray diffraction (GIXRD). The in situ GIXAS reveals that the surface oxide layer is fully reduced to metallic Cu before the onset potential for CO2RR, and the catalyst maintains the metallic state across the potentials relevant to the CO2RR. We also find a preferential surface reconstruction of the polycrystalline Cu surface toward (100) facets in the presence of CO2. Quantitative analysis of the reconstruction profiles reveals that the degree of reconstruction increases with increasingly negative applied potentials, and it persists when the applied potential returns to more positive values. These findings show that the surface of Cu electrocatalysts is dynamic during the CO2RR, and emphasize the importance of in situ characterization to understand the surface structure and its role in electrocatalysis.
Texto completo: Disponível Coleções: Bases de dados internacionais Base de dados: MEDLINE Idioma: Inglês 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 Ano de publicação: 2020 Tipo de documento: Artigo
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