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Understanding the Origin of Highly Selective CO2 Electroreduction to CO on Ni,N-doped Carbon Catalysts.
Koshy, David M; Chen, Shucheng; Lee, Dong Un; Stevens, Michaela Burke; Abdellah, Ahmed M; Dull, Samuel M; Chen, Gan; Nordlund, Dennis; Gallo, Alessandro; Hahn, Christopher; Higgins, Drew C; Bao, Zhenan; Jaramillo, Thomas F.
Afiliação
  • Koshy DM; SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, Stanford, CA, 94305, USA.
  • Chen S; SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, Stanford, CA, 94305, USA.
  • Lee DU; SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, Stanford, CA, 94305, USA.
  • Stevens MB; SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, Stanford, CA, 94305, USA.
  • Abdellah AM; Department of Chemical Engineering, McMaster University, Hamilton, ON, Canada.
  • Dull SM; SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, Stanford, CA, 94305, USA.
  • Chen G; Department of Materials Science and Engineering, Stanford University, Stanford, CA, 94305, USA.
  • Nordlund D; Stanford Synchotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, CA, 94025, USA.
  • Gallo A; SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, CA, 94025, USA.
  • Hahn C; SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, CA, 94025, USA.
  • Higgins DC; Department of Chemical Engineering, McMaster University, Hamilton, ON, Canada.
  • Bao Z; SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, Stanford, CA, 94305, USA.
  • Jaramillo TF; SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, Stanford, CA, 94305, USA.
Angew Chem Int Ed Engl ; 59(10): 4043-4050, 2020 Mar 02.
Artigo em Inglês | MEDLINE | ID: mdl-31919948
ABSTRACT
Ni,N-doped carbon catalysts have shown promising catalytic performance for CO2 electroreduction (CO2 R) to CO; this activity has often been attributed to the presence of nitrogen-coordinated, single Ni atom active sites. However, experimentally confirming Ni-N bonding and correlating CO2 reduction (CO2 R) activity to these species has remained a fundamental challenge. We synthesized polyacrylonitrile-derived Ni,N-doped carbon electrocatalysts (Ni-PACN) with a range of pyrolysis temperatures and Ni loadings and correlated their electrochemical activity with extensive physiochemical characterization to rigorously address the origin of activity in these materials. We found that the CO2 R to CO partial current density increased with increased Ni content before plateauing at 2 wt % which suggests a dispersed Ni active site. These dispersed active sites were investigated by hard and soft X-ray spectroscopy, which revealed that pyrrolic nitrogen ligands selectively bind Ni atoms in a distorted square-planar geometry that strongly resembles the active sites of molecular metal-porphyrin catalysts.
Texto completo: Disponível Coleções: Bases de dados internacionais Base de dados: MEDLINE Idioma: Inglês Revista: Angew Chem Int Ed Engl Ano de publicação: 2020 Tipo de documento: Artigo País de afiliação: Estados Unidos

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Texto completo: Disponível Coleções: Bases de dados internacionais Base de dados: MEDLINE Idioma: Inglês Revista: Angew Chem Int Ed Engl Ano de publicação: 2020 Tipo de documento: Artigo País de afiliação: Estados Unidos
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