Elucidating the Electrocatalytic CO<sub>2</sub> Reduction Reaction over a Model Single‐Atom Nickel Catalyst

  • Song Liu
    CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences 457 Zhongshan Road Dalian 116023 China
  • Hong Bin Yang
    School of Chemical and Biomedical Engineering Nanyang Technological University 62 Nanyang Drive Singapore 637459 Singapore
  • Sung‐Fu Hung
    Department of Chemistry National (Taiwan) University No. 1, Sec. 4, Roosevelt Rd Taipei 10617 Taiwan
  • Jie Ding
    CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences 457 Zhongshan Road Dalian 116023 China
  • Weizheng Cai
    School of Chemical and Biomedical Engineering Nanyang Technological University 62 Nanyang Drive Singapore 637459 Singapore
  • Linghui Liu
    CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences 457 Zhongshan Road Dalian 116023 China
  • Jiajian Gao
    School of Chemical and Biomedical Engineering Nanyang Technological University 62 Nanyang Drive Singapore 637459 Singapore
  • Xuning Li
    School of Chemical and Biomedical Engineering Nanyang Technological University 62 Nanyang Drive Singapore 637459 Singapore
  • Xinyi Ren
    CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences 457 Zhongshan Road Dalian 116023 China
  • Zhichong Kuang
    CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences 457 Zhongshan Road Dalian 116023 China
  • Yanqiang Huang
    CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences 457 Zhongshan Road Dalian 116023 China
  • Tao Zhang
    CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences 457 Zhongshan Road Dalian 116023 China
  • Bin Liu
    School of Chemical and Biomedical Engineering Nanyang Technological University 62 Nanyang Drive Singapore 637459 Singapore

書誌事項

公開日
2019-12-10
権利情報
  • http://onlinelibrary.wiley.com/termsAndConditions#vor
DOI
  • 10.1002/anie.201911995
公開者
Wiley

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説明

<jats:title>Abstract</jats:title><jats:p>Designing effective electrocatalysts for the carbon dioxide reduction reaction (CO<jats:sub>2</jats:sub>RR) is an appealing approach to tackling the challenges posed by rising CO<jats:sub>2</jats:sub> levels and realizing a closed carbon cycle. However, fundamental understanding of the complicated CO<jats:sub>2</jats:sub>RR mechanism in CO<jats:sub>2</jats:sub> electrocatalysis is still lacking because model systems are limited. We have designed a model nickel single‐atom catalyst (Ni SAC) with a uniform structure and well‐defined Ni‐N<jats:sub>4</jats:sub> moiety on a conductive carbon support with which to explore the electrochemical CO<jats:sub>2</jats:sub>RR. Operando X‐ray absorption near‐edge structure spectroscopy, Raman spectroscopy, and near‐ambient X‐ray photoelectron spectroscopy, revealed that Ni<jats:sup>+</jats:sup> in the Ni SAC was highly active for CO<jats:sub>2</jats:sub> activation, and functioned as an authentic catalytically active site for the CO<jats:sub>2</jats:sub>RR. Furthermore, through combination with a kinetics study, the rate‐determining step of the CO<jats:sub>2</jats:sub>RR was determined to be *CO<jats:sub>2</jats:sub><jats:sup>−</jats:sup>+H<jats:sup>+</jats:sup>→*COOH. This study tackles the four challenges faced by the CO<jats:sub>2</jats:sub>RR; namely, activity, selectivity, stability, and dynamics.</jats:p>

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