Intrinsic ORR Activity Enhancement of Pt Atomic Sites by Engineering the <i>d</i>‐Band Center via Local Coordination Tuning

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  • Xiaofeng Zhu
    School of Chemical Engineering University of New South Wales Sydney NSW 2052 Australia
  • Xin Tan
    Integrated Materials Design Laboratory, Department of Applied Mathematics, Research School of Physics The Australian National University Canberra ACT 2601 Australia
  • Kuang‐Hsu Wu
    School of Chemical Engineering University of New South Wales Sydney NSW 2052 Australia
  • Shu‐Chih Haw
    Nano-science Group National Synchrotron Radiation Research Center Hsinchu 30076 Taiwan
  • Chih‐Wen Pao
    Experimental Facility Division National Synchrotron Radiation Research Center Hsinchu 30076 Taiwan
  • Bing‐Jian Su
    Department of Electrophysics National Chiao Tung University Hsinchu 30076 Taiwan
  • Junjie Jiang
    School of Chemical Engineering University of New South Wales Sydney NSW 2052 Australia
  • Sean C. Smith
    Integrated Materials Design Laboratory, Department of Applied Mathematics, Research School of Physics The Australian National University Canberra ACT 2601 Australia
  • Jin‐Ming Chen
    Nano-science Group National Synchrotron Radiation Research Center Hsinchu 30076 Taiwan
  • Rose Amal
    School of Chemical Engineering University of New South Wales Sydney NSW 2052 Australia
  • Xunyu Lu
    School of Chemical Engineering University of New South Wales Sydney NSW 2052 Australia

説明

<jats:title>Abstract</jats:title><jats:p>A considerable amount of platinum (Pt) is required to ensure an adequate rate for the oxygen reduction reaction (ORR) in fuel cells and metal‐air batteries. Thus, the implementation of atomic Pt catalysts holds promise for minimizing the Pt content. In this contribution, atomic Pt sites with nitrogen (N) and phosphorus (P) co‐coordination on a carbon matrix (PtNPC) are conceptually predicted and experimentally developed to alter the d‐band center of Pt, thereby promoting the intrinsic ORR activity. PtNPC with a record‐low Pt content (≈0.026 wt %) consequently shows a benchmark‐comparable activity for ORR with an onset of 1.0 V<jats:sub>RHE</jats:sub> and half‐wave potential of 0.85 V<jats:sub>RHE</jats:sub>. It also features a high stability in 15 000‐cycle tests and a superior turnover frequency of 6.80 s<jats:sup>−1</jats:sup> at 0.9 V<jats:sub>RHE</jats:sub>. Damjanovic kinetics analysis reveals a tuned ORR kinetics of PtNPC from a mixed 2/4‐electron to a predominately 4‐electron route. It is discovered that coordinated P species significantly shifts d‐band center of Pt atoms, accounting for the exceptional performance of PtNPC.</jats:p>

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