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<p>Precisely regulating active sites is vital for promoting the oxygen reduction reaction (ORR) activity. Here we reported highly active Ni-Pd co-doped N-coordinated graphene towards ORR achieved by edge termination and O doping. Our first-principles calculations demonstrated that edge termination effectively boost the ORR activity, and armchair-edge termination was energetically more favorable than zigzag-edge termination. Notably, after O doping Ni-Pd active center, armchair edge-terminated Ni-Pd active site exhibited better ORR activity, and the lowest overpotential was only 0.31&#xa0;V. This improvement in activity was attributed to the shift of the <i>d</i>-band center of Ni atom toward the Fermi-level and the shift of the <i>d</i>-band center of Pd atom away from the Fermi-level, thus regulating the *OH adsorption strength. This work paves the way for developing highly active graphene-based dual-atom catalysts for ORR through edge and doping engineering.</p>

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Engineering the coordination environment of Ni and Pd dual active sites for promoting the oxygen reduction reaction

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年3月14日

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  • Lei Li,
  • Xiaoxia Wu,
  • Ruotong Zhang,
  • Narsu Bai,
  • Min Zhang,
  • Yuhua Wen

摘要

Precisely regulating active sites is vital for promoting the oxygen reduction reaction (ORR) activity. Here we reported highly active Ni-Pd co-doped N-coordinated graphene towards ORR achieved by edge termination and O doping. Our first-principles calculations demonstrated that edge termination effectively boost the ORR activity, and armchair-edge termination was energetically more favorable than zigzag-edge termination. Notably, after O doping Ni-Pd active center, armchair edge-terminated Ni-Pd active site exhibited better ORR activity, and the lowest overpotential was only 0.31 V. This improvement in activity was attributed to the shift of the d-band center of Ni atom toward the Fermi-level and the shift of the d-band center of Pd atom away from the Fermi-level, thus regulating the *OH adsorption strength. This work paves the way for developing highly active graphene-based dual-atom catalysts for ORR through edge and doping engineering.