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Mechanistic insight into the active centers of single/dual-atom Ni/Fe-based oxygen electrocatalysts

Author

Listed:
  • Wenchao Wan

    (University of Zurich)

  • Yonggui Zhao

    (University of Zurich)

  • Shiqian Wei

    (Leshan Normal University)

  • Carlos A. Triana

    (University of Zurich)

  • Jingguo Li

    (University of Zurich)

  • Andrea Arcifa

    (Empa, Swiss Federal Institute for Materials Science and Technology)

  • Christopher S. Allen

    (Diamond Light Source Ltd
    University of Oxford)

  • Rui Cao

    (SLAC National Accelerator Laboratory)

  • Greta R. Patzke

    (University of Zurich)

Abstract

Single-atom catalysts with maximum metal utilization efficiency show great potential for sustainable catalytic applications and fundamental mechanistic studies. We here provide a convenient molecular tailoring strategy based on graphitic carbon nitride as support for the rational design of single-site and dual-site single-atom catalysts. Catalysts with single Fe sites exhibit impressive oxygen reduction reaction activity with a half-wave potential of 0.89 V vs. RHE. We find that the single Ni sites are favorable to promote the key structural reconstruction into bridging Ni-O-Fe bonds in dual-site NiFe SAC. Meanwhile, the newly formed Ni-O-Fe bonds create spin channels for electron transfer, resulting in a significant improvement of the oxygen evolution reaction activity with an overpotential of 270 mV at 10 mA cm−2. We further reveal that the water oxidation reaction follows a dual-site pathway through the deprotonation of *OH at both Ni and Fe sites, leading to the formation of bridging O2 atop the Ni-O-Fe sites.

Suggested Citation

  • Wenchao Wan & Yonggui Zhao & Shiqian Wei & Carlos A. Triana & Jingguo Li & Andrea Arcifa & Christopher S. Allen & Rui Cao & Greta R. Patzke, 2021. "Mechanistic insight into the active centers of single/dual-atom Ni/Fe-based oxygen electrocatalysts," Nature Communications, Nature, vol. 12(1), pages 1-13, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-25811-0
    DOI: 10.1038/s41467-021-25811-0
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    Cited by:

    1. Zeyu Wang & William A. Goddard & Hai Xiao, 2023. "Potential-dependent transition of reaction mechanisms for oxygen evolution on layered double hydroxides," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    2. Zhongkai Xie & Shengjie Xu & Longhua Li & Shanhe Gong & Xiaojie Wu & Dongbo Xu & Baodong Mao & Ting Zhou & Min Chen & Xiao Wang & Weidong Shi & Shuyan Song, 2024. "Well-defined diatomic catalysis for photosynthesis of C2H4 from CO2," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    3. Cong Fang & Jian Zhou & Lili Zhang & Wenchao Wan & Yuxiao Ding & Xiaoyan Sun, 2023. "Synergy of dual-atom catalysts deviated from the scaling relationship for oxygen evolution reaction," Nature Communications, Nature, vol. 14(1), pages 1-14, December.
    4. Hongqiang Jin & Kaixin Zhou & Ruoxi Zhang & Hongjie Cui & Yu Yu & Peixin Cui & Weiguo Song & Changyan Cao, 2023. "Regulating the electronic structure through charge redistribution in dense single-atom catalysts for enhanced alkene epoxidation," Nature Communications, Nature, vol. 14(1), pages 1-10, December.

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