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Insights into the activity of single-atom Fe-N-C catalysts for oxygen reduction reaction

Author

Listed:
  • Kang Liu

    (Central South University
    Central South University)

  • Junwei Fu

    (Central South University)

  • Yiyang Lin

    (Central South University)

  • Tao Luo

    (Central South University)

  • Ganghai Ni

    (Central South University)

  • Hongmei Li

    (Central South University)

  • Zhang Lin

    (Central South University)

  • Min Liu

    (Central South University)

Abstract

Single-atom Fe-N-C catalysts has attracted widespread attentions in the oxygen reduction reaction (ORR). However, the origin of ORR activity on Fe-N-C catalysts is still unclear, which hinder the further improvement of Fe-N-C catalysts. Herein, we provide a model to understand the ORR activity of Fe-N4 site from the spatial structure and energy level of the frontier orbitals by density functional theory calculations. Taking the regulation of divacancy defects on Fe-N4 site ORR activity as examples, we demonstrate that the hybridization between Fe 3dz2, 3dyz (3dxz) and O2 π* orbitals is the origin of Fe-N4 ORR activity. We found that the Fe–O bond length, the d-band center gap of spin states, the magnetic moment of Fe site and *O2 as descriptors can accurately predict the ORR activity of Fe-N4 site. Furthermore, these descriptors and ORR activity of Fe-N4 site are mainly distributed in two regions with obvious difference, which greatly relate to the height of Fe 3d projected orbital in the Z direction. This work provides a new insight into the ORR activity of single-atom M-N-C catalysts.

Suggested Citation

  • Kang Liu & Junwei Fu & Yiyang Lin & Tao Luo & Ganghai Ni & Hongmei Li & Zhang Lin & Min Liu, 2022. "Insights into the activity of single-atom Fe-N-C catalysts for oxygen reduction reaction," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-29797-1
    DOI: 10.1038/s41467-022-29797-1
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    References listed on IDEAS

    as
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