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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
    1. Kejun Chen & Kang Liu & Pengda An & Huangjingwei Li & Yiyang Lin & Junhua Hu & Chuankun Jia & Junwei Fu & Hongmei Li & Hui Liu & Zhang Lin & Wenzhang Li & Jiahang Li & Ying-Rui Lu & Ting-Shan Chan & N, 2020. "Iron phthalocyanine with coordination induced electronic localization to boost oxygen reduction reaction," Nature Communications, Nature, vol. 11(1), pages 1-8, December.
    2. Gege Yang & Jiawei Zhu & Pengfei Yuan & Yongfeng Hu & Gan Qu & Bang-An Lu & Xiaoyi Xue & Hengbo Yin & Wenzheng Cheng & Junqi Cheng & Wenjing Xu & Jin Li & Jinsong Hu & Shichun Mu & Jia-Nan Zhang, 2021. "Regulating Fe-spin state by atomically dispersed Mn-N in Fe-N-C catalysts with high oxygen reduction activity," Nature Communications, Nature, vol. 12(1), pages 1-10, December.
    3. Daobin Liu & Xiyu Li & Shuangming Chen & Huan Yan & Changda Wang & Chuanqiang Wu & Yasir A. Haleem & Sai Duan & Junling Lu & Binghui Ge & Pulickel M. Ajayan & Yi Luo & Jun Jiang & Li Song, 2019. "Atomically dispersed platinum supported on curved carbon supports for efficient electrocatalytic hydrogen evolution," Nature Energy, Nature, vol. 4(6), pages 512-518, June.
    4. Yuanjun Chen & Shufang Ji & Shu Zhao & Wenxing Chen & Juncai Dong & Weng-Chon Cheong & Rongan Shen & Xiaodong Wen & Lirong Zheng & Alexandre I. Rykov & Shichang Cai & Haolin Tang & Zhongbin Zhuang & C, 2018. "Enhanced oxygen reduction with single-atomic-site iron catalysts for a zinc-air battery and hydrogen-air fuel cell," Nature Communications, Nature, vol. 9(1), pages 1-12, December.
    5. Travis Marshall-Roth & Nicole J. Libretto & Alexandra T. Wrobel & Kevin J. Anderton & Michael L. Pegis & Nathan D. Ricke & Troy Van Voorhis & Jeffrey T. Miller & Yogesh Surendranath, 2020. "A pyridinic Fe-N4 macrocycle models the active sites in Fe/N-doped carbon electrocatalysts," Nature Communications, Nature, vol. 11(1), pages 1-14, December.
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