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In situ modulating coordination fields of single-atom cobalt catalyst for enhanced oxygen reduction reaction

Author

Listed:
  • Meihuan Liu

    (University of Science and Technology of China
    Central South University)

  • Jing Zhang

    (University of Science and Technology of China)

  • Hui Su

    (Hunan Normal University)

  • Yaling Jiang

    (University of Science and Technology of China)

  • Wanlin Zhou

    (University of Science and Technology of China)

  • Chenyu Yang

    (University of Science and Technology of China)

  • Shuowen Bo

    (University of Science and Technology of China)

  • Jun Pan

    (Central South University)

  • Qinghua Liu

    (University of Science and Technology of China)

Abstract

Single-atom catalysts, especially those with metal−N4 moieties, hold great promise for facilitating the oxygen reduction reaction. However, the symmetrical distribution of electrons within the metal−N4 moiety results in unsatisfactory adsorption strength of intermediates, thereby limiting their performance improvements. Herein, we present atomically coordination-regulated Co single-atom catalysts that comprise a symmetry-broken Cl−Co−N4 moiety, which serves to break the symmetrical electron distribution. In situ characterizations reveal the dynamic evolution of the symmetry-broken Cl−Co−N4 moiety into a coordination-reduced Cl−Co−N2 structure, effectively optimizing the 3d electron filling of Co sites toward a reduced d-band electron occupancy (d5.8 → d5.28) under reaction conditions for a fast four-electron oxygen reduction reaction process. As a result, the coordination-regulated Co single-atom catalysts deliver a large half-potential of 0.93 V and a mass activity of 5480 A gmetal−1. Importantly, a Zn-air battery using the coordination-regulated Co single-atom catalysts as the cathode also exhibits a large power density and excellent stability.

Suggested Citation

  • Meihuan Liu & Jing Zhang & Hui Su & Yaling Jiang & Wanlin Zhou & Chenyu Yang & Shuowen Bo & Jun Pan & Qinghua Liu, 2024. "In situ modulating coordination fields of single-atom cobalt catalyst for enhanced oxygen reduction reaction," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-45990-w
    DOI: 10.1038/s41467-024-45990-w
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    References listed on IDEAS

    as
    1. Wanlin Zhou & Hui Su & Weiren Cheng & Yuanli Li & Jingjing Jiang & Meihuan Liu & Feifan Yu & Wei Wang & Shiqiang Wei & Qinghua Liu, 2022. "Regulating the scaling relationship for high catalytic kinetics and selectivity of the oxygen reduction reaction," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    2. Huishan Shang & Xiangyi Zhou & Juncai Dong & Ang Li & Xu Zhao & Qinghua Liu & Yue Lin & Jiajing Pei & Zhi Li & Zhuoli Jiang & Danni Zhou & Lirong Zheng & Yu Wang & Jing Zhou & Zhengkun Yang & Rui Cao , 2020. "Engineering unsymmetrically coordinated Cu-S1N3 single atom sites with enhanced oxygen reduction activity," Nature Communications, Nature, vol. 11(1), pages 1-11, December.
    3. Ruijie Gao & Jian Wang & Zhen-Feng Huang & Rongrong Zhang & Wei Wang & Lun Pan & Junfeng Zhang & Weikang Zhu & Xiangwen Zhang & Chengxiang Shi & Jongwoo Lim & Ji-Jun Zou, 2021. "Pt/Fe2O3 with Pt–Fe pair sites as a catalyst for oxygen reduction with ultralow Pt loading," Nature Energy, Nature, vol. 6(6), pages 614-623, June.
    4. Hui Su & Wanlin Zhou & Wu Zhou & Yuanli Li & Lirong Zheng & Hui Zhang & Meihuan Liu & Xiuxiu Zhang & Xuan Sun & Yanzhi Xu & Fengchun Hu & Jing Zhang & Tiandou Hu & Qinghua Liu & Shiqiang Wei, 2021. "In-situ spectroscopic observation of dynamic-coupling oxygen on atomically dispersed iridium electrocatalyst for acidic water oxidation," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
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    Cited by:

    1. Geng Zhang & Wei Guo & Hong Zheng & Xiang Li & Jinxin Wang & Qiuyu Zhang, 2024. "Identifying and tuning coordinated water molecules for efficient electrocatalytic water oxidation," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    2. Yanfeng Shi & Lupeng Wang & Miao Liu & Zuozheng Xu & Peilin Huang & Lizhe Liu & Yuanhong Xu, 2025. "Electron–phonon coupling and coherent energy superposition induce spin-sensitive orbital degeneracy for enhanced acidic water oxidation," Nature Communications, Nature, vol. 16(1), pages 1-13, December.
    3. Zhen Zhang & Zhenyu Xing & Xianglin Luo & Chong Cheng & Xikui Liu, 2025. "Densely populated macrocyclic dicobalt sites in ladder polymers for low-overpotential oxygen reduction catalysis," Nature Communications, Nature, vol. 16(1), pages 1-12, December.

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