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Engineering electrocatalytic activity in nanosized perovskite cobaltite through surface spin-state transition

Author

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  • Shiming Zhou

    (Hefei National Laboratory for Physics Sciences at the Microscale, Hefei Science Center, University of Science and Technology of China)

  • Xianbing Miao

    (Hefei National Laboratory for Physics Sciences at the Microscale, Hefei Science Center, University of Science and Technology of China)

  • Xu Zhao

    (Hefei National Laboratory for Physics Sciences at the Microscale, Hefei Science Center, University of Science and Technology of China)

  • Chao Ma

    (Hefei National Laboratory for Physics Sciences at the Microscale, Hefei Science Center, University of Science and Technology of China)

  • Yuhao Qiu

    (School of Physics, Nankai University)

  • Zhenpeng Hu

    (School of Physics, Nankai University
    State Key Laboratory of Luminescent Materials and Devices, South China University of Technology)

  • Jiyin Zhao

    (Hefei National Laboratory for Physics Sciences at the Microscale, Hefei Science Center, University of Science and Technology of China)

  • Lei Shi

    (Hefei National Laboratory for Physics Sciences at the Microscale, Hefei Science Center, University of Science and Technology of China)

  • Jie Zeng

    (Hefei National Laboratory for Physics Sciences at the Microscale, Hefei Science Center, University of Science and Technology of China)

Abstract

The activity of electrocatalysts exhibits a strongly dependence on their electronic structures. Specifically, for perovskite oxides, Shao-Horn and co-workers have reported a correlation between the oxygen evolution reaction activity and the eg orbital occupation of transition-metal ions, which provides guidelines for the design of highly active catalysts. Here we demonstrate a facile method to engineer the eg filling of perovskite cobaltite LaCoO3 for improving the oxygen evolution reaction activity. By reducing the particle size to ∼80 nm, the eg filling of cobalt ions is successfully increased from unity to near the optimal configuration of 1.2 expected by Shao-Horn’s principle. Consequently, the activity is significantly enhanced, comparable to those of recently reported cobalt oxides with eg∼1.2 configurations. This enhancement is ascribed to the emergence of spin-state transition from low-spin to high-spin states for cobalt ions at the surface of the nanoparticles, leading to more active sites with increased reactivity.

Suggested Citation

  • Shiming Zhou & Xianbing Miao & Xu Zhao & Chao Ma & Yuhao Qiu & Zhenpeng Hu & Jiyin Zhao & Lei Shi & Jie Zeng, 2016. "Engineering electrocatalytic activity in nanosized perovskite cobaltite through surface spin-state transition," Nature Communications, Nature, vol. 7(1), pages 1-7, September.
    • Handle: RePEc:nat:natcom:v:7:y:2016:i:1:d:10.1038_ncomms11510
    DOI: 10.1038/ncomms11510
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    Cited by:

    1. Xingyu Ding & Da Liu & Pengju Zhao & Xing Chen & Hongxia Wang & Freddy E. Oropeza & Giulio Gorni & Mariam Barawi & Miguel García-Tecedor & Víctor A. Peña O’Shea & Jan P. Hofmann & Jianfeng Li & Jongky, 2024. "Dynamic restructuring of nickel sulfides for electrocatalytic hydrogen evolution reaction," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    2. Xin Zhang & Haoyin Zhong & Qi Zhang & Qihan Zhang & Chao Wu & Junchen Yu & Yifan Ma & Hang An & Hao Wang & Yiming Zou & Caozheng Diao & Jingsheng Chen & Zhi Gen Yu & Shibo Xi & Xiaopeng Wang & Junmin , 2024. "High-spin Co3+ in cobalt oxyhydroxide for efficient water oxidation," Nature Communications, Nature, vol. 15(1), pages 1-10, December.

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