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Lanthanide-regulating Ru-O covalency optimizes acidic oxygen evolution electrocatalysis

Author

Listed:
  • Lu Li

    (Peking University)

  • Gengwei Zhang

    (Kunming University of Science and Technology)

  • Chenhui Zhou

    (Peking University)

  • Fan Lv

    (Peking University)

  • Yingjun Tan

    (Peking University)

  • Ying Han

    (Peking University)

  • Heng Luo

    (Peking University)

  • Dawei Wang

    (Peking University)

  • Youxing Liu

    (Peking University)

  • Changshuai Shang

    (Peking University)

  • Lingyou Zeng

    (Peking University)

  • Qizheng Huang

    (Peking University)

  • Ruijin Zeng

    (Peking University)

  • Na Ye

    (Peking University)

  • Mingchuan Luo

    (Peking University)

  • Shaojun Guo

    (Peking University)

Abstract

Precisely modulating the Ru-O covalency in RuOx for enhanced stability in proton exchange membrane water electrolysis is highly desired. However, transition metals with d-valence electrons, which were doped into or alloyed with RuOx, are inherently susceptible to the influence of coordination environment, making it challenging to modulate the Ru-O covalency in a precise and continuous manner. Here, we first deduce that the introduction of lanthanide with gradually changing electronic configurations can continuously modulate the Ru-O covalency owing to the shielding effect of 5s/5p orbitals. Theoretical calculations confirm that the durability of Ln-RuOx following a volcanic trend as a function of Ru-O covalency. Among various Ln-RuOx, Er-RuOx is identified as the optimal catalyst and possesses a stability 35.5 times higher than that of RuO2. Particularly, the Er-RuOx-based device requires only 1.837 V to reach 3 A cm−2 and shows a long-term stability at 500 mA cm−2 for 100 h with a degradation rate of mere 37 μV h−1.

Suggested Citation

  • Lu Li & Gengwei Zhang & Chenhui Zhou & Fan Lv & Yingjun Tan & Ying Han & Heng Luo & Dawei Wang & Youxing Liu & Changshuai Shang & Lingyou Zeng & Qizheng Huang & Ruijin Zeng & Na Ye & Mingchuan Luo & S, 2024. "Lanthanide-regulating Ru-O covalency optimizes acidic oxygen evolution electrocatalysis," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-49281-2
    DOI: 10.1038/s41467-024-49281-2
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    References listed on IDEAS

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    1. Qianqian Ji & Bing Tang & Xilin Zhang & Chao Wang & Hao Tan & Jie Zhao & Ruiqi Liu & Mei Sun & Hengjie Liu & Chang Jiang & Jianrong Zeng & Xingke Cai & Wensheng Yan, 2024. "Operando identification of the oxide path mechanism with different dual-active sites for acidic water oxidation," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    2. Chenhui Zhou & Lu Li & Zhaoqi Dong & Fan Lv & Hongyu Guo & Kai Wang & Menggang Li & Zhengyi Qian & Na Ye & Zheng Lin & Mingchuan Luo & Shaojun Guo, 2024. "Pinning effect of lattice Pb suppressing lattice oxygen reactivity of Pb-RuO2 enables stable industrial-level electrolysis," Nature Communications, Nature, vol. 15(1), pages 1-9, December.

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