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Electronic-reconstruction-enhanced hydrogen evolution catalysis in oxide polymorphs

Author

Listed:
  • Yangyang Li

    (National University of Singapore)

  • Zhi Gen Yu

    (Institute of High Performance Computing)

  • Ling Wang

    (National University of Singapore)

  • Yakui Weng

    (Nanjing University of Posts and Telecommunications (NUPT))

  • Chi Sin Tang

    (National University of Singapore
    National University of Singapore)

  • Xinmao Yin

    (National University of Singapore
    National University of Singapore)

  • Kun Han

    (Nanyang Technological University)

  • Haijun Wu

    (National University of Singapore)

  • Xiaojiang Yu

    (National University of Singapore)

  • Lai Mun Wong

    (A*STAR (Agency for Science, Technology and Research))

  • Dongyang Wan

    (National University of Singapore)

  • Xiao Renshaw Wang

    (Nanyang Technological University)

  • Jianwei Chai

    (A*STAR (Agency for Science, Technology and Research))

  • Yong-Wei Zhang

    (Institute of High Performance Computing)

  • Shijie Wang

    (A*STAR (Agency for Science, Technology and Research))

  • John Wang

    (National University of Singapore)

  • Andrew T. S. Wee

    (National University of Singapore
    National University of Singapore)

  • Mark B. H. Breese

    (National University of Singapore)

  • Stephen J. Pennycook

    (National University of Singapore
    National University of Singapore
    National University of Singapore)

  • Thirumalai Venkatesan

    (National University of Singapore
    National University of Singapore
    National University of Singapore
    National University of Singapore)

  • Shuai Dong

    (Southeast University)

  • Jun Min Xue

    (National University of Singapore)

  • Jingsheng Chen

    (National University of Singapore)

Abstract

Transition metal oxides exhibit strong structure-property correlations, which has been extensively investigated and utilized for achieving efficient oxygen electrocatalysts. However, high-performance oxide-based electrocatalysts for hydrogen evolution are quite limited, and the mechanism still remains elusive. Here we demonstrate the strong correlations between the electronic structure and hydrogen electrocatalytic activity within a single oxide system Ti2O3. Taking advantage of the epitaxial stabilization, the polymorphism of Ti2O3 is extended by stabilizing bulk-absent polymorphs in the film-form. Electronic reconstructions are realized in the bulk-absent Ti2O3 polymorphs, which are further correlated to their electrocatalytic activity. We identify that smaller charge-transfer energy leads to a substantial enhancement in the electrocatalytic efficiency with stronger hybridization of Ti 3d and O 2p orbitals. Our study highlights the importance of the electronic structures on the hydrogen evolution activity of oxide electrocatalysts, and also provides a strategy to achieve efficient oxide-based hydrogen electrocatalysts by epitaxial stabilization of bulk-absent polymorphs.

Suggested Citation

  • Yangyang Li & Zhi Gen Yu & Ling Wang & Yakui Weng & Chi Sin Tang & Xinmao Yin & Kun Han & Haijun Wu & Xiaojiang Yu & Lai Mun Wong & Dongyang Wan & Xiao Renshaw Wang & Jianwei Chai & Yong-Wei Zhang & S, 2019. "Electronic-reconstruction-enhanced hydrogen evolution catalysis in oxide polymorphs," Nature Communications, Nature, vol. 10(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-11124-w
    DOI: 10.1038/s41467-019-11124-w
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    Cited by:

    1. Han Gao & Chao Ding & Jaeseok Son & Yangyu Zhu & Mingzheng Wang & Zhi Gen Yu & Jianing Chen & Le Wang & Scott A. Chambers & Tae Won Noh & Mingwen Zhao & Yangyang Li, 2022. "Ultra-flat and long-lived plasmons in a strongly correlated oxide," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    2. Lingxi Zhou & Yangfan Shao & Fang Yin & Jia Li & Feiyu Kang & Ruitao Lv, 2023. "Stabilizing non-iridium active sites by non-stoichiometric oxide for acidic water oxidation at high current density," Nature Communications, Nature, vol. 14(1), pages 1-12, December.

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