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One-step synthesis of single-site vanadium substitution in 1T-WS2 monolayers for enhanced hydrogen evolution catalysis

Author

Listed:
  • Ali Han

    (King Abdullah University of Science and Technology
    Tsinghua University)

  • Xiaofeng Zhou

    (King Abdullah University of Science and Technology
    Shenzhen Chang Long Technology Co., Ltd)

  • Xijun Wang

    (North Carolina State University)

  • Sheng Liu

    (Nanyang Technological University)

  • Qihua Xiong

    (Nanyang Technological University
    Tsinghua University)

  • Qinghua Zhang

    (Chinese Academy of Sciences)

  • Lin Gu

    (Chinese Academy of Sciences)

  • Zechao Zhuang

    (Tsinghua University)

  • Wenjing Zhang

    (Shenzhen University)

  • Fanxing Li

    (North Carolina State University)

  • Dingsheng Wang

    (Tsinghua University)

  • Lain-Jong Li

    (King Abdullah University of Science and Technology)

  • Yadong Li

    (Tsinghua University)

Abstract

Metallic tungsten disulfide (WS2) monolayers have been demonstrated as promising electrocatalysts for hydrogen evolution reaction (HER) induced by the high intrinsic conductivity, however, the key challenges to maximize the catalytic activity are achieving the metallic WS2 with high concentration and increasing the density of the active sites. In this work, single-atom-V catalysts (V SACs) substitutions in 1T-WS2 monolayers (91% phase purity) are fabricated to significantly enhance the HER performance via a one-step chemical vapor deposition strategy. Atomic-resolution scanning transmission electron microscopy (STEM) imaging together with Raman spectroscopy confirm the atomic dispersion of V species on the 1T-WS2 monolayers instead of energetically favorable 2H-WS2 monolayers. The growth mechanism of V SACs@1T-WS2 monolayers is experimentally and theoretically demonstrated. Density functional theory (DFT) calculations demonstrate that the activated V-atom sites play vital important role in enhancing the HER activity. In this work, it opens a novel path to directly synthesize atomically dispersed single-metal catalysts on metastable materials as efficient and robust electrocatalysts.

Suggested Citation

  • Ali Han & Xiaofeng Zhou & Xijun Wang & Sheng Liu & Qihua Xiong & Qinghua Zhang & Lin Gu & Zechao Zhuang & Wenjing Zhang & Fanxing Li & Dingsheng Wang & Lain-Jong Li & Yadong Li, 2021. "One-step synthesis of single-site vanadium substitution in 1T-WS2 monolayers for enhanced hydrogen evolution catalysis," Nature Communications, Nature, vol. 12(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-20951-9
    DOI: 10.1038/s41467-021-20951-9
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    Cited by:

    1. John C. Thomas & Wei Chen & Yihuang Xiong & Bradford A. Barker & Junze Zhou & Weiru Chen & Antonio Rossi & Nolan Kelly & Zhuohang Yu & Da Zhou & Shalini Kumari & Edward S. Barnard & Joshua A. Robinson, 2024. "A substitutional quantum defect in WS2 discovered by high-throughput computational screening and fabricated by site-selective STM manipulation," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    2. Chengxin Zhou & Jian Gao & Yunlong Deng & Ming Wang & Dan Li & Chuan Xia, 2023. "Electric double layer-mediated polarization field for optimizing photogenerated carrier dynamics and thermodynamics," Nature Communications, Nature, vol. 14(1), pages 1-11, December.

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