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Accelerated water activation and stabilized metal-organic framework via constructing triangular active-regions for ampere-level current density hydrogen production

Author

Listed:
  • Fanpeng Cheng

    (Zhejiang University)

  • Xianyun Peng

    (Institute of Zhejiang University - Quzhou)

  • Lingzi Hu

    (Central China Normal University)

  • Bin Yang

    (Zhejiang University
    Institute of Zhejiang University - Quzhou)

  • Zhongjian Li

    (Zhejiang University
    Institute of Zhejiang University - Quzhou)

  • Chung-Li Dong

    (Tamkang University)

  • Jeng-Lung Chen

    (National Synchrotron Radiation Research Center)

  • Liang-Ching Hsu

    (National Synchrotron Radiation Research Center)

  • Lecheng Lei

    (Zhejiang University
    Institute of Zhejiang University - Quzhou)

  • Qiang Zheng

    (National Center for Nanoscience and Technology)

  • Ming Qiu

    (Central China Normal University)

  • Liming Dai

    (University of New South Wales)

  • Yang Hou

    (Zhejiang University
    Institute of Zhejiang University - Quzhou
    NingboTech University
    Donghai Laboratory)

Abstract

Two-dimensional metal-organic frameworks (MOFs) have been explored as effective electrocatalysts for hydrogen evolution reaction (HER). However, the sluggish water activation kinetics and structural instability under ultrahigh-current density hinder their large-scale industrial applications. Herein, we develop a universal ligand regulation strategy to build well-aligned Ni-benzenedicarboxylic acid (BDC)-based MOF nanosheet arrays with S introducing (S-NiBDC). Benefiting from the closer p-band center to the Fermi level with strong electron transferability, S-NiBDC array exhibits a low overpotential of 310 mV to attain 1.0 A cm−2 with high stability in alkaline electrolyte. We speculate the newly-constructed triangular “Ni2-S1” motif as the improved HER active region based on detailed mechanism analysis and structural characterization, and the enhanced covalency of Ni-O bonds by S introducing stabilizes S-NiBDC structure. Experimental observations and theoretical calculations elucidate that such Ni sites in “Ni2-S1” center distinctly accelerate the water activation kinetics, while the S site readily captures the H atom as the optimal HER active site, boosting the whole HER activity.

Suggested Citation

  • Fanpeng Cheng & Xianyun Peng & Lingzi Hu & Bin Yang & Zhongjian Li & Chung-Li Dong & Jeng-Lung Chen & Liang-Ching Hsu & Lecheng Lei & Qiang Zheng & Ming Qiu & Liming Dai & Yang Hou, 2022. "Accelerated water activation and stabilized metal-organic framework via constructing triangular active-regions for ampere-level current density hydrogen production," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
  • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-34278-6
    DOI: 10.1038/s41467-022-34278-6
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    1. Jiachen Li & Yuqiang Ma & Cong Zhang & Chi Zhang & Huijun Ma & Zhaoqi Guo & Ning Liu & Ming Xu & Haixia Ma & Jieshan Qiu, 2023. "Green electrosynthesis of 3,3’-diamino-4,4’-azofurazan energetic materials coupled with energy-efficient hydrogen production over Pt-based catalysts," Nature Communications, Nature, vol. 14(1), pages 1-15, December.
    2. Yiming Zhu & Malte Klingenhof & Chenlong Gao & Toshinari Koketsu & Gregor Weiser & Yecan Pi & Shangheng Liu & Lijun Sui & Jingrong Hou & Jiayi Li & Haomin Jiang & Limin Xu & Wei-Hsiang Huang & Chih-We, 2024. "Facilitating alkaline hydrogen evolution reaction on the hetero-interfaced Ru/RuO2 through Pt single atoms doping," Nature Communications, Nature, vol. 15(1), pages 1-13, December.

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