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

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 () and Yang Hou ()
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Fanpeng Cheng: Zhejiang University
Xianyun Peng: Institute of Zhejiang University - Quzhou
Lingzi Hu: Central China Normal University
Bin Yang: Zhejiang University
Zhongjian Li: Zhejiang University
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
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

Nature Communications, 2022, vol. 13, issue 1, 1-10

Abstract: 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.

Date: 2022
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DOI: 10.1038/s41467-022-34278-6

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