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The “mediated molecular”-assisted construction of Mo2N islands dispersed on Co-based nanosheets for high-efficient electrocatalytic hydrogen evolution reaction

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Abstract

The rational design of the catalysts with easily-accessible surface and high intrinsic activity is desirable for electrocatalytic hydrogen evolution reaction (HER). Here, we reported the construction of two-dimensional (2D) Co-Mo nitrides based heterojunctional catalyst for efficient HER based on a “mediated molecular” assisted route. The 2D Co(OH)2 sheet reacted partially with the “mediated molecular” (2-methylimidazole (2-MIM)) to form zeolitic imidazolate framework (ZIF)-67 at surface, giving ZIF-67/Co(OH)2 sheets. The ZIF-67 combines with [PMo12O40]3− cluster (PMo12) due to the interaction of mediated molecular with PMo12, producing 2D Mo-Co-2MIM/Co(OH)2 bimetallic precursor. After controlled nitriding, the Mo2N islands dispersed on 2D porous Co-based sheets were formed. A series of characterizations and density functional theory (DFT) calculation indicated the formation of a close contact interface, which promotes the electron transfer between Mo and Co components, enhances the electron migration/redistribution and redistribution and down-shift of d-band center and thus gives a high intrinsic activity. The 2D characteristics make the catalyst more accessible contact sites, which is favourable to promot the HER. The tests showed that the optimized catalyst exhibits an onset potential of 0 mV and an overpotential of 10 mA·cm−2 at 35.0 mV, which is quite close to that of Pt/C catalyst. It also exhibits an activity superior to Pt/C at high current density (> 100 mA·cm−2). A good stability of the catalyst was achieved with no significant decay for 100 h of continuous operation. The electrolytic cell composed of optimized catalyst and P-NiFe-layered double hydroxide (LDH) can be driven by low voltage (only 1.47 V) to reach a current density of 10 mA·cm−2.

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Acknowledgements

We gratefully acknowledge the support of this research by the National Key R&D Program of China (No. 2022YFA1503003), the National Natural Science Foundation of China (Nos. U20A20250, 91961111, and 22271081), the Natural Science Foundation of Heilongjiang Province (No. ZD2021b003), and University Nursing Program for Young Scholars with Creative Talents in Heilongjiang Province (No. UNPYSCT-2020004).

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  1. Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education of the People’s Republic of China, Heilongjiang University, Harbin, 150080, China

    Fanyi Kong, Aiping Wu, Siyu Wang, Xinhui Zhang, Chungui Tian & Honggang Fu

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  1. Fanyi Kong
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  2. Aiping Wu
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  3. Siyu Wang
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Correspondence to Chungui Tian or Honggang Fu.

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The “mediated molecular”-assisted construction of Mo2N islands dispersed on Co-based nanosheets for high-efficient electrocatalytic hydrogen evolution reaction

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Kong, F., Wu, A., Wang, S. et al. The “mediated molecular”-assisted construction of Mo2N islands dispersed on Co-based nanosheets for high-efficient electrocatalytic hydrogen evolution reaction. Nano Res. 16, 10857–10866 (2023). https://doi.org/10.1007/s12274-023-5878-5

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