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Nano Research 2023, 16(8): 10857-10866 https://doi.org/10.1007/s12274-023-5878-5
Research Article | Issue | Published: 17 July 2023

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

Show Author's Information Fanyi Kong,  Aiping Wu,  Siyu Wang,  Xinhui Zhang,  Chungui Tian( ),  Honggang Fu( )
Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education of the People’s Republic of China, Heilongjiang University, Harbin 150080, China
Keywords:
nitrides, polyoxometalates (POMs), two-dimensional heterojunctions, zeolitic imidazole framework-67 (ZIF-67), electrocatalytic hydrogen evolution reaction (HER)
Topics:
Hydrogen evolution reaction
Cite this article:
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 Research, 2023, 16(8): 10857-10866. https://doi.org/10.1007/s12274-023-5878-5
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Abstract Full text Electronic supplementary material About this article

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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Electronic supplementary material
About this article

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

Show Author's information Fanyi Kong, Aiping Wu, Siyu Wang, Xinhui Zhang, Chungui Tian( ), Honggang Fu( )
Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education of the People’s Republic of China, Heilongjiang University, Harbin 150080, China

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.

Keywords: nitrides, polyoxometalates (POMs), two-dimensional heterojunctions, zeolitic imidazole framework-67 (ZIF-67), electrocatalytic hydrogen evolution reaction (HER)

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Acknowledgements

Publication history

Received: 01 April 2023
Revised: 15 May 2023
Accepted: 29 May 2023
Published: 17 July 2023
Issue date: August 2023

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© Tsinghua University Press 2023

Acknowledgements

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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