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Ni-based transition metal nitrides (TMNs) have been regarded as promising substitutes for noble-metal electrocatalysts towards the hydrogen evolution reaction (HER) due to their low cost, excellent chemical stability, high electronic conductivity, and unique electronic structure. However, facile green synthesis and rational microstructure design of Ni-based TMNs electrocatalysts with high HER activity remain challenging. In this work, we report the fabrication of Ni/Ni3N heterostructure nanoarrays on carbon paper via a one-step magnetron sputtering method under low temperature and N2 atmosphere. The Ni/Ni3N hierarchical nanoarrays exhibit an excellent HER catalytic activity with a low overpotential of 37 mV at 10 mA·cm−2 and robust long-term durability over 100 h. Furthermore, the Ni/Ni3N||NiFeOH (NiFeOH = NiFe bimetallic hydroxide) electrolyzer requires a small voltage of 1.54 V to obtain 10 mA·cm−2 for water electrolysis. Density functional theory (DFT) calculations reveal that the heterointerface between Ni and Ni3N could directly induce electron redistribution to optimize the electronic structure, which accelerates the dissociation of water molecules and the subsequent hydrogen desorption, and thus boosting the HER kinetics.

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Publication history
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Acknowledgements

Publication history

Received: 18 October 2022
Revised: 16 November 2022
Accepted: 17 November 2022
Published: 23 December 2022
Issue date: April 2023

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 51601163, 22001081, and 22075236), the Natural Science Foundation of Fujian Province (No. 2021J011211), the Xiamen Municipal Bureau of Science and Technology (No. 3502Z20206070), the Open Fund of Fujian Provincial Key Laboratory of Functional Materials and Applications (No. fma2018012), and Xiamen University.

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