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Kinetically and thermodynamically expediting elementary steps via high-valence Cr-incorporated of nickel selenide for water electrolysis

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Abstract

Designing high-performance electrocatalysts toward hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is essential to reduce the activation barrier and optimize free adsorption energy of reactive intermediates. Herein, we report that incorporating high-valence Cr into NiSe2 (CrxNi1−xSe2) kinetically and thermodynamically expedites elementary steps of both HER and OER. The as-prepared Cr0.05Ni0.95Se2 catalyst displays excellent HER and OER activities, with low overpotentials of 89 and 272 mV at the current density of 10 mA·cm−2 (j10), respectively, and remains stable during operation for 30 h. A low cell voltage of only 1.59 V is required to drive j10 in alkaline media. In situ Raman spectroscopy reveals that Cr incorporation facilitates the formation of NiOOH active species during the OER process. Meanwhile, theoretical explorations demonstrate that high-valence Cr incorporation efficiently accelerates water dissociation kinetics and improves H* adsorption during HER process, lowering the activation barrier of OER and optimizing the adsorption energy of oxygen-based intermediate, thus kinetically and thermodynamically enhancing the intrinsic performance of NiSe2 for over water splitting. This strategy provides a new horizon to design transition metal based electrocatalysts in the clean energy field.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Nos. 12034002, 22279044, and 22202080), Jilin Province Science and Technology Development Program (No. 20210301009GX), and the fellowship of China Postdoctoral Science Foundation (No. 2022M711296). The work was carried out at LvLiang Cloud Computing Center of China.

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  1. Huafeng Fan and Dongxu Jiao contributed equally to this work.

Authors and Affiliations

  1. State Key Laboratory of Automotive Simulation and Control, School of Materials Science and Engineering, Key Laboratory of Automobile Materials of MOE, Jilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy Materials, Electron Microscopy Center, Jilin University, Changchun, 130012, China

    Huafeng Fan, Dongxu Jiao, Jinchang Fan, Dewen Wang, Bilal Zaman, Wei Zhang, Weitao Zheng & Xiaoqiang Cui

  2. College of Chemistry, Jilin University, Changchun, 130012, China

    Lei Zhang

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  1. Huafeng Fan
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Correspondence to Lei Zhang, Weitao Zheng or Xiaoqiang Cui.

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Kinetically and thermodynamically expediting elementary steps via high-valence Cr-incorporated of nickel selenide for water electrolysis

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Fan, H., Jiao, D., Fan, J. et al. Kinetically and thermodynamically expediting elementary steps via high-valence Cr-incorporated of nickel selenide for water electrolysis. Nano Res. 17, 1199–1208 (2024). https://doi.org/10.1007/s12274-023-5992-4

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