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Research Article

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

Huafeng Fan1,§, Dongxu Jiao1,§, Jinchang Fan1, Dewen Wang1, Bilal Zaman1, Wei Zhang1, Lei Zhang2( ), Weitao Zheng1( ), Xiaoqiang Cui1( )
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
College of Chemistry, Jilin University, Changchun 130012, China

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

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Graphical Abstract

A bifunctional electrocatalyst of high-valence Cr-incorporated NiSe2 was synthesized, and the as-obtained Cr0.05Ni0.95Se2 sample shows the remarkable electrocatalytic performance and the excellent durability. Density functional theory (DFT) calculations reveal that the incorporation of Cr kinetically and thermodynamically expedites elementary steps of water electrolysis.

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.

Keywords

nickel selenideelectrocatalytic water splittinghigh-valence Crdensity functional theory (DFT) calculation

Electronic Supplementary Material

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Nano Research
Volume 17 Issue 3,
March 2024
Pages 1199-1208
DOI: 10.1007/s12274-023-5992-4
Cite this article:
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 Research, 2024, 17(3): 1199-1208. https://doi.org/10.1007/s12274-023-5992-4
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Received: 18 May 2023
Revised: 27 June 2023
Accepted: 08 July 2023
Published: 12 August 2023
© Tsinghua University Press 2023
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