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Research Article

Modulating redox transition kinetics by anion regulation in Ni-Fe-X (X = O, S, Se, N, and P) electrocatalyst for efficient water oxidation

Liting Wei1,2Kaini Zhang1Rui Zhao1Lei Zhang1Yan Zhang1Suyi Yang1Jinzhan Su1( )
International Research Center for Renewable Energy & State Key Laboratory of Multiphase Flow in Power Engineering, Xi’an Jiaotong University, Xi’an 710049, China
Department of Applied Chemistry, Yuncheng University, Yuncheng 044000, China
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Graphical Abstract

The anion with lower electronegativity in NiFe-based catalyst leads to a positive shift of Ni redox peak, higher conductivity, and optimized adsorption behavior for oxygen intermediates, contributing to enhanced intrinsic electrocatalytic oxygen evolution reaction (OER) activity.

Abstract

NiFe-based electrocatalysts will experience dynamical surface reconstruction during oxygen evolution reaction (OER) process, and the derived metal (oxy)hydroxide hybrids on the surface have been considered as the actual active species for OER. Tremendous efforts have been dedicated to understanding the surface reconstruction, but there is rare research on recognizing the origin of improved performance derived from anion species of substrate. Herein, the OER electrocatalytic characteristics were tuned with different anions in NiFe-based catalyst, using NiFe-based oxides/nitride/sulfide/selenides/phosphides (NiFeX, X = O, N, S, Se, and P) as the model materials. The combination of X-ray photoelectronic spectroscopy, electrochemical tests, operando spectroscopic characterizations, and density functional theory (DFT) calculations, reveals that anion with lower electronegativity in NiFe-based catalyst leads to higher conductivity and delayed valence transition of Ni sites, as well as optimized adsorption behavior towards oxygen intermediates, contributing to enhanced OER performance. Accordingly, NiFeP electrocatalyst demonstrates an ultralow overpotential of 265 mV at 20 mA·cm−2 for OER, as well as long-term stability. This work not only offers further insights into the effect of anionic electronegativity on the intrinsic OER electrocatalytic properties of NiFe-based electrocatalyst but also provides guide to design efficient non-noble metal-based electrocatalysts for water oxidation.

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Nano Research
Pages 4720-4728
Cite this article:
Wei L, Zhang K, Zhao R, et al. Modulating redox transition kinetics by anion regulation in Ni-Fe-X (X = O, S, Se, N, and P) electrocatalyst for efficient water oxidation. Nano Research, 2024, 17(6): 4720-4728. https://doi.org/10.1007/s12274-023-6400-9
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Received: 27 September 2023
Revised: 04 December 2023
Accepted: 07 December 2023
Published: 07 February 2024
© Tsinghua University Press 2024
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