Issue 2, 2024

Molybdate ion leaching and re-adsorption facilitate structural and electronic modulation of nickel–iron catalysts for seawater electrolysis

Abstract

Developing active and robust NiFe-based catalysts as alternatives to noble metals remains a significant challenge for low-cost hydrogen generation. Generally, the original catalysts will undergo self-reconstruction to derive into oxyhydroxides (MOOH) under the operation situation. Herein, we propose a Mo oxidative leaching strategy to promote the self-reconstruction of NiFe-based pre-catalysts. Operando Raman and time-dependent X-ray photoelectron spectra revealed that, during the OER operation, Mo dopants are oxidized to soluble molybdate ions (MoO42−) and leach into the electrolyte, facilitating the reconstruction of pre-catalysts to active MOOH sites. Then, various electrochemical measurements and density functional theory calculations demonstrated that the re-adsorbed MoO42− ions modify the electronic environment of the Ni and Fe sites and enhance the adsorption of oxygenated intermediates, boosting the OER kinetics. The optimized catalysts achieve long-term stability of 150 h at 1000 mA cm−2 in simulated seawater and 200 h for overall seawater splitting. This work provides a design path for OER catalysts and enriches the understanding of the role of adsorbed oxyanions.

Graphical abstract: Molybdate ion leaching and re-adsorption facilitate structural and electronic modulation of nickel–iron catalysts for seawater electrolysis

Supplementary files

Article information

Article type
Research Article
Submitted
08 Oct 2023
Accepted
18 Nov 2023
First published
21 Nov 2023

Inorg. Chem. Front., 2024,11, 498-507

Molybdate ion leaching and re-adsorption facilitate structural and electronic modulation of nickel–iron catalysts for seawater electrolysis

J. Zhou, L. Liu, H. Ren, L. Li, W. Song, N. Li, X. Shi, C. Kou, Y. Sun, M. Han, H. Wang, J. Han, K. Liu, C. D. Momo, Y. Liu, D. Feng, W. Zhu, S. Chen, H. Jiang, Y. Liu and H. Liang, Inorg. Chem. Front., 2024, 11, 498 DOI: 10.1039/D3QI02055J

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