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亲氧钴钨氧化物与铜钴合金对水离解和氢吸附的协同效应实现pH通用析氢

Synergy effect of oxyphilic cobalt‑tungsten oxide and copper‑cobalt alloy on water dissociation and hydrogen adsorption for pH-universal hydrogen evolution.

作者信息

Zheng Jiahui, Li Mingzhe, Wang Xiaofen, Zhang Xin, Wang Yunlong, Zheng Fengchun, Chen Kepi, Zhou Wei, Lv Yuzhen, Zhang Jin

机构信息

School of Energy, Power and Mechanical Engineering, North China Electric Power University, Beijing 102206, China.

School of Energy, Power and Mechanical Engineering, North China Electric Power University, Beijing 102206, China.

出版信息

J Colloid Interface Sci. 2026 Jan 15;702(Pt 1):138889. doi: 10.1016/j.jcis.2025.138889. Epub 2025 Aug 30.

DOI:10.1016/j.jcis.2025.138889
PMID:40915291
Abstract

Developing pH-universal hydrogen evolution reaction (HER) electrocatalysts demands the simultaneous optimization of water dissociation kinetics and hydrogen adsorption. Herein, a CuCo/CoWO heterostructure with an area of 600 cm was fabricated via a facile one-step electrodeposition strategy. It only needs 193.8 and 158.1 mV overpotential to drive 1000 mA cm current density in 1 M KOH and 0.5 M HSO, respectively. Moreover, it requires 103.1 mV overpotential to reach 10 mA cm in 1 M phosphate buffered saline (PBS). Remarkably, it exhibits outstanding stability, maintaining over 99.0 % of initial activity after 1000 h of operation at 1000 mA cm in 1 M KOH and 100 mA cm in 0.5 M HSO. Experimental and density functional theoretical (DFT) analyses reveal that the superior selective adsorption capability of oxide component (*HO and *OH) and copper‑cobalt alloy (*H) significantly facilitates water dissociation at the interface. Moreover, the strong Lewis acidity of W further amplifies this effect by enhancing the oxyphilicity of the oxide component, thus resulting in a 40 % decrease in the energy barrier of water dissociation and a 58 % reduction in activation energy for HER. Meanwhile, optimized hydrogen adsorption Gibbs free energy (G) at alloy Co sites also boosts the acidic HER performance. This study presents a promising strategy to develop high-efficiency transition metal-based electrocatalysts for HER across a wide pH range.

摘要

开发pH通用析氢反应(HER)电催化剂需要同时优化水离解动力学和氢吸附。在此,通过简便的一步电沉积策略制备了面积为600 cm的CuCo/CoWO异质结构。在1 M KOH和0.5 M HSO中分别驱动1000 mA cm电流密度仅需193.8和158.1 mV的过电位。此外,在1 M磷酸盐缓冲盐水(PBS)中达到10 mA cm需要103.1 mV的过电位。值得注意的是,它表现出出色的稳定性,在1 M KOH中1000 mA cm和0.5 M HSO中100 mA cm下运行1000 h后仍保持超过99.0%的初始活性。实验和密度泛函理论(DFT)分析表明,氧化物组分(HO和OH)和铜钴合金(*H)的优异选择性吸附能力显著促进了界面处的水离解。此外,W的强路易斯酸性通过增强氧化物组分的亲氧性进一步放大了这种效应,从而使水离解的能垒降低40%,HER的活化能降低58%。同时,合金Co位点处优化的氢吸附吉布斯自由能(G)也提高了酸性HER性能。这项研究提出了一种有前景的策略,用于开发在宽pH范围内用于HER的高效过渡金属基电催化剂。

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