序贯离子交换法制备三金属催化剂,增强安培级水氧化

IF 10.3 4区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR
结构化学 Pub Date : 2026-04-01 Epub Date: 2026-01-07 DOI:10.1016/j.cjsc.2025.100861
Dequan Li , Shanshan Fan , Wenjing Liu , Zhonge Luo , Mingpeng Chen , Congcong Shen , Wangwei Liao , Bo Li , Mao Zhang , Yuewen Wu , Boxue Wang , Feng Liu , Huachuan Sun , Tong Zhou , Qingju Liu
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引用次数: 0

摘要

电催化水裂解已成为一种有前途的可持续制氢途径。然而,缓慢的析氧反应(OER)严重制约了其整体效率。本文通过顺序离子交换策略,合理设计并合成了一种三金属电催化剂。制备的Fe/NiCoO2具有多金属电子协同作用和独特的层次化结构,具有高的内在活性、丰富的活性位点和高效的质量扩散。得益于这些组成和结构上的优点,该电极在电流密度为10和500 mA cm−2时分别提供了248和353 mV的超低过电位,Tafel斜率为39.15 mV dec−1。此外,Fe/NiCoO2在500 mA cm−2的高电流密度下表现出超过200小时的长期稳定性,优于基准贵金属基催化剂。原位拉曼光谱分析表明,初始Fe/NiCoO2在OER过程中自我重构为Fe/NiCoOOH。密度泛函理论(DFT)计算证明,Fe加入NiCoO2有效地调整了三维轨道电子分布,从而优化了含氧中间体的吸附能,增强了电荷转移动力学。该研究为设计具有定制纳米结构和多活性位点配置的无贵金属催化剂提供了一种有前途的策略,以促进高效的工业规模的水氧化。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Constructing trimetallic catalyst via sequential ion-exchange for enhanced ampere-level water oxidation

Constructing trimetallic catalyst via sequential ion-exchange for enhanced ampere-level water oxidation
Electrocatalytic water splitting has emerged as a promising route for sustainable hydrogen production. However, the sluggish oxygen evolution reaction (OER) severely restricts its overall efficiency. Herein, a trimetallic electrocatalyst was rationally designed and synthesized via a sequential ion-exchange strategy. The as-prepared Fe/NiCoO2, featuring the multi-metallic electronic synergy and unique hierarchical architecture, provides high intrinsic activity, abundant active sites, and efficient mass diffusion. Benefiting from these compositional and structural merits, the electrode delivers ultralow overpotentials of 248 and 353 mV at current densities of 10 and 500 mA cm−2, respectively, with a small Tafel slope of 39.15 mV dec−1. Furthermore, Fe/NiCoO2 exhibits exceptional long-term stability over 200 h under high current densities of 500 mA cm−2, outperforming the benchmark noble-metal-based catalysts. In-situ Raman spectroscopy reveals that the initial Fe/NiCoO2 undergoes self-reconstruction into Fe/NiCoOOH during the OER process. Density functional theory (DFT) calculations certify that the incorporation of Fe into NiCoO2 effectively tunes the 3d-orbital electron distribution, which optimizes the adsorption energies of oxygen-containing intermediates and enhances charge transfer kinetics. This study provides a promising strategy for designing noble-metal-free catalysts with tailored nanostructures and multi-active site configurations to facilitate efficient industrial-scale water oxidation.
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来源期刊
结构化学
结构化学 化学-晶体学
CiteScore
4.70
自引率
22.70%
发文量
5334
审稿时长
13 days
期刊介绍: Chinese Journal of Structural Chemistry “JIEGOU HUAXUE ”, an academic journal consisting of reviews, articles, communications and notes, provides a forum for the reporting and discussion of current novel research achievements in the fields of structural chemistry, crystallography, spectroscopy, quantum chemistry, pharmaceutical chemistry, biochemistry, material science, etc. Structural Chemistry has been indexed by SCI, CA, and some other prestigious publications.
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