3D Ordered Macroporous Superstructures of High Entropy Hydroxide with Strong Orbital Coupling Enhancing Water/Seawater Oxidation.

IF 27.4 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Advanced Materials Pub Date : 2025-07-21 DOI:10.1002/adma.202506068

Xiaofeng Tian,Ruotong Liu,Weizhou Wang,Qin Yang,Zheng Huang,Yu Yang,Jishu Han,Tian Dong,Yunmei Du,Jianping Lai,Hongdong Li,Lei Wang

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引用次数: 0

Abstract

The water splitting performance is strongly influenced by intrinsic properties of the catalyst and the accessibility of the active center. Herein, high-entropy hydroxides (HEH) with 3D ordered macroporous (3DOM) structure are prepared by chemical etching method with rational design. The 3DOM structure can maximize the exposure of the active sites and also facilitates bubble transport. As demonstrated by finite element analysis, the 3DOM structure modifies the spatial curvature of the catalyst, resulting in the enrichment of OH-. Moreover, the strong orbital coupling of transition metals significantly regulates the electronic structure of the catalyst, selectively adsorbs OH- at Fe sites, and inhibits the adsorption of Cl-. Thanks to these characteristics, 3DOM-HEH-300 shows the best oxygen evolution reaction (OER) performance in 1 m KOH (182 mV@100 mA cm-2, 211 mV@500 mA cm-2), and stables operation of more than 400 h. Besides, in natural seawater, it also exhibits the best catalytic activity (245 mV@100 mA cm-2, 278 mV@500 mA cm-2), which is better than similar catalysts without 3DOM structure. This work verifies the great synergistic effect of high entropy and mass transfer on the performance of OER, which also provides a new idea for constructing high-performance electrodes.

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具有强轨道耦合的高熵氢氧化物三维有序大孔上层结构增强水/海水氧化。

催化剂的性质和活性中心的可及性对水裂解性能有很大影响。采用化学蚀刻法制备了具有三维有序大孔（3DOM）结构的高熵氢氧化物（HEH）。3DOM结构可以最大限度地暴露活性位点，也有利于气泡的传输。有限元分析表明，3DOM结构改变了催化剂的空间曲率，导致OH-富集。此外，过渡金属的强轨道偶联显著调节了催化剂的电子结构，选择性地吸附了Fe位点的OH-，抑制了Cl-的吸附。因此，3DOM- heh -300在1 m KOH条件下（182 mV@100 mA cm- 2,211 mV@500 mA cm-2）表现出最佳的析氧反应（OER）性能，稳定运行时间超过400 h。此外，在天然海水条件下，3DOM- heh -300也表现出最佳的催化活性（245 mV@100 mA cm- 2,278 mV@500 mA cm-2），优于同类无3DOM结构的催化剂。这项工作验证了高熵和传质对OER性能的巨大协同效应，也为构建高性能电极提供了新的思路。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Advanced Materials 工程技术-材料科学：综合

CiteScore

43.00

自引率

4.10%

发文量

2182

审稿时长

2 months

期刊介绍： Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.