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通过电化学重构原位合成高熵(羟基)氧化物作为高效水氧化催化剂

In Situ Synthesis of High-Entropy (Oxy)Hydroxides Via Electrochemical Reconfiguration As Catalysts For Efficient Water Oxidation.

作者信息

Shen Weilin, Du Yan, Liu Huibin, Tsang Chi-Wing, Chen Xiao, Liang Changhai

机构信息

Laboratory of Advanced Materials and Catalytic Engineering, School of Chemical Engineering, Dalian University of Technology, Dalian, 116024, China.

Faculty of Science and Technology, Technological and Higher Education Institute of Hong Kong (Thei), Hong Kong, 999077, China.

出版信息

Small. 2024 Nov;20(44):e2404379. doi: 10.1002/smll.202404379. Epub 2024 Aug 3.

DOI:10.1002/smll.202404379
PMID:39096073
Abstract

Surface reconstruction plays a pivotal role in enhancing the activity of the oxygen evolution reaction (OER), particularly in terms of the structural transformation from metal oxides to (oxy)hydroxides. Herein, a novel (oxy)hydroxide (FeCoNiCuMoOOH) with high entropy is developed by the electrochemical reconstitution of corresponding oxide (FeCoNiCuMoO). Significantly, the FeCoNiCuMoOOH exhibits much higher OER electrocatalytic activity and durability with an overpotential as low as 201 mV at a current density of 10 mA cm, and with a Tafel slope of 39.4 mV dec. The FeCoNiCuMoOOH/NF presents high stability when testing under a constant current at 100 mA cm within 1000 h. The surface reconstruction is a process of dissolution-reprecipitation of Cu and Mo species and co-hydroxylation of five metal species, which ultimately leads to the formation of FeCoNiCuMoOOH from FeCoNiCuMoOx. This study holds great significance in the realm of designing high-entropy (oxy)hydroxides catalysts with exceptional activity and stability for OER.

摘要

表面重构在提高析氧反应(OER)活性方面起着关键作用,特别是在从金属氧化物到(氧)氢氧化物的结构转变方面。在此,通过相应氧化物(FeCoNiCuMoO)的电化学重构制备了一种新型的高熵(氧)氢氧化物(FeCoNiCuMoOOH)。值得注意的是,FeCoNiCuMoOOH表现出更高的OER电催化活性和耐久性,在电流密度为10 mA cm时过电位低至201 mV,塔菲尔斜率为39.4 mV dec。FeCoNiCuMoOOH/NF在1000 h内于100 mA cm的恒定电流下测试时表现出高稳定性。表面重构是Cu和Mo物种的溶解-再沉淀以及五种金属物种的共羟基化过程,最终导致从FeCoNiCuMoOx形成FeCoNiCuMoOOH。该研究在设计具有优异活性和稳定性的高熵(氧)氢氧化物OER催化剂领域具有重要意义。

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