Plasma-driven oxygen vacancies engineering in high-entropy layered double hydroxide catalyst for enhanced oxygen evolution reaction catalysis

被引：0

作者：

Peng, Kai ^{[1
]}

Cui, Peng ^{[2
]}

Miao, Fang ^{[3
]}

机构：

[1] School of Materials Science and Engineering, Southeast University, Nanjing

[2] Department of Materials Science and Engineering, Jinzhong University, Jinzhong

[3] College of Materials Science and Engineering, North University of China, Taiyuan

来源：

International Journal of Hydrogen Energy | 2025年 / 158卷

基金：

中国博士后科学基金;

关键词：

Electronic tailoring; High-entropy effect; Layered double hydroxide; Oxygen evolution reaction; Oxygen vacancies;

D O I：

10.1016/j.ijhydene.2025.150578

中图分类号：

学科分类号：

摘要：

Tailoring high-entropy materials catalysts with unique structural attributes for improved oxygen evolution reaction (OER) performance plays a pivotal role in facilitating practical implementation of alkaline water splitting. Herein, the potential of oxygen vacancies-rich high-entropy layered double hydroxide catalyst on nickel foam substrate (P–NiFeCoMnCu-LDH/NF) fabricated via a facile hydrothermal synthesis and following Ar plasma treatment strategy is demonstrated in this work. By virtue of synergistic action of high-entropy effect and oxygen vacancies engineering, the as-optimized P–NiFeCoMnCu-LDH/NF demonstrates excellent OER catalytic efficiency in alkaline media (1 M KOH), attaining 198 mV overpotential at 10 mA‧cm−2 and a Tafel slope of 39.8 mV‧dec−1, surpassing quinary, quaternary, ternary, and binary LDH counterparts. Besides, the robust electrocatalytic stability operated continuously at 100 mA‧cm−2 for100 h of P–NiFeCoMnCu-LDH/NF is also disclosed. The advanced in-situ Raman spectroscopy analysis confirms that P–NiFeCoMnCu-LDH/NF would undergo dynamic surface reconstruction, with operando-formed γ-NiOOH identified as actual active species driving exceptional catalytic performance. Furthermore, density functional theory (DFT) calculations provide additional support, demonstrating that oxygen vacancies within P–NiFeCoMnCu-LDH/NF structure promote favorable electron delocalization at active sites, enhance charge transfer, and significantly lower energy barrier for rate-limiting O∗ to OOH∗ transition. This, in turn, accelerates OER kinetics, thereby improving the overall electrocatalytic performance. On the side, the as-integrated Pt/C||P–NiFeCoMnCu-LDH/NF electrode couple also demonstrates superior alkaline water splitting activity with exceptionally low voltage requirements (1.49 V@10 mA cm−2; 1.66 V@100 mA cm−2). This work offers an innovative strategy for designing high-entropy materials catalysts for efficient OER application based on vacancy engineering. © 2025 Hydrogen Energy Publications LLC

引用

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