Hollow-Structured and Polyhedron-Shaped High Entropy Oxide toward Highly Active and Robust Oxygen Evolution Reaction in a Full pH Range.

Miao, Kanghua; Jiang, Wendan; Chen, Zhaoqian; Luo, Yan; Xiang, Dong; Wang, Chaohui; Kang, Xiongwu · Adv Mater · 2024

basic_science · Level V

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Abstract

High entropy metal oxides (HEO) are superior to many reactions involving multi-step elementary reactions. However, controlled synthesis of hollow-structured HEO catalysts, which offers large surface area and fast mass transfer kinetics, remains challenging and unexplored due to the complicated metal precursors. Herein, a metal organic framework-templated synthesis of hollow-structured and polyhedron-shaped HEO catalysts assembled with ultra-small nanoparticles, with up to ten metal elements, can be achieved, by taking advantage of the ion-exchange method. ZnFeNiCuCoRu-O HEO catalyst displays excellent activity and ultra-stability for oxygen evolution reaction in full pH range, with an overpotential of 170 mV at a current density of 10 mA cm<sup>-2</sup> , a Tafel slope of 56 mV dec<sup>-1</sup> , and a decay of activity by 7% in 30 h in alkaline medium, as well as a 12% and 8% decay in acidic and neutral medium, respectively. DFT calculation indicates that the energy barrier of the potential determining step on Ru-Fe bridge site is significantly lower than any other Ru-related bridge sites for the unique hollow structured HEO structures. This work highlights the importance of ion-exchange method in preparing highly stable and active hollow-structured HEOs catalysts toward highly efficient energy conversion and storage devices.