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Electronic structure regulation in medium-entropy CoNiFeSe enabling efficient and durable oxygen evolution electrocatalysis

Yuxin Luan,De-Kun Liu,Yuxiang Chen,Xuezhi Song,Liang Jing,Xiao-Bing Wang,Wenqiang Sun,Yulan Meng,Chenyu Shen,Ruichen Zhou,Jinxuan Liu,Xiaofeng Wang,Zhenquan Tan

Developing highly efficient and durable electrocatalysts for oxygen evolution reaction (OER) holds great promise in revolutionizing the sustainable energy-conversion technologies, which are greatly relying on the surface electronic structures. However, constructing catalytically active medium-entropy materials encounters great challenge due to the complexed composition and the unsolved electronic structure-performance relationship. In this study, the medium-entropy metal selenide (CoFeNiSe) with cumulus-like architectures is fabricated through the selenylation of trimetallic hydroxide precursors. The medium-entropy CoFeNiSe manifests an outstanding electrocatalytic OER activity and kinetics, that is a low overpotential of 268 mV at 10 mA cm-2 and a Tafel slope of 53.33 mV dec-1, in 1 M KOH, outperforming the entropy-poor binary CoFeSe and CoNiSe, as well as unary CoSe counterparts. It has been found experimentally and theoretically that the effective modulations of the valency and the d-band center at an optimal level regulate the adsorption/desorption ability of reaction intermediates via multimetallic electron interactions. This work provides the valuable insight into the electronic structure regulation in entropy-rich materials, shedding light on the development of current green energy conversion technologies.