尖晶石
材料科学
过电位
八面体
价(化学)
化学物理
电化学
结晶学
物理化学
化学
晶体结构
电极
冶金
有机化学
作者
Q. Zhang,Zhiyang Zheng,Runhua Gao,Xiao Xiao,Menggai Jiao,Boran Wang,Guangmin Zhou,Hui‐Ming Cheng
标识
DOI:10.1002/adma.202401018
摘要
Abstract It remains a significant challenge to construct active sites to break the trade‐off between oxidation and reduction processes occurring in battery cathodes with conversion mechanism, especially for the oxygen reduction and evolution reactions (ORR/OER) involved in the Zinc‐air batteries (ZABs). Here, we propose using a high‐entropy‐driven electric dipole transition strategy to activate and stabilize the tetrahedral sites, while enhancing the activity of octahedral sites through orbital hybridization in a FeCoNiMnCrO spinel oxide, thus constructing bipolar dual‐active sites with high‐low valence states, which can effectively decouple ORR/OER. The FeCoNiMnCrO high‐entropy spinel oxide (HESO) with severe lattice distortion, exhibits a strong 1s→4s electric dipole transition and intense t 2g (Co)/e g (Ni)‐2p(O L ) orbital hybridization that regulates the electronic descriptors, e g and t 2g , which leads to the formation of low‐valence Co tetrahedral sites (Co th ) and high‐valence Ni octahedral sites (Ni oh ), resulting in a higher half‐wave potential of 0.87 V on Co th sites and a lower overpotential of 0.26 V at 10 mA cm −2 on Ni oh sites as well as a superior performance of ZABs compared to low/mild entropy spinel oxides (L/MESO). Therefore, entropy engineering presents a distinctive approach for designing catalytic sites by inducing novel electromagnetic properties in materials across various electrocatalytic reactions, particularly for decoupling systems. This article is protected by copyright. All rights reserved
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