Affiliation:
1. Shenzhen Geim Graphene Center Tsinghua‐Berkeley Shenzhen Institute and Tsinghua Shenzhen International Graduate School Tsinghua University Shenzhen 518055 China
2. Faculty of Materials Science and Energy Engineering Shenzhen Institute of Advanced Technology Shenzhen 518055 China
3. Institute of Technology for Carbon Neutrality Shenzhen Institute of Advanced Technology Chinese Academy of Sciences Shenzhen 518055 China
4. Shenyang National Laboratory for Materials Science Institute of Metal Research Chinese Academy of Sciences Shenyang 110016 China
Abstract
AbstractIt 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, using a high‐entropy‐driven electric dipole transition strategy to activate and stabilize the tetrahedral sites is proposed, 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 with severe lattice distortion, exhibits a strong 1s→4s electric dipole transition and intense t2g(Co)/eg(Ni)‐2p(OL) orbital hybridization that regulates the electronic descriptors, eg and t2g, which leads to the formation of low‐valence Co tetrahedral sites (Coth) and high‐valence Ni octahedral sites (Nioh), resulting in a higher half‐wave potential of 0.87 V on Coth sites and a lower overpotential of 0.26 V at 10 mA cm−2 on Nioh sites as well as a superior performance of ZABs compared to low/mild entropy spinel oxides. 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.
Funder
National Natural Science Foundation of China
Guangdong Innovative and Entrepreneurial Research Team Program
NSAF Joint Fund
National Key Research and Development Program of China
Cited by
3 articles.
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