文献类型：期刊文献

英文题名：Modulating metal-oxygen interactions of high-entropy oxide electrocatalysts enables highly-active and ultra-stable water oxidation

作者：Wang, Jingyu[1];Zhang, Jiahao[1];Zhang, Liyue[1];Chen, Ling[1];He, Guanjie[2];Jiang, Hao[1]

机构：[1]East China Univ Sci & Technol, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Mat Sci & Engn, Key Lab Ultrafine Mat Minist Educ, Shanghai 200237, Peoples R China;[2]UCL, Dept Chem Engn, Electrochem Innovat Lab, London WC1E 7JE, England

年份：2024

卷号：342

外文期刊名：APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY

收录：;EI(收录号：20234214915394);WOS:【SCI-EXPANDED(收录号:WOS:001091766800001)】；

基金：This work was supported by the National Natural Science Foundation of China (22208102, U22B20143) , and the Fundamental Research Funds for the Central Universities.

语种：英文

外文关键词：Electrocatalysts; High-entropy oxides; Overpotential; Oxygen evolution reaction

摘要：High-entropy oxide (HEO) electrocatalysts are appealing for multi-step catalytic reactions as their high compositional diversity and multi-element synergy effects. Herein, we find that the metal-oxygen (M-O) interactions in FeCoNi-based HEO can be well-optimized by introducing Al and Ce elements. The in-situ electrochemistry-triggered Al leaching exposes abundant newly-formed active sites with greatly reduced energy difference between TM 3d and O 2p orbitals. This fact shows the enhancement of M-O covalency, which is further quantified by the Fe/Co/Ni charge calculations. The stronger M-O covalency greatly decreases the activation energy of water oxidation at Fe/Co/Ni sites and the barrier of electrical transfer. Furthermore, the Ce element downshifts the O 2p band center, effectively refraining lattice oxygen loss. These advantages enable a supersmall overpotential of 303.7 mV at 500 mA cm-2 that maintains 95.8 % even operating for 840 h, which is the best report for the HEOs to date.