文献类型：期刊文献

英文题名：Augmented Electrochemical Oxygen Evolution by d-p Orbital Electron Coupling

作者：Sun, Ning[1];Zheng, Zhichuan[1];Lai, Zhuangzhuang[2,3];Wang, Junjie[4];Du, Peng[1];Ying, Tianping[4];Wang, Haifeng[2,3];Xu, Jianchun[1];Yu, Runze[5];Hu, Zhiwei[6];Pao, Chih-Wen[7];Huang, Wei-Hsiang[7];Bi, Ke[1];Lei, Ming[1];Huang, Kai[1]

机构：[1]Beijing Univ Posts & Telecommun, Sch Sci, State Key Lab Informat Photon & Opt Commun, Beijing 100876, Peoples R China;[2]East China Univ Sci & Technol, Ctr Computat Chem, Sch Chem & Mol Engn, State Key Lab Green Chem Engn & Ind Catalysis, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Res Inst Ind Catalysis, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[4]Chinese Acad Sci, Beijing Natl Lab Condensed Matter Phys, Inst Phys, Beijing 100190, Peoples R China;[5]Ctr High Pressure Sci & Technol Adv Res, Beijing 100193, Peoples R China;[6]Max Planck Inst Chem Phys Solids, Nothnitzer Str 40, D-01187 Dresden, Germany;[7]Natl Synchrotron Radiat Res Ctr, 101 Hsin Ann Rd, Hsinchu 300092, Taiwan

年份：2024

卷号：36

期号：39

外文期刊名：ADVANCED MATERIALS

收录：;EI(收录号：20242716601411);WOS:【SCI-EXPANDED(收录号:WOS:001258513100001)】；

基金：N.S., Z.Z., and Z.L. contributed equally to this work. This work was supported financially by the Fundamental Research Funds for the Central Universities (Grant Nos. 2023ZCJH03, 2021XD-A041), the Teaching Reform Projects at BUPT (Grant No. 2022CXCY-B03), the fund of State Key Laboratory of Information Photonics and Optical Communications (Beijing University of Posts and Telecommunications, P. R. China), the National Key Research and Development Program of China (Grant No. 2021YFA1500700), the NSFC (Grant Nos. 52272267, 22203031, 91945302, 92045303, 21873028), and the BUPT Excellent Ph.D. Students Foundation (Grant No. CX2013108).

语种：英文

外文关键词：density functional calculation; d-p orbital hybridization; electrochemical oxygen evolution; high-entropy compounds; van der Waals materials

摘要：While high-entropy alloys, high-entropy oxides, and high-entropy hydroxides, are advanced as a novel frontier in electrocatalytic oxygen evolution, their inherent activity deficiency poses a major challenge. To achieve the unlimited goal to tailor the structure-activity relationship in multicomponent systems, entropy-driven composition engineering presents substantial potential, by fabricating high-entropy anion-regulated transition metal compounds as sophisticated oxygen evolution reaction electrocatalysts. Herein, a versatile 2D high-entropy metal phosphorus trisulfide is developed as a promising and adjustable platform. Leveraging the multiple electron couplings and d-p orbital hybridizations induced by the cocktail effect, the exceptional oxygen evolution catalytic activity is disclosed upon van der Waals material (MnFeCoNiZn)PS3, exhibiting an impressively low overpotential of 240 mV at a current density of 10 mA cm-2, a minimal Tafel slope of 32 mV dec-1, and negligible degradation under varying current densities for over 96 h. Density functional theory calculations further offer insights into the correlation between orbital hybridization and catalytic performance within high-entropy systems, underscoring the contribution of active phosphorus centers on the substrate to performance enhancements. Moreover, by achieving electron redistribution to optimize the electron coordination environment, this work presents an effective strategy for advanced catalysts in energy-related applications. Stimulated by the fantastic "cocktail effect," a versatile 2D high-entropy metal phosphorus trisulfide platform is developed to accelerate oxygen evolution reaction process, where the adsorption of intermediates can be enhanced due to the elevated d-p orbital hybridization. The inherent correlation is further confirmed by advanced spectral characterizations and density functional theory analyses within this high-entropy system. image