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电子金属-载体相互作用促进Cu/InSe中*OOH中间体的生成用于电化学制氢

Electronic Metal-Support Interactions Boost *OOH Intermediate Generation in Cu/InSe for Electrochemical HO Production.

作者信息

Liu Yuepeng, Wang Pengfei, Xie Liangbo, Xia Yuguo, Zhan Sihui, Hu Wenping, Li Yi

机构信息

Key Laboratory of Organic Integrated Circuits, Ministry of Education & Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Science, Tianjin University, 300072, Tianjin, P. R. China.

MOE Key Laboratory of Pollution Processes and Environmental Criteria, Tianjin Key Laboratory of Environmental Remediation and Pollution Control, College of Environmental Science and Engineering, Nankai University, 300350, Tianjin, P. R. China.

出版信息

Angew Chem Int Ed Engl. 2024 Jun 3;63(23):e202319470. doi: 10.1002/anie.202319470. Epub 2024 Apr 25.

Abstract

Two-electron oxygen reduction reaction (2e ORR) is a promising method for the synthesis of hydrogen peroxide (HO). However, high energy barriers for the generation of key *OOH intermediates hinder the process of 2e ORR. Herein, we prepared a copper-supported indium selenide catalyst (Cu/InSe) to enhance the selectivity and yield of 2e ORR by employing an electronic metal-support interactions (EMSIs) strategy. EMSIs-induced charge rearrangement between metallic Cu and InSe is conducive to *OOH intermediate generation, promoting HO production. Theoretical investigations reveal that the inclusion of Cu significantly lowers the energy barrier of the 2e ORR intermediate and impedes the 4e ORR pathway, thus favoring the formation of HO. The concentration of HO produced by Cu/InSe is ~2 times than InSe, and Cu/InSe shows promising applications in antibiotic degradation. This research presents a valuable approach for the future utilization of EMSIs in 2e ORR.

摘要

双电子氧还原反应(2e ORR)是一种很有前景的合成过氧化氢(HO)的方法。然而,关键OOH中间体生成的高能垒阻碍了2e ORR的进程。在此,我们制备了一种铜负载硒化铟催化剂(Cu/InSe),通过采用电子金属-载体相互作用(EMSI)策略来提高2e ORR的选择性和产率。EMSI诱导的金属Cu和InSe之间的电荷重排有利于OOH中间体的生成,促进HO的产生。理论研究表明,Cu的加入显著降低了2e ORR中间体的能垒,并阻碍了4e ORR途径,从而有利于HO的形成。Cu/InSe产生的HO浓度约为InSe的2倍,并且Cu/InSe在抗生素降解方面显示出有前景的应用。这项研究为EMSI在2e ORR中的未来应用提供了一种有价值的方法。

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