文献类型：期刊文献

英文题名：Boosting Hydrogen Peroxide Electrosynthesis via Modulating the Interfacial Hydrogen-Bond Environment

作者：Fang, Yushuang[1,2];Fan, Yu[1];Xie, Kunchi[1];Ge, Wangxin[2];Zhu, Yihua[1];Qi, Zhiwen[1];Song, Zhen[1];Jiang, Hongliang[1];Li, Chunzhong[1,2]

机构：[1]East China Univ Sci & Technol, Sch Chem Engn, Key Lab Ultrafine Mat Minist Educ, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Mat Sci & Engn, Shanghai 200237, Peoples R China

年份：2023

卷号：62

期号：27

外文期刊名：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

收录：;EI(收录号：20232114137450);WOS:【SCI-EXPANDED(收录号:WOS:000992452700001)】；

基金：Acknowledgments This work was supported by the National Natural Science Foundation of China (22222804 and U22B20143), the National Key R&D program (2022YFB3808400), the Science and Technology Commission of Shanghai Municipality (22dz1205900), and the Shanghai Municipal Science and Technology Major Project. The authors thank the Shanghai Synchrotron Radiation Facility (14W1, SSRF).

语种：英文

外文关键词：Electrode-Electrolyte Interface; Electrolyte; H2O2 Electrosynthesis; Hydrogen-Bond Network; Oxygen Reduction Reaction

摘要：Designing highly efficient and stable electrode-electrolyte interface for hydrogen peroxide (H2O2) electrosynthesis remains challenging. Inhibiting the competitive side reaction, 4 e(-) oxygen reduction to H2O, is essential for highly selective H2O2 electrosynthesis. Instead of hindering excessive hydrogenation of H2O2 via catalyst modification, we discover that adding a hydrogen-bond acceptor, dimethyl sulfoxide (DMSO), to the KOH electrolyte enables simultaneous improvement of the selectivity and activity of H2O2 electrosynthesis. Spectral characterization and molecular simulation confirm that the formation of hydrogen bonds between DMSO and water molecules at the electrode-electrolyte interface can reduce the activity of water dissociation into active H* species. The suitable H* supply environment hinders excessive hydrogenation of the oxygen reduction reaction (ORR), thus improving the selectivity of 2 e(-) ORR and achieving over 90 % selectivity of H2O2. This work highlights the importance of regulating the interfacial hydrogen-bond environment by organic molecules as a means of boosting electrochemical performance in aqueous electrosynthesis and beyond.