Unveiling the chemistry behind the electrolytic production of hydrogen peroxide by oxygenated carbon

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外文摘要：Oxygenated carbon materials exhibit outstanding electrocatalytic performance in the production of hydrogen peroxide(H2O2)through a two-electron oxygen reduction reaction.The nature of the active functional group and underlying reaction mechanism,however,remain unclear.Here,a comprehensive workflow was established to identify the active sites from the numerous possible structures.The com-mon hydroxyl group at the notched edge demonstrates a key role in the two-electron process.The local chemical environment weakens the binding of OOH intermediate to substrate while enhancing interac-tion with solution,thereby promoting the H2O2 production.With increasing pH,the intramolecular hydrogen bond between OOH intermediate and hydroxyl decreases,facilitating OOH desorption.Furthermore,the rise in selectivity with increasing potential stems from the suppression of the four-electron process.The active site was further validated through experiments.Guided by theoretical under-standing,optimal performance was achieved with high selectivity(＞95％)and current density(2.06 mA/cm2)in experiment.

外文关键词：

First-principles calculationOxygen reduction reactionHydrogen peroxide productionFixed-potential methodOxygenated carbon materials

作者：

Pan Xiang、Kunshang Yang、Qihao Yang、Yang Gao、Wenwen Xu、Zhiyi Lu、Liang Chen、Zhiming Wang、Ziqi Tian

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作者单位：

Institute of Fundamental and Frontier Sciences,University of Electronic Science and Technology of China,Chengdu 610054,Sichuan,China

Key Laboratory of Advanced Fuel Cells and Electrolyzers Technology of Zhejiang Province,Ningbo Institute of Materials Technology and Engineering,Chinese Academy of Sciences,Ningbo 315201,Zhejiang,China

Institute for Advanced Study,Chengdu University,Chengdu 610106,Sichuan,China

基金：

National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaZhejiang Provincial Natural Science Foundation of ChinaFujian Institute of Innovation and Chinese Academy of Sciences.K.C.Wong Education FoundationNational Key Research and Development Program of ChinaNingbo Yongjiang Talent Introduction ProgrammeNingBo S&T Innovation 2025 Major Special Programme111 Project

项目编号：

5217102222105214LXR22B030001GJTD-2019-132019YFB22034002021A-036-B2020Z059B20030

出版年：

2024

DOI：

10.1016/j.jechem.2024.04.032

能源化学

中国科学院大连化学物理研究所中国科学院成都有机化学研究所

能源化学

CSTPCDEI

影响因子：0.654

ISSN：2095-4956

年,卷(期)：2024.96(9)