文献类型：期刊文献

英文题名：Enhanced Electrochemical Synthesis of Hydrogen Peroxide via Two-Electron Oxygen Reduction at Highly Active -SH Edge Sites

作者：Wu, Yuhan[1] Shen, Zijun[1] Yuan, Qixin[1] Zhao, Yuying[2,3] Xu, Xiang[1] Sun, Kang[2] Wang, Ao[2] Sun, Hao[2] Li, Bei[2] Hu, Shengchun[2] Xu, Ruting[2] Wang, Ziyun[3] Jiang, Jianchun[2] Fan, Mengmeng[1,2]

第一作者：Wu, Yuhan

通信作者：Fan, MM[1];Fan, MM[2];Wang, ZY[3]

机构：[1]Nanjing Forestry Univ, Coll Chem Engn, Int Innovat Ctr Forest Chem & Mat, Jiangsu Coinnovat Ctr Efficient Proc & Utilizat Fo, Nanjing 210037, Peoples R China;[2]Chinese Acad Forestry, Inst Chem Ind Forest Prod, Jiangsu Coinnovat Ctr Efficient Proc & Utilizat Fo, Key Lab Biomass Energy & Mat, Nanjing 210042, Jiangsu, Peoples R China;[3]Univ Auckland, Sch Chem Sci, Auckland 1010, New Zealand

年份：2025

卷号：13

期号：14

起止页码：5178-5189

外文期刊名：ACS SUSTAINABLE CHEMISTRY & ENGINEERING

收录：;EI(收录号：20251418191745);Scopus(收录号：2-s2.0-105001839922);WOS:【SCI-EXPANDED(收录号:WOS:001456893100001)】；

基金：M.F. acknowledges the support of this work by the Foundation Research Project of Jiangsu Province (BK20221338). Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, International Innovation Center for Forest Chemicals and Materials, Nanjing Forestry University, the Foundation of Jiangsu Key Lab of Biomass Energy and Material (JSBEM-S-202101). The computational study is supported by the Marsden Fund Council from Government funding (21-UOA-237) and Catalyst: Seeding General Grant (22-UOA-031-CGS), managed by Royal Society Te Aparangi.

语种：英文

外文关键词：sulfhydryl groups; electrocatalyst; two-electron; oxygen reduction reaction; hydrogen peroxide

摘要：Electrochemical generation of hydrogen peroxide (H2O2) through the two-electron oxygen reduction reaction (2e- ORR) represents a sustainable development strategy for bulk H2O2 manufacturing, yet crafting efficient catalysts remains a substantial challenge. Carbon materials are particularly appealing as electrochemical catalysts, owing to their diverse nanostructures and adjustable electrochemical attributes. Nonetheless, the lack of structure-property understanding has hindered the progression of metal-free carbon electrocatalysts. In this study, we fabricated porous carbon with abundant edge sulfhydryl groups (-SH) and determined that the 2e- ORR performance is roughly proportional to the edge -SH content, outperforming reported ORR catalysts in aspects such as H2O2 selectivity (90-98% over a broad potential of 0.30-0.70 V vs RHE) and stability (maintaining over 90% performance during 12 h testing) as measured in alkaline solution in a rotating ring-disk electrode setup. Furthermore, in a flow cell setup, both the H2O2 production rate (2910 mmol gcatalyst -1 h-1) and Faraday efficiency (over 80%) surpass most reported carbon- and metal-based electrocatalysts. Consequently, this research illuminates a straightforward pathway to design specific sulfur configurations in carbon-based catalysts for high-selectivity H2O2 production.