文献类型：期刊文献

英文题名：N-B-OH Site-Activated Graphene Quantum Dots for Boosting Electrochemical Hydrogen Peroxide Production

作者：Fan, Mengmeng[1,2] Wang, Zeming[3] Sun, Kang[2] Wang, Ao[2] Zhao, Yuying[2] Yuan, Qixin[1] Wang, Ruibin[1] Raj, Jithu[4] Wu, Jingjie[4] Jiang, Jianchun[1,2] Wang, Liang[3]

第一作者：Fan, Mengmeng

通信作者：Fan, MM[1];Jiang, JC[1];Fan, MM[2];Jiang, JC[2];Wang, L[3];Wu, JJ[4]

机构：[1]Nanjing Forestry Univ, Coll Chem Engn, Jiangsu Coinnovat Ctr Efficient Proc & Utilizat Fo, Int Innovat Ctr Forest Chem & Mat, 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]Shanghai Univ, Inst Nanochem & Nanobiol, Sch Environm & Chem Engn, Shanghai 200444, Peoples R China;[4]Univ Cincinnati, Dept Chem & Environm Engn, Cincinnati, OH 45221 USA

年份：0

外文期刊名：ADVANCED MATERIALS

收录：;EI(收录号：20231313803401);Scopus(收录号：2-s2.0-85150766897);WOS:【SCI-EXPANDED(收录号:WOS:000952075600001)】；

基金：M.F. acknowledges the support to this work by "The National Natural Science Foundation of China (No. 51902162, 21901154)". 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. Shanghai Pujiang Program (21PJD022), the Foundation of Jiangsu Key Lab of Biomass Energy and Material (JSBEM-S-202101).

语种：英文

外文关键词：2 e(-) electrocatalysis; graphene quantum dots; hydrogen peroxide synthesis; N-B-OH sites; oxygen reduction reaction

摘要：Carbon materials are considered promising 2/4 e(-) oxygen reduction reaction (ORR) electrocatalysts for synthesizing H2O2/H2O via regulating heteroatom dopants and functionalization. Here, various doped and functionalized graphene quantum dots (GQDs) are designed to reveal the crucial active sites of carbon materials for ORR to produce H2O2. Density functional theory (DFT) calculations predict that the edge structure involving edge N, B dopant pairs and further -OH functionalization to the B (N-B-OH) is an active center for 2e(-) ORR. To verify the above predication, GQDs with an enriched density of N-B-OH (NBO-GQDs) are designed and synthesized by the hydrothermal reaction of -NH2 edge-functionalized GQDs with H3BO3 forming six-member heterocycle containing the N-B-OH structure. When dispersed on conductive carbon substrates, the NBO-GQDs show H2O2 selectivity of over 90% at 0.7 -0.8 V versus reversible hydrogen electrode in the alkaline solution in a rotating ring-disk electrode setup. The selectivity retains 90% of the initial value after 12 h stability test. In a flow cell setup, the H2O2 production rate is up to 709 mmol g(catalyst)(-1) h(-1), superior to most reported carbon- and metal-based electrocatalysts. This work provides molecular insight into the design and formulation of highly efficient carbon-based catalysts for sustainable H2O2 production.