文献类型：期刊文献

英文题名：Toward More Efficient Carbon-Based Electrocatalysts for Hydrogen Peroxide Synthesis: Roles of Cobalt and Carbon Defects in Two-Electron ORR Catalysis

作者：Zheng, Yuanjie[1];Wang, Peng[1];Huang, Wei-Hsiang[2,3];Chen, Chi-Liang[2,3];Jia, Yanyan[4,5];Dai, Sheng[4,5];Li, Tan[1];Zhao, Yun[1];Qiu, Yongcai[1];Waterhouse, Geoffrey I. N.[6];Chen, Guangxu[1]

机构：[1]South China Univ Technol, Sch Environm & Energy, State Key Lab Luminescent Mat & Devices, Guangdong Prov Key Lab Atmospher Environm & Pollut, Guangzhou 51006, Peoples R China;[2]Natl Synchrotron Radiat Res Ctr, Hsinchu 30076, Taiwan;[3]Natl Taiwan Univ Sci & Technol, Grad Inst Appl Sci & Technol, Taipei 10607, Taiwan;[4]East China Univ Sci & Technol, Sch Chem & Mol Engn, Frontiers Sci Ctr Materiobiol & Dynam Chem, Key Lab Adv Mat,Feringa Nobel Prize Scientist Join, Shanghai 200237, Peoples R China;[5]East China Univ Sci & Technol, Inst Fine Chem, Frontiers Sci Ctr Materiobiol & Dynam Chem, Joint Int Res Lab Precis Chem & Mol Engn,Feringa N, Shanghai 200237, Peoples R China;[6]Univ Auckland, Sch Chem Sci, Auckland 1142, New Zealand

年份：2023

卷号：23

期号：3

起止页码：1100

外文期刊名：NANO LETTERS

收录：;EI(收录号：20230513467197);WOS:【SCI-EXPANDED(收录号:WOS:000924990800001)】；

基金：This work was supported by the National Natural Science Foundation of China (21971070), Natural Science Foundation of Guangdong Province (2022A1515012047), Guangdong Innovative and Entrepreneurial Research Team Program (2019ZT08L075), Guangdong Pearl River Talent Program (2019QN01L159), Guangdong Provincial Key R&D Program (2020B010188002), and Science and Technology Program of Guangzhou of China (202103040002) financially. G.I.N.W. acknowledges financial support from Greg and Kathryn Trounson (via a generous philanthropic donation) and the Royal Society Te Aparangi (via award of a James Cook Research Fellowship).

语种：英文

外文关键词：2-electron oxygen reduction reaction; carbon-based catalyst; cobalt doping

摘要：Electrochemical production of H2O2 is a cost-effective and environmentally friendly alternative to the anthraquinone-based processes. Metal-doped carbon-based catalysts are commonly used for 2 electron oxygen reduction reaction (2e-ORR) due to their high selectivity. However, the exact roles of metals and carbon defects on ORR catalysts for H2O2 production remain unclear. Herein, by varying the Co loading in the pyrolysis precursor, a Co-N/O-C catalyst with Faradaic efficiency greater than 90% in alkaline electrolyte was obtained. Detailed studies revealed that the active sites in the Co-N/O-C catalysts for 2e-ORR were carbon atoms in C-O-C groups at defect sites. The direct contribution of cobalt single atom sites and metallic Co for the 2e-ORR performance was negligible. However, Co plays an important role in the pyrolytic synthesis of a catalyst by catalyzing carbon graphitization, tuning the formation of defects and oxygen functional groups, and controlling O and N concentrations, thereby indirectly enhancing 2e-ORR performance.