Highly efficient electrosynthesis of H_(2)O_(2)in acidic electrolyte on metal-free heteroatoms co-doped carbon nanosheets and simultaneously promoting Fenton process  

作　　者：Xiaodan Wang Yingnan Liu Zhibin Liu Zhongjian Li Tao Zhang Yi Cheng Lecheng Lei Bin Yang Yang Hou 

机构地区：[1]Key Laboratory of Biomass Chemical Engineering of Ministry of Education,College of Chemical and Biological Engineering,Zhejiang University,Hangzhou 310058,China [2]Institute of Zhejiang University-Quzhou,Quzhou 324000,China [3]Donghai Laboratory,Zhoushan 316000,China [4]Ningbo Institute of Materials Technology&Engineering,University of Chinese Academy of Sciences,Ningbo 315200,China [5]School of Biological and Chemical Engineering,NingboTech University,Ningbo 315100,China [6]Zhejiang Hengyi Petrochemical Research Institute Co.,Ltd.,Hangzhou 310058,China

出　　处：《Chinese Chemical Letters》2024年第7期514-518,共5页中国化学快报（英文版）

基　　金：supported by the National Natural Science Foundation of China(Nos.U22A20432,22278364,22211530045,22178308);the Fundamental Research Funds for the Central Universities(Nos.226-2022-00044,226-2022-00055);the Research Funds of Institute of Zhejiang University-Quzhou(No.IZQ2021KJ2003);National Key Research and Development Program of China(No.2022YFB4002100);the development project of Zhejiang Province's"Jianbing"and"Lingyan"(No.2023C01226);the Startup Foundation for Hundred-Talent Program of Zhejiang University;the Science Foundation of Donghai Laboratory(No.DH_(2)022ZY0009);Zhejiang University Global Partnership Fund;the China Postdoctoral Science Foundation(No.2021M702813)。

摘　　要：Recently electrochemical synthesis of H_(2)O_(2)through oxygen reduction reaction(ORR)via 2e^(-)pathway is considered as a green and on-site route.However,it still remains a big challenge for fabricating novel metal-free catalysts under acidic solutions,since it suffers from high overpotential due to the intrinsically week*OOH adsorption.Herein,a co-doped carbon nanosheet(O/N–C)catalyst toward regulating O and N content was synthesized for improving the selectivity and activity of H_(2)O_(2)electrosynthesis process.The O/N–C exhibits outstanding 2e-ORR performance with low onset potential of 0.4 V(vs.RHE)and a selectivity of 92.4%in 0.1 mol/L HClO_(4)solutions.The in situ electrochemical impedance spectroscopy(EIS)tests reveals that the N incorporation contributes to the fast ORR kinetics.The density functional theory(DFT)calculations demonstrate that the binding strength of*OOH was optimized by the co-doping of oxygen and nitrogen at certain content,and the O/N–C–COOH site exhibits a lower theoretical overpotential for H_(2)O_(2)formation than O–C–COOH site.Furthermore,the promoted kinetics for typical organic dye degradation in simultaneous electron-Fenton process on O/N–C catalyst was demonstrated particularly for broadening its environmental application.

关 键 词：Oxygen reduction Metal-free catalyst H_(2)O_(2)electrosynthesis N doping Carbon materials 

分 类 号：TQ123.6[化学工程—无机化工] TQ426