Molecule functionalization to facilitate electrocatalytic oxygen reduction on graphdiyne

作     者：Huiying Yao Yasong Zhao Nailiang Yang Wei Hao Hu Zhao Shuzhou Li Jia Zhu Lin Shen Weihai Fang Huiying Yao;Yasong Zhao;Nailiang Yang;Wei Hao;Hu Zhao;Shuzhou Li;Jia Zhu;Lin Shen;Weihai Fang

作者机构：College of ChemistryKey Laboratory of Theoretical&Computational Photochemistry of Ministry of EducationBeijing Normal UniversityBeijing 100875China State Key Laboratory of Biochemical EngineeringInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of Materials Science and EngineeringNanyang Technological University50 Nanyang Avenue639798Singapore Department of PhysicsBeijing Normal UniversityBeijing 100875China Laboratory of Theoretical and Computational NanoscienceCAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyChinese Academy of SciencesBeijing 100190China 

出 版 物：《Journal of Energy Chemistry》 (能源化学（英文版）)

年 卷 期：2022年第31卷第2期

页      面：141-148页

核心收录：

学科分类：081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 

基　　金：supported by the National Natural Science Foundation of China(21773016,21971244,51932001) the National Key R&D Program of China(2018YFA0703504) 

主　　题：Graphdiyne F4TCNQ Density functional calculations Electronic structure Oxygen reduction reaction 

摘      要：Chemical doping is verified to be a promising strategy to regulate local electron distribution and further promote the poor intrinsic catalytic activity of ***,the current doping approach still faces problems such as precise doping for creating active sites and the destruction of graphdiyne skeleton calling for high ***,we achieved charge redistribution on graphdiyne surface through molecule functionalization.A p-type molecule–F4 TCNQ(2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodime thane)was introduced and the site-defined functionalization was *** calculations showed that the charge transfer ability is improved and graphdiyne becomes positively *** oxygen reduction electrocatalysis was conducted as a proof of principle,where the electronic states of sp hybridized C active site was tuned toward favorable reaction intermediates’*** work from both theoretical prediction and experimental validation,found that molecule functionalization is effective to promote the electrocatalytic oxygen reduction,which creates new possibilities for graphdiyne’s applications in different electrochemical reactions.