Enhanced Oxygen Reduction on Graphene via Y5Si3 Electride Substrate:a First-Principles Study  

阴离子化合物Y5Si3衬底增强石墨烯氧还原反应的第一性原理研究（英文）

作　　者：Jing-jing Lin Hai-feng Lv Xiao-jun Wu 林晶晶;吕海峰;武晓君(中国科学技术大学化学与材料科学学院合肥微尺度物质科学国家研究中心中国科学院能量转换材料重点实验室量子信息和量子科技前沿协同创新中心)

机构地区：[1]Hefei National Laboratory for Physical Science at the Microscale,School of Chemistry and Mate-rials Sciences,CAS Key Laboratory of Materials for Energy Conversion,and CAS Center for Ex-cellence in Nanoscience,University of Science and Technology of China,Hefei 230026,China Synergetic Innovation Center of Quantum Information&Quantum Physics,University of Science and Technology of China,Hefei 230026,China

出　　处：《Chinese Journal of Chemical Physics》2018年第5期649-654,735,共7页化学物理学报（英文）

基　　金：supported by the National Natural Science Foundation of China (No.21573204 and No.21421063);Ministry of Science and Technology of China (No.2016YFA0200602);Anhui Initiative in Quantum Information Technologies, Fundamental Research Funds for the Central Universities;National Program for Support of Top-notch Young Professional, Chinese Academy of Sciences Interdisciplinary Innovation Team;Super Computer Center of USTC supercomputing center and CAS supercomputing center

摘　　要：Manipulating the chemical reactivity of graphene toward oxygen reduced reduction(ORR)is of particular interest for both fundamental research and practical application in fuel cell.Deposing graphene on selected substrate provides a structure-intact strategy to enhance its chemical reactivity due to substrate-induced charge and interface effect.Here,we report the graphene deposited on one-dimensional electride Y5Si3 as an effective ORR catalyst in acidic media.Thermodynamic calculations suggest that depositing graphene on electride materials can facilitate the protonation of O2,which is the rate-determining step based on the four-electron reaction pathway and thus promote the ORR activity.Further electronic calculations reveal that low work function(3.5 eV),superior electrical conductivity and slight charge transfer from substrate to graphene result in the enhanced ORR performance of graphene.These findings shed light on the rational design of ORR catalysts based on graphitic materials and emphasize the critical role of substrates for energy-related electrochemical reactions.

关 键 词：First-principles calculations GRAPHENE Oxygen reduced reduction ELECTRIDES 

分 类 号：TM911.4[电气工程—电力电子与电力传动] TQ426[化学工程]