破悉热氨处理石墨烯法制备石墨型氮掺杂的生成机理
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- 英文论文题名：Unraveling the formation mechanism of graphitic nitrogen-doping in thermally treated graphene with ammonia
- 论文作者：李小飞 ; 连科研 ; 刘凌玲 ; 胡颖超 ; 邱琪 ; 江俊 ; 邓明森 ; 罗毅
- 英文论文作者：Xiao-Fei Li ; K.-Y.Lian ; L.Liu ; Y.Wu ; Q.Qiu ; J.Jiang ; M.Deng ; Y.Luo ; School of Optoelectronic Information ; University of Electronic Science and Technology of China ; Division of Theoretical Chemistry and Biology ; School of Biotechnology ; Royal Institute of Technology ; Hefei National Laboratory for Physical Sciences at the Microscale and Synergetic Innovation Center of Quantum Information and Quantum Physics ; University of Science and Technologyof China ; Guizhou Synergetic Innovation Center of Scientific Big Data for Advanced Manufacturing Technology ; Guizhou Education University
- 年：2016
- 作者机构：电子科技大学,光电信息学院;瑞典皇家理工学院,生物技术与理论化学系;中国科技大学,合肥微尺度物质科学国家实验室;贵州师范学院,科学云大数据开发及其产业应用协同创新中心;
- 论文关键词：氮掺杂 ; 石墨烯 ; 生成机理 ; 从头算分子动力学
- 会议召开时间：2016-07-01
- 会议录名称：中国化学会第30届学术年会摘要集-第十八分会：电子结构理论方法的发展与应用
- 语种：中文
- 分类号：O613.71
- 学会代码：ZGHY
- 会议名称：中国化学会第30届学术年会-第十八分会 ; 电子结构理论方法的发展与应用
- 会议地点：中国辽宁大连
- 主办单位：中国化学会
- 学会名称：中国化学会
- 页数：2
- 文件大小：156k
- 原文格式：D
- 会议级别：全国
摘要
氮掺杂石墨烯具有引人注目的属性而被研究多年,但其可能的生机过程至今还不清楚。本文中,我们针对热氨处理石墨烯制备氮掺杂石墨型过程进行基于从头算分子动力学的研究,提出了一种高度可行的生成机理。我们的结果表明在各种通常的石墨烯本征点缺陷中,只有单空位缺陷5-9和双空位缺陷555-777具有捕获氨基并使其脱氢的电子结构。这两个缺陷的局域结构特征与热动学效应结合在一起,对体系的复杂原子重组过程起决定作用,导致生成石墨型氮掺杂并同时完美修复相应缺陷。表明结构对称性、局域力场、多氨基之间的相互作用以及临时生成的桥位氮催化效应等在起重要作用。所获氮掺杂构型与实验发现完全一致。因此,所揭示的生成机理将对实验上目标制备具有特定属性和少缺陷的氮掺杂石墨烯具有重要指导意义。
Nitrogen-doped graphene(N-graphene) has attractive properties that have been widely studied over the years.However, its possible formation process still remains unclear.Here, we propose a highly feasible formation mechanism of the graphitic-N doing in thermally treated graphene with ammonia by performing ab initio molecular dynamic simulations at experimental conditions.Results show that among the commonly native point defects in graphene, only the single vacancy 5-9 and divacancy 555-777 have the desirable electronic structures to trap N-containing groups and to mediate the subsequent dehydrogenation processes.The local structure of the defective graphene in combining with the thermodynamic and kinetic effect plays a crucial role in dominating the complex atomic rearrangement to form graphitic-N which heals the corresponding defect perfectly.The importance of the symmetry, the localized force field, the interaction of multiple trapped N-containing groups, as well as the catalytic effect of the temporarily formed bridge-N are emphasized, and the predicted doping configuration agrees well with the experimental observation.Hence, the revealed mechanism will be helpful for realizing the targeted synthesis of N-graphene with reduced defects and desired properties.
Nitrogen-doped graphene(N-graphene) has attractive properties that have been widely studied over the years.However, its possible formation process still remains unclear.Here, we propose a highly feasible formation mechanism of the graphitic-N doing in thermally treated graphene with ammonia by performing ab initio molecular dynamic simulations at experimental conditions.Results show that among the commonly native point defects in graphene, only the single vacancy 5-9 and divacancy 555-777 have the desirable electronic structures to trap N-containing groups and to mediate the subsequent dehydrogenation processes.The local structure of the defective graphene in combining with the thermodynamic and kinetic effect plays a crucial role in dominating the complex atomic rearrangement to form graphitic-N which heals the corresponding defect perfectly.The importance of the symmetry, the localized force field, the interaction of multiple trapped N-containing groups, as well as the catalytic effect of the temporarily formed bridge-N are emphasized, and the predicted doping configuration agrees well with the experimental observation.Hence, the revealed mechanism will be helpful for realizing the targeted synthesis of N-graphene with reduced defects and desired properties.
引文
[1]Li,X.-F.;Lian,K.-Y.;Liu,L.;Wu,Y.;Qiu,Q.;Jiang,J.;Deng,M.;Luo,Y.Sci.Rep.,2016,6:23495.
[2]Li,X.-F.;Lian,K.-Y.;Qiu,Q.;Luo,Y.Nanoscale,2015,7:4156.
[2]Li,X.-F.;Lian,K.-Y.;Qiu,Q.;Luo,Y.Nanoscale,2015,7:4156.