title: Unraveling the formation mechanism of graphitic nitrogen-doping in thermally treated graphene with ammonia.
abstract: Nitrogen-doped graphene (N-graphene) has attractive properties that has 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.
authors.affiliation: School of Optoelectronic Information, University of Electronic Science and Technology of China, Chengdu, Sichuan, 610054, China.
authors.forename: Xiao-Fei
authors.initials: XF
authors.lastname: Li
authors.affiliation: Division of Theoretical Chemistry and Biology, School of Biotechnology, Royal Institute of Technology, S-106 91 Stockholm, Sweden.
authors.forename: Ke-Yan
authors.initials: KY
authors.lastname: Lian
authors.affiliation: School of Optoelectronic Information, University of Electronic Science and Technology of China, Chengdu, Sichuan, 610054, China.
authors.forename: Lingling
authors.initials: L
authors.lastname: Liu
authors.affiliation: School of Optoelectronic Information, University of Electronic Science and Technology of China, Chengdu, Sichuan, 610054, China.
authors.forename: Yingchao
authors.initials: Y
authors.lastname: Wu
authors.affiliation: School of Optoelectronic Information, University of Electronic Science and Technology of China, Chengdu, Sichuan, 610054, China.
authors.forename: Qi
authors.initials: Q
authors.lastname: Qiu
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale and Synergetic Innovation Center of Quantum Information and Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026, China.
authors.forename: Jun
authors.initials: J
authors.lastname: Jiang
authors.affiliation: Guizhou Synergetic Innovation Center of Scientific Big Data for Advanced Manufacturing Technology, Guizhou Education University, Guiyang, 550018, China.
authors.forename: Mingsen
authors.initials: M
authors.lastname: Deng
authors.affiliation: Division of Theoretical Chemistry and Biology, School of Biotechnology, Royal Institute of Technology, S-106 91 Stockholm, Sweden.|Hefei National Laboratory for Physical Sciences at the Microscale and Synergetic Innovation Center of Quantum Information and Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026, China.|Guizhou Synergetic Innovation Center of Scientific Big Data for Advanced Manufacturing Technology, Guizhou Education University, Guiyang, 550018, China.
authors.forename: Yi
authors.initials: Y
authors.lastname: Luo