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Unraveling the formation mechanism of graphitic nitrogen-doping in thermally treated graphene with ammonia
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 per...
Autores principales: | , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group
2016
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4802320/ https://www.ncbi.nlm.nih.gov/pubmed/27002190 http://dx.doi.org/10.1038/srep23495 |
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author | Li, Xiao-Fei Lian, Ke-Yan Liu, Lingling Wu, Yingchao Qiu, Qi Jiang, Jun Deng, Mingsen Luo, Yi |
author_facet | Li, Xiao-Fei Lian, Ke-Yan Liu, Lingling Wu, Yingchao Qiu, Qi Jiang, Jun Deng, Mingsen Luo, Yi |
author_sort | Li, Xiao-Fei |
collection | PubMed |
description | 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. |
format | Online Article Text |
id | pubmed-4802320 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2016 |
publisher | Nature Publishing Group |
record_format | MEDLINE/PubMed |
spelling | pubmed-48023202016-03-23 Unraveling the formation mechanism of graphitic nitrogen-doping in thermally treated graphene with ammonia Li, Xiao-Fei Lian, Ke-Yan Liu, Lingling Wu, Yingchao Qiu, Qi Jiang, Jun Deng, Mingsen Luo, Yi Sci Rep Article 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. Nature Publishing Group 2016-03-22 /pmc/articles/PMC4802320/ /pubmed/27002190 http://dx.doi.org/10.1038/srep23495 Text en Copyright © 2016, Macmillan Publishers Limited http://creativecommons.org/licenses/by/4.0/ This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ |
spellingShingle | Article Li, Xiao-Fei Lian, Ke-Yan Liu, Lingling Wu, Yingchao Qiu, Qi Jiang, Jun Deng, Mingsen Luo, Yi Unraveling the formation mechanism of graphitic nitrogen-doping in thermally treated graphene with ammonia |
title | Unraveling the formation mechanism of graphitic nitrogen-doping in thermally treated graphene with ammonia |
title_full | Unraveling the formation mechanism of graphitic nitrogen-doping in thermally treated graphene with ammonia |
title_fullStr | Unraveling the formation mechanism of graphitic nitrogen-doping in thermally treated graphene with ammonia |
title_full_unstemmed | Unraveling the formation mechanism of graphitic nitrogen-doping in thermally treated graphene with ammonia |
title_short | Unraveling the formation mechanism of graphitic nitrogen-doping in thermally treated graphene with ammonia |
title_sort | unraveling the formation mechanism of graphitic nitrogen-doping in thermally treated graphene with ammonia |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4802320/ https://www.ncbi.nlm.nih.gov/pubmed/27002190 http://dx.doi.org/10.1038/srep23495 |
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