Nitrogen-Doping Chemical Behavior of Graphene Materials with Assistance of Defluorination

Nitrogen-Doping Chemical Behavior of Graphene Materials with Assistance of Defluorination
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脱氟辅助石墨烯材料的氮掺杂化学行为

DOI:
10.1021/acs.jpcc.8b10276
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发表时间:
2018-12
影响因子:
3.7
通讯作者:
Liu Xiangyang
Liu Xiangyang
中科院分区:
化学3区
文献类型:
--
作者:
Li Yulong;Wang Xu;Wang Weimiao;Qin Rui;Lai Wenchuan;Ou Anping;Liu Yang;Liu Xiangyang

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杂原子掺杂反应是实现能源和生物领域先进石墨烯基材料的必要条件。不幸的是,到目前为止,对详细的反应途径所知甚少。本文主要研究了基于改进原位傅里叶变换红外光谱的氟化石墨烯(FG)在脱氟辅助下的氮掺杂过程。实验证明,与其他石墨烯衍生物相比,FG具有更高和更有效的氨反应性,这使得n掺杂即使在较低的温度(16.8℃)下也能在脱氟的帮助下有效地进行。300°C时N含量为%,300°C时为19.9。% N(400℃)。结合密度泛函理论证明,在n掺杂反应初始阶段,氨分子攻击FG中的C-F,并被新的C-NH2取代。依次将氨基环化成乙烯亚胺的三元环。更重要的是,分离和迁移…
Heteroatom-doping reactions are essential to achieve advanced graphene-based materials for energy and biological areas. Unfortunately, considerably less is known regarding the detailed reaction pathways up to now. Here, we focus on investigating the nitrogen (N) doping process of fluorinated graphene (FG) under the assistance of defluorination based on modified in situ Fourier transform infrared spectroscopy. It was demonstrated FG possesses a higher and more effective reactivity with ammonia in comparison with other graphene derivatives, which enable N-doping to proceed efficiently with assistance of defluorination even at a lower temperature (16.8 at. % of N at 300 °C and 19.9 at. % of N at 400 °C). Combining with Density functional theory, it was proved that, at the initial reaction step of N-doping, ammonia molecule attacked and substituted the C–F of FG by the new C-NH2. Sequentially, amino group was cyclized to the three-membered ring of ethylenimine. More importantly, the dissociation and migration...
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