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Facile preparation and the stepwise formation mechanistic investigation of gram-scale nitrogen-doped graphene quantum dots


Although nitrogen-doped graphene quantum dots (N-doped GQDs) have been widely studied for their unique properties and promising application, large scale synthesis of N-doped GQDs have been rarely reported. Besides, the foramtion mechanism was always explained simply. Herein we report a facile one-step gram-scale approach to prepare N-doped GQDs by polymerization of nitrilotriacetic acid (NTA) under high temperature and pressure in nitrogen environment. A mechanism, which is rooted in the chemical property of NTA and consisted of dehydration and nucleophilic addition, has been proposed to explain the formation of N-doped GQDs step by step. Utilizing this way, the change of structure, functional groups and FL properties can be explained intuitionisticly and clearly. Because of the significant difference of ethanol solubility between raw material and product, N-doped GQDs powder with purity higher than 99% can be easily obtained by dissolution-centrifugation-drying-dissolution-freeze drying process without tedious dialysis process. 1.38 gram of N-doped GQDs could be prepared from 3 gram of NTA. 46% of synthetic yield is higher than a large majority method reported so far. As introducing of N atom, the N-doped GQDs showed bright blue fluorescent (FL) under 365 nm ultraviolet (UV) light, exhibiting a quite high quantum yield of 45.8%. Short preparation time, low cost of raw material, simple preparation process, high synthetic yield, high quantum yield and facile purification method make this approach promising in industrial production of N-doped GQDs. Besides, the N-doped GQDs were used as handwriting FL ink in the form of aqueous and oil-like ink, used in fountain pen and ball pen namely. The words wrotten by FL ink showed strong contrast under daylight and UV light, and no obvious change can be observed for long-time high temperature treatment, indicating N-doped GQDs has obvious practicability and good stability as FL ink.

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Publication details

The article was received on 02 Jun 2017, accepted on 11 Aug 2017 and first published on 11 Aug 2017

Article type: Paper
DOI: 10.1039/C7TC02434G
Citation: J. Mater. Chem. C, 2017, Accepted Manuscript
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    Facile preparation and the stepwise formation mechanistic investigation of gram-scale nitrogen-doped graphene quantum dots

    R. Tian, S. Zhong, J. Wu, Y. Gen, B. Zhou, Q. Wang and W. Jiang, J. Mater. Chem. C, 2017, Accepted Manuscript , DOI: 10.1039/C7TC02434G

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