Facile preparation and the stepwise formation mechanistic investigation of gram-scale nitrogen-doped graphene quantum dots,Journal of Materials Chemistry C

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Facile preparation and the stepwise formation mechanistic investigation of gram-scale nitrogen-doped graphene quantum dots
Journal of Materials Chemistry C ( IF 5.7 ) Pub Date : 2017-08-11 00:00:00 , DOI: 10.1039/c7tc02434g
Renbing Tian _{1,

2,

3,

4,

5} , Suting Zhong _{1,

2,

3,

4,

5} , Juan Wu _{1,

2,

3,

4,

5} , Yongliang Geng _{2,

3,

4,

5} , Baojing Zhou _{2,

3,

4,

5} , Qinghua Wang _{5,

6,

7} , Wei Jiang _{1,

2,

3,

4,

5}

Affiliation

Although nitrogen-doped graphene quantum dots (N-doped GQDs) have been widely studied for their unique properties and promising applications, large scale synthesis of N-doped GQDs has been rarely reported. Besides, the formation 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 a nitrogen environment. A mechanism, which is rooted in the chemical properties of NTA and consists of dehydration and nucleophilic addition, has been proposed to explain the formation of N-doped GQDs step by step. Utilizing this method, the change in the structure, functional groups and FL properties can be explained intuitively and clearly. Because of the significant difference in ethanol solubility between the raw material and product, N-doped GQD powder with a purity higher than 99% can be easily obtained by a dissolution–centrifugation–drying–dissolution–freeze drying process without a tedious dialysis process. 1.38 grams of N-doped GQDs could be prepared from 3 grams of NTA. The 46% synthetic yield is higher than that obtained using a large majority of methods reported so far. With the introduction of an N atom, the N-doped GQDs showed bright blue fluorescence (FL) under 365 nm ultraviolet (UV) light, exhibiting a quite high quantum yield of 45.8%. A short preparation time, the low cost of the raw materials, a simple preparation process, high synthetic yield, high quantum yield and a facile purification method make this approach promising in the 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, and used in a fountain pen and ball pen respectively. The words written with FL ink showed strong contrast under daylight and UV light, and no obvious change can be observed after long-term high temperature treatment, indicating that the N-doped GQDs have obvious practicability and good stability as an FL ink.

中文翻译：

克级氮掺杂石墨烯量子点的制备及逐步形成机理研究

尽管已经对氮掺杂石墨烯量子点（N掺杂GQD）的独特性能和有前途的应用进行了广泛研究，但很少报道N掺杂GQD的大规模合成。此外，形成机理总是被简单地解释。本文中，我们报告了一种简便的一步法克级方法，该方法通过在高温和高压下在氮环境下聚合次氮基三乙酸（NTA）来制备N掺杂的GQD。已经提出了一种机制，该机制源于NTA的化学性质，由脱水和亲核加成组成，逐步解释了N掺杂GQD的形成。使用这种方法，可以直观，清晰地说明结构，官能团和FL特性的变化。由于原料和产品之间乙醇溶解度的显着差异，可以通过溶解-离心-干燥-溶解-冷冻干燥过程轻松地获得纯度高于99％的N掺杂GQD粉末，而无需进行繁琐的透析过程。可以从3克NTA中制备1.38克N掺杂的GQD。46％的合成产率高于迄今为止报道的使用大多数方法获得的产率。随着N原子的引入，N掺杂的GQD在365 nm紫外线（UV）下显示出明亮的蓝色荧光（FL），具有相当高的45.8％的量子产率。制备时间短，原料成本低，制备工艺简单，合成收率高，高量子产率和简便的纯化方法使该方法在N掺杂GQD的工业生产中大有前途。此外，N掺杂的GQD以水性和类油性墨水的形式用作手写FL墨水，分别用于钢笔和圆珠笔。用FL油墨书写的单词在日光和紫外线下显示出很强的对比度，经过长期高温处理后没有观察到明显的变化，这表明掺N的GQD作为FL油墨具有明显的实用性和良好的稳定性。

更新日期：2017-09-14

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