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榴莲水热法制备可控晶格硫掺杂石墨烯量子点的简便高效合成

Facile and Highly Effective Synthesis of Controllable Lattice Sulfur-Doped Graphene Quantum Dots via Hydrothermal Treatment of Durian.

机构信息

Department of Microelectronic Science and Engineering, Faculty of Science, Ningbo University , Ningbo 315211, P. R. China.

Department of Materials Science, Fudan University , Shanghai 200433, P. R. China.

出版信息

ACS Appl Mater Interfaces. 2018 Feb 14;10(6):5750-5759. doi: 10.1021/acsami.7b16002. Epub 2018 Jan 31.

Abstract

Recently, the biomass "bottom-up" approach for the synthesis of graphene quantum dots (GQDs) has attracted broad interest because of the outstanding features, including low-cost, rapid, and environmentally friendly nature. However, the low crystalline quality of products, substitutional doping with heteroatoms in lattice, and ambiguous reaction mechanism strongly challenge the further development of this technique. Herein, we proposed a facile and effective strategy to prepare controllable sulfur (S) doping in GQDs, occurring in a lattice substitution manner, by hydrothermal treatment of durian with platinum catalyst. S atoms in GQDs are demonstrated to exist in the thiophene structure, resulting in good optical and chemical stabilities, as well as ultrahigh quantum yield. Detailed mechanism of the hydrothermal reaction progress was investigated. High-efficiency reforming cyclization provided by platinum was evidenced by the coexistence of diversified sp-fused heterocyclic compounds and thiophene derivatives. Moreover, we also demonstrated that saccharides in durian with small molecular weight (<1000 Da) is the main carbon source for the forming GQDs. Because of the desulfurizing process, controllable photoluminescence properties could be achieved in the as-prepared GQDs via tuning doping concentrations.

摘要

最近,由于具有成本低、快速和环保等突出特点,基于生物质的“自上而下”方法合成石墨烯量子点(GQDs)引起了广泛关注。然而,产品结晶质量低、晶格中杂原子取代掺杂以及反应机制不明确等问题,严重阻碍了该技术的进一步发展。在此,我们提出了一种简便有效的策略,通过榴莲与铂催化剂的水热处理,制备出可控的硫(S)掺杂在晶格中的 GQDs,以取代的方式进行掺杂。实验证明,GQDs 中的 S 原子存在于噻吩结构中,具有良好的光学和化学稳定性以及超高的量子产率。详细研究了水热反应过程的机理。铂的高效重整环化作用得到了证实,因为存在多种 sp 杂化的杂环化合物和噻吩衍生物共存。此外,我们还证明了榴莲中小分子量 (<1000 Da) 的糖是形成 GQDs 的主要碳源。由于脱硫过程,通过调节掺杂浓度可以实现所制备 GQDs 的可控光致发光性能。

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