Li Liangchuan, Zhou Ming, Jin Long, Mo Youtang, Xu Enyong, Chen Huajin, Liu Lincong, Wang Mingyue, Chen Xin, Zhu Hongwei
School of Mechanical and Transportation Engineering, Guangxi University of Science and Technology, Liuzhou 545006, China.
Dongfeng Liuzhou Motor Co., Ltd., Liuzhou 545006, China.
Materials (Basel). 2020 Sep 14;13(18):4069. doi: 10.3390/ma13184069.
The large-scale preparation of stable graphene aqueous dispersion has been a challenge in the theoretical research and industrial applications of graphene. This study determined the suitable exfoliation agent for overcoming the van der Waals force between the layers of expanded graphite sheets using the liquid-phase exfoliation method on the basis of surface energy theory to prepare a single layer of graphene. To evenly and stably disperse graphene in pure water, the dispersants were selected based on Hansen solubility parameters, namely, hydrophilicity, heterocyclic structure and easy combinative features. The graphene exfoliation grade and the dispersion stability, number of layers and defect density in the dispersion were analysed under Tyndall phenomenon using volume sedimentation method, zeta potential analysis, scanning electron microscopy, Raman spectroscopy and atomic force microscopy characterization. Subsequently, the long-chain quaternary ammonium salt cationic surfactant octadecyltrimethylammonium chloride (0.3 wt.%) was electrolyzed in pure water to form ammonium ions, which promoted hydrogen bonding in the remaining oxygen-containing groups on the surface of the stripped graphene. Forming the electrostatic steric hindrance effect to achieve the stable dispersion of graphene in water can exfoliate a minimum of eight layers of graphene nanosheets; the average number of layers was less than 14. The 0.1 wt.% (sodium dodecylbenzene sulfonate: melamine = 1:1) mixed system forms π-π interaction and hydrogen bonding with graphene in pure water, which allow the stable dispersion of graphene for 22 days without sedimentation. The findings can be beneficial for the large-scale preparation of waterborne graphene in industrial applications.
在石墨烯的理论研究和工业应用中,大规模制备稳定的石墨烯水分散体一直是一项挑战。本研究基于表面能理论,采用液相剥离法确定了合适的剥离剂,以克服膨胀石墨片层间的范德华力,制备单层石墨烯。为了使石墨烯在纯水中均匀稳定地分散,基于汉森溶解度参数选择了分散剂,即亲水性、杂环结构和易于结合的特性。利用体积沉降法、zeta电位分析、扫描电子显微镜、拉曼光谱和原子力显微镜表征,在廷德尔现象下分析了石墨烯的剥离等级、分散稳定性、分散体中的层数和缺陷密度。随后,将长链季铵盐阳离子表面活性剂十八烷基三甲基氯化铵(0.3 wt.%)在纯水中电解形成铵离子,促进剥离石墨烯表面剩余含氧基团中的氢键形成。形成静电位阻效应以实现石墨烯在水中的稳定分散,可剥离出最少八层石墨烯纳米片;平均层数小于14层。0.1 wt.%(十二烷基苯磺酸钠:三聚氰胺 = 1:1)的混合体系在纯水中与石墨烯形成π-π相互作用和氢键,使石墨烯稳定分散22天不沉降。这些发现有助于在工业应用中大规模制备水性石墨烯。