Hu Te, Ye Huijian, Luo Zhenggang, Ma Junjie, Zhang Boyuan, Zhang Xuanhe, Song Jinwei, Wang Qingping, Xu Lixin
College of Materials Science and Engineering, Zhejiang University of Technology, Hangzhou 310014, China.
College of Materials Science and Engineering, Zhejiang University of Technology, Hangzhou 310014, China; Pinghu Institute of Advanced Materials, Zhejiang University of Technology, Pinghu 314212, China.
J Colloid Interface Sci. 2020 Jun 1;569:114-127. doi: 10.1016/j.jcis.2020.02.068. Epub 2020 Feb 17.
The use of stabilizer with designer structures can effectively promote graphite exfoliation in common solvents to render functionalized graphene desirable for their various applications. Herein, a hyperbranched polyethylene copolymer, HBPE@Py@Acryl, simultaneously bearing multiple pyrene terminal groups and pendant acryloyl moieties has been successfully synthesized from ethylene with a Pd-diimine catalyst based on unique chain walking mechanism. The unique structural design of the HBPE@Py@Acryl makes it capable of effectively promote graphite exfoliation in a series of common, low-boiling-point organic solvents, e.g. CHCl, to render stable graphene dispersions with concentrations effectively adjustable by changing feed concentrations of graphite and polymer or sonication time. Meanwhile, it can be irreversibly adsorbed on the exfoliated graphene surface based on the π-π interactions between them to concurrently render acryloyl-functionalized graphene free of structural defects, with majority (92.7%) of them having a thickness of 2-3 layers. This allows us to obtain graphene electrothermal films simply by filtration and UV irradiation, which exhibit outstanding stability in use. The action mechanism of the HBPE@Py@Acryl as stabilizer for promoting graphite exfoliation and the role of UV irradiation on improving the stability in use of resulting graphene films have been elucidated.
将稳定剂与设计结构相结合能够有效地促进石墨在常见溶剂中的剥离,从而制得适用于各种应用的功能化石墨烯。在此,基于独特的链行走机理,采用钯 - 二亚胺催化剂由乙烯成功合成了一种同时带有多个芘端基和丙烯酰基侧基的超支化聚乙烯共聚物HBPE@Py@Acryl。HBPE@Py@Acryl独特的结构设计使其能够在一系列常见的低沸点有机溶剂(如CHCl)中有效地促进石墨剥离,通过改变石墨和聚合物的进料浓度或超声处理时间可有效调节浓度,从而制得稳定的石墨烯分散体。同时,基于它们之间的π - π相互作用,它可以不可逆地吸附在剥离的石墨烯表面,同时使丙烯酰基功能化的石墨烯无结构缺陷,其中大部分(92.7%)的厚度为2 - 3层。这使我们能够通过过滤和紫外线照射简单地获得石墨烯电热膜,其在使用中表现出出色的稳定性。阐明了HBPE@Py@Acryl作为促进石墨剥离的稳定剂的作用机理以及紫外线照射对提高所得石墨烯膜使用稳定性的作用。