巨型表面活性剂的本体自组装研究和分子拓扑结构效应

唐雯; 岳衎; 程正迪

doi:10.11777/j.issn1000-3304.2018.18102

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巨型表面活性剂的本体自组装研究和分子拓扑结构效应

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- 巨型表面活性剂的本体自组装研究和分子拓扑结构效应
- Molecular Topology Effects in Self-assembly of Giant Surfactants
- 高分子学报 2018年0卷第8期页码：959-972
- 作者机构：
  
  华南理工大学华南软物质科学与技术高等研究院发光材料与器件国家重点实验室　广州 510640
- 作者简介：
  
  [ "岳衎，男，1986年出生. 2008年于北京大学获学士学位，2013年于美国阿克伦大学获博士学位，随后先后在美国阿克伦大学和美国哈佛大学医学院布莱根妇女医院从事博士后研究. 2017年任华南理工大学华南软物质科学与技术高等研究院研究员，博士生导师. 2017年获得中组部千人计划青年项目(第十三批)资助. 主要研究方向包括两亲性大分子自组装和新型水凝胶生物材料等" ]
  [ "程正迪，男，1949年出生. 1977年于华东师范大学获学士学位，1981年于东华大学获硕士学位，1985年于美国伦斯勒理工学院获博士学位. 1985 ~ 1987年于美国伦斯勒理工学院从事博士后研究，1987年加入美国阿克伦大学高分子科学系，历任助理教授、副教授、教授、讲席教授和杰出科研教授. 2016年起任华南理工大学华南软物质科学与技术高等研究院教授，博士生导师和院长. 2008年当选美国工程院院士，2015年获得中组部千人计划顶尖人才与创新团队项目资助，主要学术荣誉包括2013年美国物理学会高分子物理奖、2017年日本高分子学会国际奖等. 主要研究方向为软物质中的凝聚态物理问题，广泛涉及高分子、液晶分子、表面活性剂分子等体系" ]
- 基金信息：
  
  国家自然科学基金(基金号 21774038)、广东省珠江人才创新创业团队引进项目(项目号 2016ZT06C322)、科技部重点研发项目(项目号 2017YFC11050003)、中央高校基本科研业务费(基金号 2017JQ001)和第十三批国家千人计划青年项目资助()
- DOI：10.11777/j.issn1000-3304.2018.18102
  中图分类号：
- 纸质出版日期：2018-8，
  
  收稿日期：2018-4-9，
  
  修回日期：2018-5-22，
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唐雯, 岳衎, 程正迪. 巨型表面活性剂的本体自组装研究和分子拓扑结构效应[J]. 高分子学报, 2018,0(8):959-972.

Wen Tang, Kan Yue, Stephen Z. D. Cheng. Molecular Topology Effects in Self-assembly of Giant Surfactants[J]. Acta Polymerica Sinica, 2018,0(8):959-972.
唐雯, 岳衎, 程正迪. 巨型表面活性剂的本体自组装研究和分子拓扑结构效应[J]. 高分子学报, 2018,0(8):959-972. DOI： 10.11777/j.issn1000-3304.2018.18102.

Wen Tang, Kan Yue, Stephen Z. D. Cheng. Molecular Topology Effects in Self-assembly of Giant Surfactants[J]. Acta Polymerica Sinica, 2018,0(8):959-972. DOI： 10.11777/j.issn1000-3304.2018.18102.

摘要

嵌段共聚物通过本体自组装可在纳米尺度上形成多样化的有序结构，并有望为下一代微纳加工技术的发展提供平台. 近十年来，以具有三维刚性结构的笼簇状分子作为结构基元，研究者们发展了一类独特的两亲性巨型表面活性剂体系. 本文系统总结了近年来巨型表面活性剂本体自组装方向的研究进展，并特别强调了其中广泛存在的分子拓扑结构效应. 实验结果表明，巨型表面活性剂可在10 nm乃至5 nm以下的特征尺寸上形成高度有序的自组装结构. 更加重要的是，通过精心设计的分子拓扑结构的变化，逐步揭示了若干种由分子拓扑结构主导的非常规自组装结构的形成机理，包括多尾链巨型表面活性剂中的非常规球状相以及多头基巨型表面活性剂中的高度不对称的层状相等. 这些结果推进了对两亲性大分子本体自组装中的分子拓扑结构效应的理解，并为开发基于嵌段聚合物微纳加工技术提供了重要的实验基础.

Abstract

Self-assembly of block copolymers

which are composed of covalently connected incompatible polymer chains

can result in various ordered structures at the nanometer scale. This phenomenon

widely known as the microphase separation of block copolymers

may provide a technological platform for the development of next-generation nanopatterning techniques based on the " top-down” strategy. During the past decade

a unique class of novel amphiphilic macromolecules termed as giant surfactants have been reported

which are constructed from selected building blocks of cluster-like molecules having three-dimensional rigid conformations and nanometer sizes. By combining different " click-type” reactions

a highly efficient and modular synthetic method has been developed to prepare covalent conjugates of these molecular clusters and polymer chains. The resulting giant surfactants can be viewed as structural analogues of common block copolymers

and similarly

they also display interesting self-assembly behaviors both in solutions and in bulk. Herein

recent advances on the study of self-assembly of giant surfactants are summarized

with a particular emphasis on the molecular topology effects that can significantly change their self-assembly behaviors. As revealed by small angle X-ray scattering and transmission electron microscopy techniques

giant surfactants were able to self-assemble in bulk to form a series of highly ordered nanostructures with feature sizes below 10 nm or even 5 nm

with clearly shifted phase boundaries. More importantly

through rational molecular design to tune the molecular topology of giant surfactants

formation of some unusual nanostructures driven by molecular topological variations was achieved. Typical examples include several unconventional spherical phases

such as the Frank-Kasper A15 phase

the Frank-Kasper

phase

and a quasicrystalline spherical phase

which were observed in multitailed giant surfactants

and a highly asymmetric lamellar phase formed by self-assembly of multiheaded giant surfactants. It is believed that these studies provide not only insights towards understanding the molecular topological effects in macromolecular self-assembly

but also experimental foundation for the development of block copolymer lithography that can afford nanostructures with sub-10-nm feature sizes.

关键词

微相分离巨型表面活性剂分子嵌段共聚物分子拓扑结构自组装

Keywords

Microphase separationGiant surfactantsBlock copolymersMolecular topologySelf-assembly

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