基于非共价镊合作用的线形超分子聚合物

杨支帅; 田玉奎; 李子健; 敖雷; 高宗春; 汪峰

doi:10.11777/j.issn1000-3304.2017.16251

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基于非共价镊合作用的线形超分子聚合物

研究论文 | 更新时间：2021-03-12

- 基于非共价镊合作用的线形超分子聚合物
- Construction of Linear Supramolecular Polymers on the Basis of Non-covalent Molecular Tweezer/Guest Recognition
- 高分子学报 2017年第1期页码：121-128
- 作者机构：
  
  中国科学技术大学高分子科学与工程系合肥 230026
- 作者简介：
  
  E-mail: drfwang@ustc.edu.cn Feng Wang, E-mail:drfwang@ustc.edu.cn
- 基金信息：
  
  国家自然科学基金资助项目(基金号21274139)
- DOI：10.11777/j.issn1000-3304.2017.16251
  中图分类号：
- 纸质出版日期：2017-1，
  
  收稿日期：2016-8-9，
  
  修回日期：2016-9-26，
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杨支帅, 田玉奎, 李子健, 敖雷, 高宗春, 汪峰. 基于非共价镊合作用的线形超分子聚合物[J]. 高分子学报, 2017,(1):121-128.

Yang Zhi-shuai, Tian Yu-kui, Li Zi-jian, Ao Lei, Gao Zong-chun, Wang Feng. Construction of Linear Supramolecular Polymers on the Basis of Non-covalent Molecular Tweezer/Guest Recognition[J]. Acta Polymerica Sinica, 2017,(1):121-128.
杨支帅, 田玉奎, 李子健, 敖雷, 高宗春, 汪峰. 基于非共价镊合作用的线形超分子聚合物[J]. 高分子学报, 2017,(1):121-128. DOI： 10.11777/j.issn1000-3304.2017.16251.

Yang Zhi-shuai, Tian Yu-kui, Li Zi-jian, Ao Lei, Gao Zong-chun, Wang Feng. Construction of Linear Supramolecular Polymers on the Basis of Non-covalent Molecular Tweezer/Guest Recognition[J]. Acta Polymerica Sinica, 2017,(1):121-128. DOI： 10.11777/j.issn1000-3304.2017.16251.

摘要

基于“镊合导向自组装”策略构筑超分子聚合物，可实现电子给受体基元在组装体层次的精确排列，设计并制备了基于三联吡啶铂（Ⅱ）炔分子镊子主体的AA型单体分子，以及基于芘客体的BB型单体分子.通过在芘客体上引入酰胺基元，在非共价镊合过程中可产生分子间NH-N氢键作用.通过氢键和供受体相互作用力的高效协同，显著提高了非共价镊合体系的结合强度，其结合常数可达到（3.58±0.01）×10

（mol/L）

-1

，相比于未取代芘客体，其结合强度呈现出2个数量级的显著提高.在此基础之上，对AA、BB型单体分子的超分子聚合行为展开了深入的研究.结合实验及理论计算，证实在高浓度状态下，两单体分子通过自组装可获得具有高分子量特征的线形超分子聚合物.同时，考察了超分子聚合物的动态可逆性，通过温度的改变及链终止剂的加入，可实现超分子聚合物的可逆自/解组装过程.

Abstract

Supramolecular polymers represent a novel class of macromolecules

in which self-assembly serves as a powerful tool and holds the monomeric units together

via

reversible non-covalent bonds. The ideal non-covalent recognition units should concomitantly fulfill high complexation directionality

strong binding affinity and stimuli-sensitive responsiveness. To meet the requirements

hydrogen bond

metal-ligand and macrocyclic host-guest interactions have been widely served as the non-covalent driving forces for controlled supramolecular polymerization processes. The expansion of novel driving forces and the corresponding recognition motifs are of paramount importance for the current supramolecular polymers researches. In this regard

integration of donor and acceptor chromophores in a mixed supramolecular polymeric array is intriguing

since it is an efficient way to construct nano-sized optoelectronic devices. However

due to the non-specific and non-directional properties of electron donor-acceptor interactions

a variety of erratic stacking modes (such as phase segregation

random or alternating mixing) could potentially exist in the resulting supramolecular polymeric assemblies. Hence

the precise organization of multi-component

-aromatic systems is highly desirable. Our research group has recently developed a "tweezering directed self-assembly" strategy for the construction of well-ordered supramolecular donor-acceptor polymers. As a research extension

herein a novel alkynylplatinum (Ⅱ) terpyridine molecular tweezer/pyrene recognition motif is investigated

which features with intermolecular NH-N hydrogen bond between the amide unit on the guest and the pyridine moiety on the molecular tweezer. Ascribing to the elaborate combination of donor-acceptor and hydrogen-bonding interactions

it demonstrates rather strong binding affinity (

=3.58×10

(mol/L)

-1

). Moreover

by modulating the intermolecular NH-N hydrogen bonds involved in the system

its binding affinity exhibits significantly large variations towards external stimuli. Such non-covalent recognition motifs are further employed as the connecting units for the fabrication of high-molecular-weight supramolecular polymers. Moreover

the resulting polymeric assemblies exhibit interesting dynamic temperature-responsive behaviors

which are promising for the development of adaptive

-functional materials.

关键词

超分子聚合物分子识别供受体相互作用力自组装环境响应性

Keywords

Supramolecular polymersMolecular recognitionDonor-acceptor interactionsSelf-assemblyStimuli-responsiveness

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