文献类型：期刊文献

中文题名：双亲性DNA嵌段共聚物胶束构建超结构的模拟研究

英文题名：Computational Investigation on the Superstructures of Micelles from Amphiphilic DNA Block Copolymers

作者：李小霞[1];谷梦鑫[1];张良顺[1];林嘉平[1]

机构：[1]华东理工大学,上海市先进聚合物材料重点实验室,材料科学与工程学院,上海200237

年份：2020

卷号：51

期号：11

起止页码：1257

中文期刊名：高分子学报

外文期刊名：Acta Polymerica Sinica

收录：CSTPCD;;Scopus;WOS:【SCI-EXPANDED(收录号:WOS:000580620000008)】；北大核心:【北大核心2017】；CSCD:【CSCD2019_2020】；

基金：国家自然科学基金(基金号21574040,21873029,51833003)资助项目.

语种：中文

中文关键词：DNA;超结构;嵌段共聚物;粗粒化模型

外文关键词：DNA;Superstructures;Block copolymers;Coarse-grained model

摘要：构建了双亲性DNA嵌段共聚物的粗粒化模型,采用布朗动力学模拟方法,开展了DNA嵌段共聚物多层次自组装行为的研究.模拟结果表明,DNA嵌段共聚物首先自组装形成纳米尺度胶束,随后在DNA嵌段杂化的引导下共聚物胶束相互连接形成多种超结构,如网络状、支化状、星型和线型拓扑等.DNA嵌段序列、化学计量比和温度等因素可以显著地改变超结构的拓扑特征.模拟结果与已有实验发现一致.模拟结果预测,胶束共组装超结构与胶束配位数和DNA嵌段杂化率等微观量紧密相关.
Amphiphilic DNA block copolymers,which are composed of DNA and polymeric blocks linked by covalent bonds,are regared as novel building units for creating hierarchically self-assembled superstructures at the mesoscales.However,insufficient understanding of the formation mechanisms and the regulation rules of selfassembled superstructures seriously impedes their potential utility in the field of nanomedicines.In this work,we build a coarse-grained model for amphiphilic block copolymers consisting of DNA blocks in selective solution,and propose a stepwise self-assembly strategy of DNA block copolymers on the basis of Brownian dynamics simulations.It is computationally demonstrated that the amphiphilic DNA block copolymers self-assemble into spherical micelles due to the solvophobic effect of polymeric blocks in the first-step of coarse-grained simulations.Driven by the hybridization of complementary DNA blocks,the binary mixtures of nano-sized micelles in the second-step of simulations are programmed to co-assemble into a series of hierarchical superstructures such as network-like,branched-like,star-like and linear topologies.The DNA-programmed superstructures of micelles can be regulated by finely tuning the sequence of DNA blocks,the stoichiometric ratio of binary mixtures of micelles and the reduced temperature of simulation system.The simulation results turn out to be in agreement with the available experimental findings.Furthermore,it is corroborated that the DNA-programmed superstructures of micelles have a close connection with the coordination number of micelles and the hybridization fraction of DNA blocks at the microscopic level.