文献类型：期刊文献

中文题名：DNA非均匀功能化纳米粒子的可编程自组装行为

英文题名：Programmable Self-Assembly of Non-Uniformly DNA-Functionalized Nanoparticles

作者：谷梦鑫[1];张良顺[1];林嘉平[1]

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

年份：2020

卷号：33

期号：3

起止页码：269

中文期刊名：功能高分子学报

外文期刊名：Journal of Functional Polymers

收录：CSTPCD;;北大核心:【北大核心2017】；CSCD:【CSCD_E2019_2020】；

基金：国家自然科学基金(21574040)。

语种：中文

中文关键词：分子动力学模拟;粗粒化模型;DNA可编程自组装;纳米粒子

外文关键词：molecular dynamics simulation;coarse-grained model;DNA-programmable self-assembly;nanoparticles

摘要：DNA非均匀功能化纳米粒子作为一种可编程原子等价物,在多层次自组装结构领域具有重要的应用前景。构建了DNA非均匀功能化纳米粒子的粗粒化模型,并利用分子动力学模拟其自组装过程。通过计算机模拟发现,互补DNA序列间发生杂化反应,纳米粒子形成三维网络状和支化超结构;通过构建纳米粒子自组装结构的几何模型,能够正确预测纳米粒子之间的相对位置及其分布;通过调节互补的DNA功能化纳米粒子的化学计量比,显著地改变了自组装超结构和动力学行为。
DNA-functionalized nanoparticles,regarded as the programmable atom equivalent,enable the realization of hierarchically self-assembled superstructures.The self-assembled superstructures possessing unique mechanic,optical and electronic properties have prospective applications in the field of energy conservation,catalysis and medical diagnostics.With the development of nanotechnology,non-uniformly DNA-functionalized nanoparticles with DNA strands regioselectively distributed on the surfaces have been successfully synthesized.Recently,by utilizing the non-uniformly DNA-functionalized nanoparticles,researchers have created nanoparticle superstructures with complex architecture in the lab,such as discrete planet-satellite nanostructures,one-dimensional nanoparticle chains,and even three-dimensional networks.However,the mechanism and design rules of self-assembly of non-uniformly DNA-functionalized nanoparticles remain to be explored.Herein,the coarse-grained model of non-uniformly DNA-functionalized nanoparticles is constructed,and molecular dynamics is utilized to simulate the self-assembly process of DNA-programmable nanoparticles.It is demonstrated that the nonuniformly DNA-functionalized nanoparticles self-assemble into branched or even network-like superstructures through the hybridization of complementary DNA strands.The geometrical model of self-assembled superstructures is proposed to predict the relative position and distribution of nanoparticles inside the superstructures.Sparked by the molecular polymerization,we further explored the effect of stoichiometric ratio on the self-assembly of nanoparticles.The stoichiometric ratio of nanoparticles has remarkable effects on both the architecture of superstructures and the kinetics of DNA-programmable selfassembly of nanoparticles.As the stoichiometric ratio increased from 1.0 to 5.7,the self-assembled superstructures switch from the spanning networks to discrete branched clusters.