Sequence-Regulated Supracolloidal Copolymers via Copolymerization-Like Coassembly of Binary Mixtures of Patchy Nanoparticles
Sequence-Regulated Supracolloidal Copolymers via Copolymerization-Like Coassembly of Binary Mixtures of Patchy Nanoparticles
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通过片状纳米颗粒二元混合物的类共聚共组装实现序列调节的超胶体共聚物
DOI：
10.1021/acsnano.8b08431
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发表时间：
2019
期刊：
影响因子：
17.1
通讯作者：
Xiaohui Tian
中科院分区：
文献类型：
--
作者：
Xiaodong Ma;Mengxin Gu;Liangshun Zhang;Jiaping Lin;Xiaohui Tian
分子系统的合成共聚物启发了通过非等距纳米粒子的共组装来创建一维共聚物样超结构。与共价和分子共聚物相比，类共聚物超结构的形成机理以及决定其长度和排列的纳米粒子序列的因素仍然知之甚少。在这里，我们提出了一个联合的理论-计算框架来探讨片状纳米颗粒二元混合物的共组装机理和动力学。通过粗粒分子动力学模拟表明，片状纳米粒子的共组装与分子阶梯生长共聚的许多方面非常相似，并且片状纳米粒子在共聚物样超结构中的顺序可以通过相对活性、片状纳米粒子的初始成分以及共组装策略进行精细调节。建立了一个定量的类共聚模型来解释片状纳米粒子的共聚动力学和排列的纳米粒子的序列分布，所有这些都受较低层建筑单元的精心设计所支配。理论和模拟相结合的研究为片状纳米粒子二元混合物的共聚反应动力学和序列预测提供了机理上的见解，为合理设计具有不同序列和功能的共聚物类超结构铺平了道路。
Synthetic copolymers of molecular systems serve as an inspiration for creation of one-dimensional copolymer-like superstructures via coassembly of anisometric nanoparticles. In contrast to the covalent and molecular copolymers, the details of formation mechanisms of copolymer-like superstructures, as well as the factors determining their length and the sequences of arranged nanoparticles, are still poorly understood. Herein, we propose a joint theoretical–computational framework to probe into the coassembly mechanism and kinetics of binary mixtures of patchy nanoparticles. By applying the coarse-grained molecular dynamics simulations, it is demonstrated that the coassembly of patchy nanoparticles markedly resembles many aspects of molecular step-growth copolymerization, and the sequences of nanoparticles inside the copolymer-like superstructures can be finely regulated by the relative activity and the initial ingredient of patchy nanoparticles as well as the coassembly strategy. A quantitatively copolymerization-like model is developed to account for the coassembly kinetics of patchy nanoparticles and the sequence distribution of arranged nanoparticles, all governed by the elaborate design of lower-level building units. The jointly theoretical and simulated studies offer mechanistic insights into the copolymerization-like kinetics and the sequence prediction for the coassembly of binary mixtures of patchy nanoparticles, paving the way toward the rational design of copolymer-like superstructures with various sequences and functionalities.