凝聚
化学物理
冷凝
界面聚合
材料科学
序列(生物学)
纳米技术
自组装
相(物质)
聚合
单体
聚合物
化学
有机化学
色谱法
热力学
物理
生物化学
作者
Ye Wang,Chao Li,Lei Ma,Xiyu Wang,Kai Wang,Xinhua Lu,Yuanli Cai
出处
期刊:Macromolecules
[American Chemical Society]
日期:2021-06-08
卷期号:54 (12): 5577-5585
被引量:16
标识
DOI:10.1021/acs.macromol.1c00756
摘要
Development of spatially restricted liquid–liquid phase separation (LLPS) systems emulating biomolecular condensates is a major challenge in coacervating materials science, due to lack of approaches for spatially restricted coacervation of sequence-defined zwitterionic segments resembling intrinsically disordered proteins. Herein, we present interfacial LLPS-driven polymerization-induced electrostatic self-assembly, namely, interfacial LLPS-PIESA. The asymmetric charge sequence patterning of zwitterionic growing segments is achieved via spontaneous polymerization of ion-pair monomers within a nanoparticle core–shell interface. We show that charge sequence can profoundly affect the self-coacervation, leading to droplet dispersions, dense coacervates, and free-standing hydrogels. Moreover, the interfacial LLPS-PIESA shows a programmed hierarchical condensation self-assembly mechanism involving vesicles-to-lamellae transition, interfacial self-coacervation, lamellae-to-sheets transition, layer-by-layer sheet self-assembly, spatially restricted condensation and agglomeration, and redispersing into fibril network condensates under dynamic evolving surface charge regulation. The spatially restricted asymmetric charge sequence patterning, interfacial self-coacervation, and programmed hierarchical condensation self-assembly, all these elements can serve as the primary principles for the asymmetric charge sequence patterning design of hierarchically nanostructured condensates that emulate cellular biomolecular condensates.
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