Interfacial Liquid-Liquid Phase Separation-Driven Polymerization-Induced Electrostatic Self-Assembly

被引:27
|
作者
Wang, Ye [1 ]
Li, Chao [1 ]
Ma, Lei [1 ]
Wang, Xiyu [1 ]
Wang, Kai [1 ]
Lu, Xinhua [1 ]
Cai, Yuanli [1 ]
机构
[1] Soochow Univ, Coll Chem Chem Engn & Mat Sci, State Local Joint Engn Lab Novel Funct Polymer Ma, Suzhou 215123, Peoples R China
基金
中国国家自然科学基金;
关键词
VISIBLE-LIGHT; COMPLEX COACERVATION; RAFT POLYMERIZATION; COPOLYMER VESICLES; NANOPARTICLES; MONOMERS; WATER;
D O I
10.1021/acs.macromol.1c00756
中图分类号
O63 [高分子化学(高聚物)];
学科分类号
070305 ; 080501 ; 081704 ;
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 nanopartide 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.
引用
收藏
页码:5577 / 5585
页数:9
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