Ma Lei, Xiong Weixing, Yu Kaiwen, Wang Xiyu, Cao Ying, Lu Xinhua, Cai Yuanli
State-Local Joint Engineering Laboratory for Novel Functional Polymer Materials, College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou 215123, China.
ACS Macro Lett. 2021 Nov 16;10(11):1410-1415. doi: 10.1021/acsmacrolett.1c00557. Epub 2021 Oct 21.
Macromolecular crowding plays a key role in liquid-phase condensation of proteins and membraneless organelles yet is largely unexplored for artificial liquid materials. Herein, we present a strategy for direct access to multiphase liquid condensates with individual charged/neutral subdomains, by introducing macromolecular crowding to our previous protocol of liquid-liquid phase-separation-driven polymerization-induced electrostatic self-assembly (LLPS-PIESA). We show that reversible addition fragmentation chain transfer (RAFT) aqueous dispersion photo-copolymerization of a charged monomer with a specific neutral monomer, in the presence of a polar macrochain transfer agent (CTA) and an oppositely charged polyion, can induce self-sorting and macromolecular crowding. LLPS-PIESA proceeds via liquid-phase condensation of as-assembled nascent clusters up to biologically important nanostructured multiphase condensates with individual charged/neutral subdomains.
大分子拥挤效应在蛋白质和无膜细胞器的液相凝聚过程中起着关键作用，但在人工液体材料方面却 largely unexplored。在此，我们提出了一种策略，通过在我们之前的液-液相分离驱动的聚合诱导静电自组装（LLPS-PIESA）方案中引入大分子拥挤效应，直接获得具有单个带电/中性子域的多相液体凝聚物。我们表明，在极性大分子链转移剂（CTA）和带相反电荷的聚离子存在下，带电单体与特定中性单体的可逆加成-断裂链转移（RAFT）水分散体光共聚合可以诱导自分类和大分子拥挤效应。LLPS-PIESA通过组装的新生簇的液相凝聚进行，直至形成具有单个带电/中性子域的具有生物学重要性的纳米结构多相凝聚物。
