荷兰埃因霍温理工大学Meijer, E. W.团队报道了超分子聚合物通过液-液相分离形成水性液滴。相关研究成果发表在2024年2月28日出版的国际学术期刊《自然》。

生物聚合物的液-液相分离（LLPS）最近被证明，在具有多种生物功能的无膜细胞器的形成中起着核心作用。LLPS和大分子缩合之间的相互作用是持续研究的一部分。合成超分子聚合物是大分子的非共价等价物，但尚未报道其发生LLPS。

该文中，研究表明，通过合成组分的超分子聚合获得的连续生长的原纤维，负责通过熵驱动途径将相分离为高度各向异性的水性液滴（tactoid）。由右旋糖酐浓度调节的拥挤环境不仅影响超分子聚合的动力学，还影响LLPS的性质，包括相分离动力学、形态、内部有序性、流动性和最终水性液滴的机械性能。

此外，基底-液体和液体-液体界面被证明能够加速超分子聚合物的LLPS，能够产生无数的三维有序结构，包括表面微米长的三角体的高度有序阵列。几种超分子聚合物证明了超分子聚合控制新兴形态的普遍性和许多可能性，开辟了一个从通过稳定LLPS的高度结构化水溶液到纳米级软物质的新物质领域。

附：英文原文

Title: Supramolecular polymers form tactoids through liquid–liquid phase separation

Author: Fu, Hailin, Huang, Jingyi, van der Tol, Joost J. B., Su, Lu, Wang, Yuyang, Dey, Swayandipta, Zijlstra, Peter, Fytas, George, Vantomme, Ghislaine, Dankers, Patricia Y. W., Meijer, E. W.

Issue&Volume: 2024-02-28

Abstract: Liquid–liquid phase separation (LLPS) of biopolymers has recently been shown to play a central role in the formation of membraneless organelles with a multitude of biological functions1,2,3. The interplay between LLPS and macromolecular condensation is part of continuing studies4,5. Synthetic supramolecular polymers are the non-covalent equivalent of macromolecules but they are not reported to undergo LLPS yet. Here we show that continuously growing fibrils, obtained from supramolecular polymerizations of synthetic components, are responsible for phase separation into highly anisotropic aqueous liquid droplets (tactoids) by means of an entropy-driven pathway. The crowding environment, regulated by dextran concentration, affects not only the kinetics of supramolecular polymerizations but also the properties of LLPS, including phase-separation kinetics, morphology, internal order, fluidity and mechanical properties of the final tactoids. In addition, substrate–liquid and liquid–liquid interfaces proved capable of accelerating LLPS of supramolecular polymers, allowing the generation of a myriad of three-dimensional-ordered structures, including highly ordered arrays of micrometre-long tactoids at surfaces. The generality and many possibilities of supramolecular polymerizations to control emerging morphologies are demonstrated with several supramolecular polymers, opening up a new field of matter ranging from highly structured aqueous solutions by means of stabilized LLPS to nanoscopic soft matter.

DOI: 10.1038/s41586-024-07034-7

Source: https://www.nature.com/articles/s41586-024-07034-7