Data relating to Fuel-Driven Macromolecular Coacervation in Complex Coacervate Core Micelles

In this work a chemical reaction network (CRN) is used to drive the coacervation of macromolecular species. The CRN enables transient quaternization of tertiary amine substrates, driven by the conversion of electron deficient allyl acetates and thiol or amine nucleophiles. By incorporating tertiary amine functionality into block copolymers, we demonstrate chemical triggered complex coacervate core micelle (C3M) assembly and disassembly. In contrast to most dynamic coacervate systems, this CRN operates at constant physiological pH without the need for complex biomolecules. By varying the allyl acetate fuel, deactivating nucleophile and reagent ratios, we achieved both sequential signal-induced C3M (dis)assembly, as well as transient non-equilibrium (dis)assembly.

本研究中采用化学反应网络（chemical reaction network, CRN）驱动大分子物种的凝聚过程。该CRN以缺电子乙酸烯丙酯与硫醇或胺类亲核试剂的转化为驱动力，实现叔胺底物的瞬态季铵化。将叔胺官能团引入嵌段共聚物后，我们成功实现了化学触发的复合凝聚核胶束（complex coacervate core micelle, C3M）的组装与解组装。与多数动态凝聚体系相比，本CRN可在恒定生理pH环境下运行，无需依赖复杂生物分子。通过调控乙酸烯丙酯燃料、失活亲核试剂与反应物的配比，我们可同时实现顺序信号诱导的C3M（去）组装与瞬态非平衡（去）组装过程。