Organelle-like structural evolution of coacervate droplets induced by photopolymerization

The dynamic study of coacervates in vitro contributes our understanding of phase separation mechanisms in cells due to complex intracellular physiology. However, current researches mainly involve the use of exogenous auxiliary agents to form multi-compartmental coacervates with short-term stability. Herein, we report the endogenous self-organizing of multi-component coacervates (HA/PDDA/BSA/DMAEMA) induced by a dynamic stimulation process of protein-mediated photopolymerization. As polymerization proceeds, the cycled structural evolution and maturation from coacervate droplets into multi-compartmental coacervates, coacervate vesicles and coacervate droplets are revealed, which are driven by electrostatic interaction and osmotic pressure difference supported by dynamic and thermodynamic control. Specially, by regulating the light stimulation time, a type of multi-compartmental coacervates can be widely obtained with high structural stability over 300 days. Being a promising artificial cell model, it shows the special characteristic of compartmentalized encapsulation of substrates, efficiently improving enzymatic interfacial catalytic efficiency of organelle-like communication. Our study holds great potential for advancing the understanding of the structural evolution mechanism of membraneless organelles and provides an instructive technique for constructing multi-compartmental coacervates with long-term stability.