Enzymatically reconfigurable liquid crystalline coacervate microdroplets as protocell models

Reconfigurable cell-sized compartments can act as artificial cellular models that dynamically respond to environmental stimuli, mimicking the adaptive behaviors of living cells. In this study, we present enzymatically active liquid crystalline (LC) coacervate microdroplets as a protocell model, which undergoes differentiation into helicoidal vesicles and eventually membranous protocells containing artificial organelles. The LC protocell microdroplets are developed through electrostatic complexation between a negatively charged polysaccharide and a cationic surfactant. We identify the amylase-mediated hydrolysis of polysaccharide as the molecular mechanism that is accounted for two-step structural changes of protocells, in which electrostatic complexation plays a crucial role. Notably, by integrating affinitive biomolecules into the LC microdroplets, we demonstrate the reconfiguration of protocells into yolk-shell coacervate vesicles that support biochemical reactions. Our findings illustrate the potential to build protocell models to mimic the differentiation behaviors of cellular materials and shed light to the understanding of the structural reconfiguration of protocells.