Spontaneous Membranization in a Silk‐Based Coacervate Protocell Model

/dk/atira/pure/core/keywords/max_planck_bristol_ Silk 600 Artificial Cells 02 engineering and technology /dk/atira/pure/core/keywords/biodesign_SRI name=Bristol BioDesign Institute 0210 nano-technology 01 natural sciences Communications name=Max Planck Bristol 620 0104 chemical sciences
DOI: 10.1002/anie.202202302 Publication Date: 2022-02-17T21:09:06Z
ABSTRACT
AbstractMolecularly crowded coacervate micro‐droplets are useful protocell constructs but the absence of a physical membrane limits their application as cytomimetic models. Auxiliary surface‐active agents have been harnessed to stabilize the coacervate droplets by irreversible shell formation but endogenous processes of reversible membranization have received minimal attention. Herein, we describe a dynamic alginate/silk coacervate‐based protocell model in which membrane‐less droplets are reversibly reconfigured and inflated into semipermeable coacervate vesicles by spontaneous self‐organization of amphiphilic silk polymers at the droplet surface under non‐neutral charge conditions in the absence of auxiliary agents. We show that membranization can be reversibly controlled endogenously by programming the pH within the protocells using an antagonistic enzyme system such that structural reconfigurations in the protocell microstructure are coupled to the trafficking of water‐soluble solutes. Our results open new perspectives in the design of hybrid protocell models with dynamical structural properties.
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