Peptide‐Based Coacervate‐Core Vesicles with Semipermeable Membranes

Abbas, Manzar; Law, Jack O.; Grellscheid, Sushma N.; Huck, Wilhelm T.S.; Spruijt, Evan

Abstract

Coacervates droplets have long been considered as potential protocells to mimic living cells. However, these droplets lack a membrane and are prone to coalescence, limiting their ability to survive, interact, and organize into higher-order assemblies. This work shows that tyrosine-rich peptide conjugates can undergo liquid–liquid phase separation in a well-defined pH window and transform into stable membrane-enclosed protocells by enzymatic oxidation and cross-linking at the liquid–liquid interface. The oxidation of the tyrosine-rich peptides into dityrosine creates a semipermeable, flexible membrane around the coacervates with tunable thickness, which displays strong intrinsic fluorescence, and stabilizes the coacervate protocells against coalescence. The membranes have an effective molecular weight cut-off of 2.5 kDa, as determined from the partitioning of small dyes and labeled peptides, RNA, and polymers into the membrane-enclosed coacervate protocells. Flicker spectroscopy reveals a membrane bending rigidity of only 0.1kBT, which is substantially lower than phospholipid bilayers despite a larger membrane thickness. Finally, it is shown that enzymes can be stably encapsulated inside the protocells and be supplied with substrates from outside, which opens the way for these membrane-bound compartments to be used as molecularly crowded artificial cells capable of communication or as a vehicle for drug delivery.

Citation

Abbas, M., Law, J. O., Grellscheid, S. N., Huck, W. T., & Spruijt, E. (2022). Peptide‐Based Coacervate‐Core Vesicles with Semipermeable Membranes. Advanced Materials, 34(34), Article 2202913. https://doi.org/10.1002/adma.202202913

• Journal Article Type: Article
• Acceptance Date: Jul 7, 2022
• Online Publication Date: Jul 22, 2022
• Publication Date: Aug 25, 2022
• Deposit Date: Aug 17, 2022
• Publicly Available Date: Mar 14, 2023
• Journal: Advanced Materials
• Print ISSN: 0935-9648
• Electronic ISSN: 1521-4095
• Publisher: Wiley
• Peer Reviewed: Peer Reviewed
• Volume: 34
• Issue: 34
• Article Number: 2202913
• DOI: https://doi.org/10.1002/adma.202202913
• Public URL: https://durham-repository.worktribe.com/output/1194297