Peptide-Based Coacervate-Core Vesicles with Semipermeable Membranes

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

Research output: Contribution to journalArticlepeer-review

31 Scopus citations

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.

Original languageBritish English
Article number2202913
JournalAdvanced Materials
Volume34
Issue number34
DOIs
StatePublished - 25 Aug 2022

Keywords

  • coacervate-core vesicles
  • enzyme compartmentalization
  • liquid–liquid phase separation
  • membranes
  • protocells

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