Abstract

Cell membranes exhibit elaborate lipidic patterning to carry out a myriad of functions such as signaling and trafficking. Domain formation in giant unilamellar vesicles (GUVs) is thus of interest for understanding fundamental biological processes and to provide new prospects for biocompatible soft materials. Lipid rearrangements in lipidic GUVs and lipid/polymer GUVs are extensively studied whereas polymer/polymer hybrid GUVs remain evasive. Here, the focus is on the thermodynamically driven phase separation of amphiphilic polymers in GUVs. It is demonstrated that polymer phase separation is entropically dictated by hydrophobic block incompatibilities and that films topology can help to determine the outcome of polymeric phase separation in GUVs. Lastly, Janus-GUVs are obtained and GUVs exhibit a single large domain by using a compatibilizing hydrophobic block copolymer.

Highlights

  • Cell membranes exhibit elaborate lipidic patterning to carry out a myriad of functions such as signaling and trafficking

  • It is demonstrated that polymer phase sepachemical and geometrical incompatibility ration is entropically dictated by hydrophobic block incompatibilities and that between lipids and polymers.[2b]. If the films topology can help to determine the outcome of polymeric phase separation in giant unilamellar vesicles (GUVs)

  • We showed that PB-b-PEEP behave differently to the traditionally used polymeric amphiphiles because they are entropically favored to form GUVs in aqueous media to lipids

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Summary

Polymer Synthesis and Unipolymeric GUVs

We recently developed a novel block copolymer, polybutadieneblock-poly(ethylene ethyl phosphate) (PB-b-PEEP), which hydrophilic block PEEP resembles natural phospholipids.[14]. This mild technique helps to minimize phase separation artefacts caused by the method of self-assembly rather than pure physicochemical immiscibility Other techniques such as electroformation, gel-assisted hydration and double emulsion might force the mixing of the polymers as it has been shown for hybrid liposomes.[21] We modified our original procedure by letting the film hydrate overnight rather than 1 h in order to maximize the number of vesicles, to diminish artefacts and variability caused by short hydration times and to observe the GUVs in their thermodynamic state.

Binary Polymer Mixture in GUVs
Polymer Film Topology
Ternary Polymer Mixed GUVs
Conclusion
Experimental Section
Conflict of Interest
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