Issue 16, 2022

Fuel-driven macromolecular coacervation in complex coacervate core micelles

Abstract

Fuel-driven macromolecular coacervation is an entry into the transient formation of highly charged, responsive material phases. In this work, we used a chemical reaction network (CRN) to drive the coacervation of macromolecular species readily produced using radical polymerisation methods. The CRN enables transient quaternization of tertiary amine substrates, driven by the conversion of electron deficient allyl acetates and thiol or amine nucleophiles. By incorporating tertiary amine functionality into block copolymers, we demonstrate chemical triggered complex coacervate core micelle (C3M) assembly and disassembly. In contrast to most dynamic coacervate systems, this CRN operates at constant physiological pH without the need for complex biomolecules. By varying the allyl acetate fuel, deactivating nucleophile and reagent ratios, we achieved both sequential signal-induced C3M (dis)assembly, as well as transient non-equilibrium (dis)assembly. We expect that timed and signal-responsive control over coacervate phase formation at physiological pH will find application in nucleic acid delivery, nano reactors and protocell research.

Graphical abstract: Fuel-driven macromolecular coacervation in complex coacervate core micelles

Supplementary files

Article information

Article type
Edge Article
Submitted
08 Feb 2022
Accepted
30 Mar 2022
First published
31 Mar 2022
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY license

Chem. Sci., 2022,13, 4533-4544

Fuel-driven macromolecular coacervation in complex coacervate core micelles

R. W. Lewis, B. Klemm, M. Macchione and R. Eelkema, Chem. Sci., 2022, 13, 4533 DOI: 10.1039/D2SC00805J

This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. You can use material from this article in other publications without requesting further permissions from the RSC, provided that the correct acknowledgement is given.

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