Fuel-driven macromolecular coacervation in complex coacervate core micelles

Journal Article (2022)
Author(s)

R.W. Lewis (TU Delft - ChemE/Advanced Soft Matter)

B. Klemm (TU Delft - ChemE/Advanced Soft Matter)

M. Macchione (TU Delft - ChemE/Advanced Soft Matter)

R Eelkema (TU Delft - ChemE/Advanced Soft Matter)

Research Group
ChemE/Advanced Soft Matter
Copyright
© 2022 R.W. Lewis, B. Klemm, M. Macchione, R. Eelkema
DOI related publication
https://doi.org/10.1039/d2sc00805j
More Info
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Publication Year
2022
Language
English
Copyright
© 2022 R.W. Lewis, B. Klemm, M. Macchione, R. Eelkema
Research Group
ChemE/Advanced Soft Matter
Issue number
16
Volume number
13
Pages (from-to)
4533-4544
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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.