Gel phase formation in dilute triblock copolyelectrolyte complexes

Samanvaya Srivastava, Marat Andreev, Adam E. Levi, David J. Goldfeld, Jun Mao, William T. Heller, Vivek M. Prabhu, Juan J. De Pablo, Matthew V. Tirrell

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96 Scopus citations

Abstract

Assembly of oppositely charged triblock copolyelectrolytes into phase-separated gels at low polymer concentrations (<1% by mass) has been observed in scattering experiments and molecular dynamics simulations. Here we show that in contrast to uncharged, amphiphilic block copolymers that form discrete micelles at low concentrations and enter a phase of strongly interacting micelles in a gradual manner with increasing concentration, the formation of a dilute phase of individual micelles is prevented in polyelectrolyte complexation-driven assembly of triblock copolyelectrolytes. Gel phases form and phase separate almost instantaneously on solvation of the copolymers. Furthermore, molecular models of self-assembly demonstrate the presence of oligo-chain aggregates in early stages of copolyelectrolyte assembly, at experimentally unobservable polymer concentrations. Our discoveries contribute to the fundamental understanding of the structure and pathways of complexation-driven assemblies, and raise intriguing prospects for gel formation at extraordinarily low concentrations, with applications in tissue engineering, agriculture, water purification and theranostics.

Original languageEnglish (US)
Article number14131
JournalNature communications
Volume8
DOIs
StatePublished - Feb 23 2017
Externally publishedYes

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© 2017 The Author(s).

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