Gel phase formation in dilute triblock copolyelectrolyte complexes

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

doi:10.1038/ncomms14131

Title: Gel phase formation in dilute triblock copolyelectrolyte complexes

Journal Article · 22 February 2017 · Nature Communications

DOI: https://doi.org/10.1038/ncomms14131 · OSTI ID:1345009

Srivastava, Samanvaya ^[1]; Andreev, Marat ^[2]; Levi, Adam E. ^[2]; Goldfeld, David J. ^[2]; Mao, Jun ^[1]; Heller, William T. ^[3]; Prabhu, Vivek M. ^[4]; de Pablo, Juan J. ^[1]; Tirrell, Matthew V. ^[1]

The Univ. of Chicago, Chicago, IL (United States); Argonne National Lab. (ANL), Lemont, IL (United States)
The Univ. of Chicago, Chicago, IL (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
National Institute of Standards and Technology, Gaithersburg, MD (United States)

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. Finally, 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.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1345009

Alternate ID(s):: OSTI ID: 1345421; OSTI ID: 1421606

Journal Information:: Nature Communications, Journal Name: Nature Communications Vol. 8; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Mapping the phase behavior of coacervate-driven self-assembly in diblock copolyelectrolytes Ong, Gary M. C.; Sing, Charles E. Soft Matter, Vol. 15, Issue 25 https://doi.org/10.1039/c9sm00741e	journal	January 2019
Topologically frustrated dynamics of crowded charged macromolecules in charged hydrogels Jia, Di; Muthukumar, Murugappan Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-04661-3	journal	June 2018
Sequence and entropy-based control of complex coacervates Chang, Li-Wei; Lytle, Tyler K.; Radhakrishna, Mithun Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/s41467-017-01249-1	journal	November 2017
Micro- to macro-phase separation transition in sequence-defined coacervates Sing, Charles E. The Journal of Chemical Physics, Vol. 152, Issue 2 https://doi.org/10.1063/1.5140756	journal	January 2020

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Title: Gel phase formation in dilute triblock copolyelectrolyte complexes

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