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Issue 6, 2015
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Phase behavior of electrostatically complexed polyelectrolyte gels using an embedded fluctuation model

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Abstract

Nanostructured, responsive hydrogels formed due to electrostatic interactions have promise for applications such as drug delivery and tissue mimics. These physically cross-linked hydrogels are composed of an aqueous solution of oppositely charged triblocks with charged end-blocks and neutral, hydrophilic mid-blocks. Due to their electrostatic interactions, the end-blocks microphase separate and form physical cross-links that are bridged by the mid-blocks. The structure of this system was determined using a new, efficient embedded fluctuation (EF) model in conjunction with self-consistent field theory. The calculations using the EF model were validated against unapproximated field-theoretic simulations with complex Langevin sampling and were found consistent with small angle X-ray scattering (SAXS) measurements on an experimental system. Using both the EF model and SAXS, phase diagrams were generated as a function of end-block fraction and polymer concentration. Several structures were observed including a body-centered cubic sphere phase, a hexagonally packed cylinder phase, and a lamellar phase. Finally, the EF model was used to explore how parameters that directly relate to polymer chemistry can be tuned to modify the resulting phase diagram, which is of practical interest for the development of new hydrogels.

Graphical abstract: Phase behavior of electrostatically complexed polyelectrolyte gels using an embedded fluctuation model

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Publication details

The article was received on 20 Oct 2014, accepted on 01 Dec 2014 and first published on 03 Dec 2014


Article type: Paper
DOI: 10.1039/C4SM02299H
Author version available: Download Author version (PDF)
Citation: Soft Matter, 2015,11, 1214-1225
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    Phase behavior of electrostatically complexed polyelectrolyte gels using an embedded fluctuation model

    D. J. Audus, J. D. Gopez, D. V. Krogstad, N. A. Lynd, E. J. Kramer, C. J. Hawker and G. H. Fredrickson, Soft Matter, 2015, 11, 1214
    DOI: 10.1039/C4SM02299H

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