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Title: Effects of Polymer and Salt Concentration on the Structure and Properties of Triblock Copolymer Coacervate Hydrogels

Abstract

Structure-property relationships were established for complex coacervate hydrogels formed from binary aqueous solutions of oppositely charged ABA triblock copolymers. The charged triblock copolymers were synthesized by functionalizing poly[(allyl glycidyl ether)-b-(ethylene oxide)-b-(allyl glycidyl ether)] with either guanidinium or sulfonate functional groups. When aqueous solutions (ca. 5-40 wt %) of these oppositely charged polymers were mixed, the electrostatic interactions of the functionalized blocks led to the association of the oppositely charged end-blocks into phase-separated complex coacervate domains bridged by the uncharged, hydrophilic PEO midblock. The resulting structures were studied by small-angle X-ray scattering (SAXS) and dynamic mechanical spectroscopy. The organization of the coacervate domains was shown to affect substantially the viscoelastic properties of the hydrogels, with the storage modulus increasing significantly as the mixtures transformed from a disordered array of domains to an ordered BCC structure with increasing block copolymer concentration. As the polymer concentration was further increased to 30 wt %, a hexagonal structure appeared, which coincided with a 25% drop in the modulus. Further structural changes, resulting in variations in the viscoelastic response, were also induced through changes in salt concentration. The viscoelastic properties and the physical nature of the cross-links have important implications for the applicability of these gelsmore » as injectable drug delivery systems.« less

Authors:
; ; ; ; ; ;
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
University of Chicago - Institute for Molecular Engineering; USDOE Office of Science - Office of Basic Energy Sciences - Materials Sciences and Engineering Division; National Science Foundation (NSF)
OSTI Identifier:
1395152
DOE Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article
Journal Name:
Macromolecules
Additional Journal Information:
Journal Volume: 46; Journal Issue: 4; Journal ID: ISSN 0024-9297
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English

Citation Formats

Krogstad, Daniel V., Lynd, Nathaniel A., Choi, Soo-Hyung, Spruell, Jason M., Hawker, Craig J., Kramer, Edward J., and Tirrell, Matthew V. Effects of Polymer and Salt Concentration on the Structure and Properties of Triblock Copolymer Coacervate Hydrogels. United States: N. p., 2013. Web. doi:10.1021/ma302299r.
Krogstad, Daniel V., Lynd, Nathaniel A., Choi, Soo-Hyung, Spruell, Jason M., Hawker, Craig J., Kramer, Edward J., & Tirrell, Matthew V. Effects of Polymer and Salt Concentration on the Structure and Properties of Triblock Copolymer Coacervate Hydrogels. United States. https://doi.org/10.1021/ma302299r
Krogstad, Daniel V., Lynd, Nathaniel A., Choi, Soo-Hyung, Spruell, Jason M., Hawker, Craig J., Kramer, Edward J., and Tirrell, Matthew V. Tue . "Effects of Polymer and Salt Concentration on the Structure and Properties of Triblock Copolymer Coacervate Hydrogels". United States. https://doi.org/10.1021/ma302299r.
@article{osti_1395152,
title = {Effects of Polymer and Salt Concentration on the Structure and Properties of Triblock Copolymer Coacervate Hydrogels},
author = {Krogstad, Daniel V. and Lynd, Nathaniel A. and Choi, Soo-Hyung and Spruell, Jason M. and Hawker, Craig J. and Kramer, Edward J. and Tirrell, Matthew V.},
abstractNote = {Structure-property relationships were established for complex coacervate hydrogels formed from binary aqueous solutions of oppositely charged ABA triblock copolymers. The charged triblock copolymers were synthesized by functionalizing poly[(allyl glycidyl ether)-b-(ethylene oxide)-b-(allyl glycidyl ether)] with either guanidinium or sulfonate functional groups. When aqueous solutions (ca. 5-40 wt %) of these oppositely charged polymers were mixed, the electrostatic interactions of the functionalized blocks led to the association of the oppositely charged end-blocks into phase-separated complex coacervate domains bridged by the uncharged, hydrophilic PEO midblock. The resulting structures were studied by small-angle X-ray scattering (SAXS) and dynamic mechanical spectroscopy. The organization of the coacervate domains was shown to affect substantially the viscoelastic properties of the hydrogels, with the storage modulus increasing significantly as the mixtures transformed from a disordered array of domains to an ordered BCC structure with increasing block copolymer concentration. As the polymer concentration was further increased to 30 wt %, a hexagonal structure appeared, which coincided with a 25% drop in the modulus. Further structural changes, resulting in variations in the viscoelastic response, were also induced through changes in salt concentration. The viscoelastic properties and the physical nature of the cross-links have important implications for the applicability of these gels as injectable drug delivery systems.},
doi = {10.1021/ma302299r},
url = {https://www.osti.gov/biblio/1395152}, journal = {Macromolecules},
issn = {0024-9297},
number = 4,
volume = 46,
place = {United States},
year = {2013},
month = {2}
}