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Polymers 2014, 6(9), 2451-2472; doi:10.3390/polym6092451

Polyplex Formation Influences Release Mechanism of Mono- and Di-Valent Ions from Phosphorylcholine Group Bearing Hydrogels

1
Center for Bioelectronics, Biosensors and Biochips (C3B), Clemson University Advanced Materials Center, 100 Technology Drive, Anderson, SC 29625, USA
2
Department of Chemical and Biomolecular Engineering, 132 Earle Hall, Clemson University, Clemson, SC 29634, USA
3
Department of Bioengineering, 132 Earle Hall, Clemson University, Clemson, SC 29634, USA
4
Holcombe Department of Electrical and Computer Engineering, 132 Earle Hall, Clemson University, Clemson, SC 29634, USA
5
ABTECH Scientific, Inc., Biotechnology Research Park, 800 East Leigh Street, Richmond, VA 23219, USA
*
Author to whom correspondence should be addressed.
Received: 14 July 2014 / Revised: 3 September 2014 / Accepted: 9 September 2014 / Published: 25 September 2014
(This article belongs to the Special Issue Complex Macromolecular Architectures)
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Abstract

The release of monovalent potassium and divalent calcium ions from zwitterionic phosphorylcholine containing poly(2-hydroxyethyl methacrylate) (pHEMA)-based hydrogels was studied and the effects of polymer swelling, ion valence and temperature were investigated. For comparison, ions were loaded during hydrogel formulation or loaded by partitioning following construct synthesis. Using the Koshmeyer-Peppas release model, the apparent diffusion coefficient, Dapp, and diffusional exponents, n, were Dapp (pre-K+) = 2.03 × 105, n = 0.4 and Dapp (post-K+) = 1.86 × 105, n = 0.33 respectively, indicative of Fickian transport. The Dapp (pre-Ca2+) = 3.90 × 106, n = 0.60 and Dapp (post-Ca2+) = 2.85 × 106, n = 0.85, respectively, indicative of case II and anomalous transport. Results indicate that divalent cations form cation-polyelectrolyte anion polymer complexes while monovalent ions do not. Temperature dependence of potassium ion release was shown to follow an Arrhenius-type relation with negative apparent activation energy of −19 ± 15 while calcium ion release was temperature independent over the physiologically relevant range (25–45 °C) studied. The negative apparent activation energy may be due to temperature dependent polymer swelling. No effect of polymer swelling on the diffusional exponent or rate constant was found suggesting polymer relaxation occurs independent of polymer swelling. View Full-Text
Keywords: polyplexes; hydrogels; electromigration; release; transport; diffusional exponent polyplexes; hydrogels; electromigration; release; transport; diffusional exponent
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MDPI and ACS Style

Wilson, A.N.; Blenner, M.; Guiseppi-Elie, A. Polyplex Formation Influences Release Mechanism of Mono- and Di-Valent Ions from Phosphorylcholine Group Bearing Hydrogels. Polymers 2014, 6, 2451-2472.

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