Biotechnical Properties of Poly(HEMA- co-HPMA) Hydrogels Are Governed by Distribution among Water States

Sara Abasi, Daria Anna Podstawczyk, Alycia Farida Sherback, Anthony Guiseppi-Elie

Research output: Contribution to journalArticle

7 Scopus citations

Abstract

Controlling the biotechnical properties of synthetic hydrogels allows their application in a wide range of biomedical fields. Cross-linker concentration and monomer mole ratio of poly(2-hydroxyethylmethacrylate-co-N-(2-hydroxypropyl) methacrylamide) [poly(HEMA-co-HPMA)]-based hydrogels were used to control the degree of hydration and water distribution within constructs. Cross-linker concentrations corresponding to 0.1, 0.5, 1.0, and 3.0 mol % tetraethylene glycol (TEGDA) with HEMA/HPMA mole ratios of 1:0 and 4:1, and poly(HEMA-co-HPMA) of cross-linker concentration corresponding to 1.0 mol % TEGDA with a HEMA/HPMA ratio of 1:1 were investigated for their degree of hydration, water distribution, and corresponding physiochemical and mechanical properties. Copolymerization of HEMA and HPMA was confirmed by Fourier-transform infrared spectroscopy. Both cross-linker concentration and chemical composition (HEMA/HPMA) systematically changed the water content and free/bound water distribution in the polymer, which resulted in different biochemical and transport properties. The addition of 20% HPMA (poly(HEMA-co-HPMA) (4:1)) increased total hydration (25%) and glass-transition temperature (9%) and decreased elastic modulus (31%) and nonfreezable bound water (33%) of the hydrogel. Increasing cross-linker concentration resulted in a stiffer hydrogel with less total water but larger nonfreezable water content. Evaluation of poly(HEMA-co-HPMA) (1:1) revealed that further increase of HPMA content increased the degree of hydration by 25% and decreased nonfreezable water content and elastic modulus by 33 and 16%, respectively, compared to that of poly(HEMA-co-HPMA) (4:1). The hydrogel correspondingly had a higher void fraction and rougher freeze-fractured surface. The diffusion-related processes depended more on water distribution within the hydrogel. The poly(HEMA) showed the fastest swelling kinetics with a concomitant burst release profile of fluorescein isothiocyanate-dextran (a drug surrogate), while the compositions containing HPMA showed a sustained release pattern. The biotechnical properties are illustrative examples of key properties that are influenced by the water distribution rather than the absolute water content of hydrogels.

Original languageEnglish (US)
Pages (from-to)4994-5004
Number of pages11
JournalACS Biomaterials Science and Engineering
Volume5
Issue number10
DOIs
StatePublished - Oct 14 2019

Keywords

  • elastic modulus
  • hydration
  • hydrogels
  • release
  • water distribution

ASJC Scopus subject areas

  • Biomaterials
  • Biomedical Engineering

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