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Synthesis, characterization and properties of a physically and chemically gelling polymer system using poly(NIPAAm-co-HEMA-acrylate) and poly(NIPAAm-co-cysteamine).

Abstract

The aim of this work was to develop a simultaneous physically and chemically gelling system using NIPAAm co-polymers. The in situ polymer gel was obtained by synthesizing poly(NIPAAm-co-HEMAacrylate) and poly(NIPAAm-co-cysteamine) through free radical polymerization and further nucleophilic substitution. The purpose of the dual gelation is that physical gelation would take place at higher temperatures as the NIPAAm chains associate, while chemical gelation would occur through a Michael-type addition reaction, resulting in a cross-link forming through a nucleophilic attack of the thiolate on the acrylate. The structure of each co-polymer was then verified using (1)H-NMR and FT-IR spectroscopy. The corresponding lower critical solution temperature and phase transition behavior of each co-polymer was analyzed through cloud point and DSC, while mechanical properties were investigated through rheology. Swelling behavior was also monitored at different temperatures. The resulting polymer system demonstrated properties compatible with physiological conditions, forming a gel at pH 7.4 and at temperatures near body temperature. The hydrogel also showed reduced viscoelastic flow at low frequency stress, and increased strength than purely physical or chemical gels. Swelling behavior was determined to be temperature-dependent; however, no difference was observed in swelling percent beyond 48 h. Having the ability to alter these co-polymers through various synthesis parameters and techniques, this hydrogel can potentially be used as an injectable, waterborne gelling material for biomedical applications such as endovascular embolization.

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  • Authors+Show Affiliations

    ,

    a The School of Biological and Health Systems Engineering, Center for Interventional Biomaterials, ECG 334, Arizona State University, Tempe, AZ 85287-9709, USA.

    , ,

    Source

    MeSH

    Acrylamides
    Acrylic Resins
    Cysteamine
    Gels
    Hydrogen-Ion Concentration
    Materials Testing
    Molecular Structure
    Polyhydroxyethyl Methacrylate
    Polymers
    Proton Magnetic Resonance Spectroscopy
    Spectroscopy, Fourier Transform Infrared
    Temperature
    Time Factors

    Pub Type(s)

    Journal Article
    Research Support, Non-U.S. Gov't

    Language

    eng

    PubMed ID

    20594409

    Citation

    TY - JOUR T1 - Synthesis, characterization and properties of a physically and chemically gelling polymer system using poly(NIPAAm-co-HEMA-acrylate) and poly(NIPAAm-co-cysteamine). AU - Bearat,Hanin H, AU - Lee,Bae Hoon, AU - Valdez,Jorge, AU - Vernon,Brent L, PY - 2010/7/3/entrez PY - 2010/7/3/pubmed PY - 2016/6/9/medline KW - CHEMICAL CROSS-LINK KW - IN SITU POLYMER GEL KW - LOWER CRITICAL SOLUTION TEMPERATURE (LCST) KW - MICHAEL-TYPE ADDITION REACTION KW - PHYSICAL GEL KW - POLY(NIPAAM) KW - RHEOLOGY SP - 1299 EP - 318 JF - Journal of biomaterials science. Polymer edition JO - J Biomater Sci Polym Ed VL - 22 IS - 10 N2 - The aim of this work was to develop a simultaneous physically and chemically gelling system using NIPAAm co-polymers. The in situ polymer gel was obtained by synthesizing poly(NIPAAm-co-HEMAacrylate) and poly(NIPAAm-co-cysteamine) through free radical polymerization and further nucleophilic substitution. The purpose of the dual gelation is that physical gelation would take place at higher temperatures as the NIPAAm chains associate, while chemical gelation would occur through a Michael-type addition reaction, resulting in a cross-link forming through a nucleophilic attack of the thiolate on the acrylate. The structure of each co-polymer was then verified using (1)H-NMR and FT-IR spectroscopy. The corresponding lower critical solution temperature and phase transition behavior of each co-polymer was analyzed through cloud point and DSC, while mechanical properties were investigated through rheology. Swelling behavior was also monitored at different temperatures. The resulting polymer system demonstrated properties compatible with physiological conditions, forming a gel at pH 7.4 and at temperatures near body temperature. The hydrogel also showed reduced viscoelastic flow at low frequency stress, and increased strength than purely physical or chemical gels. Swelling behavior was determined to be temperature-dependent; however, no difference was observed in swelling percent beyond 48 h. Having the ability to alter these co-polymers through various synthesis parameters and techniques, this hydrogel can potentially be used as an injectable, waterborne gelling material for biomedical applications such as endovascular embolization. SN - 1568-5624 UR - https://www.unboundmedicine.com/medline/citation/20594409/Synthesis_characterization_and_properties_of_a_physically_and_chemically_gelling_polymer_system_using_poly_NIPAAm_co_HEMA_acrylate__and_poly_NIPAAm_co_cysteamine__ L2 - http://www.tandfonline.com/doi/full/10.1163/092050610X504774 ER -