Poly(γ-glutamic acid)/silica hybrids with calcium incorporated in the silica network by use of a calcium alkoxide precursor

Gowsihan Poologasundarampilla, Bobo Yu, Olga Tsigkou, Daming Wang, Frederik Romer, Vineet Bhakhri, Finn Giuliani, Molly M. Stevens, David S. McPhail, Mark E. Smith, John V. Hanna, Julian R. Jones

    Research output: Contribution to journalArticlepeer-review

    Abstract

    Current materials used for bone regeneration are usually bioactive ceramics or glasses. Although they bond to bone, they are brittle. There is a need for new materials that can combine bioactivity with toughness and controlled biodegradation. Sol-gel hybrids have the potential to do this through their nanoscale interpenetrating networks (IPN) of inorganic and organic components. Poly(γ-glutamic acid) (γ-PGA) was introduced into the sol-gel process to produce a hybrid of γ-PGA and bioactive silica. Calcium is an important element for bone regeneration but calcium sources that are used traditionally in the sol-gel process, such as Ca salts, do not allow Ca incorporation into the silicate network during low-temperature processing. The hypothesis for this study was that using calcium methoxyethoxide (CME) as the Ca source would allow Ca incorporation into the silicate component of the hybrid at room temperature. The produced hybrids would have improved mechanical properties and controlled degradation compared with hybrids of calcium chloride (CaCl2), in which the Ca is not incorporated into the silicate network. Class II hybrids, with covalent bonds between the inorganic and organic species, were synthesised by using organosilane. Calcium incorporation in both the organic and inorganic IPNs of the hybrid was improved when CME was used. This was clearly observed by using FTIR and solid-state NMR spectroscopy, which showed ionic cross-linking of γ-PGA by Ca and a lower degree of condensation of the Si species compared with the hybrids made with CaCl 2 as the Ca source. The ionic cross-linking of γ-PGA by Ca resulted in excellent compressive strength and reduced elastic modulus as measured by compressive testing and nanoindentation, respectively. All hybrids showed bioactivity as hydroxyapatite (HA) was formed after immersion in simulated body fluid (SBF). Organic/inorganic hybrid materials: Calcium methoxyethoxide (CME) was found to be an effective precursor for successfully introducing calcium into organic/inorganic hybrid materials (see figure). The Ca2+ ions were found to successfully cross-link the polymer chains, thereby avoiding a burst release of polymer and Ca2+ in buffered media. CME was found to distribute within the inorganic silica network thanks to the high reactivity of CME with hydroxyl groups. © 2014 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA. This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.
    Original languageEnglish
    Pages (from-to)8149-8160
    Number of pages11
    JournalChemistry - A European Journal
    Volume20
    Issue number26
    DOIs
    Publication statusPublished - 23 Jun 2014

    Keywords

    • bioactivity
    • calcium methoxyethoxide
    • hybrid materials
    • poly(γ-glutamic acid)
    • sol-gel process

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