Mechanically tuneable physical nanocomposite hydrogels from polyelectrolyte complex templated silica nanoparticles for anionic therapeutic delivery.
Mechanically tuneable physical nanocomposite hydrogels from polyelectrolyte complex templated silica nanoparticles for anionic therapeutic delivery.
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DOI：
10.1016/j.jcis.2022.02.052
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发表时间：
2022-02
影响因子：
9.9
通讯作者：
George Newham;S. Evans;Z. Ong
中科院分区：
文献类型：
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作者：
George Newham;S. Evans;Z. Ong
水凝胶在药物输送和组织工程方面显示出巨大的前景，但由于机械性能差，在实际应用中受到限制。聚合物接枝二氧化硅纳米颗粒作为化学或物理交联剂掺入原位聚合纳米复合水凝胶中，以提高其机械性能已被广泛研究。尽管纳米复合水凝胶具有增强的机械刚度、抗拉强度和自愈性能，但仍需要开发更简单和模块化的方法来获得纳米复合水凝胶。在此，我们报告了一种简单的聚电解质复合物（PEC）模板合成有机-无机杂化聚亚胺功能化二氧化硅纳米颗粒（PEI-SiNPs）的方法，并将其作为多功能静电交联剂与透明质酸（HA）形成纳米复合水凝胶。混合后，阳离子PEI-SiNPs和阴离子HA之间的静电相互作用导致形成凝聚状纳米复合水凝胶，具有增强的机械刚度，可以通过改变PEI-SiNPs和HA的比例来调节。水凝胶网络中的可逆静电相互作用也使其具有自愈和触变特性。PEI-SiNPs中存在的过量正电荷促进了高负载，并延缓了阴离子抗癌药物甲氨蝶呤从纳米复合水凝胶中的释放。此外，PEI- sinp和HA的静电络合被发现可以减轻与使用高分子量PEI相关的血液毒性问题。本文提出的方法提供了一种更简单和更通用的策略，用于制造具有可调机械刚度和自修复性能的凝聚状纳米复合水凝胶，用于药物输送应用。
Hydrogels have shown great promise for drug delivery and tissue engineering but can be limited in practical applications by poor mechanical performance. The incorporation of polymer grafted silica nanoparticles as chemical or physical crosslinkers inin situpolymerised nanocomposite hydrogels has been widely researched to enhance their mechanical properties. Despite the enhanced mechanical stiffness, tensile strength, and self-healing properties, there remains a need for the development of simpler and modular approaches to obtain nanocomposite hydrogels. Herein, we report a facile protocol for the polyelectrolyte complex (PEC) templated synthesis of organic-inorganic hybrid poly(ethylenimine) functionalised silica nanoparticles (PEI-SiNPs) and their use as multifunctional electrostatic crosslinkers with hyaluronic acid (HA) to form nanocomposite hydrogels. Upon mixing, electrostatic interactions between cationic PEI-SiNPs and anionic HA resulted in the formation of a coacervate nanocomposite hydrogel with enhanced mechanical stiffness that can be tuned by varying the ratios of PEI-SiNPs and HA present. The reversible electrostatic interactions within the hydrogel networks also enabled self-healing and thixotropic properties. The excess positive charge present within the PEI-SiNPs facilitated high loading and retarded the release of the anionic anti-cancer drug methotrexate from the nanocomposite hydrogel. Furthermore, the electrostatic complexation of PEI-SiNP and HA was found to mitigate haemotoxicity concerns associated with the use of high molecular weight PEI. The method presented herein offers a simpler and more versatile strategy for the fabrication of coacervate nanocomposite hydrogels with tuneable mechanical stiffness and self-healing properties for drug delivery applications.