Department of Chemical Engineering and Koch Institute for Integrative Cancer Research, Massachusetts Institute of Technology, Cambridge, MA 02139, USA.
Department of Chemical Engineering and Koch Institute for Integrative Cancer Research, Massachusetts Institute of Technology, Cambridge, MA 02139, USA; Department of Materials, University of Oxford, 16 Parks Road, Oxford OX1 3PH, UK.
Biomaterials. 2018 Jul;170:127-135. doi: 10.1016/j.biomaterials.2018.04.010. Epub 2018 Apr 6.
Covalently cross-linked gels are utilized in a broad range of biomedical applications though their synthesis often compromises easy implementation. Cross-linking reactions commonly utilize catalysts or conditions that can damage biologics and sensitive compounds, producing materials that require extensive post processing to achieve acceptable biocompatibility. As an alternative, we report a batch synthesis platform to produce covalently cross-linked materials appropriate for direct biomedical application enabled by green chemistry and commonly available food grade ingredients. Using caffeine, a mild base, to catalyze anhydrous carboxylate ring-opening of diglycidyl-ether functionalized monomers with citric acid as a tri-functional crosslinking agent we introduce a novel poly(ester-ether) gel synthesis platform. We demonstrate that biocompatible Caffeine Catalyzed Gels (CCGs) exhibit dynamic physical, chemical, and mechanical properties, which can be tailored in shape, surface texture, solvent response, cargo release, shear and tensile strength, among other potential attributes. The demonstrated versatility, low cost and facile synthesis of these CCGs renders them appropriate for a broad range of customized engineering applications including drug delivery constructs, tissue engineering scaffolds, and medical devices.
尽管共价交联凝胶在广泛的生物医学应用中得到了应用，但它们的合成通常会影响其易于实施的程度。交联反应通常使用催化剂或条件来破坏生物制剂和敏感化合物，从而产生需要大量后处理才能达到可接受的生物相容性的材料。作为替代方案，我们报告了一种批量合成平台，该平台可使用绿色化学和常用的食品级成分来生产适用于直接生物医学应用的共价交联材料。我们使用咖啡因（一种温和的碱）来催化具有柠檬酸的二缩水甘油基醚官能化单体的无水羧酸盐开环反应，作为三官能交联剂，我们引入了一种新型的聚（酯-醚）凝胶合成平台。我们证明了生物相容性的咖啡因催化凝胶（CCG）具有动态的物理、化学和机械性能，可以通过形状、表面纹理、溶剂响应、载药释放、剪切和拉伸强度等其他潜在特性进行定制。这些 CCG 具有多功能性、低成本和简便的合成，使其适用于广泛的定制工程应用，包括药物输送结构、组织工程支架和医疗器械。
