Tunable microphase-regulated silk fibroin/poly (lactic acid) biocomposite materials generated from ionic liquids
Tunable microphase-regulated silk fibroin/poly (lactic acid) biocomposite materials generated from ionic liquids
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DOI：
10.1016/j.ijbiomac.2021.12.060
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发表时间：
2022-02-01
影响因子：
8.2
通讯作者：
Hu, Xiao
中科院分区：
文献类型：
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作者：
Deng, Qianqian;Wang, Fang;Hu, Xiao
开发具有独特、可调结构和物理化学性质的新型生物材料的最有效和最有前途的策略之一是利用离子液体创造将合成聚合物与天然蛋白质相结合的复合材料。本研究将可生物降解的聚(D，L-乳酸)与丝素蛋白(SF)共混，利用离子液体为基础的二元溶剂体系(1-丁基-3-甲基咪唑氯/N，N-二甲基甲酰胺)制备生物相容薄膜，以保持蛋白质/聚合物的相对分子质量，并促进分子间的相互作用。通过扫描电子显微镜(SEM)、傅里叶变换红外光谱(FTIR)、X射线衍射仪(XRD)、差示扫描量热仪(DSC)、热重分析(TGA)、水接触角测试、细胞毒性分析和酶降解等手段，研究了不同比例的聚乳酸与聚硅氧烷的作用效果。结果表明，复合膜在宏观上是均匀共混的，表现出典型的全互溶聚合物共混特征。通过增加SF在复合材料中的含量，薄膜中的β-片层数量显著增加，从而允许SF作为物理交联剂来维持蛋白质-聚合物网络的稳定性。此外，SF显著提高了材料的亲水性和生物相容性，促进了胶束结构在生物复合材料中的自组装。薄膜中不同的拓扑结构也为细胞的黏附、生长和增殖提供了有利的表面形态。总体而言，这项研究展示了一种将合成聚合物和蛋白质结合在一起的微调聚合物混合物的有效制造方法，用于广泛的生物医学和绿色材料应用。
One of the most effective and promising strategies to develop novel biomaterials with unique, tunable structure and physicochemical properties is by creating composite materials that combine synthetic polymers with natural proteins using ionic liquids. In this study, biodegradable poly(D,L-lactic acid) (PDLLA) was blended with silk fibroin (SF) to create biocompatible films using an ionic liquid-based binary solvent system (1-butyl-3-methylimidazolium chloride/N,N-dimethylformamide), which can maintain the molecular weights of the proteins/polymers and encourage intermolecular interactions between the molecules. The effects of varying the ratio of PLA to SF were studied using scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), differential scanning calorimetry (DSC), thermogravimetric analysis (TGA), water contact angle testing, and cytotoxicity analysis as well as enzymatic degradation. Results showed that the composite films were homogeneously blended on the macroscopic scale and exhibited typical fully miscible polymer blend characteristics. By increasing the SF content in the composites, the amounts of beta-sheets in the films were significantly increased, allowing for SF to act as a physical crosslinker to maintain the stability of the protein-polymer network. Additionally, SF significantly improved the hydrophilicity and biocompatibility of the material and promoted the self-assembly of micelle structures in the biocomposites. Different topologies in the films also provided beneficial surface morphology for cell adhesion, growth, and proliferation. Overall, this study demonstrated an effective fabrication method for a fine-tuned polymer blends combining synthetic polymer and protein for a wide variety of biomedical and green material applications.