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生物相容性、可降解、光固化的聚氨酯基弹性水凝胶的合成与表征

Synthesis and characterization of biocompatible, degradable, light-curable, polyurethane-based elastic hydrogels.

作者信息

Zhang Changhong, Zhang Ning, Wen Xuejun

机构信息

Clemson--MUSC Bioengineering Program, Department of Bioengineering, Clemson University, Charleston, South Carolina 29425, USA.

出版信息

J Biomed Mater Res A. 2007 Sep 1;82(3):637-50. doi: 10.1002/jbm.a.30992.

Abstract

A series of degradable polyurethane-based light-curable elastic hydrogels were synthesized from polycaprolactone diol, polyethylene glycol (PEG), lysine diisocyanate (LDI), and 2-hydroxyethyl methacrylate (HEMA) through UV light initiated polymerization reaction. LDI was used as hard segment and polycaprolactone (PCL) and/or PEG were used as soft segments. By changing the PCL to PEG ratio during the prepolymer synthesis, polyurethanes with different soft segmental structures, hydrophilicity, and cytophilicity were obtained after light-initiated polymerization. The chemical structures of the synthesized polymers were characterized using differential scanning calorimetry and Fourier transform infrared spectroscopy. Physical properties such as swelling, mechanical properties, and in vitro degradation were evaluated. Materials containing a higher ratio of PEG exhibit higher water absorbance, higher degradation rate in vitro, and lower mechanical strength in the hydrated state. Mouse embryonal carcinoma-derived clonal chondrocytes were used as a model cell type to study the cytocompatibility of the synthesized polymers. Chondrocyte attachment, proliferation rates, and morphologies varied with changes in the PCL/PEG ratio. With a higher PEG ratio, lower cell attachment and proliferation were observed. To improve the cell attachment and proliferation on high PEG content hydrogels, bioactive molecules, such as peptides and proteins, were conjugated or immobilized in the gel matrix during the light-curing process. In this study, a short peptide, Arg-Gly-Asp-Ser, was used as a model biomolecule and incorporated into the gels during the light-curing process and improved cell growth was observed. In summary, the use of PCL/PEG at different ratios, as well as the introduction of HEMA into polyurethane, allows the synthesis of a series of biocompatible elastic hydrogels with tunable physical and cytophilic properties through light-initiated polymerization. This series of materials also allows for controlling cell attachment and growth by incorporating bioactive molecules during the light-curing process.

摘要

通过紫外光引发聚合反应,由聚己内酯二醇、聚乙二醇(PEG)、赖氨酸二异氰酸酯(LDI)和甲基丙烯酸2-羟乙酯(HEMA)合成了一系列可降解的基于聚氨酯的光固化弹性水凝胶。LDI用作硬段,聚己内酯(PCL)和/或PEG用作软段。通过在预聚物合成过程中改变PCL与PEG的比例,光引发聚合后获得了具有不同软段结构、亲水性和细胞亲和性的聚氨酯。使用差示扫描量热法和傅里叶变换红外光谱对合成聚合物的化学结构进行了表征。评估了诸如溶胀、机械性能和体外降解等物理性能。含有较高PEG比例的材料表现出更高的吸水率、更高的体外降解率以及在水合状态下更低的机械强度。将小鼠胚胎癌衍生的克隆软骨细胞用作模型细胞类型,以研究合成聚合物的细胞相容性。软骨细胞的附着、增殖率和形态随PCL/PEG比例的变化而变化。PEG比例越高,观察到的细胞附着和增殖越低。为了改善高PEG含量水凝胶上的细胞附着和增殖,在光固化过程中将生物活性分子(如肽和蛋白质)缀合或固定在凝胶基质中。在本研究中,短肽Arg-Gly-Asp-Ser用作模型生物分子,并在光固化过程中掺入凝胶中,观察到细胞生长得到改善。总之,以不同比例使用PCL/PEG以及将HEMA引入聚氨酯中,使得通过光引发聚合能够合成一系列具有可调物理和细胞亲和性能的生物相容性弹性水凝胶。这一系列材料还允许通过在光固化过程中掺入生物活性分子来控制细胞附着和生长。

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