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Photo-active collagen systems with controlled triple helix architecture

机译：具有受控三螺旋结构的光敏胶原蛋白系统

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The design of photo-active collagen systems is presented as a basis for establishing biomimetic materials with varied network architecture and programmable macroscopic properties. Following in-house isolation of type I collagen, reaction with vinyl-bearing compounds of varied backbone rigidity, i.e. 4-vinylbenzyl chloride (4VBC) and glycidyl methacrylate (GMA), was carried out. TNBS colorimetric assay, 1H-NMR and ATR-FTIR confirmed covalent and tunable functionalization of collagen lysines. Depending on the type and extent of functionalization, controlled stability and thermal denaturation of triple helices were observed via circular dichroism (CD), whereby the hydrogen-bonding capability of introduced moieties was shown to play a major role. Full gel formation was observed following photo-activation of functionalized collagen solutions. The presence of a covalent network only slightly affected collagen triple helix conformation (as observed by WAXS and ATR-FTIR), confirming the structural organization of functionalized collagen precursors. Photo-activated hydrogels demonstrated an increased denaturation temperature (DSC) with respect to native collagen, suggesting that the formation of the covalent network successfully stabilized collagen triple helices. Moreover, biocompatibility and mechanical competence of obtained hydrogels were successfully demonstrated under physiologically-relevant conditions. These results demonstrate that this novel synthetic approach enabled the formation of biocompatible collagen systems with defined network architecture and programmable macroscopic properties, which can only partially be obtained with current synthetic methods.
机译：介绍了光敏胶原蛋白系统的设计，作为建立具有多种网络结构和可编程宏观特性的仿生材料的基础。在内部分离出I型胶原之后，与具有不同骨架刚性的含乙烯基化合物，即4-乙烯基苄基氯（4VBC）和甲基丙烯酸缩水甘油酯（GMA）进行反应。 TNBS比色分析， 1 H-NMR和ATR-FTIR证实了胶原赖氨酸的共价和可调功能。取决于官能化的类型和程度，通过圆二色性（CD）观察到三重螺旋的受控稳定性和热变性，从而表明引入的部分的氢键合能力起主要作用。光活化功能化胶原蛋白溶液后观察到完全凝胶形成。共价网络的存在仅轻微影响胶原蛋白三螺旋构象（通过WAXS和ATR-FTIR观察到），证实了功能化胶原蛋白前体的结构组织。光活化水凝胶显示出相对于天然胶原蛋白而言更高的变性温度（DSC），这表明共价网络的形成成功地稳定了胶原蛋白三螺旋。此外，在生理相关条件下成功地证明了获得的水凝胶的生物相容性和机械能力。这些结果表明，这种新颖的合成方法能够形成具有确定的网络架构和可编程的宏观特性的生物相容性胶原蛋白系统，而这只能通过当前的合成方法部分获得。

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