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Facile preparation of photodegradable hydrogels by photopolymerization

机译：光聚合的可光降解水凝胶的舒适性

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Photodegradable hydrogels have emerged as a powerful material platform for studying and directing cell behaviors, as well as for delivering drugs. The premise of this technique is to use a cytocompatible light source to cleave linkers within a hydrogel, thus causing reduction of matrix stiffness or liberation of matrix-tethered biomolecules in a spatial-temporally controlled manner. The most commonly used photodegradable units are molecules containing nitrobenzyl moieties that absorb light in the ultraviolet (UV) to lower visible wavelengths (~280 to 450 nm). Because photodegradable linkers and hydrogels reported in the literature thus far are all sensitive to UV light, highly efficient UV-mediated photopolymerizations are less likely to be used as the method to prepare these hydrogels. As a result, currently available photodegradable hydrogels are formed by redox-mediated radical polymerizations, emulsion polymerizations, Michael-type addition reactions, or orthogonal click chemistries. Here, we report the first photodegradable poly(ethylene glycol)-based hydrogel system prepared by step-growth photopolymerization. The model photolabile peptide cross-linkers, synthesized by conventional solid phase peptide synthesis, contained terminal cysteines for step-growth thiol-ene photo-click reactions and a UV-sensitive 2-nitrophenylalanine residue in the peptide backbone for photo-cleavage. Photolysis of this peptide was achieved through adjusting UV light exposure time and intensity. Photopolymerization of photodegradable hydrogels containing photolabile peptide cross-linkers was made possible via a highly efficient visible light-mediated thiol-ene photo-click reaction using a non-cleavage type photoinitiator eosin-Y. Rapid gelation was confirmed by in situ photo-rheometry. Flood UV irradiation at controlled wavelength and intensity was used to demonstrate the photodegradability of these photopolymerized hydrogels.
机译：可光降解的水凝胶已成为研究和指导细胞行为以及传递药物的强大材料平台。该技术的前提是使用细胞相容性光源切割水凝胶中的接头，从而导致以空间-时间控制的方式降低基质刚度或释放基质束缚的生物分子。最常用的可光降解单元是含有硝基苄基部分的分子，该分子吸收紫外线（UV）中的光以降低可见光波长（〜280至450 nm）。由于迄今为止在文献中报道的可光降解的连接剂和水凝胶都对紫外线敏感，因此高效的紫外线介导的光聚合不太可能用作制备这些水凝胶的方法。结果，通过氧化还原介导的自由基聚合，乳液聚合，迈克尔型加成反应或正交点击化学形成了当前可用的可光降解水凝胶。在这里，我们报告通过逐步增长的光聚合制备的第一个可光降解的基于聚乙二醇的水凝胶体系。通过常规固相肽合成法合成的模型光不稳定肽交联剂包含用于逐步生长的硫醇-烯光点击反应的末端半胱氨酸和用于光裂解的肽骨架中的UV敏感的2-硝基苯丙氨酸残基。该肽的光解是通过调节紫外线的曝光时间和强度来实现的。通过使用非裂解型光引发剂曙红-Y的高效可见光介导的硫醇-烯光点击反应，使得包含光不稳定肽交联剂的可光降解水凝胶的光聚合成为可能。通过原位流变仪确认快速凝胶化。使用在控制的波长和强度下的泛紫外辐射来证明这些光聚合水凝胶的光降解性。

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