Methacrylation induces rapid, temperature-dependent, reversible self-assembly of type-I collagen.
Methacrylation induces rapid, temperature-dependent, reversible self-assembly of type-I collagen.
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DOI：
10.1021/la502418s
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发表时间：
2014-09-23
期刊：
影响因子：
--
通讯作者：
Shreiber DI
中科院分区：
文献类型：
--
作者：
Drzewiecki KE;Parmar AS;Gaudet ID;Branch JR;Pike DH;Nanda V;Shreiber DI
I型胶原在生理温度和pH下自组装成纤维状凝胶，提供细胞粘附性、支撑性和结构网络结构。因此，它是一种有吸引力的、受欢迎的支架，用于体外评估细胞行为和组织工程应用。本研究对I型胶原进行了改性，在赖氨酸残基的游离胺上引入甲基丙烯酸酯基团，合成了胶原蛋白甲基丙烯酰胺(CMA)。CMA保留了胶原的自组装、生物降解性和自然生物活性等特性，但也具有光活性，在光引发剂存在的情况下，在紫外光照射下，可以快速与丙烯酸酯分子交联或功能化。CMA还表现出独特的温度依赖行为。对于天然的I型胶原，在低于其变性点的温度下加热和冷却后，纤维网络结构的总体结构在几个小时的时间尺度上基本保持不变。然而，CMA是快速热可逆的，当温度在10到37°C之间调节时，它将在液体大分子悬浮液和半固态纤维水凝胶之间振荡。使用一系列机械、散射和光谱方法，我们证明了结构可逆性在多个尺度上明显，从三螺旋的蛋白质拓扑到CMA水凝胶的流变特性。CMA经不同阶段加热和冷却后的电子显微镜图像显示，纤维的典型胶原样D-周期带状超微结构保持不变。一种快速热可逆的胶原基水凝胶作为一种生物功能、生物相容的材料，有望在组织工程和药物输送应用中得到广泛的应用。热可逆性也使CMA成为研究分级胶原自组装复杂过程的有力模型。
Type-I collagen self-assembles into a fibrillar gel at physiological temperature and pH to provide a cell-adhesive, supportive, structural network. As such, it is an attractive, popular scaffold for in vitro evaluations of cellular behavior and for tissue engineering applications. In this study, type-I collagen is modified to introduce methacrylate groups on the free amines of the lysine residues to create collagen methacrylamide (CMA). CMA retains the properties of collagen such as self-assembly, biodegradability, and natural bioactivity but is also photoactive and can be rapidly cross-linked or functionalized with acrylated molecules when irradiated with ultraviolet light in the presence of a photoinitiator. CMA also demonstrates unique temperature-dependent behavior. For natural type-I collagen, the overall structure of the fiber network remains largely static over time scales of a few hours upon heating and cooling at temperatures below its denaturation point. CMA, however, is rapidly thermoreversible and will oscillate between a liquid macromer suspension and a semisolid fibrillar hydrogel when the temperature is modulated between 10 and 37 °C. Using a series of mechanical, scattering, and spectroscopic methods, we demonstrate that structural reversibility is manifest across multiple scales from the protein topology of the triple helix up through the rheological properties of the CMA hydrogel. Electron microscopy imaging of CMA after various stages of heating and cooling shows that the canonical collagen-like D-periodic banding ultrastructure of the fibers is preserved. A rapidly thermoreversible collagen-based hydrogel is expected to have wide utility in tissue engineering and drug delivery applications as a biofunctional, biocompatible material. Thermal reversibility also makes CMA a powerful model for studying the complex process of hierarchical collagen self-assembly.
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影响因子：
13.1
作者：
Cheung, Hoi-Yan;Lau, Kin-Tak;Hui, David
通讯作者：
Hui, David
DOI：
10.1073/pnas.0800291105
发表时间：
2008-06-24
影响因子：
11.1
作者：
Cejas, Mabel A.;Kinnney, William A.;Maryanoff, Bruce E.
通讯作者：
Maryanoff, Bruce E.
影响因子：
2.9
作者：
Kar, Karunakar;Ibrar, Sajjad;Nanda, Vikas;Getz, Todd M.;Kunapuli, Satya P.;Brodsky, Barbara
通讯作者：
Brodsky, Barbara
影响因子：
4.1
作者：
Monteiro, Gary A.;Fernandes, Anthony V.;Shreiber, David I.
通讯作者：
Shreiber, David I.
影响因子：
2.4
作者：
Harris, J. Robin;Soliakov, Andrei;Lewis, Richard J.
通讯作者：
Lewis, Richard J.