Jain Era, Hill Lindsay, Canning Erin, Sell Scott A, Zustiak Silviya P
Department of Biomedical Engineering, Saint Louis University, Saint Louis, MO 63103, USA.
J Mater Chem B. 2017 Apr 14;5(14):2679-2691. doi: 10.1039/c6tb03050e. Epub 2017 Mar 24.
Tuning hydrogel properties through minor modifications of the crosslinker structure is a beneficial approach for hydrogel design that could result in hydrogels with wide range of properties to match a desired application. In this study, we analyzed the relationship between the dithiol crosslinker chemical and physical structure and the resulting properties of polyethylene glycol (PEG) hydrogels formed via Michael-type addition reaction. Specifically, the dithiol crosslinker properties and chemical structure were correlated with gelation time, hydrolytic degradation rate, reaction rate constant, crosslink density and storage modulus of PEG hydrogels. By changing the properties and structure of the crosslinker, hydrogels with controlled degradation ranging from 10 h to 22 d were obtained. It was also established that hydrogel gelation times correlated closely with degradation times. By extensive characterization of the dithiol crosslinker chemical structure and physical properties, we identified two sets of conditions which yielded fast-gelling, fast-degrading hydrogels and slow-gelling, slow-degrading hydrogels. Uniquely, the hydrogel storage moduli could be controlled by the dithiol crosslinker chemical identity independent of the degradation time of the hydrogel or the mesh size.
通过对交联剂结构进行微小修饰来调节水凝胶性能,是一种有利于水凝胶设计的方法,这可能会产生具有广泛性能的水凝胶,以匹配所需的应用。在本研究中,我们分析了二硫醇交联剂的化学和物理结构与通过迈克尔型加成反应形成的聚乙二醇(PEG)水凝胶的最终性能之间的关系。具体而言,二硫醇交联剂的性能和化学结构与PEG水凝胶的凝胶化时间、水解降解速率、反应速率常数、交联密度和储能模量相关。通过改变交联剂的性能和结构,获得了降解时间从10小时到22天不等的可控降解水凝胶。还确定了水凝胶的凝胶化时间与降解时间密切相关。通过对二硫醇交联剂化学结构和物理性质的广泛表征,我们确定了两组条件,分别产生快速凝胶化、快速降解的水凝胶和缓慢凝胶化、缓慢降解的水凝胶。独特的是,水凝胶的储能模量可以由二硫醇交联剂的化学特性控制,而与水凝胶的降解时间或网孔大小无关。
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