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首页> 外文期刊>ACS applied materials & interfaces >Hydrogel Patterning by Diffusion through the Matrix and Subsequent Light-Triggered Chemical Immobilization
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Hydrogel Patterning by Diffusion through the Matrix and Subsequent Light-Triggered Chemical Immobilization

机译：通过基质扩散和随后的光触发化学固定形成水凝胶图案

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摘要

A novel approach to hyaluronic acid (HA) hydrogel with a chemical gradient of the matrix-linked bisphosphonate (BP) groups is presented. The method consists of two steps, including initial generation of physical gradient patterns of BPs by diffusion of BP acrylamide reagent into HA matrix carrying thiol groups and subsequent chemical immobilization of the BP groups by UV light-triggered thiolene addition reaction. This gradient hydrogel permits spatial three-dimensional regulation of secondary interactions of different molecules with the polymer matrix. In particular, graded amounts of cytochrome c (cyt c) were reversibly absorbed in the hydrogel, thus enabling the subsequent spatially controlled release of the therapeutic protein. The obtained patterned hydrogel acts also as a unique reactor in which peroxidase-catalyzed oxidation of a substrate is determined by spatial position of the enzyme (cyt c) in the matrix resulting in a range of product concentrations. As an example, matrix template-assisted oxidation of 3,3',5,5'-tetarmethylbenzydine (TMB) in the presence of H2O2 occurs simultaneously at different rates within the gradient hydrogel. Moreover, calcium binding to the gradient HABP hydrogel reflects the pattern of immobilized BP groups eventually leading to the graded biomineralization of the matrix. This approach opens new possibilities for use of hydrogels as dynamic models for biologic three-dimensional structures such as extracellular matrix.
机译：提出了一种新的透明质酸（HA）水凝胶的方法，该方法具有基质连接的双膦酸酯（BP）基团的化学梯度。该方法包括两个步骤，包括通过将BP丙烯酰胺试剂扩散到带有硫醇基团的HA基质中，初步生成BPs的物理梯度图谱，以及随后通过紫外光触发的硫烯加成反应将BP基团化学固定。该梯度水凝胶允许不同分子与聚合物基质的次级相互作用的空间三维调节。尤其是，渐变量的细胞色素c（cyt c）可逆地吸收在水凝胶中，因此可以在空间上释放治疗性蛋白质。所获得的图案化水凝胶还可以充当独特的反应器，其中过氧化物酶催化的底物氧化取决于酶（cyt c）在基质中的空间位置，从而导致一定范围的产物浓度。例如，在H2O2存在下，基质模板辅助的3,3'，5,5'-酒石酸甲基苯丙胺（TMB）氧化在梯度水凝胶中以不同的速率同时发生。而且，钙与梯度HABP水凝胶的结合反映了固定的BP基团的模式，最终导致基质的生物矿化梯度化。这种方法为将水凝胶用作生物三维结构（例如细胞外基质）的动力学模型开辟了新的可能性。

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