Podevyn Annelore, Van Vlierberghe Sandra, Dubruel Peter, Hoogenboom Richard
Supramolecular Chemistry Group, Centre of Macromolecular Chemistry (CMaC), Department of Organic and Macromolecular Chemistry, Ghent University, Krijgslaan 281, 9000 Ghent, Belgium.
Polymer Chemistry and Biomaterials Group (PBM), Centre of Macromolecular Chemistry (CMaC), Department of Organic and Macromolecular Chemistry, Ghent University, Krijgslaan 281, 9000 Ghent, Belgium.
Gels. 2022 Jan 18;8(2):64. doi: 10.3390/gels8020064.
The combination of natural and synthetic polymers to form hybrid hydrogels offers the potential of fabricating new materials that possess a combination of properties resulting from both types of polymer classes. Within this work, two alkene-functionalized poly(2-alkyl/aryl-2-oxazoline) (PAOx) copolymers and one gelatin derivative, thiolated gelatin (gel-SH), are synthesized as precursors for hybrid hydrogels through a photo-induced radical thiol-ene crosslinking process. In-situ photo-rheology revealed an increased mechanical stability for hydrogels that possess an excess amount of PAOx precursor. A final qualitative investigation of the thermo-responsive properties of a P(EtOx-norbornenOx):gel-SH (2:1) hydrogel film revealed a cloud point temperature (T) in the same range as the T of the P(EtOx-norbornenOx) polymer precursor, which is around 30 °C. This promising result demonstrates that thermo-responsive hybrid poly(2-oxazoline)-gelatin hydrogels could be prepared with predictable Ts and that further investigation into this appealing feature might be of interest. Ultimately, this work shows a proof-of-concept of using PAOx as potential hybrid hydrogel precursor in combination with cell-interactive gelatin derivatives to potentially improve the mechanical stability of the final scaffolds and introduce additional features such as thermo-responsiveness for the purpose of drug delivery.
天然聚合物与合成聚合物相结合形成杂化水凝胶，为制造具有两类聚合物特性组合的新材料提供了可能。在这项工作中，通过光引发自由基硫醇-烯交联过程，合成了两种烯烃功能化的聚（2-烷基/芳基-2-恶唑啉）（PAOx）共聚物和一种明胶衍生物——硫醇化明胶（gel-SH），作为杂化水凝胶的前体。原位光流变学表明，对于含有过量PAOx前体的水凝胶，其机械稳定性有所提高。对P（EtOx-降冰片烯氧化物）：gel-SH（2:1）水凝胶薄膜的热响应特性进行的最终定性研究表明，其浊点温度（T）与P（EtOx-降冰片烯氧化物）聚合物前体的T在相同范围内，约为30℃。这一有前景的结果表明，可以制备出具有可预测浊点温度的热响应性杂化聚（2-恶唑啉）-明胶水凝胶，对这一吸引人的特性进行进一步研究可能会很有意义。最终，这项工作展示了一个概念验证，即使用PAOx作为潜在的杂化水凝胶前体，与细胞相互作用的明胶衍生物相结合，有可能提高最终支架的机械稳定性，并引入诸如热响应性等附加特性，用于药物递送目的。
