不同反应体系合成明胶甲基丙烯酰基 (GelMA) 的结构与性质,Biomacromolecules

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不同反应体系合成明胶甲基丙烯酰基 (GelMA) 的结构与性质
Biomacromolecules ( IF 5.5 ) Pub Date : 2023-05-22 , DOI: 10.1021/acs.biomac.3c00302
Shangsi Chen ₁ , Yue Wang ₁ , Jiahui Lai ₁ , Shenglong Tan _{2,

3} , Min Wang ₁

Affiliation

明胶甲基丙烯酰 (GelMA) 水凝胶由于其良好的生物相容性、生物降解性和可控的光固化效率，已广泛用于药物输送和组织工程应用。磷酸盐缓冲溶液 (PBS) 是 GelMA 合成中使用最广泛的反应体系。然而，碳酸盐-碳酸氢盐缓冲溶液 (CBS) 由于其高反应效率，最近已尝试用于合成 GelMA。然而，对于分别在 PBS 和 CBS 中合成的 GelMA 的结构和性质可能存在的差异，缺乏系统的研究。因此，在目前的研究中，分别在 PBS 和 CBS 反应系统下，在可比较的条件下合成了具有两个甲基丙烯酰化度（~20 和~80%）的 GelMA 分子。结果表明，由于明胶链中甲基丙烯酸酯基团的功能化，可能会干扰链内和链间的相互作用，例如氢键，因此在 PBS 中合成的 GelMA 分子具有不同的物理结构，并且与在 PBS 中制备的 GelMA 分子相比表现出不同的性质。哥伦比亚广播公司。在 PBS 中合成的 GelMA 水凝胶表现出更高的凝胶-溶胶转变温度和更好的光固化效率、机械强度和生物特性。相比之下，在 CBS 中生产的 GelMA 水凝胶在溶胀性能和微观结构（例如孔径和孔隙率）方面表现出优势。此外，在 PBS 中合成并具有高度甲基丙烯酰化（“GelMA-PH”聚合物）的 GelMA 显示出三维 (3D) 生物打印的巨大潜力。

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Structure and Properties of Gelatin Methacryloyl (GelMA) Synthesized in Different Reaction Systems

Gelatin methacryloyl (GelMA) hydrogels have been extensively used for drug delivery and tissue engineering applications due to their good biocompatibility, biodegradability, and controllable photocurable efficiency. Phosphate buffer solution (PBS) is the most widely used reaction system for GelMA synthesis. However, carbonate–bicarbonate buffer solution (CBS) has been tried recently for synthesizing GelMA due to its high reaction efficiency. However, there is a lack of systematic investigation into possible differences in the structure and properties of GelMA synthesized in PBS and CBS, respectively. Therefore, in the current study, GelMA molecules with two degrees of methacryloylation (∼20 and ∼80%) were synthesized under PBS and CBS reaction systems, respectively, in comparable conditions. The results showed that because of the functionalization of methacrylate groups in gelatin chains, which could interfere with the intrachain and interchain interactions, such as hydrogen bonding, the GelMA molecules synthesized in PBS had distinct physical structures and exhibited different properties in comparison with those produced in CBS. GelMA hydrogels synthesized in PBS exhibited higher gel–sol transition temperatures and better photocurable efficiencies, mechanical strength, and biological properties. In contrast, GelMA hydrogels produced in CBS showed advantages in swelling performance and microstructures, such as pore sizes and porosities. In addition, GelMA synthesized in PBS and possessing a high degree of methacryloylation (the “GelMA-PH” polymer) showed great potential for three-dimensional (3D) bioprinting. This focused study has gained helpful new insights into GelMA and can provide guidance on the application of GelMA in 3D printing and tissue engineering.

更新日期：2023-05-22

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