Synthesis and characterisation of photocurable poly(glycerol sebacate)-co-poly(ethylene glycol) methacrylates
Synthesis and characterisation of photocurable poly(glycerol sebacate)-co-poly(ethylene glycol) methacrylates
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DOI：
10.1016/j.mtadv.2023.100410
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发表时间：
2023-08
影响因子：
10
通讯作者：
Mina Aleemardani;Louis Johnson;M. Trikić;N. Green;F. Claeyssens
中科院分区：
文献类型：
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作者：
Mina Aleemardani;Louis Johnson;M. Trikić;N. Green;F. Claeyssens
聚甘油癸二酸酯-共聚乙二醇共聚物（PGS-co-PEG）具有多功能性和可调性，是一种极具潜力的高性能生物材料。然而，这些材料的应用目前受到恶劣交联条件的限制，包括高温和长反应时间。在本研究中，为了克服这些限制，对PGS-co-PEG进行甲基丙烯酸化处理，得到光固化(PGS-co-PEG)-M共聚物。首次研究了以聚乙二醇（PEG2）或聚乙氧基甘油（PEG3）为原料制备的PGS-co-PEG的甲基丙烯酸化反应。（PGS-co-PEG2）-M和(PGS-co-PEG3)-M具有可生物降解、生物相容性、生物粘附性、ph响应性和光固化性。甲基丙烯酸基化后，多功能特征仍然存在，但它们被彻底改变了。（PGS-co-PEG）-M共聚物的机械强度显著提高。（PGS-co-PEG2）-M样品的拉伸杨氏模量范围为0.08 ~ 0.48 MPa, (PGS-co-PEG3)-M样品的拉伸杨氏模量范围为2.67 ~ 35.47 MPa，表明材料的力学性能可以通过交联密度调节。相比之下，由于甲基丙烯酸基化，生物粘附性能，如lap-shear和粘附强度几乎减少了一半。降解和溶胀率略有降低，但在pH = 5.0, 7.4和9.1时仍观察到pH响应行为。reazurin和PicoGreen®检测细胞代谢活性和双链DNA含量，证明(PGS-co-PEG)-M共聚物具有生物相容性。光固化(PGS-co-PEG)-M共聚物促进了一种简单且用户友好的固化过程（光交联），可用于生物医学应用。此外，这些光固化共聚物直接或间接地有利于各种生物制造方法，包括乳液技术和增材制造。
Poly (glycerol sebacate)-co-poly (ethylene glycol) (PGS-co-PEG) copolymers have multifunctional and tunable properties and great potential as high-performance biomaterials. However, the application of these materials is currently limited by harsh crosslinking conditions that include high temperatures and long reaction times. In this study, in order to overcome these limitations, the methacrylation process was conducted on PGS-co-PEG, resulting in photocurable (PGS-co-PEG)-M copolymers. Methacrylation of PGS-co-PEG, formulated respectively from polyethylene glycol (PEG2) or glycerol ethoxylate (PEG3), was investigated for the first time. (PGS-co-PEG2)-M and (PGS-co-PEG3)-M were found to be biodegradable, biocompatible, bioadhesive, pH-responsive and photocurable. Multifunctional characteristics remained after methacrylation, they were, however, drastically altered. Mechanical strength was enhanced significantly for (PGS-co-PEG)-M copolymers. Tensile Young's moduli of (PGS-co-PEG2)-M samples ranged from 0.08 to 0.48 MPa, while those of (PGS-co-PEG3)-M ranged from 2.67 to 35.47 MPa, indicating the mechanical properties of the materials can be tuned via crosslinking density. In contrast, bioadhesive properties, such as lap-shear and adhesion strengths, were almost halved due to methacrylation. The degradation and swelling rates were slightly reduced, but pH-responsive behaviours at pH = 5.0, 7.4 and 9.1 were still observed. Cell metabolic activity and double-stranded DNA content, investigated by resazurin and PicoGreen® assays, demonstrated that the (PGS-co-PEG)-M copolymers were biocompatible. Photocurable (PGS-co-PEG)-M copolymers facilitate a simple and user-friendly curing process (photocrosslinking) that could be used for biomedical applications. Moreover, these photocurable copolymers are beneficial for various biofabrication methods, including emulsion techniques and additive manufacturing, either directly or indirectly.