Biomaterials and Tissue Engineering Group, Department of Materials Science and Engineering, Kroto Research Institute, The University of Sheffield, Sheffield S3 7HQ, UK.
Insigneo Institute for in Silico Medicine, The Pam Liversidge Building, Sir Robert Hadfield Building, Mappin Street, Sheffield S1 3JD, UK.
Biomater Sci. 2022 Dec 6;10(24):7015-7031. doi: 10.1039/d2bm01335e.
Poly(glycerol sebacate) (PGS), a synthetic biorubber, is characterised by its biocompatibility, high elasticity and tunable mechanical properties; however, its inherent hydrophobicity and insolubility in water make it unsuitable for use in advanced biomaterials like hydrogels fabrication. Here, we developed new hydrophilic PGS-based copolymers that enable hydrogel formation through use of two different types of polyethylene glycol (PEG), polyethylene glycol (PEG2) or glycerol ethoxylate (PEG3), combined at different ratios. A two-step polycondensation reaction was used to produce poly(glycerol sebacate)--polyethylene glycol (PGS--PEG) copolymers that were then crosslinked thermally without the use of initiators or crosslinkers, resulting in PGS--PEG2 and PGS--PEG3 amphiphilic polymers. It has been illustrated that the properties of PGS--PEG copolymers can be controlled by altering the type and amount of PEG. PGS--PEG copolymers containing PEG ≥ 40% showed high swelling, flexibility, stretching, bioadhesion and biocompatibility, and good enzymatic degradation and mechanical properties. Also, the addition of PEG created hydrogels that demonstrated pH-responsive behaviours, which can be used for bioapplications requiring responding to physicochemical dynamics. Interestingly, PGS--40PEG2 and PGS--60PEG3 had the highest shear strengths, 340.4 ± 49.7 kPa and 336.0 ± 35.1 kPa, and these are within the range of commercially available sealants or bioglues. Due to the versatile multifunctionalities of these new copolymer hydrogels, they can have great potential in soft tissue engineering and biomedicine.
聚（癸二酸甘油酯）（PGS）是一种合成的生物橡胶，具有生物相容性、高弹性和可调节的机械性能；然而，其固有疏水性和不溶于水使其不适合用于高级生物材料的制造，如水凝胶的制备。在这里，我们开发了新的亲水性 PGS 基共聚物，通过使用两种不同类型的聚乙二醇（PEG），即聚乙二醇 2（PEG2）或甘油乙氧基化物（PEG3），并以不同的比例组合，使水凝胶的形成成为可能。采用两步缩聚反应制备聚（癸二酸甘油酯）-聚乙二醇（PGS-PEG）共聚物，然后无需引发剂或交联剂即可通过热交联，得到 PGS-PEG2 和 PGS-PEG3 两亲聚合物。已经表明，PGS-PEG 共聚物的性质可以通过改变 PEG 的类型和用量来控制。含有 PEG≥40%的 PGS-PEG 共聚物表现出高的溶胀性、柔韧性、拉伸性、生物黏附性和生物相容性，以及良好的酶降解性和机械性能。此外，PEG 的添加形成了具有 pH 响应行为的水凝胶，可用于需要响应物理化学动力学的生物应用。有趣的是，PGS-40PEG2 和 PGS-60PEG3 具有最高的剪切强度，分别为 340.4±49.7 kPa 和 336.0±35.1 kPa，这在商业上可用的密封剂或生物胶的范围内。由于这些新的共聚物水凝胶具有多功能性，它们在软组织工程和生物医学中有很大的应用潜力。
