Brewer Kyle, Gundsambuu Batjargal, Facal Marina Paula, Barry Simon C, Blencowe Anton
Applied Chemistry and Translational Biomaterials (ACTB) Group, School of Pharmacy and Medical Sciences, University of South Australia, Adelaide, South Australia 5000, Australia.
Cooperative Research Centre for Cell Therapy Manufacturing, University of South Australia, Adelaide, South Australia 5000, Australia.
Polymers (Basel). 2020 Feb 7;12(2):367. doi: 10.3390/polym12020367.
Injectable, thermoresponsive hydrogels are promising candidates for the delivery, maintenance and controlled release of adoptive cell therapies. Therefore, there is significant interest in the development of cytocompatible and biodegradable thermoresponsive hydrogels with appropriate gelling characteristics. Towards this end, a series of thermoresponsive copolymers consisting of poly(caprolactone) (PCL), poly(ethylene glycol) (PEG) and poly(propylene glycol) (PPG) segments, with various PEG:PPG ratios, were synthesised via ring-opening polymerisation (ROP) of ε-caprolactone and epoxy-functionalised PEG and PPG derivatives. The resultant PCL-PEG-PPG copolymers were characterised via proton nuclear magnetic resonance (1H NMR) spectroscopy, gel permeation chromatography (GPC) and differential scanning calorimetry (DSC). The thermoresponsive characteristics of the aqueous copolymer solutions at various concentrations was investigated using the inversion method. Whilst all of the copolymers displayed thermoresponsive properties, the copolymer with a ratio of 1:2 PEG:PPG exhibited an appropriate sol-gel transition (28 °C) at a relatively low concentration (10 wt%), and remained a gel at 37 °C. Furthermore, the copolymers were shown to be enzymatically degradable in the presence of lipases and could be used for the encapsulation of CD4+ T-cell lymphocytes. These results demonstrate that the thermoresponsive PCL-PEG-PPG hydrogels may be suitable for use as an adoptive cell therapy (ACT) delivery vehicle.
可注射的热响应水凝胶是过继性细胞疗法的递送、维持和控释的有前景的候选材料。因此，开发具有适当凝胶化特性的细胞相容性和可生物降解的热响应水凝胶引起了极大的兴趣。为此，通过ε-己内酯与环氧官能化的聚乙二醇（PEG）和聚丙二醇（PPG）衍生物的开环聚合（ROP），合成了一系列由聚己内酯（PCL）、聚乙二醇（PEG）和聚丙二醇（PPG）链段组成的、具有不同PEG:PPG比例的热响应共聚物。通过质子核磁共振（1H NMR）光谱、凝胶渗透色谱（GPC）和差示扫描量热法（DSC）对所得的PCL-PEG-PPG共聚物进行了表征。使用倒置法研究了不同浓度的共聚物水溶液的热响应特性。虽然所有共聚物都表现出热响应特性，但PEG:PPG比例为1:2的共聚物在相对较低的浓度（10 wt%）下表现出合适的溶胶-凝胶转变温度（28 °C），并在37 °C时保持为凝胶状态。此外，这些共聚物在脂肪酶存在下可被酶解，并且可用于封装CD4+ T淋巴细胞。这些结果表明，热响应性PCL-PEG-PPG水凝胶可能适合用作过继性细胞疗法（ACT）的递送载体。
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