Investigation of the Thermogelation of a Promising Biocompatible ABC Triblock Terpolymer and Its Comparison with Pluronic F127.

Investigation of the Thermogelation of a Promising Biocompatible ABC Triblock Terpolymer and Its Comparison with Pluronic F127.
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DOI:
10.1021/acs.macromol.1c02123
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发表时间:
2022-03-08
期刊:
影响因子:
5.5
通讯作者:
Georgiou, Theoni K.
Georgiou, Theoni K.
中科院分区:
化学1区
文献类型:
--
作者:
Constantinou, Anna P.;Nele, Valeria;Doutch, James J.;Correia, Joana S.;Moiseev, Roman, V;Cihova, Martina;Gaboriau, David C. A.;Krell, Jonathan;Khutoryanskiy, Vitaliy V.;Stevens, Molly M.;Georgiou, Theoni K.

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具有适当结构的热敏聚合物在温度变化时形成物理网络,在配方科学、组织工程和药物输送方面具有实用价值。在这里,我们报告了一种具有成本效益的生物兼容替代品,即OEGMA30015-b-BuMA26-b-DEGMA13,它在低浓度(低至2%w/w)下形成凝胶;OEGMA300、Buma和DEGMA分别代表低聚(乙二醇甲基醚)甲基丙烯酸酯(MM=300gmol-1)、甲基丙烯酸丁酯和甲基丙烯酸二乙二醇甲醚。对这种聚合物进行了深入的研究,并与其商业上可用的同类产品泊洛沙姆P407(Pluronic F127)进行了比较。为了阐明它们宏观凝胶行为的差异,我们用小角中子散射的方法研究了它们在纳米尺度上的自组装,同时记录了它们的流变性。揭示了两种不同的凝胶化机理。三嵌段共聚物固有地形成拉长的胶束,胶束的长度随着温度的增加而增加,形成蠕虫状的胶束,从而促进凝胶。相比之下,Pluronic F127的S胶束化是温度驱动的,其胶凝作用归因于胶束的紧密堆积。通过低温扫描和透射电子显微镜对凝胶结构进行了分析。对房内注射的体外凝胶研究表明,它在改善药物在眼内滞留方面具有很好的应用潜力。
Thermoresponsive polymers with the appropriate structure form physical networks upon changes in temperature, and they find utility in formulation science, tissue engineering, and drug delivery. Here, we report a cost-effective biocompatible alternative, namely OEGMA30015-b-BuMA26-b-DEGMA13, which forms gels at low concentrations (as low as 2% w/w); OEGMA300, BuMA, and DEGMA stand for oligo(ethylene glycol) methyl ether methacrylate (MM = 300 g mol–1), n-butyl methacrylate, and di(ethylene glycol) methyl ether methacrylate, respectively. This polymer is investigated in depth and is compared to its commercially available counterpart, Poloxamer P407 (Pluronic F127). To elucidate the differences in their macroscale gelling behavior, we investigate their nanoscale self-assembly by means of small-angle neutron scattering and simultaneously recording their rheological properties. Two different gelation mechanisms are revealed. The triblock copolymer inherently forms elongated micelles, whose length increases by temperature to form worm-like micelles, thus promoting gelation. In contrast, Pluronic F127’s micellization is temperature-driven, and its gelation is attributed to the close packing of the micelles. The gel structure is analyzed through cryogenic scanning and transmission electron microscopy. Ex vivo gelation study upon intracameral injections demonstrates excellent potential for its application to improve drug residence in the eye.
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