Polymer Architecture Effects on Poly(N,N-Diethyl Acrylamide)-b-Poly(Ethylene Glycol)-b-Poly(N,N-Diethyl Acrylamide) Thermoreversible Gels and Their Evaluation as a Healthcare Material.

Polymer Architecture Effects on Poly(N,N-Diethyl Acrylamide)-b-Poly(Ethylene Glycol)-b-Poly(N,N-Diethyl Acrylamide) Thermoreversible Gels and Their Evaluation as a Healthcare Material.
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聚合物结构对聚(N,N-二乙基丙烯酰胺)-b-聚(乙二醇)-b-聚(N,N-二乙基丙烯酰胺)热可逆凝胶的影响及其作为保健材料的评估。

DOI:
10.1002/mabi.202100432
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发表时间:
2022
影响因子:
4.6
通讯作者:
Haddow PJ
Haddow PJ
中科院分区:
工程技术3区
文献类型:
--
作者:
Haddow PJ

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热可逆凝胶在加热时在液体状和固体状状态之间转变,使重要的新型医疗保健技术成为可能。聚(N,N-二乙基丙烯酰胺)(PDEA)是一种温敏聚合物,可用作形成热可逆凝胶的触发剂,但其在这些材料中的应用有限,关键的设计原理尚不清楚。本文合成了具有结构PDEA-B-聚(乙二醇)(PEG)-B-PDEA的阿坝共聚物,以得到具有不同分子量的PDEA和PEG嵌段的四种嵌段共聚物。对嵌段共聚物溶液的流变测定表明,需要高分子量PEG嵌段来形成具有主要固体状行为的热可逆凝胶。此外,小角X射线散射阐明了共聚物库的纳米结构的明显差异,这可能与不同的流变行为有关。通过优化聚合物浓度和离子强度,设计了基于PDEA(20 kDa)-B-PEG(10 kDa)-B-PDEA(20 kDa)的热可逆凝胶制剂。发现该凝胶具有粘膜粘附性、稳定性和无毒性,并可控制疏水性药物的释放。总体而言,本研究提供了深入了解聚合物结构对PDEA-B-PEG-B-PDEA的纳米结构和流变学的影响,并提出了一种高功能性热可逆凝胶的开发,具有很高的医疗保健应用前景。
Thermoreversible gels which transition between liquid‐like and solid‐like states when warmed have enabled significant novel healthcare technologies. Poly(N,N‐diethyl acrylamide) (PDEA) is a thermoresponsive polymer which can be used as a trigger to form thermoreversible gels, however its use in these materials is limited and crucial design principles are unknown. Herein ABA copolymers with the structure PDEA‐b‐poly(ethylene glycol) (PEG)‐b‐PDEA are synthesized to give four block copolymers with varied molecular weight of PDEA and PEG blocks. Rheometry on solutions of the block copolymers reveals that high molecular weight PEG blocks are required to form thermoreversible gels with predominantly solid‐like behavior. Furthermore, small‐angle X‐ray scattering elucidates clear differences in the nanostructure of the copolymer library which can be linked to distinct rheological behaviors. A thermoreversible gel formulation based on PDEA (20 kDa)‐b‐PEG (10 kDa)‐b‐PDEA (20 kDa) is designed by optimizing the polymer concentration and ionic strength. It is found that the gel is mucoadhesive, stable, and non‐toxic, as well as giving controlled release of a hydrophobic drug. Overall, this study provides insight into the effect of polymer architecture on the nanostructure and rheology of PDEA‐b‐PEG‐b‐PDEA and presents the development of a highly functional thermoreversible gel with high promise for healthcare applications.