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通过调控聚乳酸-乙醇酸共聚物-聚乙二醇-聚乳酸-乙醇酸共聚物(PLGA-PEG-PLGA)水凝胶的聚乳酸-乙醇酸共聚物(PLGA)单体序列来调节其热响应特性。

Modulating the Thermoresponsive Characteristics of PLGA-PEG-PLGA Hydrogels via Manipulation of PLGA Monomer Sequences.

作者信息

Jo SeongHoon, Roh Soonjong, Shim Jaemin, Yu Ji Woong, Jung Youngmee, Jang Woo Young, Seo Bumjoon, Won You-Yeon, Yoo Jin

机构信息

Center of Biomaterials, Biomedical Research Institute, Korea Institute of Science and Technology (KIST), Seoul 02792, Republic of Korea.

Department of Applied Bioengineering, Graduate School of Convergence Science and Technology, Seoul National University, Seoul 08826, Republic of Korea.

出版信息

Biomacromolecules. 2024 Aug 12;25(8):5374-5386. doi: 10.1021/acs.biomac.4c00817. Epub 2024 Jul 16.

Abstract

Hydrogels are promising materials for biomedical applications, particularly in drug delivery and tissue engineering. This study highlights thermoresponsive hydrogels, specifically poly(lactic--glycolic acid) (PLGA)-poly(ethylene glycol) (PEG)-PLGA triblock copolymers, and introduces a feed rate-controlled polymerization (FRCP) method. By utilizing an organic catalyst and regulating the monomer feed rate, the sequence distribution of PLGA within the triblock copolymer is controlled. Various analyses, including C NMR and rheological measurements, were conducted to investigate the impact of sequence distribution. Results show that altering sequence distribution significantly influences the sol-gel transition, hydrophobicity-hydrophilicity balance, and drug release profile. Increased sequence uniformity lowers the glass transition temperature, raises the sol-gel transition temperature due to enhanced hydrophilicity, and promotes a more uniform drug (curcumin) distribution within the PLGA domain, resulting in a slower release rate. This study emphasizes the importance of PLGA sequence distribution in biomedical applications and the potential of FRCP to tailor thermoresponsive hydrogels for biomedical advancements.

摘要

水凝胶是生物医学应用中很有前景的材料,尤其是在药物递送和组织工程领域。本研究重点关注热响应性水凝胶,特别是聚(乳酸-乙醇酸)(PLGA)-聚(乙二醇)(PEG)-PLGA三嵌段共聚物,并介绍了一种进料速率控制聚合(FRCP)方法。通过使用有机催化剂并调节单体进料速率,可控制三嵌段共聚物中PLGA的序列分布。进行了各种分析,包括碳核磁共振(C NMR)和流变学测量,以研究序列分布的影响。结果表明,改变序列分布会显著影响溶胶-凝胶转变、疏水性-亲水性平衡和药物释放曲线。序列均匀性的提高会降低玻璃化转变温度,由于亲水性增强而提高溶胶-凝胶转变温度,并促进药物(姜黄素)在PLGA域内更均匀地分布,从而导致释放速率减慢。本研究强调了PLGA序列分布在生物医学应用中的重要性以及FRCP为生物医学进步定制热响应性水凝胶的潜力。

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