Strengthening of hydrogels made from enantiomeric block copolymers of polylactide (PLA) and poly(ethylene glycol) (PEG) by the chain extending Diels-Alder reaction at the hydrophilic PEG terminals
Strengthening of hydrogels made from enantiomeric block copolymers of polylactide (PLA) and poly(ethylene glycol) (PEG) by the chain extending Diels-Alder reaction at the hydrophilic PEG terminals
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DOI：
10.1016/j.polymer.2015.04.026
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发表时间：
2015-06-12
期刊：
影响因子：
4.6
通讯作者：
Kimura, Yoshiharu
中科院分区：
文献类型：
--
作者：
Hsu, Yu-I;Masutani, Kazunari;Kimura, Yoshiharu
使用部分呋喃基化的PEG作为大分子引发剂，通过L-和D-丙交酯的ROP容易地合成具有不同组成的F-PEG-PLA的呋喃（F）封端的AB二嵌段共聚物和PLA-PEG-PLA的阿坝三嵌段共聚物（PEG：聚（环氧乙烷），PEA：聚（L-丙交酯）（PLLA）或聚（D-丙交酯）（PDLA），取决于对映体嵌段链）的混合物。在偶联剂1，8-二（马来酰亚胺基）二甘醇（BMG）存在和不存在下制备了对映体共聚物混合物（F-PEG-PDLA/PDLA-PEG-PDLA + F-PEG-PLLA/PLLA-PEG-PLLA）的混合胶束溶液。无BMG和添加BMG的混合胶束溶液都经历了溶胶-凝胶转变，并且其中发现添加BMG的胶束溶液的凝胶强度变得更高，达到11 kPa的水平。这些水凝胶系统被认为是控制的双重交联机制的凝胶形成：立体复合物的形成之间的对映异构体的PLA块和Diels-Alder耦合的PEG块上的呋喃基末端与BMG。这些溶胶-凝胶系统产生的强化凝胶是通用的，可用作组织工程中的可注射支架。(C)2015爱思唯尔有限公司版权所有。
Mixtures of furan (F)-terminated AB diblock copolymer of F-PEG-PLA and ABA triblock copolymer of PLA-PEG-PLA (PEG: poly(oxyethylene), PEA: poly(L-lactide) (PLLA) or poly(D-lactide) (PDLA) depending on the enantiomeric block chain) having different compositions were readily synthesized by ROP of L- and D-lactides using partially furanylated PEGs as the macro initiators. Mixed micelle solutions of the enantiomeric copolymer mixtures (F-PEG-PDLA/PDLA-PEG-PDLA + F-PEG-PLLA/PLLA-PEG-PLLA) were prepared in the presence and absence of a coupling agent 1,8-bis(maleimido)diethylene glycol (BMG). Both the BMG-free and BMG-added mixed micelle solutions underwent sol gel transition, and in which the gel strength was found to become much higher in the BMG-added micelle solutions, reaching a level of 11 kPa. These hydrogel systems were thought to be controlled by the dual cross-linking mechanisms for the gel formation: stereocomplex formation between the enantiomeric PLA blocks and Diels-Alder coupling of the furanyl terminals on PEG blocks with BMG. These sol gel systems producing strengthened gels are versatile for use as injectable scaffolds in the tissue engineering. (C) 2015 Elsevier Ltd. All rights reserved.