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Development of Novel Biodegradable Aliphatic Polyesters Prepared by Catalysts Containing Metals

含金属催化剂制备新型可生物降解脂肪族聚酯的开发

基本信息

批准号：
11217211
负责人：
SHIRAHAMA Hiroyuki
金额：
$ 9.98万
依托单位：
Hiroshima University
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research on Priority Areas
财政年份：
1999
资助国家：
日本
起止时间：
1999 至 2002
项目状态：
已结题

项目摘要

Poly (L-1actic acid), namely poly (L-lactide) [poly (L-LA)] has such advantages as good biocompatibility and mechanical properties. However, the major problems of poly (L-LA) are its brittleness and low biodegradability. Therefore, in this work, to improve these disadvantages of poly (L-LA), but keeping its advantages, we have prepared novel biodegradable aliphatic polyesters. The following significant results were obtainedImprovement of biodegradability of poly (L-LA) by introducing depsipetide (DP) units ; The enzymatic degradation of poly (L-LA) was much improved by copolymerizing DP monomer (DPs were synthsized from various amino asids and hydoxy acid derivatives). Furthermore, it was found that the biodegradability was most improved by using DP monmers prepared from L-isomers of amino asids.Improvement of brittleness of poly (L-LA) chains ; The introduction of caprolactone (CL) or its derivative (4-alkylated caprolactone) units into poly (L-LA) chains resulted in a greater improvement of the brittleness of poly (L-LA). And this enabled us to regulate the degradability of copolymers.The above results rendered us to prepare DP/CL/L-LA terpolymers. The terpolymer with composition ratio about 5/20/75 was found to be the best polymer judging by the balance of biodegradability and properties.For many applications of biodegradable polymers, functionalizations of these polymers are very important. We have therefore prepared L-LA copolymers having various **nctinal groups. For example, CL/L-LA copolymers with hydroxy group was found to be highly biodegradable compared with poly (L-LA). Further, we have synthesized the copolymers with multifunctional groups (double bond/epoxy/diol) by transforming the reactive double bond of polymers into these functional groups. Finally, we have succeeded in developing cross-linked hydrogel polymers by chemical modification of these groups.

聚（L-1-乳酸），即聚（L-乳酸）[poly（L-LA）]，具有良好的生物相容性和力学性能。然而，聚（L-LA）的主要问题是它的脆性和低生物降解性。因此，在本工作中，为了改善聚（L-LA）的这些缺点，但保持其优点，我们制备了新型的可生物降解的脂肪族聚酯。结果表明：缩肽（DP）的引入改善了聚L-乳酸的生物降解性; DP单体（DP是由各种氨基酸和羟基酸衍生物合成的）的共聚改善了聚L-乳酸的酶降解性。聚（L-LA）分子链脆性的改善：在聚（L-LA）分子链中引入己内酯（CL）或其衍生物（4-烷基化己内酯）单元，可使聚（L-LA）分子链的脆性得到较大改善。上述结果为制备DP/CL/L-LA三元共聚物提供了依据。通过综合性能和生物降解性的综合评价，确定了组成比为5/20/75左右的聚合物为最佳聚合物。对于生物降解聚合物的许多应用，功能化是非常重要的。因此，我们制备了具有各种 **nctinal基团的L-LA共聚物。例如，与聚（L-LA）相比，具有羟基的CL/L-LA共聚物被发现是高度可生物降解的。此外，我们还通过将聚合物的反应性双键转化为多官能团（双键/环氧/二醇），合成了具有这些官能团的共聚物。最后，我们已经成功地开发了交联的水凝胶聚合物通过化学修饰这些基团。