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南极假丝酵母脂肪酶和猪胰脂肪酶对源自碳酸三亚甲基酯和乙交酯的可生物降解聚合物的酶催化降解作用

Enzyme-catalyzed degradation of biodegradable polymers derived from trimethylene carbonate and glycolide by lipases from Candida antarctica and Hog pancreas.

作者信息

Liu Feng, Yang Jian, Fan Zhongyong, Li Suming, Kasperczyk Janusz, Dobrzynski Piotr

机构信息

a Department of Materials Science , Fudan University , Shanghai , 200433 , China.

出版信息

J Biomater Sci Polym Ed. 2012;23(10):1355-68. doi: 10.1163/092050611X581525. Epub 2012 May 8.

DOI:10.1163/092050611X581525
PMID:21722422
Abstract

Enzyme-catalyzed degradation of poly(trimethylene carbonate) homo-polymer (PTMC) and poly(trimethylene carbonate-co-glycolide) co-polymer (PTGA) was investigated in the presence of lipases from Candida antarctica and Hog pancreas. Degradation was monitored by gravimetry, size-exclusion chromatography (SEC), nuclear magnetic resonance (NMR), tensiometry and environmental scanning electron microscopy (ESEM). PTMC can be rapidly degraded by Candida antarctica lipase with 98% mass loss after 9 days, while degradation by Hog pancreas lipase leads to 27% mass loss. Introduction of 16% glycolide units in PTMC chains strongly affects the enzymatic degradation. Hog pancreas lipase becomes more effective to PTGA co-polymer with a mass loss of 58% after 9 days, while Candida antarctica lipase seems not able to degrade PTGA. Bimodal molecular weight distributions are observed during enzymatic degradation of both PTMC and PTGA, which can be assigned to the fact that the surface is largely degraded while the internal part remains intact. The composition of the PTGA co-polymer remains constant, and ESEM shows that the polymers are homogeneously eroded during enzymatic degradation. Contact angle measurements confirm the enzymatic degradation mechanism, i.e., enzyme adsorption on the polymer surface followed by enzyme-catalyzed chain cleavage.

摘要

在南极假丝酵母脂肪酶和猪胰脂肪酶存在的情况下,研究了聚碳酸三亚甲基酯均聚物(PTMC)和聚碳酸三亚甲基酯-乙交酯共聚物(PTGA)的酶催化降解。通过重量法、尺寸排阻色谱法(SEC)、核磁共振(NMR)、张力测定法和环境扫描电子显微镜(ESEM)监测降解过程。PTMC可被南极假丝酵母脂肪酶快速降解,9天后质量损失98%,而猪胰脂肪酶降解导致质量损失27%。在PTMC链中引入16%的乙交酯单元会强烈影响酶促降解。猪胰脂肪酶对PTGA共聚物的降解更有效,9天后质量损失58%,而南极假丝酵母脂肪酶似乎无法降解PTGA。在PTMC和PTGA的酶促降解过程中均观察到双峰分子量分布,这可以归因于表面大量降解而内部部分保持完整的事实。PTGA共聚物的组成保持不变,ESEM表明聚合物在酶促降解过程中均匀侵蚀。接触角测量证实了酶促降解机制,即酶吸附在聚合物表面,随后发生酶催化的链断裂。

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