高等学校化学学报 ›› 2015, Vol. 36 ›› Issue (3): 568-574.doi: 10.7503/cjcu20140966

• 高分子化学 • 上一篇    下一篇

亲水改性PBS基共聚物的N435酶降解差异性及分子模拟

张敏1(), 张祎1, 李成涛1, 覃家祥1, 高让1, 马晓宁1, 邱建辉2   

  1. 1. 陕西科技大学轻化工助剂化学与技术教育部重点实验室, 西安 710021
    2. 日本秋田县立大学, 秋田 015-0055
  • 收稿日期:2014-10-22 出版日期:2015-03-10 发布日期:2015-01-15
  • 作者简介:联系人简介: 张 敏, 女, 博士, 教授, 博士生导师, 主要从事可生物降解材料的合成、 降解和机理研究. E-mail: yanjiushi206@163.com
  • 基金资助:
    高等学校博士学科点专项基金(批准号: 20126125110001)和国家“八六三”计划项目(批准号: 2011AA100503)资助

N435 Enzymatic Degradation Difference and Molecular Modeling of Hydrophilic Modified PBS-based Copolymer

ZHANG Min1,*(), ZHANG Yi1, LI Chengtao1, QIN Jiaxiang1, Gao Rang2, MA Xiaoning1, QIU Jianhui2   

  1. 1. Key Laboratory of Auxiliary Chemistry & Technology for Chemical Industry, Ministry of Education,Shaanxi University of Science & Technology, Xi’an 710021, China
    2. Akita Prefecture University, Akita 015-0055, Japan
  • Received:2014-10-22 Online:2015-03-10 Published:2015-01-15
  • Contact: ZHANG Min E-mail:yanjiushi206@163.com

摘要:

在水相体系中, 采用脂肪酶Novozym435对聚丁二酸丁二醇酯(PBS)分子主链中氧醚键在醇段和酸段的不同位置的共聚物聚(丁二酸丁二醇-co-丁二酸二甘醇酯)[P(BS-co-BDGA)]和聚(丁二酸丁二醇-co-二甘醇酸丁二醇酯)[P(BS-co-DEGS)]进行酶促降解研究. 以分子对接模拟探讨了酶对亲水性底物的识别及相互作用机制. 通过对降解前后不同摩尔比的共聚物薄膜的质量损失率、 亲水性、 热性能以及降解产物的分析, 研究了PBS改性共聚物的降解规律. 结果表明, 随着降解时间的推移, 所有共聚物薄膜的质量损失率升高, 亲水性增强, 热分解温度升高; 降解5 d后, P(BS-co-BDGA)降解产生的低聚物种类比P(BS-co-DEGS)的多. 分子对接结果表明, 醚键在酸段的P(BS-co-BDGA)型酯键与Novozym435酶活性位点的结合比醚键在醇段的P(BS-co-DEGS)型酯键更稳定, 因此, 在N435脂肪酶作用下, P(BS-co-BDGA)比P(BS-co-DEGS)的降解效果好. 实验结果表明, 当DGA摩尔分数为20%时, 降解效果最佳.

关键词: 聚丁二酸丁二醇酯, 氧醚键, 脂肪酶N435, 酶促降解, 分子对接模拟

Abstract:

By lipase Novozym435, enzymatic degradation of copolymers poly(butylene succinate-diglycolic butanediol)ester[P(BS-co-BDGA)] and poly(butylene succinate-diethylene glycol succinate)ester[P(BS-co-DEGS)] which contain ether oxygen bond at different positions of alcohol binding segment and acid binding segment in the main chain of PBS, was performed in the aqueous system. And molecular docking simulations explore the recognition of enzyme on hydrophilic substrate and the interaction mechanisms. In order to study the degradation law of PBS modified copolymers, the mass loss rate, hydrophilicity and thermal properties of the copolymer films and the degradation products were investigated. The results show that: with the passage of time, mass loss rate of the copolymer films is increased, increasing the hydrophilicity and the thermal decomposition temperature; after degradation for 5 d, oligomeric species of P(BS-co-BDGA) are more than P(BS-co-DEGS). Combined with the results of molecular docking, P(BS-co-BDGA) ester bond of ether bond in an acid binding segment docking with the Novozym435 enzyme active sites is more stable than P(BS-co-DEGS) ester bond of ether bond in an alcohol binding segment, so under the action of the enzyme. The degradation effect of P(BS-co-BDGA) is better than P(BS-co-DEGS); and in the synthesized composition range, when the addition amount of DGA is 20%(molar fraction), degradation effect is best.

Key words: Polybutylene succinate, Oxygen ether bond, Lipase Novozym 435, Enzymatic degradation, Molecular docking simulation

中图分类号: