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Characterisation and kinetic modelling of a novel convergent enzymatic cascade for epsilon-caprolactone synthesis employing a double-smart cosubstrate with in situ polymerisation

采用双智能共底物原位聚合合成ε-己内酯的新型聚合酶级联的表征和动力学建模

基本信息

批准号：
288779125
负责人：
Professorin Dr.-Ing. Selin Kara
金额：
--
依托单位：
Institut für Technische Chemie
依托单位国家：
德国
项目类别：
Research Grants
财政年份：
2015
资助国家：
德国
起止时间：
2014-12-31 至 2019-12-31
项目状态：
已结题

来源：
https://gepris.dfg.de/gepris/projekt/288779125?language=en
关键词：
Characterisation kinetic modelling novel convergent

项目摘要

Biocatalytic synthesis of epsilon-caprolactone (ECL) and oligomers/polymers thereof is of high interest owing to important advantages compared to chemical approach concerning resource efficiency, selectivity, environment and safety. A novel redox-neutral convergent cascade for the synthesis of ECL in a bi-enzymatic system consisting of an alcohol dehydrogenase (ADH) and a Baeyer-Villiger monooxygenase (BVMO) has been recently introduced. One of the main limitations identified in the preliminary studies was the product inhibition and enzyme deactivation owing to ECL accumulation, and hence its removal from the reaction medium becomes necessary. The research project aims at the development of a rational approach for highly productive synthesis of ECL in convergent BVMO-ADH cascade system coupled with an effective in situ Ring-Opening-Polymerisation (ROP) of ECL for enhancing enzymatic performances. At the same time, oligomer/polymer products will be synthesised and hence the waste generated by separation and purification steps will be reduced. To achieve these goals, key reaction parameters, kinetic and thermodynamic effects influencing the productivity in the synthesis of ECL and its oligomer/polymer products will be systematically described and quantitatively evaluated. The development of a reliable model describing the kinetics of the system is required for the effective design of the multi-enzymatic cascade. Overall, the proposed approach has not been investigated yet and it represents a unique approach, which possess an absolutely considerable potential for future development studies. The research presented here will establish a highly efficient and environmentally benign synthesis of ECL and polymers/oligomers thereof, which will alleviate the severe drawbacks observed in the current chemical approach.

ε-己内酯（ECL）及其低聚物/聚合物的生物催化合成由于与化学方法相比在资源效率、选择性、环境和安全性方面的重要优点而受到高度关注。最近介绍了一种新的氧化还原中性收敛级联反应，用于在由醇脱氢酶（ADH）和Baeyer-Villiger单加氧酶（BVMO）组成的双酶系统中合成ECL。在初步研究中确定的主要限制之一是由于ECL积累导致的产物抑制和酶失活，因此必须将其从反应介质中去除。该研究项目旨在开发一种合理的方法，用于在收敛的BVMO-ADH级联系统中高效合成ECL，并结合ECL的有效原位开环聚合（ROP）以提高酶的性能。同时，将合成低聚物/聚合物产品，因此将减少分离和纯化步骤产生的废物。为了实现这些目标，关键的反应参数，动力学和热力学影响的ECL及其低聚物/聚合物产品的合成生产率将系统地描述和定量评估。一个可靠的模型描述的动力学系统的发展是必要的多酶级联的有效设计。总的来说，所提出的方法还没有被调查，它代表了一种独特的方法，具有绝对相当大的潜力，为未来的发展研究。本文提出的研究将建立ECL及其聚合物/低聚物的高效和环境友好的合成，这将减轻在当前化学方法中观察到的严重缺点。