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

• Applicant: Professorin Dr.-Ing. Selin Kara
• Subject Area: Biological Process Engineering ; Technical Chemistry
• Term: from 2015 to 2020
• Project identifier: Deutsche Forschungsgemeinschaft (DFG) - Project number 288779125

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.

• DFG Programme: Research Grants
• International Connection: Denmark