Siritanaratkul Bhavin
Stephenson Institute for Renewable Energy and the Department of Chemistry University of Liverpool, Liverpool, L69 7ZF, UK.
Phys Chem Chem Phys. 2023 Mar 29;25(13):9357-9363. doi: 10.1039/d3cp00540b.
The study of enzymes by direct electrochemistry has been extended to enzyme cascades, with a key development being the 'electrochemical leaf': an electroactive enzyme is immobilized within a porous electrode, providing cofactor (NADP(H)) regeneration for a co-immobilized downstream enzyme. This system has been further developed to include multiple downstream enzymes, and it has become an important tool in biocatalysis, however, the local environment within the porous electrode has not been investigated in detail. Here, we constructed a 1D reaction-diffusion model, comprising the porous electrode with 2 kinds of enzymes immobilized, and an enzyme-free electrolyte diffusion layer. The modelling results show that the rate of the downstream enzyme is a key parameter, and that substrate transport within the porous electrode is not a main limiting factor. The insights obtained from this model can guide future rational design and improvement of these electrodes and immobilized enzyme cascade systems.
通过直接电化学对酶的研究已扩展到酶级联反应，其中一个关键进展是“电化学叶”：一种电活性酶固定在多孔电极内，为共固定的下游酶提供辅因子（NADP(H)）再生。该系统已进一步发展为包含多种下游酶，并且已成为生物催化中的重要工具，然而，多孔电极内的局部环境尚未得到详细研究。在此，我们构建了一个一维反应扩散模型，该模型包括固定有两种酶的多孔电极以及无酶电解质扩散层。建模结果表明，下游酶的速率是一个关键参数，并且多孔电极内的底物传输不是主要限制因素。从该模型获得的见解可以指导未来对这些电极和固定化酶级联系统的合理设计和改进。
