Understanding Benefits and Trade-offs in Coupling Cathodic and Anodic Processes in Continuous Electroenzymatic Reaction Cascades

本研究计划介绍了一种将成对电极过程与酶反应级联相结合的方法，使氧化还原-中性过程能够在流动系统中连续进行。总体目标是调查的优势和权衡与耦合还原和氧化过程在不同的配对电极配置。所提出的模型级联包括葡萄糖完全转化为乙醇和二氧化碳，在氧化还原中性和ph中性的系统中使用六种酶。在整个研究过程中，几个关键的研究问题将被解决。这些包括评估电极电位对耦合生物催化过程的影响，研究还原电位对生物电催化速率和选择性的影响，以及制定解决系统内浓度梯度的策略。此外，在反应不理想平衡的情况下，将努力使系统稳定。在成对的生物电催化条件下，所选酶的稳定性和性能也将被彻底检查。此外，该研究将探讨进行连续氧化和裂解反应的利弊，以及同时进行多个氧化反应的优势。拟议的研究将分成不同的工作包，每个工作包针对成对的电-生物催化过程的特定方面。本研究结果对于推进基于耦合反应的高效生物电化学电池的设计具有重要的潜力。这些发现不仅将加深我们对这些系统内复杂相互作用的理解，而且还将为优化酶级联提供有价值的见解，这些酶级联对许多工业过程至关重要。总的来说，这项研究旨在释放成对电-生物催化过程的全部潜力，为可持续和环境友好的技术应用开辟新的途径。

This research proposal introduces an approach that integrates paired electrode processes with enzymatic reaction cascades, enabling redox-neutral processes to be carried out continuously in a flow system. The overarching objective is to investigate the advantages and trade-offs associated with coupling reductive and oxidative processes in diverse paired electrode configurations. The proposed model cascade involves the complete conversion of glucose into ethanol and carbon dioxide, employing six enzymes in a redox-neutral and pH-neutral system. Throughout the study, several critical research questions will be addressed. These include assessing the influence of electrode potential on coupled biocatalytic processes, studying the effect of reduction potentials on bioelectrocatalytic rate and selectivity, and developing strategies to address concentration gradients within the system. Additionally, efforts will be made to stabilize the system in cases where reactions are not ideally equilibrated. The stability and performance of selected enzymes under paired bioelectrocatalytic conditions will also be thoroughly examined. Furthermore, the investigation will explore the trade-offs and benefits of performing continuous oxidative and lytic reactions, as well as the advantages of conducting multiple oxidative reactions concurrently. The proposed research will be structured into various work packages, each targeting specific aspects of the paired electro-biocatalytic processes. The outcomes of this study hold significant potential for advancing the design of efficient bioelectrochemical cells based on coupled reactions. The findings will not only deepen our understanding of complex interactions within such systems but also offer valuable insights for optimizing enzyme cascades crucial for numerous industrial processes. Overall, this research aims to unlock the full potential of paired electro-biocatalytic processes, opening new avenues for sustainable and environmentally friendly technological applications.