Periodic Reporting for period 1 - ReLay (Enabling Incompatible Tandem Reactions through Spatial Separation of Reaction Layers)
Período documentado: 2022-09-01 hasta 2024-08-31
Today’s technology for the biocatalytic production of base chemicals is fossil-fuel based. Moving away from non-renewable and carbon-based energy feedstocks towards renewable hydrogen is a key challenge for current chemical processes. However, biocatalysis has yet to see H2 implemented as a energy source, simply because such H2-consuming reactions are sensitive to O2, whereas many enzymatic reactions driving product formation require O2 as a cosubstrate. H2-driven biocatalysis is not realized today on a large scale because of this need for both O2-sensitive and O2-dependent reactions to operate in tandem. The goal of this Marie Skłodowska-Curie individual fellowship project is to deliver the theoretical framework and experimental validation for novel biohybrid catalytic microdisks capable of carrying out seemingly incompatible tandem reactions by controlling the spatial separation of reaction layers (ReLay). These actions will create a universal platform for H2-driven biocatalysis, which can be implemented directly in current bioreactors.
Driven by both theory and simulation, the optimal conditions were found to create both anaerobic and aerobic domains allowing O2-sensitive and O2-dependent reactions to take place within a single particle. A reaction-diffusion model and simulation toolbox was built to establish the theoretical framework of spatially separated reaction layers in these catalytic micodisks. Second, the parameter space was explored using the model and simulations to find the best performing components and conditions.
A new methodology for mapping the parameter space and identifying kinetic regimes of a general electrochemical system was developed. By introducing a geometric interpretation of kinetic zone diagrams, it was possible to automate the procedure for constructing zone diagrams using computational techniques. This allows for mapping the kinetic behavior of complex electrochemical systems encompassing chemical reactions coupled to mass transport and locating optimal kinetic regimes within large dimensional parameter spaces.