Enabling Incompatible Tandem Reactions through Spatial Separation of Reaction Layers

ended

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 Postdoctoral 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). Driven by both theory and simulation, the optimal conditions will be found to create both anaerobic and aerobic domains allowing O2-sensitive and O2-dependent reactions to take place within a single particle. This will be accomplished by, first, building a reaction-diffusion model and simulation toolbox to establish the theoretical framework of spatially separated reaction layers in these catalytic micodisks. Second, the parameter space will be explored using the model and simulations to find the best performing components and conditions. Finally, these predictions will be validated with an experimental case-study, comparing the expected output from the model with the actual reaction rates and concentrations gradients measured experimentally for an O2-dependent oxyfunctionalization driven by H2 within the catalytic microdisks. These actions will create a universal platform for H2-driven biocatalysis, which can be implemented directly in current bioreactors.