The ability to synthesize chemical products from renewable feedstocks is key component of a sustainable chemical production. Here, we describe our efforts combine microbial bio-oxidation with organocatalytic upgrading in a single flask to convert aliphatic alcohols to industrially relevant α,β-unsaturated aldehyde products in aqueous buffer at 28°C. This hybrid one-pot process works with a range of C<sub>2</sub>−C<sub>6</sub> alcohol substrates and yields homodimers and crossed aldol products. We demonstrate that the inclusion of an organocatalyst intercepts microbially produced aldehyde and redirects flux to the target aldol condensation product. Finally, we show that this methodology is readily merged with enzymatic biocatalytic oxidation and yeast whole-cell biocatalysis. Taken together, our work reveals a new strategy to expand the scope of products from biosynthetic processes.

Combining chemical catalysis and microbial biocatalysis in one-flask systems for sustainable chemical production

ACS Spring 2022

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