One-pot chemobiological cascade strategy for synthesizing furyl hydroxymethyl ketone from corncob

Abstract

Furyl hydroxymethyl ketone (FHK) is essential in synthesizing pharmaceuticals and biologically active molecules. However, green and sustainable methods for synthesizing FHK from renewable feedstocks remain challenging. This research proposed a simple one-pot chemobiocatalytic cascade strategy for effectually transforming renewable biomass into FHK via solid acid catalysis and whole-cells hydroxymethylation. Using whole-cells (SMPDC cells) containing pyruvate decarboxylase and small ubiquitin-like modifier (SUMO) fusion tag as biocatalysts, non-natural substrates furfural and formaldehyde were introduced into a C-C ligation bioreaction, establishing a biocatalytic pathway for FHK synthesis. SMPDC cells exhibited excellent biocatalytic activity and high tolerance to high furfural concentrations (up to 200 mM), a well-known effective microbial inhibitor. Optimal reaction conditions were identified, enabling the manufacturing of FHK from corncob- and D-xylose-derived furfural with productivities of 0.12 g FHK/(1 g corncob + 0.09 g HCHO) and 0.39 g FHK/(1 g D-xylose + 0.28 g HCHO), respectively. This strategy demonstrated the potential for synthesizing valuable chemicals from low-cost biomass, providing a sustainable alternative to traditional chemical synthesis.