Upgrading glycerol to sorbose via a tandem photoelectrocatalysis–enzyme catalysis relay
摘要
The selective conversion of glycerol, an abundant biomass-derived platform chemical, into longer carbon chain, high-value compounds is appealing but highly challenging. Conventional oxidation processes are prone to C–C bond cleavage, resulting in the inefficient utilization of the glycerol three-carbon backbone. Here we report a spatially decoupled photoelectrocatalytic–biocatalytic relay system that is able to efficiently upgrade glycerol to sorbose, an important six-carbon sugar used in the food, pharmaceutical and cosmetic industries. This system uses a WO3–Bi photoanode to selectively oxidize glycerol into two distinct three-carbon products: glyceraldehyde and dihydroxyacetone. Subsequently, these two three-carbon products are coupled via an aldol addition reaction, driven by a mutant fructose-6-phosphate aldolase catalyst. Continuous tandem operation enables the highly selective conversion of glycerol into a single six-carbon product, sorbose. Furthermore, coupling the WO3–Bi photoanode with an Si photocathode followed by enzyme catalysis relay achieves a sorbose yield of 31.66 mmol genzyme−1 h−1 under solar light irradiation without the need of external energy input. This work presents a sustainable platform for upgrading biomass-derived glycerol into valuable six-carbon chemicals under mild conditions, providing a green and efficient route for biomass valorization.