Chemoenzymatic platform with coordinated cofactor self-circulation for lignin valorization
摘要
Lignin valorization is vital for achieving economically viable and sustainable lignocellulosic biorefineries. However, the value-added utilization of lignin constituents is hampered by the requirement of expensive cofactors and low conversions. Here, by integrating coenzyme regeneration and cell-free expression, we report an in vitro multienzyme-coordinated expression with cofactor self-circulation (iMECS) strategy to achieve efficient lignin-to-molecule conversion. The iMECS system established a catalytic bridge with high atom economy for converting lignin waste into valuable aromatic compounds. Curcumin, vanillin and raspberry ketone were efficiently synthesized in a coenzyme-free manner, with a conversion of over 90%. We also demonstrated the flexibility of the iMECS platform, through which a wide array of phenylpropanoids could be easily obtained by enzyme swapping and pathway extension. By integrating chemical depolymerization with the iMECS system, lignin-rich agricultural waste was directly converted into valuable chemicals, and the overall catalytic efficiency was enhanced by up to 48-fold compared with the reported titres. This efficient, general platform can facilitate the utilization of lignocellulosic biomass, thereby promoting zero-waste biorefineries for a more sustainable future.