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Regioselective O -demethylation of lignin-derived aryl ethers is a key yet challenging step in lignin valorization, governing the efficient conversion of lignin into high-value aromatic chemicals. Here, we report an artificial peroxygenase system that integrates engineered P450BM3 with glucose oxidase (GOx) and a dual-functional small molecule (DFSM) to enable efficient O -demethylation driven by in situ H 2 O 2 generation. This strategy circumvents the dependence on costly NADPH and improves catalytic sustainability and operational robustness. The engineered F87A/T268D/A328F mutant achieved efficient double O -demethylation of syringol with a turnover number (TON) of 583 ± 7, while the F87A/V78A mutant exhibited a 68.2-fold enhancement in catalytic efficiency toward anisole (TON = 341 ± 8) compared to wild-type P450BM3. Precise regulation of oxidative catalysis and H 2 O 2 supply afforded high efficiency, selectivity, and stability. This work establishes a scalable and environmentally benign biocatalytic platform for upgrading lignin-derived aromatic monomers, advancing sustainable biomass utilization.
Zhao et al. (Wed,) studied this question.