A H2O2 generation-detection-regulation integrated platform for boosting the efficiency of peroxygenase-catalysed C-H oxidative hydroxylation.

The peroxygenases are ideal biocatalysts for the selective oxyfunctionalisation of stable C-H bonds. However, the catalytic efficiency of this approach is limited due to enzyme lability toward oxidant H₂O₂. Although the reported in-situ H₂O₂ generation system enables the stable biocatalytic process without deactivating the enzyme, the greatest catalytic potential of peroxygenases still cannot be fulfilled effectively. To address the above issue, a H₂O₂ generation-detection-regulation platform that integrated an effective organocatalyst-driven H₂O₂ generation system, a precise electrochemical H₂O₂ real-time detection device, and a convenient H₂O₂ regulation strategy was first developed. The suitable range of H₂O₂ generation rate for maximizing the catalytic efficiency of perox-ygenases while minimizing inactivation of the enzyme was firstly obtained by simply adjusting the amount of organocatalyst. According to the determined suitable range, the C-H oxyfunctionalisation efficiency of peroxygenases for each substrate was significantly boosted, achieving ~3-fold of the reported highest turnover frequency. [ABSTRACT FROM AUTHOR]