Tracking light-induced electron transfer toward O2 in a hybrid photoredox-laccase system

摘要: Summary Photobiocatalysis uses light to perform specific chemical transformations in a selective and efficient way. The intention is couple photoredox cycle with an enzyme performing multielectronic catalytic activities. Laccase, robust multicopper oxidase, can be envisioned use dioxygen as clean electron sink when coupled oxidation photocatalyst. Here, we provide detailed study of the coupling [Ru(bpy)3]2+ photosensitizer laccase. We demonstrate that laccase reduction requires relay like methyl viologen. In presence dioxygen, electrons transiently stored superoxide ions are scavenged by form water instead H2O2. net result photo accumulation highly oxidizing [Ru(bpy)3]3+. This provides ground for tandem light-driven oxidative process O2 one-electron transfer four-electron substrate sustainable final acceptor photocatalytic process.