Abstract
Photocatalytic ozonation of wastewater pollutants by sunlight is a highly attractive technology close to real application. Understanding this process on the atomic scale and under realistic working conditions is challenging but vital for the rational design of catalysts and photocatalytic decontamination systems. Here we study two highly active C3N4 photocatalysts (bulk C3N4 and a nanosheet-structured C3N4) under simultaneous visible-light irradiation and O3 bubbling in water by in situ EPR spectroscopy coupled with an online spin-trapping technique. The photoexcitation of electrons to the conduction band (CB-e–), their further trapping by dissolved O2 and O3, and the evolution of reactive oxygen species (ROS) have been semiquantitatively visualized. A dual role of O3 in boosting the CB-e– to •OH conversion is confirmed: (i) an inlet 2.1 mol % O3/O2 gas mixture can trap about 2–3 times more CB-e– upon aqueous C3N4 suspension than pure O2 and further produce •OH by a robust •O3–-mediated one-electron-reduc...
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