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TiO₂ is one of the most promising heterogeneous photoredox catalysts employed in oxidative pollutant destruction, CO₂ reduction, water splitting, disinfection, solar cell design and organic synthesis. Due to the wide bandgap of TiO₂, visible light energy is not sufficient for its activation, and electron/hole pairs generated upon UV irradiation demonstrate limited selectivity for application in organic synthesis. Thus, the development of TiO₂-based catalytic systems activated by visible light is highly attractive. In the present work we demonstrate the generation of <i>t</i>-BuOO• radicals from <i>tert</i>-butylhydroperoxide catalyzed using commercially available unmodified TiO₂ under visible light. This finding was used for the highly selective CH-peroxidation of barbituric acids, which contrasts with the behavior of the known TiO₂/H₂O₂/UV photocatalytic system used for deep oxidation of organic pollutants.