Selective Photocatalytic Benzene Oxidation Using Iron‐Carbon Nitride Fragments Functionalized with Cyamelurate‐Like Groups

Carbon nitrides have emerged as promising supports for catalytically active metals in various chemical reactions. Among these, the selective oxidation of benzene to phenol stands out as particularly challenging within the chemical industry due to its traditionally low yields and complex reaction pathways. In our current investigation, we have focused on the synthesis of ionic carbon nitride fragments via a straightforward alkaline hydrolysis method. These fragments demonstrate a remarkable ability to stabilize iron cations within the carbon nitride structure (Frag‐Fe), resulting in a highly efficient photocatalyst for benzene oxidation. Employing hydrogen peroxide as the oxidant in a single‐step reaction, we achieved an impressive 47% yield of phenol using Frag‐Fe at 12 hours, with negligible production of CO2 as a byproduct. This compelling outcome underscores the effectiveness of our alkaline synthesis approach in generating carbon nitride‐based photocatalysts with exceptional activity for C‐H oxidation reactions. Our findings not only contribute to the advancement of carbon nitride‐based catalysis, but also hold significant promise for the development of more sustainable and efficient chemical processes in the future.