Organic/Inorganic Heterogeneous Silica‐Based Photoredox Catalyst for Aza‐Henry Reactions

The transformation of light into chemical energy is a leitmotiv in the development of sustainable and environmentally concerned chemical processes. Chemists invented original concepts to address this purpose, like photoredox catalysis, which became a wonderful tool to transform simple organic compounds into high‐value products. Nevertheless, the most relevant transition metal based photocatalysts suffer from major disadvantages like toxicity, cost, and poor recyclability potential. To circumvent this, we propose a new generation of heterogeneous photoredox catalysts resulting from the combination of porous silica materials and Rose Bengal. They promote carbon–carbon bond formations under visible‐light in environmentally benign solvent using air as the only stoichiometric redox partner. The pure covalent photocatalytic system provides a robust and recyclable system for greener catalysis. This report would be of broad significance because it addresses important sustainability issues: recycling, non‐toxic metal‐free photocatalysts, and less‐waste‐producing chemical process. The combination of porous materials based on silica with an organic dye allowed the development of a cheap, robust, and recyclable hybrid system with proven efficiency in oxidation and reduction processes. It opens the doors to the design of new hybrid systems for sustainable photoredox catalysis.