Counterbalancing Cations in Ru(III)–Zeolites to Fine-Tune the Catalytic Activity during the Dehydrogenative Aerobic Imination of Benzyl Alcohols

The dehydrogenative imination of alcohols is an attractive reaction in organic synthesis that circumvents the use of unstable aldehyde intermediates and gives access to a variety of amine derivate products. However, most of the protocols reported so far employ soluble metal complex catalysts, which often allow a fine-tuned control of the reactivity through the ligand–metal interactions but lack any recoverability at the end of the reaction. Here, we show that RuCl3 exchanged into commercially available Y and X zeolites (faujasites) acts as a heterogeneous, reusable catalyst for the imination of benzyl alcohols under air. The alkaline counterbalancing cations naturally present in the Ru3+–faujasite framework (ranging from H+ to Cs+) finely control the catalytic activity of the Ru(III) site during the reaction, thereby combining the benefits of a simple, recoverable solid catalyst with finely tuned reactivity.