Aluminum–Ligand Cooperative N–H Bond Activation and an Example of Dehydrogenative Coupling

Activation of N–H bonds by a molecular aluminum complex via metal–ligand cooperation is described. (PhI2P2–)­AlH (1b), in which PhI2P2– is a tridentate bis­(imino)­pyridine ligand, reacts with anilines to give the N–H-activated products (PhHI2P–)­AlH­(NHAr) (2). When heated, 2 releases H2 and affords (PhI2P–)­Al­(NHAr) (3). Complex 1b catalyzes the dehydrogenative coupling of benzylamine to afford H2, NH3, and N-(phenylmethylene)­benzenemethanamine.