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Coordination studies of new lutidine-derived hybrid NHC/phosphine ligands (CNP) to Pd and Ir have been performed. Treatment of the square-planar [Pd(CNP)Cl](AgCl 2 ) complex 2a with KHMDS produces the selective deprotonation at the CH 2 P arm of the pincer to yield the pyridine-dearomatised complex 3a. A series of cationic [Ir(CNP)(cod)] + complexes 4 has been prepared by reaction of the imidazolium salts 1 with Ir(acac)(cod). These derivatives exhibit in the solid state, and in solution, a distorted trigonal bipyramidal structure in which the CNP ligands adopt an unusual C (axial) -N (equatorial) -P (equatorial) coordination mode. Reactions of complexes 4 with CO and H 2 yield the carbonyl species 5a(Cl) and 6a(Cl), and the dihydrido derivatives 7, respectively. Furthermore, upon reaction of complex 4b(Br) with base, selective deprotonation at the methylene CH 2 P arms is observed. The, thus formed, deprotonated Ir complex 8b reacts with H 2 in a ligand-assisted process leading to the trihydrido complex 9b, which can also be obtained by reaction of 7b(Cl) with H 2 in the presence of KO t Bu. Finally, the catalytic activity of Ir-CNP complexes in the hydrogenation of ketones has been briefly assessed.

Synthesis, structure and reactivity of Pd and Ir complexes based on new lutidine-derived NHC/phosphine mixed pincer ligands