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The unique synthesis and reactivity of [( R PNP*)NiH] complexes ( 1a , b ), based on metal-ligand cooperation (MLC), are presented ( R PNP* = deprotonated PNP ligand, R = i Pr, t Bu). Unexpectedly, the dearomatized complexes 1a , b were obtained by reduction of the dicationic complexes [( R PNP)Ni(MeCN)](BF 4 ) 2 with sodium amalgam or by reaction of the free ligand with Ni 0 (COD) 2 . Complex 1b reacts with CO via MLC, to give a rare case of a distorted-octahedral PNP-based pincer complex, the Ni(0) complex 3b . Complexes 1a , b also react with CO 2 via MLC to form a rare example of η 1 binding of CO 2 to nickel, complexes 4a , b . An unusual CO 2 cleavage process by complex 4b , involving C-O and C-P cleavage and C-C bond formation, led to the Ni-CO complex 3b and to the new complex [(P i Pr 2 NC 2 O 2 )Ni(P(O) i Pr 2 )] ( 5b ). All complexes have been fully characterized by NMR and X-ray crystallography.

Metal–Ligand Cooperation as Key in Formation of Dearomatized NiII–H Pincer Complexes and in Their Reactivity toward CO and CO2

Metal–Ligand Cooperation as Key in Formation of Dearomatized Ni^II–H Pincer Complexes and in Their Reactivity toward CO and CO₂