FORMATION OF N-IMIDOYLIMIDATORUTHENIUM(II) COMPLEXES VIA RUTHENIUM-PROMOTED HYDRATION OF NITRILES

The hydridoruthenium(II) complex [RuCl(H)(CO)(PPh(3))(3)] 1 reacted wi th aromatic nitriles at 120 degrees C in the presence of water to give novel N-imidoylimidatoruthenium(II) complexes [RuCl(NH=CRN=CRO)(CO)(P Ph(3))(2)] (R = C(6)H(4)Me-p 2, Ph 3, or C(6)H(4)Me-m 4). In contrast, reaction of o-toluonitrile with 1 gave a small amount of the correspo nding N-imidoylimidato complex and a considerable amount of o-toluamid e. When 1 was heated at 120 degrees C in a 1 : 1 mixture of an amide R (1)CONH(2) and a nitrile R(2)CN a cross-linked N-imidoylimidato comple x [RuCl(NH=CR(2)N=CR(1)O)(CO)(PPh(3))(2)] 6 (R(1) = Ph, R(2) = C(6)H(4 )Me-p) or 7 (R(1) = C(6)H(4)Me-p, R(2) = Ph) was obtained. Single-crys tal structure analyses of 2 and 6 have been performed.