Unsymmetrical Ni II –Imidoylamidine Complexes Derived from a Novel Oxime‐Mediated Single‐Pot Reaction of Nitriles

The neutral bisimidoylamidine (or 1,3,5‐triazapentadiene) Ni II complexes [Ni{H N C(R)N C(C 6 H 4 CO) N } 2 ] {R=Me, Et, n Pr, i Pr, (CH 2 ) 3 Cl}, bearing an iminoisoindolinone moiety, have been generated by a novel 2‐propanone oxime‐mediated single‐pot reaction of phthalonitrile and nickel(II) acetate in solution of the corresponding alkylnitrile (RCN). Single‐crystal X‐ray diffraction analyses indicate a square‐planar geometry of the imidoylamidine core. The synthesised compounds represent rare specimens of genuine unsymmetrical imidoylamidine complexes as well as their first examples generated from nitriles in a single‐pot reaction.