X‐ray structure and density functional theory studies of an unexpected product: trans‐bis{2‐[(2‐cyanoethyl)iminomethyl]phenolato}copper(II)

The title compound, [Cu(C₁₀H₉N₂O)₂] or [Cu^II(CYMB)₂], (I), was obtained in an attempt to reduce trans‐bis(2‐{[3,5‐bis(trifluoromethyl)phenyl]iminomethyl}phenolato)copper(II), [Cu(TIMB)₂], (II), with bis(pentamethylcyclopentadienyl)cobalt(II) [decamethylcobaltocene, Cp*₂Co, (III)]. The molecular structure of (I) has the Cu^II centre located on an inversion centre of the C2/c space group. A density functional theory (DFT) analysis at the B3LYP/Lanl2dz(CuF);6‐31G**(CHNO) level performed in order to optimize the structures of the free ligands CYMB⁻ and TIMB⁻, and the metal complexes [Cu^I/II(CYMB)₂]^−/0 and [Cu^I/II(TIMB)₂]^−/0, reproduced well the X‐ray diffraction structure and allowed us to infer the insertion of the cyanomethide anion on the 3,5‐bis(trifluoromethyl)phenyl system from an evaluation of the Mulliken atomic charges and the electronic energies.