The hydrothermal reaction of V2O5, Ni(NO3)2·6H2O, ethylenediamine and H2O in the molar ratio of 1∶1∶3.5∶519 at 180 °C yields black plates of [Ni(en)2][V6O14]. This compound has been characterized structurally, magnetically, electrically, and spectroscopically. The crystal structure consists of novel mixed-valence vanadium oxide layers and interlayer metal coordination complexes. Each of the three VO5 square pyramids share two edges to form a V3O11 group. The V3O11 groups are connected through sharing edges to produce a linear ribbon. Adjacent strips share corners to form a layer structure. The two oxygen atoms from the neighbouring vanadium oxide layers are coordinated to each nickel atom in a trans-fashion, and form a three-dimensional framework structure. An EHT (Extended Hückel
Theory) calculation was performed to analyze the electronic structure, and the electrical resistivity measurements confirmed the expected semiconducting behavior of [Ni(en)2][V6O14].
