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[C4H11N8NiO4]+[C12H4N4]-, Mr = 498.09 is triclinic, P1̄, a = 3.7718(6), b = 7.436(2), c = 17.511(4) Å, α = 88.67(2), β = 86.93(2), γ = 85.05(2)°, V = 488.51 Å3, Z = 1, dc = 1.69 gcm-3, final Rw = 0.035 for 1454 observed independent reflections. The crystals consist of segregated regular parallel stacks of planar metal complex cations and tenq- counterions with intermolecular H bonds stabilizing the structure. The compound is metallic at room temperature. A metal to semiconductor transition around 230 K shows up in thermopower data, in the microwave conduc­tivity and epr around 170 K. It is not visible in the static magnetic susceptibility.

The average unit cell of the methanol solvate [Ni(C2H5N4O2)2] × C14H8N4 × 2CH3OH, MΓ = 589.22 is triclinic. Ρ1̄, a = 8.539(3). b = 8.937(3). c = 9.418(3) Å, α = 103.39(3). β = 100.12(2), γ = 105.39(2)°, V = 652.2 Å3 Z = 1, dc = 1.50 gem-3, final Rw = 0.050 for 1580 observed independent reflections. Satellite reflections hint at a modulation of the structure in the ac plane. Mixed stacks of alternating and mainly neutral metal complex and Me2tcnq molecules are formed.Crystals grown with electrochemical reduction show a weak activated paramagnetism, those grown without electrochemical support are diamagnetic.