Keywords: Cluster compounds / Cobalt / Mixed-valent compounds / Magnetic properties / Density functional calculations / EPR spectroscopyWe have synthesised and structurally characterised a new pentanuclear mixed-valent cobalt cluster of formula [Co II 3 Co III 2 (OH) 2 (piv) 6 (L) 2 (H 2 O) 4 ] (piv = trimethylacetate, H 2 L = salicylideneanthranillic acid) from reaction of a dinuclear cobalt pivalate precursor with a Schiff base type ligand under mild reaction conditions. The core structure can be conveniently described as two fused Co 3 -μ 3 -OH triangles with a strict unique sharing vertex point. A complete picture of the magnetic behaviour of this compound is presented. Through combined use of susceptibility, magnetisation, and[a]

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