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Tetraphenylphosphonium salts of Co and Fe complexes with alkyl-substituted, er -butyl ( b ), and isopropyl ( dp ) 2,3-thiophenedithiolate (α-tpdt) ligands, namely, TPP[Co(α- b -tpdt) 2 ] ( 3 ), TPP 2 [Fe(α- b -tpdt) 2 ] 2 ( 4a - b ), TPP[Co(α- dp -tpdt) 2 ] ( 5 ), and TPP[Fe(α- dp -tpdt) 2 ] ( 6 ) were prepared and characterized by cyclic voltammetry, single crystal X-ray diffraction, magnetic susceptibility measurements, and 57 Fe Mössbauer spectroscopy. Compound 3 and 5 are isostructural with their Au and Ni analogues with a square-planar coordination geometry. Compound 4 presents two polymorphs ( 4a - b ) both showing a Fe(III) bisdithiolene dimerization. The magnetic susceptibility of 3 and 5 exhibits behavior dominated by antiferromagnetic interactions, with room-temperature magnetic moments of 3.40 and 3.36 μB, respectively, indicating that these square-planar Co(III) complexes assume an intermediate spin electronic configuration ( S = 1) as supported by multiconfigurational and DFT calculations.

[Co/Fe(α-Alkyl-tpdt)2]x−: Alkyl-Substituted Cobalt and Iron Bis-dithiolenethiophenic Complexes

[Co/Fe(α-Alkyl-tpdt)₂]^x−: Alkyl-Substituted Cobalt and Iron Bis-dithiolenethiophenic Complexes