BEDT-TTF Salts Formed with Tetrahedrally Coordinated Zinc(II) Complex Anions

Abstract

12 kinds of bis(ethylenedithio)tetrathiafulvalene (BEDT-TTF or ET) cation salts with tetrahedrally coordinated zinc(II) complex anions were obtained by electrocrystallization; most of them were produced via the additional reaction of Lewis-basic cyano-containing anions [N(CN)2-, C(CN)3-, and Au(CN)2-] with ZnX2 (X = Cl-, Brand nd SCN-) occurred during electrocrystallization. Based on the charge and arrangement of ET molecules, these salts were predominantly categorized into four groups: (A) isolated ET •+ dimers or tetramers, (B) infinite ET •+ ribbon, (C) infinite layers either with a peculiar ET 0.5+ arrangement or of ET molecules with partial charges other than +0.5, and (D) infinite layers of ET 0.5+ molecules. In A, zinc(II) complex anions including a unidentate-coordinated C(CN)3 or Au(CN)2 group spatially interrupt the infinite arrangement of ET molecules. The ET •+ ribbon in B runs parallel to the pseudo-polymeric chain of disordered Zn[C(CN)3]2Br2 2ions. In C, two salts are semiconductive, whereas the remaining two salts behave metallic at room temperature and undergo a metal-insulator transition on cooling. The ET molecules in D are arranged in a θ42+40-like packing motif, due to the non-planar anionic layers. All salts

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