The crystal structure of the title compound, 2,2‐dimethyl‐1,3‐propanediammonium chromate, (C5H16N2)[CrO4], consists of layers built up from CrO42− tetrahedra alternating with diprotonated 2,2‐dimethylpropylendiamine molecules. N—H⋯O hydrogen bonds ensure the cohesion and stability of the structure.
The electrochemical combination of the paramagnetic anion [Cr(NCS) 6 ] 3with the organic p-donors bis(ethylenedithio)tetrathiafulvalene (ET) and 4,5-bis(2-hydroxyethylthio)-4',5'-ethylenedithiotetrathiafulvalene (DHET-EDTTTF) leads to two new radical cation salts, namely (ET) 4 [Cr(NCS) 6 ]•PhCN (1) and (DHET-EDTTTF) 2 (NEt 4 )[Cr(NCS) 6 ] (2). Both have been characterized by X-ray crystallography, magnetic and resistivity measurements. The structure of 1 consists of alternating inorganic layers generated by the anions and organic layers in which the PhCN molecules are inserted; the organic sub-lattice is built up from four different ET units, three of them with a charge distribution of +1, the fourth being neutral. The organic sub-lattice of 2 contains a centrosymmetric [(DHET-EDTTTF • ) 2 ] 2+ dimer, in which the overlap mode is of the eclipsed type. Conductivity measurements indicate that compounds 1 and 2 are semiconductors with room temperature conductivities of 1.4 × 10 -2 and 6.1 × 10 -5 S cm -1 and activation energies of 0.24 and 0.23 eV, in 1 and 2, respectively. For both salts, magnetic measurements indicate (i) that the organic and inorganic parts are magnetically independent, and (ii) that the organic units are antiferromagnetically coupled. To cite this article: F.
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