Abstract
Chemical oxidation of the linear tricobalt compound Co3(dpa)4Cl2 (1) with 1 equiv of NOBF4 yields the one-electron oxidized species [Co3(dpa)4Cl2]+ (1+), which crystallizes from dichloromethane as a solvate [Co3(dpa)4Cl2][BF4]·2CH2Cl2 (2·2CH2Cl2). The crystal structure of 2·xCH2Cl2 (with x varying from 1.125 to 2.0) has been determined at 100, 213, and 300 K, showing very little variation and an essentially symmetrical arrangement of three Co atoms in the cation 1+ with Co−Co distances of 2.3168(8) and 2.3289(8) A. The terminal cobalt to axial chloride distances are 2.350(1) and 2.376(1) A at 100 K. The cation maintains its symmetrical structure at ambient temperature (300 K) with only a slight lengthening (0.01−0.02 A) of Co−Co and Co−N distances. Temperature studies of the magnetic properties for 2 in both solution and solid state have revealed a spin-crossover behavior occurring in two gradual steps, indicating that 2 exhibits a diamagnetic ground state and thermally accessible triplet and quintet spin...
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