Pressure and temperature effects on octahedral-tetrahedral equilibria in 3-methylpyridine solutions of some cobalt(II) halides.
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The visible absorption spectra of CoX<SUB>2</SUB> (X=Cl, Br) in 3-methylpyridine (3-Me-py) solutions have been measured in the pressure range of 1 bar—3 kbar at room temperature, and in the temperature range of ≈5–≈76 °C at 1 bar. The equilibrium, [CoX<SUB>2</SUB>(3-Me-py)<SUB>2</SUB>] (tetrahedral)+2(3-Me-py)\rightleftharpoons[CoX<SUB>2</SUB>(3-Me-py)<SUB>4</SUB>] (octahedral), is found to be followed over this pressure range. Higher pressures favor the octahedral species with the volume changes −18–−19 cm<SUP>3</SUP> mol<SUP>−1</SUP> at 1 bar. On the other hand, the above equilibrium holds fairly well at temperatures up to about 40 °C. Higher temperatures favor the tetrahedral species, the heats of reaction, being 56.7 kJ mol<SUP>−1</SUP> (5.0–44.8 °C) and 58.6 kJ mol<SUP>−1</SUP> (4.8–34.2 °C) for the chloro and bromo complexes, respectively. An intense and broad band appears around 400 nm at elevated temperatures especially for the bromo complex solution. This band may be assigned to a charge-transfer band occurring in a contact ion pair of solvent molecule 3-Me-py with X<SUP>−</SUP> arising from the dissociation of the tetrahedral species [CoX<SUB>2</SUB>(3-Me-py)<SUB>2</SUB>].
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