Solubility Thermodynamics of CyMe 4 -BTBP in Various Diluents Mixed with TBP

Jenny Halleröd, Chrisitan Ekberg, Ivan Kajan, Emma Aneheim
Journal of Solution Chemistry 2018, 47 (6): 1021-1036
The two organic ligands 6,6'-bis(5,5,8,8-tetramethyl-5,6,7,8-tetrahydrobenzo[1,2,4]triazin-3-yl)[2,2']bipyridine (CyMe <mml:math xmlns:mml=""&gt; <mml:msub> <mml:mrow/> <mml:mn>4</mml:mn> </mml:msub> </mml:math> -BTBP) and tri-butyl phosphate (TBP) have previously been investigated in different diluents for use within recycling of used nuclear fuel through solvent extraction. The thermodynamic parameters, <mml:math xmlns:mml=""&gt; <mml:msub> <mml:mi>K</mml:mi> <mml:mi>S</mml:mi> </mml:msub> </mml:math> , <mml:math xmlns:mml=""&gt; <mml:mrow> <mml:mi>Δ</mml:mi> <mml:msub> <mml:mi>C</mml:mi> <mml:mi>p</mml:mi> </mml:msub> </mml:mrow> </mml:math> , <mml:math xmlns:mml=""&gt; <mml:mrow> <mml:mi>Δ</mml:mi> <mml:msup> <mml:mi>H</mml:mi> <mml:mn>0</mml:mn> </mml:msup> </mml:mrow> </mml:math> and <mml:math xmlns:mml=""&gt; <mml:mrow> <mml:mi>Δ</mml:mi> <mml:msup> <mml:mi>S</mml:mi> <mml:mn>0</mml:mn> </mml:msup> </mml:mrow> </mml:math> , of the CyMe <mml:math xmlns:mml=""&gt; <mml:msub> <mml:mrow/> <mml:mn>4</mml:mn> </mml:msub> </mml:math> -BTBP solubility in three diluents (cyclohexanone, octanol and phenyl trifluoromethyl sulfone) mixed with TBP have been studied at 288, 298 and 308 K, both as pristine solutions and pre-equilibrated with 4 mol <mml:math xmlns:mml=""&gt; <mml:mo>·</mml:mo> </mml:math> L <mml:math xmlns:mml=""&gt; <mml:msup> <mml:mrow/> <mml:mrow> <mml:mo>-</mml:mo> <mml:mn>1</mml:mn> </mml:mrow> </mml:msup> </mml:math> nitric acid. In addition, the amount of acid in the organic phase and density change after pre-equilibration have been measured. The solubility of CyMe <mml:math xmlns:mml=""&gt; <mml:msub> <mml:mrow/> <mml:mn>4</mml:mn> </mml:msub> </mml:math> -BTBP increases with an increased temperature in all systems, especially after acid pre-equilibration. This increased CyMe <mml:math xmlns:mml=""&gt; <mml:msub> <mml:mrow/> <mml:mn>4</mml:mn> </mml:msub> </mml:math> -BTBP solubility after pre-equilibration could be explained by acid dissolution into the solvent. Comparing the <mml:math xmlns:mml=""&gt; <mml:mrow> <mml:mi>Δ</mml:mi> <mml:msup> <mml:mi>H</mml:mi> <mml:mn>0</mml:mn> </mml:msup> </mml:mrow> </mml:math> and <mml:math xmlns:mml=""&gt; <mml:mrow> <mml:mi>Δ</mml:mi> <mml:msup> <mml:mi>S</mml:mi> <mml:mn>0</mml:mn> </mml:msup> </mml:mrow> </mml:math> calculated using <mml:math xmlns:mml=""&gt; <mml:mrow> <mml:mi>Δ</mml:mi> <mml:msub> <mml:mi>C</mml:mi> <mml:mi>p</mml:mi> </mml:msub> </mml:mrow> </mml:math> with the same parameters derived from a linear fit indicates temperature independence of all three thermodynamic systems. The change in enthalpy is positive in all solutions.

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