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Report No.

A Novel microemulsion phase transition; Toward the elucidation of third-phase formation in spent nuclear fuel reprocessing

Mu, J.*; Motokawa, Ryuhei   ; Akutsu, Kazuhiro*; Nishitsuji, Shotaro*; Masters, A. J.*

We present evidence that the transition between organic and third phases, which is an unusual transition between two isotropic, bi-continuous micro-emulsion phases. This system contains quaternary; water, n-dodecane, nitric acid, tributyl phosphate (TBP). This quaternary system has been shown to exhibit, under appropriate conditions, three coexisting phases: a light organic phase, an aqueous phase, and the so-called third phase. In this work, we focused on the coexistence of the light organic phase with the third phase using methods of molecular dynamics (MD) simulation and small-angle X-ray scattering (SAXS). Snapshots from the MD simulations as well as a cluster analysis of the organic and third phases revealed structures akin to bi-continuous micro-emulsion phases, with the polar species residing within a mesh, and with the surface of the mesh formed by amphiphilic TBP molecules. The non-polar n-dodecane molecules were observed in these snapshots to be outside this mesh. The only large-scale structural differences observed between the two phases were the dimensions of the mesh. Evidence for the correctness of these structures was provided by the results of SAXS studies, where the profiles obtained for both the organic and third phases agreed well with those calculated from simulation.



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Category:Chemistry, Physical



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