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A mass spectrometric investigation of the vaporisation behaviour in the (U+Pu+O) system

Authors
  • Gotcu-Freis, Petronela
  • Colle, Jean-Yves
  • Hiernaut, Jean-Pol
  • Beneš, Ondrej
  • Guéneau, Christine
  • Konings, Rudy J.M.1, 2, 3, 4, 5, 6
  • 1 European Commission
  • 2 Joint Research Centre
  • 3 Institute for Transuranium Elements
  • 4 Delft University of Technology
  • 5 Faculty of Applied Sciences
  • 6 CEA, DEN, SCCME, LM2T
Type
Published Article
Journal
The Journal of Chemical Thermodynamics
Publication Date
Jan 01, 2013
Accepted Date
Dec 07, 2013
Volume
71
Pages
212–220
Identifiers
DOI: 10.1016/j.jct.2013.12.004
Source
Elsevier
Keywords
License
Unknown

Abstract

The vaporisation behaviour of (U,Pu)O2 mixed oxides (Pu/M=0.25, 0.50 and 0.75, with M=U+Pu) was studied by means of mass spectrometry. Hyperstoichiometric samples were heated in a Knudsen cell up to T=2300K. The evolution of the uranium and plutonium bearing gaseous species was studied as a function of time in order to evaluate the congruent vapour composition. Ionisation efficiency measurements were performed and the partial pressures of the gaseous species involved in the vaporisation process were determined. The vapour pressure has also been calculated using a thermochemical model for the (U+Pu+O) system. A quasi congruent composition with respect to the O/M ratio has been assumed, in agreement with the experiments. Nevertheless, the evaluation of all the experimental and calculated results shows that a total congruent composition exists for a single composition of the mixed oxide (MOX) samples with a Pu/M content slightly lower than 0.50. A good agreement is obtained between the calculated and experimental vapour pressure data, as well as the quasi congruent vaporisation compositions.

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