Title: A mass spectrometric investigation of the vaporisation behaviour in the (U+Pu+O) system
Authors: GOTCU PetronelaCOLLE Jean-YvesHIERNAUT Jean-PolBENES ONDREJGUENEAU ChristineKONINGS Rudy
Citation: JOURNAL OF CHEMICAL THERMODYNAMICS vol. 71 p. 212 - 220
Publisher: ACADEMIC PRESS LTD- ELSEVIER SCIENCE LTD
Publication Year: 2014
JRC N°: JRC68726
ISSN: 0021-9614
URI: http://www.sciencedirect.com/science/article/pii/S0021961413004692
http://publications.jrc.ec.europa.eu/repository/handle/JRC68726
DOI: 10.1016/j.jct.2013.12.004
Type: Articles in periodicals and books
Abstract: The vaporisation behaviour of (U,Pu)O2‐x 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 2300 K. 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 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 overview of all the experimental and calculated results show that a total congruent composition exists for a single composition of the MOX 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. Keywords: Knudsen cell, mass spectrometry, vapour pressure, thermodynamics, U‐Pu‐O system.
JRC Directorate:Nuclear Safety and Security

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