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

被引:6
作者
Gotcu-Freis, Petronela [1 ,2 ]
Colle, Jean-Yves [1 ]
Hiernaut, Jean-Pol [1 ]
Benes, Ondrej [1 ]
Gueneau, Christine [3 ]
Konings, Rudy J. M. [1 ]
机构
[1] Commiss European Communities, Joint Res Ctr, Inst Transuranium Elements, D-76125 Karlsruhe, Germany
[2] Delft Univ Technol, Fac Sci Appl, NL-2629 JB Delft, Netherlands
[3] CEA, DEN, SCCME, LM2T, F-91191 Gif Sur Yvette, France
关键词
Knudsen cell; Mass spectrometry; Vapour pressure; Thermodynamics; (U plus Pu plus O) system; PLUTONIUM; URANIUM; OXIDE;
D O I
10.1016/j.jct.2013.12.004
中图分类号
O414.1 [热力学];
学科分类号
摘要
The vaporisation behaviour of (U, Pu)O-2 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 = 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 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. (C) 2013 Elsevier Ltd. All rights reserved.
引用
收藏
页码:212 / 220
页数:9
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