Thermochemistry of UO2 - ThO2 and UO2 - ZrO2 fluorite solid solutions

被引:22
作者
Zhang, Lei [1 ,2 ,3 ]
Shelyug, Anna [1 ,2 ]
Navrotsky, Alexandra [1 ,2 ]
机构
[1] Univ Calif Davis, Peter A Rock Thermochem Lab, Davis, CA 95616 USA
[2] Univ Calif Davis, NEAT ORU, Davis, CA 95616 USA
[3] Univ Notre Dame, Dept Civil & Environm Engn & Earth Sci, Notre Dame, IN 46556 USA
关键词
UO2; ThO2; ZrO2; Solid solution thermodynamics; Calorimetry; Nuclear fuel; THERMODYNAMIC MIXING PROPERTIES; HIGH-TEMPERATURE CALORIMETRY; X-RAY; URANIUM-OXIDES; ZIRCONIA; SYSTEM; THORIA; PHASE; DIRECTIONS; ENERGETICS;
D O I
10.1016/j.jct.2017.05.026
中图分类号
O414.1 [热力学];
学科分类号
摘要
The enthalpies of formation of cubic urania - thoria (c-ThxU(1) O-x(2+y)) and urania - zirconia (c-ZrxU(1) O-x(2), x < 0.3) solid solutions at 25 degrees C from end-member binary oxides (c-UO2, and c-ThO2 or m-ZrO2) have been measured by high temperature oxide melt solution calorimetry. The enthalpies of mixing for both systems are zero within experimental error. The interaction parameters for binary solid solutions MO2 - M'O-2 (M, M' = U, Th, Ce, Zr, and Hf), fitted by regular and subregular thermodynamic models using both calorimetric and computational data, increase linearly with the corresponding volume mismatch. Cubic UO2 - ZrO2 appears to be an exception to this correlation and shows a zero heat of mixing despite large size mismatch, suggestive of some short-range ordering and/or incipient phase separation to mitigate the strain. The incorporation of ZrO2 into UO2 stabilizes the system and makes it a potential candidate for immobilization and disposal of nuclear waste. (C) 2017 Elsevier Ltd.
引用
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页码:48 / 54
页数:7
相关论文
共 48 条
  • [1] Thermochemistry of Lanthana- and Yttria-Doped Thoria
    Aizenshtein, Michael
    Shvareva, Tatiana Y.
    Navrotsky, Alexandra
    [J]. JOURNAL OF THE AMERICAN CERAMIC SOCIETY, 2010, 93 (12) : 4142 - 4147
  • [2] A NEW FUEL MATERIAL FOR ONCE-THROUGH WEAPONS PLUTONIUM BURNING
    AKIE, H
    MUROMURA, T
    TAKANO, H
    MATSUURA, S
    [J]. NUCLEAR TECHNOLOGY, 1994, 107 (02) : 182 - 192
  • [3] Theoretical study of mixing energetics in homovalent fluorite-structured oxide solid solutions
    Alexandrov, Vitaly
    Gronbech-Jensen, Niels
    Navrotsky, Alexandra
    Asta, Mark
    [J]. JOURNAL OF NUCLEAR MATERIALS, 2014, 444 (1-3) : 292 - 297
  • [4] THE OXIDES OF URANIUM .4. THE SYSTEM UO2-THO2-O
    ANDERSON, JS
    EDGINGTON, DN
    ROBERTS, LEJ
    WAIT, E
    [J]. JOURNAL OF THE CHEMICAL SOCIETY, 1954, (OCT): : 3324 - 3331
  • [5] THERMODYNAMIC PROPERTIES OF NONSTOICHIOMETRIC URANIA-THORIA SOLID SOLUTIONS
    ARONSON, S
    CLAYTON, JC
    [J]. JOURNAL OF CHEMICAL PHYSICS, 1960, 32 (03) : 749 - 754
  • [6] The solidification behaviour of the UO2-ThO2 system in a laser heating study
    Bohler, R.
    Quaini, A.
    Capriotti, L.
    Cakir, P.
    Benes, O.
    Boboridis, K.
    Guiot, A.
    Luzzi, L.
    Konings, R. J. M.
    Manara, D.
    [J]. JOURNAL OF ALLOYS AND COMPOUNDS, 2014, 616 : 5 - 13
  • [7] A METALLOGRAPHIC AND X-RAY STUDY OF THE UO2-ZRO2 SYSTEM
    COHEN, I
    SCHANER, BE
    [J]. JOURNAL OF NUCLEAR MATERIALS, 1963, 9 (01) : 18 - 52
  • [8] Characterization of zirconia-thoria-urania ceramics by X-ray and electron interactions
    Curran, G
    Sevestre, Y
    Rattray, W
    Allen, P
    Czerwinski, KR
    [J]. JOURNAL OF NUCLEAR MATERIALS, 2003, 323 (01) : 41 - 48
  • [9] Thermodynamic investigations of ThO2-UO2 solid solutions
    Dash, Smruti
    Parida, S. C.
    Singh, Ziley
    Sen, B. K.
    Venugopal, V.
    [J]. JOURNAL OF NUCLEAR MATERIALS, 2009, 393 (02) : 267 - 281
  • [10] QUANTITATIVE CORRELATIONS OF DEVIATIONS FROM IDEALITY IN BINARY AND PSEUDOBINARY SOLID-SOLUTIONS
    DAVIES, PK
    NAVROTSKY, A
    [J]. JOURNAL OF SOLID STATE CHEMISTRY, 1983, 46 (01) : 1 - 22