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Title: Thermal expansion in UO 2 determined by high-energy X-ray diffraction

Abstract

In this study, we present crystallographic analyses of high-energy X-ray diffraction data on polycrystalline UO 2 up to the melting temperature. The Rietveld refinements of our X-ray data are in agreement with previous measurements, but are systematically located around the upper bound of their uncertainty, indicating a slightly steeper trend of thermal expansion compared to established values. This observation is consistent with recent first principles calculations.

Authors:
 [1];  [2];  [3];  [4];  [4];  [5];  [2]
  1. European Spallation Source ESS AB, Lund (Sweden)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States); Stony Brook Univ., Stony Brook, NY (United States); Materials Development, Inc., Arlington Heights, IL (United States)
  4. Argonne National Lab. (ANL), Argonne, IL (United States); Materials Development, Inc., Arlington Heights, IL (United States)
  5. Stony Brook Univ., Stony Brook, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1346746
Alternate Identifier(s):
OSTI ID: 1328451
Report Number(s):
BNL-113574-2017-JA
Journal ID: ISSN 0022-3115; TRN: US1701819
Grant/Contract Number:
SC00112704; AC02-06CH11357; DE SC0007564; FG02-09ER46650
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Nuclear Materials
Additional Journal Information:
Journal Volume: 479; Journal Issue: C; Journal ID: ISSN 0022-3115
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS

Citation Formats

Guthrie, M., Benmore, C. J., Skinner, L. B., Alderman, O. L. G., Weber, J. K. R., Parise, J. B., and Williamson, M. Thermal expansion in UO2 determined by high-energy X-ray diffraction. United States: N. p., 2016. Web. doi:10.1016/j.jnucmat.2016.06.042.
Guthrie, M., Benmore, C. J., Skinner, L. B., Alderman, O. L. G., Weber, J. K. R., Parise, J. B., & Williamson, M. Thermal expansion in UO2 determined by high-energy X-ray diffraction. United States. doi:10.1016/j.jnucmat.2016.06.042.
Guthrie, M., Benmore, C. J., Skinner, L. B., Alderman, O. L. G., Weber, J. K. R., Parise, J. B., and Williamson, M. Fri . "Thermal expansion in UO2 determined by high-energy X-ray diffraction". United States. doi:10.1016/j.jnucmat.2016.06.042. https://www.osti.gov/servlets/purl/1346746.
@article{osti_1346746,
title = {Thermal expansion in UO2 determined by high-energy X-ray diffraction},
author = {Guthrie, M. and Benmore, C. J. and Skinner, L. B. and Alderman, O. L. G. and Weber, J. K. R. and Parise, J. B. and Williamson, M.},
abstractNote = {In this study, we present crystallographic analyses of high-energy X-ray diffraction data on polycrystalline UO2 up to the melting temperature. The Rietveld refinements of our X-ray data are in agreement with previous measurements, but are systematically located around the upper bound of their uncertainty, indicating a slightly steeper trend of thermal expansion compared to established values. This observation is consistent with recent first principles calculations.},
doi = {10.1016/j.jnucmat.2016.06.042},
journal = {Journal of Nuclear Materials},
number = C,
volume = 479,
place = {United States},
year = {Fri Jun 24 00:00:00 EDT 2016},
month = {Fri Jun 24 00:00:00 EDT 2016}
}

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  • Here we present crystallographic analyses of high-energy X-ray diffraction data on polycrystalline UO2 up to the melting temperature. The Rietveld refinements of our X-ray data are in agreement with previous measurements, but are systematically located around the upper bound of their uncertainty, indicating a slightly steeper trend of thermal expansion compared to established values. This observation is consistent with recent first principles calculations.
  • The high-temperature phase relationship and thermal expansion coefficient of YBa{sub 2}Cu{sub 3}O{sub 7{minus}x} under constant oxygen nonstoichiometry, x, were determined by high-temperature powder X-ray diffraction analysis under controlled oxygen partial pressure at temperatures up to 800 C. The results are discussed based on reported nonstoichiometry data. The present study showed an orthorhombic-to-tetragonal transition near the composition x = 0.5. The lattice parameter c, perpendicular to the Cu-O plane, showed a maximum at around x = 0.7 to 0.8. In the orthorhombic phase, the lattice parameters a and b along the Cu-O plane were essentially constant for x < 0.2. Formore » 0.2 < x < {approximately}0.5, a increased and b decreased with x. In the tetragonal phase, with x > {approximately}0.5, the lattice parameter a decreased with x. The thermal expansion coefficient, {alpha}, along the c-axis ranged from 19 {times} 10{sup {minus}6} to 25 {times} 10{sup {minus}6}{center_dot}K{sup {minus}1}, whereas {alpha} along the a- and b-axes ranged form 12 {times} 10{sup {minus}6} to 22 {times} 10{sup {minus}6}{center_dot}K{sup {minus}1} at 400 to 800 C, and these values were very small below 400 C. It was found that a, b, and {alpha} along the a- and b-axes are smaller when the oxygen content along the respective axes is less, while the area of the ab plane and its thermal expansion coefficient are larger when the deviation of the oxygen content from the stoichiometric compositions of YBa{sub 2}Cu{sub 3}O{sub 7} or YBa{sub 2}Cu{sub 3}O{sub 6}is larger. Changes of x and temperature affected c more strongly than a and b.« less
  • The thermal expansion behavior of Ba{sub 2}ZnSi{sub 2}O{sub 7}, BaZnSiO{sub 4} and BaZn{sub 2}Si{sub 2}O{sub 7} is characterized by both high-temperature X-ray diffraction (HT-XRD) and dilatometry. Ba{sub 2}ZnSi{sub 2}O{sub 7} and BaZnSiO{sub 4} show a thermal expansion (100-800 Degree-Sign C) in the range from 8.9 to 10.4 Multiplication-Sign 10{sup -6} K{sup -1}. By contrast, BaZn{sub 2}Si{sub 2}O{sub 7} has a much higher thermal expansion in the low-temperature modification and shows a phase transition at 280 Degree-Sign C which runs parallel with a steep increase in cell volume. This phase transition is also observed in the solid solution series BaZn{sub 2-x}Mg{submore » x}Si{sub 2}O{sub 7}, but it is shifted to higher temperatures and to a smaller volume change with increasing Mg{sup 2+} concentration. This solid solution series is characterized by dilatometry, X-ray diffraction and differential scanning calorimetry. An adjustment of the MgO/ZnO-ratio enables the preparation of materials with a large variety of thermal expansions. - Graphical abstract: XRD-patterns of Ba{sub 2}ZnSi{sub 2}O{sub 7} were recorded at different temperatures (left). For each XRD-pattern a Rietveld-refinement was performed, the image in the middle shows the XRD-pattern measured at room temperature (circles), the Rietveld calculation (red line) and the difference between them (blue line). The lattice parameters derived hereof were plottet against the temperature and fitted to a polynomial (right picture). From those polynomials the lattice expansion was calculated. Highlights: Black-Right-Pointing-Pointer We examined the thermal expansion of Ba{sub 2}ZnSi{sub 2}O{sub 7}, BaZnSiO{sub 4} and BaZn{sub 2-x}Mg{sub x}Si{sub 2}O{sub 7}. Black-Right-Pointing-Pointer Thermal expansions were determined by dilatometry and high-temperature X-ray diffraction. Black-Right-Pointing-Pointer High-temperature X-ray diffraction enabled to determine anisotropic thermal expansion. Black-Right-Pointing-Pointer BaZn{sub 2}Si{sub 2}O{sub 7} exhibits the highest thermal expansion due to a phase transition. Black-Right-Pointing-Pointer Substitution of small amounts of Zn{sup 2+} for Mg{sup 2+} leads to a decrease in thermal expansion.« less