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Title: Structure and bulk modulus of Ln-doped UO 2 (Ln = La, Nd) at high pressure

Abstract

The structure of lanthanide-doped uranium dioxide, Ln xU 1-xO 2-0.5x+y (Ln = La, Nd), was investigated at pressures up to ~50–55 GPa. Samples were synthesized with different lanthanides at different concentrations (x ~ 0.2 and 0.5), and all were slightly hyperstoichiometric (y ~ 0.25–0.4). In situ high-pressure synchrotron X-ray diffraction was used to investigate their high-pressure phase behavior and determine their bulk moduli. All samples underwent a fluorite-to-cotunnite phase transformation with increasing pressure. The pressure of the phase transformation increased with increasing hyperstoichiometry, which is consistent with results from previous computational simulations. Bulk moduli are inversely proportional to both the ionic radius of the lanthanide and its concentration, as quantified using a weighted cationic radius ratio. As a result, this trend was found to be consistent with the behavior of other elastic properties measured for Ln-doped UO 2, such as Young's modulus.

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1];  [2]; ORCiD logo [3];  [3];  [2];  [4];  [1]
  1. Stanford Univ., Stanford, CA (United States)
  2. Univ. of California, Davis, CA (United States)
  3. Univ. of Tennessee, Knoxville, TN (United States)
  4. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1369255
Alternate Identifier(s):
OSTI ID: 1419350
Grant/Contract Number:  
AC02-76SF00515; SC0001089; NA0001974; FG02-99ER45775; AC02-05CH11231; EAR 1606856; NA0002006
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Nuclear Materials
Additional Journal Information:
Journal Volume: 490; 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; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Rittman, Dylan R., Park, Sulgiye, Tracy, Cameron L., Zhang, Lei, Palomares, Raul I., Lang, Maik, Navrotsky, Alexandra, Mao, Wendy L., and Ewing, Rodney C. Structure and bulk modulus of Ln-doped UO2 (Ln = La, Nd) at high pressure. United States: N. p., 2017. Web. doi:10.1016/j.jnucmat.2017.04.007.
Rittman, Dylan R., Park, Sulgiye, Tracy, Cameron L., Zhang, Lei, Palomares, Raul I., Lang, Maik, Navrotsky, Alexandra, Mao, Wendy L., & Ewing, Rodney C. Structure and bulk modulus of Ln-doped UO2 (Ln = La, Nd) at high pressure. United States. doi:10.1016/j.jnucmat.2017.04.007.
Rittman, Dylan R., Park, Sulgiye, Tracy, Cameron L., Zhang, Lei, Palomares, Raul I., Lang, Maik, Navrotsky, Alexandra, Mao, Wendy L., and Ewing, Rodney C. Mon . "Structure and bulk modulus of Ln-doped UO2 (Ln = La, Nd) at high pressure". United States. doi:10.1016/j.jnucmat.2017.04.007. https://www.osti.gov/servlets/purl/1369255.
@article{osti_1369255,
title = {Structure and bulk modulus of Ln-doped UO2 (Ln = La, Nd) at high pressure},
author = {Rittman, Dylan R. and Park, Sulgiye and Tracy, Cameron L. and Zhang, Lei and Palomares, Raul I. and Lang, Maik and Navrotsky, Alexandra and Mao, Wendy L. and Ewing, Rodney C.},
abstractNote = {The structure of lanthanide-doped uranium dioxide, LnxU1-xO2-0.5x+y (Ln = La, Nd), was investigated at pressures up to ~50–55 GPa. Samples were synthesized with different lanthanides at different concentrations (x ~ 0.2 and 0.5), and all were slightly hyperstoichiometric (y ~ 0.25–0.4). In situ high-pressure synchrotron X-ray diffraction was used to investigate their high-pressure phase behavior and determine their bulk moduli. All samples underwent a fluorite-to-cotunnite phase transformation with increasing pressure. The pressure of the phase transformation increased with increasing hyperstoichiometry, which is consistent with results from previous computational simulations. Bulk moduli are inversely proportional to both the ionic radius of the lanthanide and its concentration, as quantified using a weighted cationic radius ratio. As a result, this trend was found to be consistent with the behavior of other elastic properties measured for Ln-doped UO2, such as Young's modulus.},
doi = {10.1016/j.jnucmat.2017.04.007},
journal = {Journal of Nuclear Materials},
number = C,
volume = 490,
place = {United States},
year = {Mon Apr 10 00:00:00 EDT 2017},
month = {Mon Apr 10 00:00:00 EDT 2017}
}

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