Radionuclide incorporation in negative thermal expansion α-Zr(WO4)2: A density functional theory study

Kim, Eunja; Weck, Philippe F.; Greathouse, Jeffery A.; Gordon, Margaret E.; Bryan, Charles R.

doi:10.1016/j.cplett.2020.137172

Radionuclide incorporation in negative thermal expansion α-Zr(WO₄)₂: A density functional theory study

Journal Article · Wed Apr 01 00:00:00 EDT 2020 · Chemical Physics Letters

DOI:https://doi.org/10.1016/j.cplett.2020.137172· OSTI ID:1617302

^[1]; Weck, Philippe F. ^[2]; Greathouse, Jeffery A. ^[2]; Gordon, Margaret E. ^[2]; Bryan, Charles R. ^[2]

Univ. of Nevada, Las Vegas, NV (United States)
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

The incorporation of uranium, plutonium and technetium in the negative thermal expansion (NTE) α-Zr (WO₄)₂ has been investigated within the framework of density functional theory (DFT). It is found that the vacancy formation energies of the charged vacancies are overall larger than that of its counterpart neutral Frenkel defects and Schottky defects. DFT calculations suggest that U and Pu substitutions for the Zr site are preferred in α-Zr (WO₄)₂. In case of Tc substitution, both Tc(IV) for the Zr site and Tc(VII) for the W site are considered under oxygen-poor and oxygen-rich conditions, while Tc(VII) substitution can be improved significantly by including Y₂O₃ (charge compensation).

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE), Fuel Cycle Technologies

Grant/Contract Number:: AC04-94AL85000

OSTI ID:: 1617302

Alternate ID(s):: OSTI ID: 1703137

Report Number(s):: SAND--2019-14350J; 682693

Journal Information:: Chemical Physics Letters, Journal Name: Chemical Physics Letters Vol. 744; ISSN 0009-2614

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (26)

Structure of Zr2(WO4)(PO4)2 from Powder X-Ray Data: Cation Ordering with No Superstructure Evans, J. S. O.; Mary, T. A.; Sleight, A. W. Journal of Solid State Chemistry, Vol. 120, Issue 1 https://doi.org/10.1006/jssc.1995.1383	journal	November 1995
Ordered and Defect Structures in the UO2–WO3System, Revealed by HREM Sundberg, Margareta; Marinder, Bengt-Olov Journal of Solid State Chemistry, Vol. 121, Issue 1 https://doi.org/10.1006/jssc.1996.0024	journal	January 1996
Negative Thermal Expansion in a Large Molybdate and Tungstate Family Evans, J. S. O.; Mary, T. A.; Sleight, A. W. Journal of Solid State Chemistry, Vol. 133, Issue 2 https://doi.org/10.1006/jssc.1997.7605	journal	November 1997
Synthesis of novel nanomaterials and their application in efficient removal of radionuclides Wang, Xiangxue; Chen, Long; Wang, Lin Science China Chemistry, Vol. 62, Issue 8 https://doi.org/10.1007/s11426-019-9492-4	journal	June 2019
Heat capacities, third-law entropies and thermodynamic functions of the negative thermal expansion materials, cubic α-ZrW2O8 and cubic ZrMo2O8, from K Stevens, Rebecca; Linford, Jessica; Woodfield, Brian F. The Journal of Chemical Thermodynamics, Vol. 35, Issue 6 https://doi.org/10.1016/S0021-9614(03)00050-8	journal	June 2003
Phonon density of states and thermodynamic properties in cubic and orthorhombic phases of ZrW2O8 Mittal, R.; Chaplot, S. L. Solid State Communications, Vol. 115, Issue 6 https://doi.org/10.1016/S0038-1098(00)00180-0	journal	June 2000
Lattice dynamics and thermomechanical properties of zirconium(IV) chloride: Evidence for low-temperature negative thermal expansion Kim, Eunja; Weck, Philippe F.; Borjas, Rosendo Chemical Physics Letters, Vol. 691 https://doi.org/10.1016/j.cplett.2017.10.065	journal	January 2018
Assessing exchange-correlation functionals for elasticity and thermodynamics of α - ZrW 2 O 8 : A density functional perturbation theory study Weck, Philippe F.; Kim, Eunja; Greathouse, Jeffery A. Chemical Physics Letters, Vol. 698 https://doi.org/10.1016/j.cplett.2018.03.025	journal	April 2018
Negative Thermal Expansion in ZrW ₂ O ₈ and HfW ₂ O ₈ Evans, J. S. O.; Mary, T. A.; Vogt, T. Chemistry of Materials, Vol. 8, Issue 12 https://doi.org/10.1021/cm9602959	journal	January 1996
The immobilization of high level radioactive wastes using ceramics and glasses Donald, I. W.; Metcalfe, B. L.; Taylor, R. N. J. Journal of Materials Science, Vol. 32, Issue 22, p. 5851-5887 https://doi.org/10.1023/A:1018646507438	journal	January 1997
Mechanical properties of zirconium alloys and zirconium hydrides predicted from density functional perturbation theory Weck, Philippe F.; Kim, Eunja; Tikare, Veena Dalton Transactions, Vol. 44, Issue 43 https://doi.org/10.1039/C5DT03403E	journal	January 2015
Assessing Hubbard-corrected AM05+U and PBEsol+U density functionals for strongly correlated oxides CeO ₂ and Ce ₂ O ₃ Weck, Philippe F.; Kim, Eunja Physical Chemistry Chemical Physics, Vol. 18, Issue 38 https://doi.org/10.1039/C6CP05479J	journal	January 2016
Technetium incorporation in scheelite: insights from first-principles Ackerman, Matthew; Kim, Eunja; Weck, Philippe F. Dalton Transactions, Vol. 45, Issue 45 https://doi.org/10.1039/C6DT03626K	journal	January 2016
Nuclear waste forms for actinides Ewing, R. C. Proceedings of the National Academy of Sciences, Vol. 96, Issue 7 https://doi.org/10.1073/pnas.96.7.3432	journal	March 1999
Self-radiation damage and recovery in Pu-doped zircon Weber, W. J. Radiation Effects and Defects in Solids, Vol. 115, Issue 4 https://doi.org/10.1080/10420159108220580	journal	January 1991
Negative thermal expansion and associated anomalous physical properties: review of the lattice dynamics theoretical foundation Dove, Martin T.; Fang, Hong Reports on Progress in Physics, Vol. 79, Issue 6 https://doi.org/10.1088/0034-4885/79/6/066503	journal	May 2016
Special points for Brillouin-zone integrations Monkhorst, Hendrik J.; Pack, James D. Physical Review B, Vol. 13, Issue 12, p. 5188-5192 https://doi.org/10.1103/PhysRevB.13.5188	journal	June 1976
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
Negative thermal expansion in cubic ZrW 2 O 8 : Role of phonons in the entire Brillouin zone from ab initio calculations Gupta, M. K.; Mittal, R.; Chaplot, S. L. Physical Review B, Vol. 88, Issue 1 https://doi.org/10.1103/PhysRevB.88.014303	journal	July 2013
First-Principles Mode Gruneisen Parameters and Negative Thermal Expansion in α − ZrW 2 O 8 Gava, V.; Martinotto, A. L.; Perottoni, C. A. Physical Review Letters, Vol. 109, Issue 19 https://doi.org/10.1103/PhysRevLett.109.195503	journal	November 2012
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Large Low Temperature Specific Heat in the Negative Thermal Expansion Compound ZrW 2 O 8 Ramirez, A. P.; Kowach, G. R. Physical Review Letters, Vol. 80, Issue 22 https://doi.org/10.1103/PhysRevLett.80.4903	journal	June 1998
Negative Thermal Expansion from 0.3 to 1050 Kelvin in ZrW2O8 Mary, T. A.; Evans, J. S. O.; Vogt, T. Science, Vol. 272, Issue 5258 https://doi.org/10.1126/science.272.5258.90	journal	April 1996
Compressibility, Phase Transitions, and Oxygen Migration in Zirconium Tungstate, ZrW2O8 Evans, J. S. O. Science, Vol. 275, Issue 5296 https://doi.org/10.1126/science.275.5296.61	journal	January 1997
Technetium in the Nuclear Fuel Cycle, in Medicine and in the Environment Lieser, K. H. Radiochimica Acta, Vol. 63, Issue s1 https://doi.org/10.1524/ract.1993.63.special-issue.5	journal	January 1993
Zircon: A host-phase for the disposal of weapons plutonium Ewing, R. C.; Lutze, Werner; Weber, William J. Journal of Materials Research, Vol. 10, Issue 2 https://doi.org/10.1557/JMR.1995.0243	journal	February 1995

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Radionuclide incorporation
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Radionuclide incorporation in negative thermal expansion α-Zr(WO4)2: A density functional theory study

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Radionuclide incorporation in negative thermal expansion α-Zr(WO₄)₂: A density functional theory study