A density functional theory and neutron diffraction study of the ambient condition properties of sub-stoichiometric yttrium hydride
Abstract
Several mechanical and thermophysical properties are required as a function of non-stoichiometry for the successful implementation of YH2-x for nuclear reactor moderator applications. Density functional theory calculations, in combination with neutron diffraction experiments, were used to study the structural and mechanical properties of YH2-x. Point defect analysis indicated H occupation primarily at the tetrahedral site within an fcc Y sub-lattice, confirming a fluorite YH2 structure. The small positive formation energy for H vacancies under Y-rich conditions predicted that hypo-stoichiometry is accommodated by Y+YH2 at ambient conditions and by H vacancies in the YH2-x single phase that is relevant to high temperatures. Neutron diffraction studies were used to confirm both the occupation of H on tetrahedral sites and the near-stoichiometric composition of the hydride phase in the two-phase Y+YH2 region of the phase diagram that dominates at room temperature. Energy minimized special-quasirandom-structures of H vacancies were used to calculate lattice parameters, elastic constants, and several other properties as a function of composition for the single phase YH2-x. The lattice parameter of YH2-x decreased by only 0.004 Å with increasing H/Y for the range indicating a negligible effect on lattice parameters due to vacancy formation. In the two-phase region, however, calculations predicted the density of to increase with decreasing H/Y at lower temperatures due to the increased fraction of high-density Y metal. Additionally, for the high temperature single phase, decreasing H/Y reduced the density as a consequence of the lattice expansion associated with vacancy formation. All elastic constants and moduli increased with increasing hydrogen content in single-phase YH2-x.
- Authors:
-
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Georgia Institute of Technology, Atlanta, GA (United States)
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Civilian Nuclear Energy Programs
- Georgia Institute of Technology, Atlanta, GA (United States)
- Publication Date:
- Research Org.:
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Office of Nuclear Energy (NE). Nuclear Reactor Technologies; USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1764213
- Alternate Identifier(s):
- OSTI ID: 1810975
- Report Number(s):
- LA-UR-20-24029
Journal ID: ISSN 0022-3115; TRN: US2206430
- Grant/Contract Number:
- 89233218CNA000001; 20190649DI
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Nuclear Materials
- Additional Journal Information:
- Journal Volume: 547; Journal ID: ISSN 0022-3115
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; DFT; high temperature moderators; neutron diffraction; mechanical properties; yttrium hydride; crystal structure
Citation Formats
Mehta, Vedant Kiritkumar, Vogel, Sven C., Shivprasad, Aditya Prahlad, Luther, Erik Paul, Andersson, Anders David Ragnar, Rao, Dasari V., Kotlyar, Dan, Cooper, Michael William Donald, and Clausen, Bjorn. A density functional theory and neutron diffraction study of the ambient condition properties of sub-stoichiometric yttrium hydride. United States: N. p., 2021.
Web. doi:10.1016/j.jnucmat.2021.152837.
Mehta, Vedant Kiritkumar, Vogel, Sven C., Shivprasad, Aditya Prahlad, Luther, Erik Paul, Andersson, Anders David Ragnar, Rao, Dasari V., Kotlyar, Dan, Cooper, Michael William Donald, & Clausen, Bjorn. A density functional theory and neutron diffraction study of the ambient condition properties of sub-stoichiometric yttrium hydride. United States. https://doi.org/10.1016/j.jnucmat.2021.152837
Mehta, Vedant Kiritkumar, Vogel, Sven C., Shivprasad, Aditya Prahlad, Luther, Erik Paul, Andersson, Anders David Ragnar, Rao, Dasari V., Kotlyar, Dan, Cooper, Michael William Donald, and Clausen, Bjorn. Sat .
"A density functional theory and neutron diffraction study of the ambient condition properties of sub-stoichiometric yttrium hydride". United States. https://doi.org/10.1016/j.jnucmat.2021.152837. https://www.osti.gov/servlets/purl/1764213.
@article{osti_1764213,
title = {A density functional theory and neutron diffraction study of the ambient condition properties of sub-stoichiometric yttrium hydride},
author = {Mehta, Vedant Kiritkumar and Vogel, Sven C. and Shivprasad, Aditya Prahlad and Luther, Erik Paul and Andersson, Anders David Ragnar and Rao, Dasari V. and Kotlyar, Dan and Cooper, Michael William Donald and Clausen, Bjorn},
abstractNote = {Several mechanical and thermophysical properties are required as a function of non-stoichiometry for the successful implementation of YH2-x for nuclear reactor moderator applications. Density functional theory calculations, in combination with neutron diffraction experiments, were used to study the structural and mechanical properties of YH2-x. Point defect analysis indicated H occupation primarily at the tetrahedral site within an fcc Y sub-lattice, confirming a fluorite YH2 structure. The small positive formation energy for H vacancies under Y-rich conditions predicted that hypo-stoichiometry is accommodated by Y+YH2 at ambient conditions and by H vacancies in the YH2-x single phase that is relevant to high temperatures. Neutron diffraction studies were used to confirm both the occupation of H on tetrahedral sites and the near-stoichiometric composition of the hydride phase in the two-phase Y+YH2 region of the phase diagram that dominates at room temperature. Energy minimized special-quasirandom-structures of H vacancies were used to calculate lattice parameters, elastic constants, and several other properties as a function of composition for the single phase YH2-x. The lattice parameter of YH2-x decreased by only 0.004 Å with increasing H/Y for the range 1.31≤H/Y≤2.0 indicating a negligible effect on lattice parameters due to vacancy formation. In the two-phase region, however, calculations predicted the density of zY+(1-z)YH2-x to increase with decreasing H/Y at lower temperatures due to the increased fraction of high-density Y metal. Additionally, for the high temperature single phase, decreasing H/Y reduced the density as a consequence of the lattice expansion associated with vacancy formation. All elastic constants and moduli increased with increasing hydrogen content in single-phase YH2-x.},
doi = {10.1016/j.jnucmat.2021.152837},
journal = {Journal of Nuclear Materials},
number = ,
volume = 547,
place = {United States},
year = {Sat Jan 23 00:00:00 EST 2021},
month = {Sat Jan 23 00:00:00 EST 2021}
}
Works referenced in this record:
gsaslanguage: a GSAS script language for automated Rietveld refinements of diffraction data
journal, July 2011
- Vogel, Sven C.
- Journal of Applied Crystallography, Vol. 44, Issue 4
Analytical Bond-order Potential for hcp‐Y
journal, October 2013
- Fan, Kai‐min; Yang, Li; Tang, Jing
- Chinese Journal of Chemical Physics, Vol. 26, Issue 5
Generalized Gradient Approximation Made Simple
journal, October 1996
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
The crystal structures and lattice parameters of high-purity scandium, yttrium and the rare earth metals
journal, July 1956
- Spedding, F. H.; Daane, A. H.; Herrmann, K. W.
- Acta Crystallographica, Vol. 9, Issue 7
Crystal structure of and by neutron diffraction
journal, March 1980
- Khatamian, D.; Kamitakahara, W. A.; Barnes, R. G.
- Physical Review B, Vol. 21, Issue 6
XCII. Relations between the elastic moduli and the plastic properties of polycrystalline pure metals
journal, August 1954
- Pugh, S. F.
- The London, Edinburgh, and Dublin Philosophical Magazine and Journal of Science, Vol. 45, Issue 367
High-Temperature Diffusion of Hydrogen in YH x (1.80≤x≤1.97)*
journal, January 1989
- Stuhr, Uwe; Schlereth, Michael; Steinbinder, Detlef
- Zeitschrift für Physikalische Chemie, Vol. 164, Issue Part_1
Determination of pole figure coverage for texture measurements with neutron time-of-flight diffractometers
journal, June 2018
- Takajo, Shigehiro; Vogel, Sven C.
- Journal of Applied Crystallography, Vol. 51, Issue 3
�ber die W�rmebewegung in festen und fl�ssigen K�rpern
journal, August 1926
- Frenkel, J.
- Zeitschrift f�r Physik, Vol. 35, Issue 8-9
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996
- Kresse, G.; Furthmüller, J.
- Computational Materials Science, Vol. 6, Issue 1, p. 15-50
Hydrides as neutron moderator and reflector materials
journal, February 1971
- Vetrano, J. B.
- Nuclear Engineering and Design, Vol. 14, Issue 3
Theoretical predictions of structure and related properties of intermetallics
journal, April 1992
- Pettifor, D. G.
- Materials Science and Technology, Vol. 8, Issue 4
A six-axis robotic sample changer for high-throughput neutron powder diffraction and texture measurements
journal, November 2014
- Losko, Adrian S.; Vogel, Sven C.; Reiche, H. Matthias
- Journal of Applied Crystallography, Vol. 47, Issue 6
Extra-electron induced covalent strengthening and generalization of intrinsic ductile-to-brittle criterion
journal, October 2012
- Niu, Haiyang; Chen, Xing-Qiu; Liu, Peitao
- Scientific Reports, Vol. 2, Issue 1
Dynamical evidence of hydrogen sublattice melting in metal-hydrogen systems
journal, February 1987
- Barnes, R. G.; Borsa, F.; Jerosch-Herold, M.
- Journal of the Less Common Metals, Vol. 129
Thermodynamic modelling of Y–H and Y–Zr–H system aided by first-principles and its application in bulk hydride moderator fabrication
journal, April 2020
- Peng, Jiaqing; Wu, Ming; Du, Fu
- Journal of Nuclear Materials, Vol. 531
Experimental investigation and thermodynamic assessment of the yttrium-hydrogen binary system
journal, June 2018
- Fu, Kai; Jiang, Xiaojing; Guo, Yanru
- Progress in Natural Science: Materials International, Vol. 28, Issue 3
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996
- Kresse, G.; Furthmüller, J.
- Physical Review B, Vol. 54, Issue 16, p. 11169-11186
The Voigt‐Reuss‐Hill Approximation and Elastic Moduli of Polycrystalline MgO, CaF 2 , β‐ZnS, ZnSe, and CdTe
journal, May 1967
- Chung, D. H.; Buessem, W. R.
- Journal of Applied Physics, Vol. 38, Issue 6
Mechanical properties of yttrium hydride
journal, May 2005
- Setoyama, Daigo; Ito, Masato; Matsunaga, Junji
- Journal of Alloys and Compounds, Vol. 394, Issue 1-2
Elastic moduli of high-density, sintered monoliths of yttrium dihydride
journal, June 2020
- Shivprasad, A. P.; Frazer, D. M.; Mehta, V. K.
- Journal of Alloys and Compounds, Vol. 826
Electronic structure of metal hydrides. I. Optical studies of Sc , Y , and Lu
journal, May 1979
- Weaver, J. H.; Rosei, R.; Peterson, D. T.
- Physical Review B, Vol. 19, Issue 10
Preparation and Refining of Yttrium Metal by Y-Mg Alloy Process
journal, January 1960
- Carlson, O. N.; Haefling, J. A.; Schmidt, F. A.
- Journal of The Electrochemical Society, Vol. 107, Issue 6
Texture measurements using the new neutron diffractometer HIPPO and their analysis using the Rietveld method
journal, March 2004
- Vogel, Sven C.; Hartig, Christian; Lutterotti, Luca
- Powder Diffraction, Vol. 19, Issue 1
Poisson'S Ratio for Metals and Alloys
journal, January 1961
- KÖSter, Werner; Franz, H.
- International Materials Reviews, Vol. 6, Issue 1
DFT in a nutshell
journal, July 2012
- Burke, Kieron; Wagner, Lucas O.
- International Journal of Quantum Chemistry, Vol. 113, Issue 2
Pressure-Temperature-Composition Relationships of the Yttrium-Hydrogen System
journal, January 1962
- Lundin, C. E.; Blackledge, J. P.
- Journal of The Electrochemical Society, Vol. 109, Issue 9
Selection of a Space Reactor Moderator Using Lessons Learned from SNAP and ANP Programs
conference, August 2019
- Mehta, Vedant K.; McClure, Patrick; Kotlyar, Dan
- AIAA Propulsion and Energy 2019 Forum
Ab initio study of the structural, mechanical, and dynamical properties of the rare-earth dihydrides XH2 (X=Sc, Y, and La)
journal, November 2013
- Yang, Jin Wen; Gao, Tao; Guo, Lin Yuan
- Physica B: Condensed Matter, Vol. 429
Ab Initio Calculation of Elastic Constants of Ceramic Crystals
journal, October 2007
- Yao, Hongzhi; Ouyang, Lizhi; Ching, Wai-Yim
- Journal of the American Ceramic Society, Vol. 90, Issue 10
The Thermodynamics of the Yttrium-Hydrogen System 1
journal, August 1965
- Yannopoulos, L. N.; Edwards, R. K.; Wahlbeck, P. G.
- The Journal of Physical Chemistry, Vol. 69, Issue 8
Special quasirandom structures
journal, July 1990
- Zunger, Alex; Wei, S.-H.; Ferreira, L. G.
- Physical Review Letters, Vol. 65, Issue 3, p. 353-356
The H−Y (Hydrogen-Yttrium) system
journal, June 1988
- Khatamian, D.; Manchester, F. D.
- Bulletin of Alloy Phase Diagrams, Vol. 9, Issue 3
Ab initiomolecular dynamics for liquid metals
journal, January 1993
- Kresse, G.; Hafner, J.
- Physical Review B, Vol. 47, Issue 1, p. 558-561
Hydrogen Diffusion in f.c.c. TiH x and YH x : Two Distinct Examples for Diffusion in a Concentrated Lattice Gas
journal, September 1992
- Stuhr, U.; Steinbinder, D.; Wipf, H.
- Europhysics Letters (EPL), Vol. 20, Issue 2
Neutron scattering studies of the structure and dynamics of rare-earth hydrides and deuterides
journal, May 1997
- Udovic, T. J.; Rush, J. J.; Huang, Q.
- Journal of Alloys and Compounds, Vol. 253-254
Multicomponent multisublattice alloys, nonconfigurational entropy and other additions to the Alloy Theoretic Automated Toolkit
journal, June 2009
- van de Walle, Axel
- Calphad, Vol. 33, Issue 2
The Los Alamos Neutron Science Center
journal, June 2006
- Lisowski, Paul W.; Schoenberg, Kurt F.
- Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 562, Issue 2
High-precision sampling for Brillouin-zone integration in metals
journal, August 1989
- Methfessel, M.; Paxton, A. T.
- Physical Review B, Vol. 40, Issue 6
A profile refinement method for nuclear and magnetic structures
journal, June 1969
- Rietveld, H. M.
- Journal of Applied Crystallography, Vol. 2, Issue 2, p. 65-71
Necessary and sufficient elastic stability conditions in various crystal systems
journal, December 2014
- Mouhat, Félix; Coudert, François-Xavier
- Physical Review B, Vol. 90, Issue 22
Temperature dependence of hydrogen site occupancy in Yttrium dihydride
journal, February 1984
- Goldstone, J. A.; Eckert, J.; Richards, P. M.
- Solid State Communications, Vol. 49, Issue 5
Mechanical properties of metal dihydrides
journal, February 2016
- Schultz, Peter A.; Snow, Clark S.
- Modelling and Simulation in Materials Science and Engineering, Vol. 24, Issue 3
Standard x-ray diffraction patterns
journal, April 1951
- Swanson, H. E.; Tatge, E.
- Journal of Research of the National Bureau of Standards, Vol. 46, Issue 4
Efficient stochastic generation of special quasirandom structures
journal, September 2013
- van de Walle, A.; Tiwary, P.; de Jong, M.
- Calphad, Vol. 42
Texture analysis with the new HIPPO TOF diffractometer
journal, December 2003
- Wenk, H. -R.; Lutterotti, L.; Vogel, S.
- Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 515, Issue 3
Hydrogen locations, diffusion and the electronic density of states in yttrium dihydrides: A nuclear magnetic resonance investigation
journal, September 1980
- Anderson, D. L.; Barnes, R. G.; Hwang, T. Y.
- Journal of the Less Common Metals, Vol. 73, Issue 2