First-principles study of the surface properties of γ-LiAlO2: Stability and tritium adsorption
Abstract
γ-LiAlO2 enriched with 6Li isotope exhibits excellent performance under neutron radiation and is used in tritium-producing burnable absorber rods (TPBARs) to produce tritium (T, 3H) in pressurized water reactor (PWR). Here, to better understand the 3H formation and diffusion on the surfaces, the first-principles calculations are performed to study the stability of γ-LiAlO2 surface and the 3H adsorption on the surface. By considering all possible symmetrical stoichiometric and nonstoichiometric low-index surfaces, two most stable surfaces, one stoichiometric (100) and one nonstoichiometric (101), were identified. The 3H adsorption and diffusion on the most stable (100) surface were further explored, and the obtained results show that there are four stable sites (three O and one Al atop) for 3H adsorption. The calculated Bader charges of atoms reflect that 3H adsorption on the top of O site is a reduction process, while on the top of Al site is an oxidation one. Under low adsorption coverage of 1/4 per surface unit cell, 3H atoms are adsorbed on the most stable OA atop site. With increasing 3H diffused from bulk to surface, the AlG site is the second choice for 3H adsorption, and then the OB site. The coverage of 2/4 is the mostmore »
- Authors:
-
[1]
- National Energy Technology Lab. (NETL), Pittsburgh, PA (United States)
- Chinese Academy of Sciences, Hefei (China)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Publication Date:
- Research Org.:
- National Energy Technology Laboratory (NETL), Pittsburgh, PA, Morgantown, WV (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1582395
- Alternate Identifier(s):
- OSTI ID: 1547427
- Report Number(s):
- NETL-PUB-22174
Journal ID: ISSN 0022-3115; TRN: US2100868
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Nuclear Materials
- Additional Journal Information:
- Journal Volume: 522; Journal Issue: C; Journal ID: ISSN 0022-3115
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Jia, Ting, Zeng, Zhi, Paudel, Hari, Senor, David J., and Duan, Yuhua. First-principles study of the surface properties of γ-LiAlO2: Stability and tritium adsorption. United States: N. p., 2019.
Web. doi:10.1016/j.jnucmat.2019.05.007.
Jia, Ting, Zeng, Zhi, Paudel, Hari, Senor, David J., & Duan, Yuhua. First-principles study of the surface properties of γ-LiAlO2: Stability and tritium adsorption. United States. https://doi.org/10.1016/j.jnucmat.2019.05.007
Jia, Ting, Zeng, Zhi, Paudel, Hari, Senor, David J., and Duan, Yuhua. Tue .
"First-principles study of the surface properties of γ-LiAlO2: Stability and tritium adsorption". United States. https://doi.org/10.1016/j.jnucmat.2019.05.007. https://www.osti.gov/servlets/purl/1582395.
@article{osti_1582395,
title = {First-principles study of the surface properties of γ-LiAlO2: Stability and tritium adsorption},
author = {Jia, Ting and Zeng, Zhi and Paudel, Hari and Senor, David J. and Duan, Yuhua},
abstractNote = {γ-LiAlO2 enriched with 6Li isotope exhibits excellent performance under neutron radiation and is used in tritium-producing burnable absorber rods (TPBARs) to produce tritium (T, 3H) in pressurized water reactor (PWR). Here, to better understand the 3H formation and diffusion on the surfaces, the first-principles calculations are performed to study the stability of γ-LiAlO2 surface and the 3H adsorption on the surface. By considering all possible symmetrical stoichiometric and nonstoichiometric low-index surfaces, two most stable surfaces, one stoichiometric (100) and one nonstoichiometric (101), were identified. The 3H adsorption and diffusion on the most stable (100) surface were further explored, and the obtained results show that there are four stable sites (three O and one Al atop) for 3H adsorption. The calculated Bader charges of atoms reflect that 3H adsorption on the top of O site is a reduction process, while on the top of Al site is an oxidation one. Under low adsorption coverage of 1/4 per surface unit cell, 3H atoms are adsorbed on the most stable OA atop site. With increasing 3H diffused from bulk to surface, the AlG site is the second choice for 3H adsorption, and then the OB site. The coverage of 2/4 is the most favorable 3H adsorption state due to the counteracted charge transfer. Finally, when the coverage is up to 4/4, the interaction between 3H atoms leads to partial formation of T2 molecule that desorbs from surface. Therefore, T2 molecule should be the main product from the perfect surface of γ-LiAlO2 at high 3H coverage.},
doi = {10.1016/j.jnucmat.2019.05.007},
journal = {Journal of Nuclear Materials},
number = C,
volume = 522,
place = {United States},
year = {Tue May 07 00:00:00 EDT 2019},
month = {Tue May 07 00:00:00 EDT 2019}
}
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Works referenced in this record:
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
TEACUP: A Tritium Management and Supplemental Core Follow Program
journal, March 2017
- Lyons, Jennifer; Love, Edward; Burns, Kim
- Fusion Science and Technology, Vol. 71, Issue 4
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
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
Ceramic breeder material development
journal, September 1998
- Roux, N.; Tanaka, S.; Johnson, C.
- Fusion Engineering and Design, Vol. 41, Issue 1-4
Nanostructural evolution and behavior of H and Li in ion-implanted γ-LiAlO2
journal, October 2017
- Jiang, Weilin; Zhang, Jiandong; Edwards, Danny J.
- Journal of Nuclear Materials, Vol. 494
Nano-composite solid polymer electrolytes for solid state ionic devices
journal, May 2004
- Lakshman Dissanayake, M. A. K.
- Ionics, Vol. 10, Issue 3-4
Effects of radiation on lithium aluminate samples properties
journal, November 1986
- Botter, F.; Lefevre, F.; Rasneur, B.
- Journal of Nuclear Materials, Vol. 141-143
Special points for Brillouin-zone integrations
journal, June 1976
- Monkhorst, Hendrik J.; Pack, James D.
- Physical Review B, Vol. 13, Issue 12, p. 5188-5192
-type doping of and
journal, July 2005
- Persson, Clas; Zhao, Yu-Jun; Lany, Stephan
- Physical Review B, Vol. 72, Issue 3
Tritium diffusivity in lithium-based ceramic breeders irradiated with neutrons
journal, January 1989
- Okuno, Kenji; Kudo, Hiroshi
- Fusion Engineering and Design, Vol. 8
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
LiAlO-coated LiCoO as cathode material for lithium ion batteries
journal, March 2005
- Cao, H.; Xia, B.; Zhang, Y.
- Solid State Ionics, Vol. 176, Issue 9-10
Lithium transport through lithium-ion battery cathode coatings
journal, January 2015
- Xu, Shenzhen; Jacobs, Ryan M.; Nguyen, Ha M.
- Journal of Materials Chemistry A, Vol. 3, Issue 33
Chemical potential dependence of defect formation energies in GaAs: Application to Ga self-diffusion
journal, October 1991
- Zhang, S.; Northrup, John
- Physical Review Letters, Vol. 67, Issue 17
Tritium behavior in lithium ceramics
journal, April 1999
- Johnson, C. E.
- Journal of Nuclear Materials, Vol. 270, Issue 1-2
Self-doping of cadmium stannate in the inverse spinel structure
journal, February 2002
- Zhang, S. B.; Wei, Su-Huai
- Applied Physics Letters, Vol. 80, Issue 8
Commentary: The Materials Project: A materials genome approach to accelerating materials innovation
journal, July 2013
- Jain, Anubhav; Ong, Shyue Ping; Hautier, Geoffroy
- APL Materials, Vol. 1, Issue 1
Insights on Amorphization of Lithium Aluminate from Atomistic Simulation
journal, March 2017
- Setyawan, Wahyu; Senor, David J.; Devanathan, Ram
- The Journal of Physical Chemistry C, Vol. 121, Issue 14
Improved adsorption energetics within density-functional theory using revised Perdew-Burke-Ernzerhof functionals
journal, March 1999
- Hammer, B.; Hansen, L. B.; Nørskov, J. K.
- Physical Review B, Vol. 59, Issue 11
Release behavior of bred tritium from LiAlO2
journal, October 2004
- Nishikawa, M.; Kinjyo, T.; Ishizaka, T.
- Journal of Nuclear Materials, Vol. 335, Issue 1
Identification of cathode materials for lithium batteries guided by first-principles calculations
journal, April 1998
- Ceder, G.; Chiang, Y. -M.; Sadoway, D. R.
- Nature, Vol. 392, Issue 6677
Irradiation effects and hydrogen behavior in H2+ and He+ implanted γ-LiAlO2 single crystals
journal, February 2017
- Jiang, Weilin; Zhang, Jiandong; Kovarik, Libor
- Journal of Nuclear Materials, Vol. 484
Tritium inventory in a LiAlO2 blanket
journal, July 1997
- Nishikawa, Masabumi; Baba, Atsushi; Kawamura, Yoshinori
- Journal of Nuclear Materials, Vol. 246, Issue 1
Diffusion-controlled tritium release from neutron-irradiated γ-LiAlO2
journal, April 1986
- Okuno, Kenji; Kudo, Hiroshi
- Journal of Nuclear Materials, Vol. 138, Issue 2-3
Tritium Diffusion Pathways in γ-LiAlO 2 Pellets Used in TPBAR: A First-Principles Density Functional Theory Investigation
journal, April 2018
- Paudel, Hari P.; Lee, Yueh-Lin; Senor, David J.
- The Journal of Physical Chemistry C, Vol. 122, Issue 18
Ab initiomolecular dynamics for liquid metals
journal, January 1993
- Kresse, G.; Hafner, J.
- Physical Review B, Vol. 47, Issue 1, p. 558-561
Properties and performance of tritium breeding ceramics
journal, September 1992
- Roux, N.; Johnson, C.; Noda, K.
- Journal of Nuclear Materials, Vol. 191-194
The stability of ionic crystal surfaces
journal, November 1979
- Tasker, P. W.
- Journal of Physics C: Solid State Physics, Vol. 12, Issue 22
Simplified generalized-gradient approximation and anharmonicity: Benchmark calculations on molecules
journal, March 1997
- Patton, David C.; Porezag, Dirk V.; Pederson, Mark R.
- Physical Review B, Vol. 55, Issue 12
Correlation behavior of lithium and tritium in some solid breeder materials
journal, August 1985
- Ohno, H.; Konishi, S.; Nagasaki, T.
- Journal of Nuclear Materials, Vol. 133-134
Oxidation energies of transition metal oxides within the framework
journal, May 2006
- Wang, Lei; Maxisch, Thomas; Ceder, Gerbrand
- Physical Review B, Vol. 73, Issue 19
Solid Tritium Breeder Materials-Li 2 O and LiAlO 2 : A Data Base Review
journal, September 1985
- Liu, Yung Y.; Billone, Michael C.; Fischer, A. K.
- Fusion Technology, Vol. 8, Issue 2P1
Chemical imaging and diffusion of hydrogen and lithium in lithium aluminate
journal, December 2018
- Jiang, Weilin; Spurgeon, Steven R.; Zhu, Zihua
- Journal of Nuclear Materials, Vol. 511
Density functional theory study of the point defect energetics in γ-LiAlO2, Li2ZrO3 and Li2TiO3 materials
journal, December 2018
- Lee, Yueh-Lin; Holber, Jamie; Paudel, Hari P.
- Journal of Nuclear Materials, Vol. 511
In-Situ Tritium Release Experiment from Solid Breeder γ-LiAlO 2 in SWINPC
journal, October 1995
- Cao, Xiaohua; Shen, Wende; Wan, Jingping
- Fusion Technology, Vol. 28, Issue 3P1
Tritium recovery from nanostructured LiAlO2
journal, December 2001
- Carrera, L. M.; Jiménez-Becerril, J.; Basurto, R.
- Journal of Nuclear Materials, Vol. 299, Issue 3
Nitride semiconductors free of electrostatic fields for efficient white light-emitting diodes
journal, August 2000
- Waltereit, P.; Brandt, O.; Trampert, A.
- Nature, Vol. 406, Issue 6798