First-principles study of the surface properties of γ-LiAlO2: Stability and tritium adsorption

Jia, Ting; Zeng, Zhi; Paudel, Hari; Senor, David J.; Duan, Yuhua

doi:10.1016/j.jnucmat.2019.05.007

Title: First-principles study of the surface properties of γ-LiAlO₂: Stability and tritium adsorption

Journal Article · Tue May 07 00:00:00 EDT 2019 · Journal of Nuclear Materials

DOI:https://doi.org/10.1016/j.jnucmat.2019.05.007· OSTI ID:1582395

Jia, Ting ^[1]; Zeng, Zhi ^[2]; Paudel, Hari ^[1]; Senor, David J. ^[3];

^[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)

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 O_A atop site. With increasing ³H diffused from bulk to surface, the Al_G 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.

View Accepted Manuscript (DOE)

View Accepted Manuscript (Publisher)

Cite

Export

Save

Research Organization:: National Energy Technology Laboratory (NETL), Pittsburgh, PA, Morgantown, WV (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

OSTI ID:: 1582395

Alternate ID(s):: OSTI ID: 1547427

Report Number(s):: NETL-PUB-22174; TRN: US2100868

Journal Information:: Journal of Nuclear Materials, Vol. 522, Issue C; ISSN 0022-3115

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 9 works

Citation information provided by
Web of Science

References (38)

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
TEACUP: A Tritium Management and Supplemental Core Follow Program Lyons, Jennifer; Love, Edward; Burns, Kim Fusion Science and Technology, Vol. 71, Issue 4 https://doi.org/10.1080/15361055.2017.1290944	journal	March 2017
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set Kresse, G.; Furthmüller, J. Computational Materials Science, Vol. 6, Issue 1, p. 15-50 https://doi.org/10.1016/0927-0256(96)00008-0	journal	July 1996
Ceramic breeder material development Roux, N.; Tanaka, S.; Johnson, C. Fusion Engineering and Design, Vol. 41, Issue 1-4 https://doi.org/10.1016/S0920-3796(97)00140-3	journal	September 1998
Nanostructural evolution and behavior of H and Li in ion-implanted γ-LiAlO2 Jiang, Weilin; Zhang, Jiandong; Edwards, Danny J. Journal of Nuclear Materials, Vol. 494 https://doi.org/10.1016/j.jnucmat.2017.07.048	journal	October 2017
Nano-composite solid polymer electrolytes for solid state ionic devices Lakshman Dissanayake, M. A. K. Ionics, Vol. 10, Issue 3-4 https://doi.org/10.1007/BF02382820	journal	May 2004
Effects of radiation on lithium aluminate samples properties Botter, F.; Lefevre, F.; Rasneur, B. Journal of Nuclear Materials, Vol. 141-143 https://doi.org/10.1016/S0022-3115(86)80066-6	journal	November 1986
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
$n$ -type doping of $CuIn {Se}_{2}$ and $CuGa {Se}_{2}$ Persson, Clas; Zhao, Yu-Jun; Lany, Stephan Physical Review B, Vol. 72, Issue 3 https://doi.org/10.1103/PhysRevB.72.035211	journal	July 2005
Tritium diffusivity in lithium-based ceramic breeders irradiated with neutrons Okuno, Kenji; Kudo, Hiroshi Fusion Engineering and Design, Vol. 8 https://doi.org/10.1016/S0920-3796(89)80131-0	journal	January 1989
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
LiAlO-coated LiCoO as cathode material for lithium ion batteries Cao, H.; Xia, B.; Zhang, Y. Solid State Ionics, Vol. 176, Issue 9-10 https://doi.org/10.1016/j.ssi.2004.12.001	journal	March 2005
Lithium transport through lithium-ion battery cathode coatings Xu, Shenzhen; Jacobs, Ryan M.; Nguyen, Ha M. Journal of Materials Chemistry A, Vol. 3, Issue 33 https://doi.org/10.1039/C5TA01664A	journal	January 2015
Chemical potential dependence of defect formation energies in GaAs: Application to Ga self-diffusion Zhang, S.; Northrup, John Physical Review Letters, Vol. 67, Issue 17 https://doi.org/10.1103/PhysRevLett.67.2339	journal	October 1991
Tritium behavior in lithium ceramics Johnson, C. E. Journal of Nuclear Materials, Vol. 270, Issue 1-2 https://doi.org/10.1016/S0022-3115(98)00905-2	journal	April 1999
Self-doping of cadmium stannate in the inverse spinel structure Zhang, S. B.; Wei, Su-Huai Applied Physics Letters, Vol. 80, Issue 8 https://doi.org/10.1063/1.1452789	journal	February 2002
Commentary: The Materials Project: A materials genome approach to accelerating materials innovation Jain, Anubhav; Ong, Shyue Ping; Hautier, Geoffroy APL Materials, Vol. 1, Issue 1 https://doi.org/10.1063/1.4812323	journal	July 2013
Insights on Amorphization of Lithium Aluminate from Atomistic Simulation Setyawan, Wahyu; Senor, David J.; Devanathan, Ram The Journal of Physical Chemistry C, Vol. 121, Issue 14 https://doi.org/10.1021/acs.jpcc.6b12562	journal	March 2017
Improved adsorption energetics within density-functional theory using revised Perdew-Burke-Ernzerhof functionals Hammer, B.; Hansen, L. B.; Nørskov, J. K. Physical Review B, Vol. 59, Issue 11 https://doi.org/10.1103/PhysRevB.59.7413	journal	March 1999
Release behavior of bred tritium from LiAlO2 Nishikawa, M.; Kinjyo, T.; Ishizaka, T. Journal of Nuclear Materials, Vol. 335, Issue 1 https://doi.org/10.1016/j.jnucmat.2004.07.032	journal	October 2004
Identification of cathode materials for lithium batteries guided by first-principles calculations Ceder, G.; Chiang, Y. -M.; Sadoway, D. R. Nature, Vol. 392, Issue 6677 https://doi.org/10.1038/33647	journal	April 1998
Irradiation effects and hydrogen behavior in H2+ and He+ implanted γ-LiAlO2 single crystals Jiang, Weilin; Zhang, Jiandong; Kovarik, Libor Journal of Nuclear Materials, Vol. 484 https://doi.org/10.1016/j.jnucmat.2016.03.014	journal	February 2017
Tritium inventory in a LiAlO2 blanket Nishikawa, Masabumi; Baba, Atsushi; Kawamura, Yoshinori Journal of Nuclear Materials, Vol. 246, Issue 1 https://doi.org/10.1016/S0022-3115(97)00091-3	journal	July 1997
Diffusion-controlled tritium release from neutron-irradiated γ-LiAlO2 Okuno, Kenji; Kudo, Hiroshi Journal of Nuclear Materials, Vol. 138, Issue 2-3 https://doi.org/10.1016/0022-3115(86)90007-3	journal	April 1986
Tritium Diffusion Pathways in γ-LiAlO ₂ Pellets Used in TPBAR: A First-Principles Density Functional Theory Investigation Paudel, Hari P.; Lee, Yueh-Lin; Senor, David J. The Journal of Physical Chemistry C, Vol. 122, Issue 18 https://doi.org/10.1021/acs.jpcc.8b01108	journal	April 2018
Ab initiomolecular dynamics for liquid metals Kresse, G.; Hafner, J. Physical Review B, Vol. 47, Issue 1, p. 558-561 https://doi.org/10.1103/PhysRevB.47.558	journal	January 1993
Properties and performance of tritium breeding ceramics Roux, N.; Johnson, C.; Noda, K. Journal of Nuclear Materials, Vol. 191-194 https://doi.org/10.1016/S0022-3115(09)80005-6	journal	September 1992
The stability of ionic crystal surfaces Tasker, P. W. Journal of Physics C: Solid State Physics, Vol. 12, Issue 22 https://doi.org/10.1088/0022-3719/12/22/036	journal	November 1979
Simplified generalized-gradient approximation and anharmonicity: Benchmark calculations on molecules Patton, David C.; Porezag, Dirk V.; Pederson, Mark R. Physical Review B, Vol. 55, Issue 12 https://doi.org/10.1103/PhysRevB.55.7454	journal	March 1997
Correlation behavior of lithium and tritium in some solid breeder materials Ohno, H.; Konishi, S.; Nagasaki, T. Journal of Nuclear Materials, Vol. 133-134 https://doi.org/10.1016/0022-3115(85)90130-8	journal	August 1985
Oxidation energies of transition metal oxides within the $GGA + U$ framework Wang, Lei; Maxisch, Thomas; Ceder, Gerbrand Physical Review B, Vol. 73, Issue 19 https://doi.org/10.1103/PhysRevB.73.195107	journal	May 2006
Solid Tritium Breeder Materials-Li ₂ O and LiAlO ₂ : A Data Base Review Liu, Yung Y.; Billone, Michael C.; Fischer, A. K. Fusion Technology, Vol. 8, Issue 2P1 https://doi.org/10.13182/FST85-A24573	journal	September 1985
Chemical imaging and diffusion of hydrogen and lithium in lithium aluminate Jiang, Weilin; Spurgeon, Steven R.; Zhu, Zihua Journal of Nuclear Materials, Vol. 511 https://doi.org/10.1016/j.jnucmat.2018.08.057	journal	December 2018
Density functional theory study of the point defect energetics in γ-LiAlO2, Li2ZrO3 and Li2TiO3 materials Lee, Yueh-Lin; Holber, Jamie; Paudel, Hari P. Journal of Nuclear Materials, Vol. 511 https://doi.org/10.1016/j.jnucmat.2018.09.030	journal	December 2018
In-Situ Tritium Release Experiment from Solid Breeder γ-LiAlO ₂ in SWINPC Cao, Xiaohua; Shen, Wende; Wan, Jingping Fusion Technology, Vol. 28, Issue 3P1 https://doi.org/10.13182/FST95-A30460	journal	October 1995
Tritium recovery from nanostructured LiAlO2 Carrera, L. M.; Jiménez-Becerril, J.; Basurto, R. Journal of Nuclear Materials, Vol. 299, Issue 3 https://doi.org/10.1016/S0022-3115(01)00693-6	journal	December 2001
Nitride semiconductors free of electrostatic fields for efficient white light-emitting diodes Waltereit, P.; Brandt, O.; Trampert, A. Nature, Vol. 406, Issue 6798 https://doi.org/10.1038/35022529	journal	August 2000

Similar Records

First-principles study of the surface properties of y-LiAlO2: Stability and tritium adsorption

Journal Article · Thu Aug 15 00:00:00 EDT 2019 · Journal of Nuclear Materials · OSTI ID:1582395

Jia, Ting; Zeng, Zhi; Paudel, Hari; +2 more

First-principles study of the surface properties of LiAl₅O₈: Stability and tritiated water formation

Journal Article · Mon Nov 01 00:00:00 EDT 2021 · Journal of Nuclear Materials · OSTI ID:1582395

Jia, Ting; Senor, David J.; Duan, Yuhua

First-principles Studies of Tritium Reactivity and Diffusivity on Defective and Carbon Doped Surfaces of $\gamma$-LiAlO₂ Pellets (Tritium Science Program Report FY 2019 )

Technical Report · Sat Dec 28 00:00:00 EST 2019 · OSTI ID:1582395

Jia, Ting; Duan, Yuhua

Related Subjects

36 MATERIALS SCIENCE

Title: First-principles study of the surface properties of γ-LiAlO2: Stability and tritium adsorption

Citation Formats

References (38)

Similar Records

Related Subjects

Title: First-principles study of the surface properties of γ-LiAlO₂: Stability and tritium adsorption