Tritium Diffusion Pathways in y-LiAlO2 Pellets Used in TPBAR: A First-Principles Density Functional Theory Investigation

Paudel, Hari; Lee, Yueh-Lin; Senor, David J.; Duan, Yuhua

doi:10.1021/acs.jpcc.8b01108

Tritium Diffusion Pathways in y-LiAlO2 Pellets Used in TPBAR: A First-Principles Density Functional Theory Investigation

Journal Article · Thu May 10 04:00:00 EDT 2018 · Journal of Physical Chemistry C

DOI:https://doi.org/10.1021/acs.jpcc.8b01108· OSTI ID:1576574

Paudel, Hari ^[1]; Lee, Yueh-Lin ^[1]; Senor, David J. ^[2]; Duan, Yuhua ^[1]

National Energy Technology Laboratory
BATTELLE (PACIFIC NW LAB)

With superior thermophysical and thermochemical properties, gamma-LiAlO2 has high compatibility with other blanket materials and is used in the form of an annular pellet in tritium-producing burnable absorber rods (TPBARs) to produce tritium by thermal neutron irradiation of Li-6. In radiation damaged gamma-LiAlO2, different types of vacancies, defects of its constituent elements, and other trapping sites hinder the diffusion process of tritium. In this study, the first-principles density functional theory approach is used to study the diffusion mechanisms of tritium defect and its species, such as interstitial and substitutional tritium defects, oxygen-tritium vacancy defects, and interaction of tritium with oxygen vacancies in defective and nondefective gamma-LiAlO2. The obtained results provide an understanding of how such defects hamper the diffusivity and solubility of tritium. By calculating several different diffusion pathways, our results show that the smallest activation energy barrier is 0.63 eV for substitutional tritium diffusion with a diffusion coefficient of 3.25 X 10(-12) m(2)/s. The smallest oxygen-tritium diffusion barrier is found to be 2.17 eV, which is around 3.5 times higher than the tritium diffusion barrier alone.

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 1576574

Report Number(s):: PNNL-SA-136350

Journal Information:: Journal of Physical Chemistry C, Journal Name: Journal of Physical Chemistry C Journal Issue: 18 Vol. 122

Country of Publication:: United States

Language:: English

References (39)

Interstitial Lithium Diffusion Pathways in γ-LiAlO ₂ : A Computational Study Islam, Mazharul M.; Bredow, Thomas The Journal of Physical Chemistry Letters, Vol. 6, Issue 22 https://doi.org/10.1021/acs.jpclett.5b01780	journal	October 2015
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
A hydrolysis-hydrothermal route for the synthesis of ultrathin LiAlO ₂ -inlaid LiNi _0.5 Co _0.2 Mn _0.3 O ₂ as a high-performance cathode material for lithium ion batteries Li, Lingjun; Chen, Zhaoyong; Zhang, Qiaobao Journal of Materials Chemistry A, Vol. 3, Issue 2 https://doi.org/10.1039/C4TA05902F	journal	January 2015
Ab initio study of tritium defects in lithium oxide Shah, R.; Vita, A. De; Payne, M. C. Journal of Physics: Condensed Matter, Vol. 7, Issue 35 https://doi.org/10.1088/0953-8984/7/35/005	journal	August 1995
Lattice-geometry effects in garnet solid electrolytes: a lattice-gas Monte Carlo simulation study Morgan, Benjamin J. Royal Society Open Science, Vol. 4, Issue 11 https://doi.org/10.1098/rsos.170824	journal	November 2017
Optimization methods for finding minimum energy paths Sheppard, Daniel; Terrell, Rye; Henkelman, Graeme The Journal of Chemical Physics, Vol. 128, Issue 13 https://doi.org/10.1063/1.2841941	journal	April 2008
Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium Kresse, G.; Hafner, J. Physical Review B, Vol. 49, Issue 20, p. 14251-14269 https://doi.org/10.1103/PhysRevB.49.14251	journal	May 1994
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
Lithium diffusion in γ-LiAlO2, a molecular dynamics simulation Jacobs, Jean-Paul; San Miguel, Miguel Angel; Alvarez, Luis Javier Journal of Nuclear Materials, Vol. 232, Issue 2-3 https://doi.org/10.1016/S0022-3115(96)00435-7	journal	September 1996
Finite Elastic Strain of Cubic Crystals Birch, Francis Physical Review, Vol. 71, Issue 11 https://doi.org/10.1103/PhysRev.71.809	journal	June 1947
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
A generalized solid-state nudged elastic band method Sheppard, Daniel; Xiao, Penghao; Chemelewski, William The Journal of Chemical Physics, Vol. 136, Issue 7 https://doi.org/10.1063/1.3684549	journal	February 2012
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
Li ion diffusion in LiAlO 2 investigated by Raman spectroscopy Hu, Qiwei; Lei, Li; Jiang, Xiaodong Solid State Sciences, Vol. 37 https://doi.org/10.1016/j.solidstatesciences.2014.08.017	journal	November 2014
Point Defects and Non-stoichiometry in Li ₂ TiO ₃ Murphy, Samuel T.; Hine, Nicholas D. M. Chemistry of Materials, Vol. 26, Issue 4 https://doi.org/10.1021/cm4038473	journal	February 2014
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
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
Correlation Between Annihilation of Radiation Defects and Tritium Release in Neutron-Irradiated LiAlO ₂ Oyaidzu, M.; Takeda, T.; Kimura, H. Fusion Science and Technology, Vol. 48, Issue 1 https://doi.org/10.13182/FST05-A1006	journal	August 2005
Tritium Solubility in Li ₂ TiO ₃ from First-Principles Simulations Murphy, Samuel T. The Journal of Physical Chemistry C, Vol. 118, Issue 51 https://doi.org/10.1021/jp508875y	journal	December 2014
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
Ceramic breeder materials: Status and needs Johnson, C. E.; Noda, K.; Roux, N. Journal of Nuclear Materials, Vol. 258-263 https://doi.org/10.1016/S0022-3115(98)00357-2	journal	October 1998
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
Chemical states of tritium and interaction with radiation damages in Li2O crystals Okuno, Kenji; Kudo, Hiroshi Journal of Nuclear Materials, Vol. 138, Issue 1 https://doi.org/10.1016/0022-3115(86)90251-5	journal	March 1986
Unravelling Ultraslow Lithium-Ion Diffusion in γ-LiAlO ₂ : Experiments with Tracers, Neutrons, and Charge Carriers Wiedemann, Dennis; Nakhal, Suliman; Rahn, Johanna Chemistry of Materials, Vol. 28, Issue 3 https://doi.org/10.1021/acs.chemmater.5b04608	journal	January 2016
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
First-Principles Calculation of Self-Diffusion Coefficients Mantina, M.; Wang, Y.; Arroyave, R. Physical Review Letters, Vol. 100, Issue 21 https://doi.org/10.1103/PhysRevLett.100.215901	journal	May 2008
Li Ion Dynamics in a LiAlO ₂ Single Crystal Studied by ⁷ Li NMR Spectroscopy and Conductivity Measurements Indris, Sylvio; Heitjans, Paul; Uecker, Reinhard The Journal of Physical Chemistry C, Vol. 116, Issue 27 https://doi.org/10.1021/jp3042928	journal	June 2012
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
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
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
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
Fully Ab Initio Finite-Size Corrections for Charged-Defect Supercell Calculations Freysoldt, Christoph; Neugebauer, Jörg; Van de Walle, Chris G. Physical Review Letters, Vol. 102, Issue 1 https://doi.org/10.1103/PhysRevLett.102.016402	journal	January 2009
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
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
Order vs. disorder—a huge increase in ionic conductivity of nanocrystalline LiAlO ₂ embedded in an amorphous-like matrix of lithium aluminate Wohlmuth, D.; Epp, V.; Bottke, P. J. Mater. Chem. A, Vol. 2, Issue 47 https://doi.org/10.1039/C4TA02923B	journal	January 2014
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
Preparation, characterization, and chemistry of solid ceramic breeder materials Arons, R. M.; Poeppel, R. B.; Tetenbaum, M. Journal of Nuclear Materials, Vol. 103 https://doi.org/10.1016/0022-3115(82)90660-2	journal	January 1981
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
The crystal structure and anomalous dispersion of γ-LiAlO ₂ Marezio, M. Acta Crystallographica, Vol. 19, Issue 3 https://doi.org/10.1107/S0365110X65003511	journal	September 1965

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