Effect of Mg and Ni impurities on tritium diffusion in lithium ceramics through cluster dynamics simulations

Roy, Ankit; Pitike, Krishna Chaitanya; Matthews, Christopher; Andersson, David A.; Casella, Andrew M.; Devanathan, Ram; Senor, David J.

doi:10.1016/j.jnucmat.2025.155736

Effect of Mg and Ni impurities on tritium diffusion in lithium ceramics through cluster dynamics simulations

Journal Article · Tue Mar 04 23:00:00 EST 2025 · Journal of Nuclear Materials

DOI:https://doi.org/10.1016/j.jnucmat.2025.155736· OSTI ID:2588696

^[1]; Pitike, Krishna Chaitanya ^[1]; Matthews, Christopher ^[2]; Andersson, David A. ^[2]; ^[1]; ^[1]; ^[1]

Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

This study investigates the impact of Mg and Ni doping on tritium diffusion in LiAlO₂ and LiAl₅O₈ ceramics, that are used in tritium-producing burnable absorber rods (TPBARs). Utilizing Centipede simulations across a broad temperature range (500 K to 1250 K), we explore the interplay between defect dynamics, cluster formation, and tritium mobility. In LiAlO₂, Mg doping significantly enhances tritium diffusivity by increasing tritium interstitial concentrations and diffusion coefficients of key species, thereby doubling the overall tritium diffusivity. Ni doping, while shifting the dominant defect to Li vacancies, maintains high tritium mobility due to the low binding energy of Li vacancy-tritium complexes, which ensures effective tritium migration. In LiAl₅O₈, Mg and Ni doping results in a slight reduction in the diffusion coefficients of key species, yet the dramatic increase in tritium interstitial concentrations compensates, leading to a net small increase in tritium diffusivity. In conclusion, the findings highlight the critical role of defects in tritium transport and the effect of Mg and Ni defects on the performance of these ceramics in demanding nuclear environments.

View Accepted Manuscript (DOE)

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

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

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 2588696

Report Number(s):: PNNL-SA--204584

Journal Information:: Journal of Nuclear Materials, Journal Name: Journal of Nuclear Materials Vol. 608; ISSN 0022-3115

Publisher:: Elsevier BVCopyright Statement

Country of Publication:: United States

Language:: English

References (27)

Effect of the damping function in dispersion corrected density functional theory Grimme, Stefan; Ehrlich, Stephan; Goerigk, Lars Journal of Computational Chemistry, Vol. 32, Issue 7 https://doi.org/10.1002/jcc.21759	journal	March 2011
Enhanced tritium transport and release by solids modification Kopasz, J. P.; Tam, S. W.; Johnson, C. E. Journal of Nuclear Materials, Vol. 179-181 https://doi.org/10.1016/0022-3115(91)90213-Q	journal	March 1991
Vacancy formation energies and migration barriers in multi-principal element alloys Roy, Ankit; Singh, Prashant; Balasubramanian, Ganesh Acta Materialia, Vol. 226 https://doi.org/10.1016/j.actamat.2021.117611	journal	March 2022
Atomistic simulations to reveal HIP-bonding mechanisms of Al6061/Al6061 Roy, Ankit; Kalsar, Rajib; Song, Miao Acta Materialia, Vol. 281 https://doi.org/10.1016/j.actamat.2024.120402	journal	December 2024
Low energy atomic traps sluggardize the diffusion in compositionally complex refractory alloys Roy, Ankit; Munshi, Joydeep; Balasubramanian, Ganesh Intermetallics, Vol. 131 https://doi.org/10.1016/j.intermet.2021.107106	journal	April 2021
Accumulation of helium in tungsten irradiated by helium and neutrons Xu, Q.; Yoshida, N.; Yoshiie, T. Journal of Nuclear Materials, Vol. 367-370 https://doi.org/10.1016/j.jnucmat.2007.03.078	journal	August 2007
Cluster dynamics modeling of accumulation and diffusion of helium in neutron irradiated tungsten Li, Y. G.; Zhou, W. H.; Huang, L. F. Journal of Nuclear Materials, Vol. 431, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2011.12.015	journal	December 2012
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
Atomistic modeling of out-of-pile xenon diffusion by vacancy clusters in UO2 Perriot, Romain; Matthews, Christopher; Cooper, Michael W. D. Journal of Nuclear Materials, Vol. 520 https://doi.org/10.1016/j.jnucmat.2019.03.050	journal	July 2019
Cluster dynamics simulation of uranium self-diffusion during irradiation in UO2 Matthews, Christopher; Perriot, Romain; Cooper, Michael W. D. Journal of Nuclear Materials, Vol. 527 https://doi.org/10.1016/j.jnucmat.2019.151787	journal	December 2019
Cluster dynamics simulation of xenon diffusion during irradiation in UO2 Matthews, Christopher; Perriot, Romain; Cooper, M. W. D. Journal of Nuclear Materials, Vol. 540 https://doi.org/10.1016/j.jnucmat.2020.152326	journal	November 2020
Molecular dynamics simulations of radiation response of LiAlO2 and LiAl5O8 Roy, Ankit; Senor, David J.; Casella, Andrew M. Journal of Nuclear Materials, Vol. 576 https://doi.org/10.1016/j.jnucmat.2023.154280	journal	April 2023
Insights into radiation resistance of titanium alloys from displacement cascade simulations Roy, Ankit; Senor, David J.; Edwards, Danny J. Journal of Nuclear Materials, Vol. 586 https://doi.org/10.1016/j.jnucmat.2023.154695	journal	December 2023
Microstructural and compositional evolutions in γ-LiAlO2 pellets during ion irradiation at an elevated temperature Jiang, Weilin; Kovarik, Libor; Wirth, Mark G. Journal of Nuclear Materials, Vol. 591 https://doi.org/10.1016/j.jnucmat.2024.154925	journal	April 2024
Cluster dynamics simulations of tritium and helium diffusion in lithium ceramics Roy, Ankit; Sassi, Michel; Pitike, Krishna Chaitanya Journal of Nuclear Materials, Vol. 592 https://doi.org/10.1016/j.jnucmat.2024.154970	journal	April 2024
Formation of interstitial loops in tungsten under helium ion irradiation: Rate theory modeling and experiment Watanabe, Y.; Iwakiri, H.; Yoshida, N. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 255, Issue 1 https://doi.org/10.1016/j.nimb.2006.11.008	journal	February 2007
MOOSE: Enabling massively parallel multiphysics simulation Permann, Cody J.; Gaston, Derek R.; Andrš, David SoftwareX, Vol. 11 https://doi.org/10.1016/j.softx.2020.100430	journal	January 2020
Comprehensive Analysis of Hydrogen, Deuterium, Tritium and Isotopic Ratios of Other Light Elements in Neutron Irradiated TPBAR Components Devaraj, Arun; Matthews, Bethany; Arey, Bruce Microscopy and Microanalysis, Vol. 25, Issue S2 https://doi.org/10.1017/S1431927619002137	journal	August 2019
First-Principles Study of Tritium Trapping in γ-LiAlO₂ Nanovoids Sassi, Michel; Spurgeon, Steven R.; Matthews, Bethany E. The Journal of Physical Chemistry C, Vol. 126, Issue 12 https://doi.org/10.1021/acs.jpcc.2c00381	journal	March 2022
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
A review of displacement cascade simulations using molecular dynamics emphasizing interatomic potentials for TPBAR components Roy, Ankit; Nandipati, Giridhar; Casella, Andrew M. npj Materials Degradation, Vol. 9, Issue 1 https://doi.org/10.1038/s41529-024-00536-9	journal	January 2025
Molecular dynamics study of grain boundaries as defect sinks under irradiation in LiAlO2 and LiAl5O8 Roy, Ankit; Jiang, Weilin; Nandipati, Giridhar npj Materials Degradation, Vol. 9, Issue 1 https://doi.org/10.1038/s41529-025-00565-y	journal	February 2025
Molecular dynamics simulations of displacement cascades in LiAlO2 and LiAl5O8 ceramics Roy, Ankit; Casella, Andrew M.; Senor, David J. Scientific Reports, Vol. 14, Issue 1 https://doi.org/10.1038/s41598-024-51222-4	journal	January 2024
A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu Grimme, Stefan; Antony, Jens; Ehrlich, Stephan The Journal of Chemical Physics, Vol. 132, Issue 15 https://doi.org/10.1063/1.3382344	journal	April 2010
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
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

Similar Records

Cluster dynamics simulations of tritium and helium diffusion in lithium ceramics

Journal Article · Thu Feb 15 23:00:00 EST 2024 · Journal of Nuclear Materials · OSTI ID:2406926

Microstructure-dependent rate theory model of defect segregation and phase stability in irradiated polycrystalline LiAlO₂

Journal Article · Mon Dec 20 23:00:00 EST 2021 · Modelling and Simulation in Materials Science and Engineering · OSTI ID:1915261

Molecular dynamics study of grain boundaries as defect sinks under irradiation in LiAlO₂ and LiAl₅O₈

Journal Article · Wed Feb 26 23:00:00 EST 2025 · npj Materials Degradation · OSTI ID:2565344

Related Subjects

Cluster dynamics
DFT
Defect clusters
LiAl5O8
LiAlO2
Mg and Ni impurities
Tritium diffusion

Effect of Mg and Ni impurities on tritium diffusion in lithium ceramics through cluster dynamics simulations

Citation Formats

References (27)

Similar Records

Related Subjects