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Title: Tritium Diffusion Pathways in γ-LiAlO 2 Pellets Used in TPBAR: A First-Principles Density Functional Theory Investigation

Abstract

With superior thermophysical and thermochemical properties, γ-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 6Li. In radiation damaged γ-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 γ-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 × 10–12 m2/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.

Authors:
 [1];  [1];  [2]; ORCiD logo [1]
  1. National Energy Technology Lab. (NETL), Pittsburgh, PA, (United States)
  2. 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); USDOE Office of Fossil Energy (FE)
OSTI Identifier:
1461484
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 122; Journal Issue: 18; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Paudel, Hari P., Lee, Yueh-Lin, Senor, David J., and Duan, Yuhua. Tritium Diffusion Pathways in γ-LiAlO 2 Pellets Used in TPBAR: A First-Principles Density Functional Theory Investigation. United States: N. p., 2018. Web. https://doi.org/10.1021/acs.jpcc.8b01108.
Paudel, Hari P., Lee, Yueh-Lin, Senor, David J., & Duan, Yuhua. Tritium Diffusion Pathways in γ-LiAlO 2 Pellets Used in TPBAR: A First-Principles Density Functional Theory Investigation. United States. https://doi.org/10.1021/acs.jpcc.8b01108
Paudel, Hari P., Lee, Yueh-Lin, Senor, David J., and Duan, Yuhua. Wed . "Tritium Diffusion Pathways in γ-LiAlO 2 Pellets Used in TPBAR: A First-Principles Density Functional Theory Investigation". United States. https://doi.org/10.1021/acs.jpcc.8b01108. https://www.osti.gov/servlets/purl/1461484.
@article{osti_1461484,
title = {Tritium Diffusion Pathways in γ-LiAlO 2 Pellets Used in TPBAR: A First-Principles Density Functional Theory Investigation},
author = {Paudel, Hari P. and Lee, Yueh-Lin and Senor, David J. and Duan, Yuhua},
abstractNote = {With superior thermophysical and thermochemical properties, γ-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 6Li. In radiation damaged γ-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 γ-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 × 10–12 m2/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.},
doi = {10.1021/acs.jpcc.8b01108},
journal = {Journal of Physical Chemistry. C},
number = 18,
volume = 122,
place = {United States},
year = {2018},
month = {4}
}

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Works referenced in this record:

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
  • DOI: 10.1038/35022529

LiAlO-coated LiCoO as cathode material for lithium ion batteries
journal, March 2005


Nano-composite solid polymer electrolytes for solid state ionic devices
journal, May 2004


Effects of radiation on lithium aluminate samples properties
journal, November 1986


Preparation, characterization, and chemistry of solid ceramic breeder materials
journal, January 1981


Tritium behavior in lithium ceramics
journal, April 1999


Ceramic breeder materials: Status and needs
journal, October 1998


Release behavior of bred tritium from LiAlO2
journal, October 2004


Diffusion-controlled tritium release from neutron-irradiated γ-LiAlO2
journal, April 1986


Ceramic breeder material development
journal, September 1998


Properties and performance of tritium breeding ceramics
journal, September 1992


Interstitial Lithium Diffusion Pathways in γ-LiAlO 2 : A Computational Study
journal, October 2015


Lithium diffusion in γ-LiAlO2, a molecular dynamics simulation
journal, September 1996

  • Jacobs, Jean-Paul; San Miguel, Miguel Angel; Alvarez, Luis Javier
  • Journal of Nuclear Materials, Vol. 232, Issue 2-3
  • DOI: 10.1016/S0022-3115(96)00435-7

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
  • DOI: 10.1021/acs.jpcc.6b12562

Tritium Solubility in Li 2 TiO 3 from First-Principles Simulations
journal, December 2014

  • Murphy, Samuel T.
  • The Journal of Physical Chemistry C, Vol. 118, Issue 51
  • DOI: 10.1021/jp508875y

Point Defects and Non-stoichiometry in Li 2 TiO 3
journal, February 2014

  • Murphy, Samuel T.; Hine, Nicholas D. M.
  • Chemistry of Materials, Vol. 26, Issue 4
  • DOI: 10.1021/cm4038473

Li Ion Dynamics in a LiAlO 2 Single Crystal Studied by 7 Li NMR Spectroscopy and Conductivity Measurements
journal, June 2012

  • Indris, Sylvio; Heitjans, Paul; Uecker, Reinhard
  • The Journal of Physical Chemistry C, Vol. 116, Issue 27
  • DOI: 10.1021/jp3042928

Tritium recovery from nanostructured LiAlO2
journal, December 2001


Tritium diffusivity in lithium-based ceramic breeders irradiated with neutrons
journal, January 1989


Nanostructural evolution and behavior of H and Li in ion-implanted γ-LiAlO2
journal, October 2017


Irradiation effects and hydrogen behavior in H2+ and He+ implanted γ-LiAlO2 single crystals
journal, February 2017


Chemical states of tritium and interaction with radiation damages in Li2O crystals
journal, March 1986


Correlation Between Annihilation of Radiation Defects and Tritium Release in Neutron-Irradiated LiAlO 2
journal, August 2005

  • Oyaidzu, M.; Takeda, T.; Kimura, H.
  • Fusion Science and Technology, Vol. 48, Issue 1
  • DOI: 10.13182/FST05-A1006

Ab initiomolecular dynamics for liquid metals
journal, January 1993


Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium
journal, May 1994


Projector augmented-wave method
journal, December 1994


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
  • DOI: 10.1103/PhysRevLett.77.3865

Optimization methods for finding minimum energy paths
journal, April 2008

  • Sheppard, Daniel; Terrell, Rye; Henkelman, Graeme
  • The Journal of Chemical Physics, Vol. 128, Issue 13
  • DOI: 10.1063/1.2841941

A generalized solid-state nudged elastic band method
journal, February 2012

  • Sheppard, Daniel; Xiao, Penghao; Chemelewski, William
  • The Journal of Chemical Physics, Vol. 136, Issue 7
  • DOI: 10.1063/1.3684549

Fully Ab Initio Finite-Size Corrections for Charged-Defect Supercell Calculations
journal, January 2009


The crystal structure and anomalous dispersion of γ-LiAlO 2
journal, September 1965


Finite Elastic Strain of Cubic Crystals
journal, June 1947


First-Principles Calculation of Self-Diffusion Coefficients
journal, May 2008


Lattice-geometry effects in garnet solid electrolytes: a lattice-gas Monte Carlo simulation study
journal, November 2017


    Works referencing / citing this record:

    Atomistic Simulations of the Defect Chemistry and Self-Diffusion of Li-ion in LiAlO2
    journal, July 2019

    • Kuganathan, N.; Dark, J.; Sgourou, E. N.
    • Energies, Vol. 12, Issue 15
    • DOI: 10.3390/en12152895