Fission gas in thoria

Navaratnarajah Kuganathan, Partha S. Ghosh, Conor O.T. Galvin, Ashok K. Arya, Bijon K. Dutta, Gautam K. Dey, Robin W. Grimes

Research output: Contribution to journalArticle

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Abstract

The fission gases Xe and Kr, formed during normal reactor operation, are known to degrade fuel performance, particularly at high burn-up. Using first-principles density functional theory together with a dispersion correction (DFT + D), in ThO2 we calculate the energetics of neutral and charged point defects, the di-vacancy (DV), different neutral tri-vacancies (NTV), the charged tetravacancy (CTV) defect cluster geometries and their interaction with Xe and Kr. The most favourable incorporation point defect site for Xe or Kr in defective ThO2 is the fully charged thorium vacancy. The lowest energy NTV in larger supercells of ThO2 is NTV3, however, a single Xe atom is most stable when accommodated within a NTV1. The di-vacancy (DV) is a significantly less favoured incorporation site than the NTV1 but the CTV offers about the same incorporation energy. Incorporation of a second gas atom in a NTV is a high energy process and more unfavourable than accommodation within an existing Th vacancy. The bi-NTV (BNTV) cluster geometry studied will accommodate one or two gas atoms with low incorporation energies but the addition of a third gas atom incurs a high energy penalty. The tri-NTV cluster (TNTV) forms a larger space which accommodates three gas atoms but again there is a penalty to accommodate a fourth gas atom. By considering the energy to form the defect sites, solution energies were generated showing that in ThO2−x the most favourable solution equilibrium site is the NTV1 while in ThO2 it is the DV.

Original languageEnglish
Pages (from-to)47-55
Number of pages9
JournalJournal of Nuclear Materials
Volume485
Early online date20 Dec 2016
DOIs
Publication statusPublished - 1 Mar 2017
Externally publishedYes

Fingerprint

Thoria
Vacancies
fission
Gases
gases
Atoms
atoms
Point defects
energy
penalties
point defects
Thorium
Reactor operation
Defects
Geometry
thorium
defects
accommodation
geometry
Discrete Fourier transforms

Keywords

  • Defects
  • DFT
  • Krypton
  • Nuclear fuel
  • Thoria
  • Xenon

ASJC Scopus subject areas

  • Nuclear and High Energy Physics
  • Materials Science(all)
  • Nuclear Energy and Engineering

Cite this

Kuganathan, N., Ghosh, P. S., Galvin, C. O. T., Arya, A. K., Dutta, B. K., Dey, G. K., & Grimes, R. W. (2017). Fission gas in thoria. Journal of Nuclear Materials, 485, 47-55. https://doi.org/10.1016/j.jnucmat.2016.12.011

Fission gas in thoria. / Kuganathan, Navaratnarajah; Ghosh, Partha S.; Galvin, Conor O.T.; Arya, Ashok K.; Dutta, Bijon K.; Dey, Gautam K.; Grimes, Robin W.

In: Journal of Nuclear Materials, Vol. 485, 01.03.2017, p. 47-55.

Research output: Contribution to journalArticle

Kuganathan, N, Ghosh, PS, Galvin, COT, Arya, AK, Dutta, BK, Dey, GK & Grimes, RW 2017, 'Fission gas in thoria' Journal of Nuclear Materials, vol. 485, pp. 47-55. https://doi.org/10.1016/j.jnucmat.2016.12.011
Kuganathan N, Ghosh PS, Galvin COT, Arya AK, Dutta BK, Dey GK et al. Fission gas in thoria. Journal of Nuclear Materials. 2017 Mar 1;485:47-55. https://doi.org/10.1016/j.jnucmat.2016.12.011
Kuganathan, Navaratnarajah ; Ghosh, Partha S. ; Galvin, Conor O.T. ; Arya, Ashok K. ; Dutta, Bijon K. ; Dey, Gautam K. ; Grimes, Robin W. / Fission gas in thoria. In: Journal of Nuclear Materials. 2017 ; Vol. 485. pp. 47-55.
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