Rights statement: This is the author’s version of a work that was accepted for publication in Solid State Ionics. Changes resulting from the publishing process, such as peer review, editing, corrections, structural formatting, and other quality control mechanisms may not be reflected in this document. Changes may have been made to this work since it was submitted for publication. A definitive version was subsequently published in Solid State Ionics, 373, 2022 DOI: 10.1016/j.ssi.2021.115813
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Available under license: CC BY-NC-ND
Final published version
Research output: Contribution to Journal/Magazine › Journal article › peer-review
Research output: Contribution to Journal/Magazine › Journal article › peer-review
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TY - JOUR
T1 - The accommodation of lithium in bulk ZrO2
AU - Stephens, G.F.
AU - Than, Y.R.
AU - Neilson, W.
AU - Evitts, L.J.
AU - Wenman, M.R.
AU - Murphy, S.T.
AU - Grimes, R.W.
AU - Cole-Baker, A.
AU - Ortner, S.
AU - Gotham, N.
AU - Rushton, M.J.D.
AU - Lee, W.E.
AU - Middleburgh, S.C.
N1 - This is the author’s version of a work that was accepted for publication in Solid State Ionics. Changes resulting from the publishing process, such as peer review, editing, corrections, structural formatting, and other quality control mechanisms may not be reflected in this document. Changes may have been made to this work since it was submitted for publication. A definitive version was subsequently published in Solid State Ionics, 373, 2022 DOI: 10.1016/j.ssi.2021.115813
PY - 2021/12/15
Y1 - 2021/12/15
N2 - Lithium is known to accelerate the corrosion of zirconium alloys in light water reactor conditions. Identifying the mechanism by which this occurs will allow alloying additions and alternative coolant chemistries to be proposed with the aim of improved performance. Accommodation mechanisms for Li in bulk ZrO2 were investigated using density functional theory (DFT). Defects including oxygen and zirconium vacancies along with lithium, zirconium and oxygen interstitials and several small clusters were modelled. Predicted formation energies were used to construct Brouwer diagrams. These show how competing defect species concentrations change across the monoclinic and tetragonal oxide layers. The solubility of Li into ZrO2 was determined to be very low indicating that Li solution into the bulk, under equilibrium conditions, is an unlikely cause for accelerated corrosion.
AB - Lithium is known to accelerate the corrosion of zirconium alloys in light water reactor conditions. Identifying the mechanism by which this occurs will allow alloying additions and alternative coolant chemistries to be proposed with the aim of improved performance. Accommodation mechanisms for Li in bulk ZrO2 were investigated using density functional theory (DFT). Defects including oxygen and zirconium vacancies along with lithium, zirconium and oxygen interstitials and several small clusters were modelled. Predicted formation energies were used to construct Brouwer diagrams. These show how competing defect species concentrations change across the monoclinic and tetragonal oxide layers. The solubility of Li into ZrO2 was determined to be very low indicating that Li solution into the bulk, under equilibrium conditions, is an unlikely cause for accelerated corrosion.
KW - Brouwer diagram
KW - Fermi-Dirac
KW - Lithium accelerated corrosion
KW - Solubility
KW - Zirconia
KW - Corrosion
KW - Density functional theory
KW - Light water reactors
KW - Lithium
KW - Oxygen
KW - Zircaloy
KW - Accelerated corrosion
KW - Alloying additions
KW - Brouwe diagram
KW - Coolant chemistry
KW - Density-functional-theory
KW - Light water reactor conditions
KW - Oxygen interstitials
KW - Performance
U2 - 10.1016/j.ssi.2021.115813
DO - 10.1016/j.ssi.2021.115813
M3 - Journal article
VL - 373
JO - Solid State Ionics
JF - Solid State Ionics
SN - 0167-2738
M1 - 115813
ER -