Characterization of zirconium oxides part I: Raman mapping and spectral feature analysis

Raman mapping of sectioned zirconium cladding oxides was performed to analyze different spectral features before and after breakaway, as well as between zirconium and its alloys Zr-2.65Nb, Zry-3, and Zry-4. Oxide phase composition, or percent tetragonality, was defined to compare tetragonal to monoc...

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Main Authors: Corey M. Efaw, Jordan L. Vandegrift, Michael Reynolds, Samuel McMurdie, Brian J. Jaques, Hongqiang Hu, Hui Xiong, Michael F. Hurley
Format: Article
Language:English
Published: Elsevier 2019-12-01
Series:Nuclear Materials and Energy
Online Access:http://www.sciencedirect.com/science/article/pii/S2352179119300523
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author Corey M. Efaw
Jordan L. Vandegrift
Michael Reynolds
Samuel McMurdie
Brian J. Jaques
Hongqiang Hu
Hui Xiong
Michael F. Hurley
author_facet Corey M. Efaw
Jordan L. Vandegrift
Michael Reynolds
Samuel McMurdie
Brian J. Jaques
Hongqiang Hu
Hui Xiong
Michael F. Hurley
author_sort Corey M. Efaw
collection DOAJ
description Raman mapping of sectioned zirconium cladding oxides was performed to analyze different spectral features before and after breakaway, as well as between zirconium and its alloys Zr-2.65Nb, Zry-3, and Zry-4. Oxide phase composition, or percent tetragonality, was defined to compare tetragonal to monoclinic zirconia. Percent tetragonality was spatially mapped to support distinction of zirconia phase distribution. A tetragonal-rich layer was seen at the metal/oxide interface, while post-breakaway samples exhibited increased amount of tetragonal phase in the bulk of their oxides. Spatial mapping of spectral peak location and half-width at half-maximum was accomplished to distinguish differences in stability mechanisms of tetragonal-rich zirconia phase. Shifts in monoclinic peak positions provided mapping of relative stress state, supporting the differences in stabilization of tetragonal phase near the metal/oxide interface and tetragonal phase in the bulk of the oxide. Tetragonal phase near the metal/oxide interface is stabilized through support of oxygen sub-stoichiometry and compressive stress. Tetragonal phase observed in the bulk of the oxide is stabilized through oxygen sub-stoichiometry, void of compressive stress. A linear trend between percent tetragonality and stress state was determined. This resulted in a connection between mechanism of tetragonal to monoclinic phase transformation and a cladding's ability to resist oxidation and breakaway. Poor performing samples displayed greater stress gradients, driven by lattice mismatch at the metal/oxide interface, as well as between tetragonal and monoclinic phase boundaries. Tetragonal phase at the metal/oxide interface for superior performing samples have reduced epitaxial growth of tetragonal grains, lowering compressive stress gradients and provided more resistant inner-oxide layers. With increased utility of Raman spectroscopy for characterizing zirconium cladding materials, different degradation mechanisms can be further understood. Keywords: Zirconium alloys, Cladding, Oxidation, Breakaway, Raman mapping
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spelling doaj.art-f9d464e9d6ad414c9d8693be6c771fdb2022-12-21T22:52:08ZengElsevierNuclear Materials and Energy2352-17912019-12-0121Characterization of zirconium oxides part I: Raman mapping and spectral feature analysisCorey M. Efaw0Jordan L. Vandegrift1Michael Reynolds2Samuel McMurdie3Brian J. Jaques4Hongqiang Hu5Hui Xiong6Michael F. Hurley7Micron School of Materials Science and Engineering, Boise State University, 1910 W University Dr, Boise, ID 83725, USA; Center for Advanced Energy Studies, 995 University Blvd, Idaho Falls, ID 83401, USAMicron School of Materials Science and Engineering, Boise State University, 1910 W University Dr, Boise, ID 83725, USA; Center for Advanced Energy Studies, 995 University Blvd, Idaho Falls, ID 83401, USAMicron School of Materials Science and Engineering, Boise State University, 1910 W University Dr, Boise, ID 83725, USAMicron School of Materials Science and Engineering, Boise State University, 1910 W University Dr, Boise, ID 83725, USAMicron School of Materials Science and Engineering, Boise State University, 1910 W University Dr, Boise, ID 83725, USA; Center for Advanced Energy Studies, 995 University Blvd, Idaho Falls, ID 83401, USAIdaho National Laboratory, 2525 Fremont Ave, Idaho Falls, ID 83402, USAMicron School of Materials Science and Engineering, Boise State University, 1910 W University Dr, Boise, ID 83725, USA; Center for Advanced Energy Studies, 995 University Blvd, Idaho Falls, ID 83401, USAMicron School of Materials Science and Engineering, Boise State University, 1910 W University Dr, Boise, ID 83725, USA; Center for Advanced Energy Studies, 995 University Blvd, Idaho Falls, ID 83401, USA; Corresponding author at: Micron School of Materials Science and Engineering, Boise State University, 1910 W University Dr, Boise, ID 83725, USA.Raman mapping of sectioned zirconium cladding oxides was performed to analyze different spectral features before and after breakaway, as well as between zirconium and its alloys Zr-2.65Nb, Zry-3, and Zry-4. Oxide phase composition, or percent tetragonality, was defined to compare tetragonal to monoclinic zirconia. Percent tetragonality was spatially mapped to support distinction of zirconia phase distribution. A tetragonal-rich layer was seen at the metal/oxide interface, while post-breakaway samples exhibited increased amount of tetragonal phase in the bulk of their oxides. Spatial mapping of spectral peak location and half-width at half-maximum was accomplished to distinguish differences in stability mechanisms of tetragonal-rich zirconia phase. Shifts in monoclinic peak positions provided mapping of relative stress state, supporting the differences in stabilization of tetragonal phase near the metal/oxide interface and tetragonal phase in the bulk of the oxide. Tetragonal phase near the metal/oxide interface is stabilized through support of oxygen sub-stoichiometry and compressive stress. Tetragonal phase observed in the bulk of the oxide is stabilized through oxygen sub-stoichiometry, void of compressive stress. A linear trend between percent tetragonality and stress state was determined. This resulted in a connection between mechanism of tetragonal to monoclinic phase transformation and a cladding's ability to resist oxidation and breakaway. Poor performing samples displayed greater stress gradients, driven by lattice mismatch at the metal/oxide interface, as well as between tetragonal and monoclinic phase boundaries. Tetragonal phase at the metal/oxide interface for superior performing samples have reduced epitaxial growth of tetragonal grains, lowering compressive stress gradients and provided more resistant inner-oxide layers. With increased utility of Raman spectroscopy for characterizing zirconium cladding materials, different degradation mechanisms can be further understood. Keywords: Zirconium alloys, Cladding, Oxidation, Breakaway, Raman mappinghttp://www.sciencedirect.com/science/article/pii/S2352179119300523
spellingShingle Corey M. Efaw
Jordan L. Vandegrift
Michael Reynolds
Samuel McMurdie
Brian J. Jaques
Hongqiang Hu
Hui Xiong
Michael F. Hurley
Characterization of zirconium oxides part I: Raman mapping and spectral feature analysis
Nuclear Materials and Energy
title Characterization of zirconium oxides part I: Raman mapping and spectral feature analysis
title_full Characterization of zirconium oxides part I: Raman mapping and spectral feature analysis
title_fullStr Characterization of zirconium oxides part I: Raman mapping and spectral feature analysis
title_full_unstemmed Characterization of zirconium oxides part I: Raman mapping and spectral feature analysis
title_short Characterization of zirconium oxides part I: Raman mapping and spectral feature analysis
title_sort characterization of zirconium oxides part i raman mapping and spectral feature analysis
url http://www.sciencedirect.com/science/article/pii/S2352179119300523
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