Site-specific nanoscale characterization of zirconium hydrides in the hydride rim structure of hydrogen-charged zircaloy-4 cladding

Rittenhouse, Joshua Eddy; Pradhan, Arnold; Kamerman, David W.; Burns, Jatuporn; Xu, Fei; Wen, Haiming; Yao, Tiankai

doi:10.1016/j.matchar.2025.115006

Site-specific nanoscale characterization of zirconium hydrides in the hydride rim structure of hydrogen-charged zircaloy-4 cladding

Journal Article · Wed Apr 02 00:00:00 EDT 2025 · Materials Characterization

DOI:https://doi.org/10.1016/j.matchar.2025.115006· OSTI ID:2583266

^[1]; Pradhan, Arnold ^[1]; ^[1]; ^[1]; Xu, Fei ^[1]; ^[2]; ^[1]

Idaho National Laboratory (INL), Idaho Falls, ID (United States)
Missouri Univ. of Science and Technology, Rolla, MO (United States)

Zircaloy-4 cladding tubes were hydrogen-charged using a static pressure hydrogen charging method to experimentally produce a zirconium-hydride rim structure similar to that observed in Zircaloy-4 cladding tubes after operation in commercial light-water nuclear reactors. Detailed characterization was performed using electron energy loss spectroscopy (EELS) and four-dimensional scanning transmission electron microscopy (4D-STEM). By mapping the position of the plasmon peak in the low-loss EELS spectrum, it was determined that the zirconium hydrides formed were predominantly solid δ-phase zirconium hydrides. 4D-STEM was used to generate phase and strain maps at nanoscale. The interactions between two zirconium hydride platelets less than 200 nm apart leads to the localized lattice rotations and possible phase change, revealing a potential hydride growth mechanism.

View Accepted Manuscript (DOE)

Research Organization:: Idaho National Laboratory (INL), Idaho Falls, ID (United States)

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE)

Grant/Contract Number:: AC07-05ID14517

OSTI ID:: 2583266

Report Number(s):: INL/JOU--24-77839-Rev000

Journal Information:: Materials Characterization, Journal Name: Materials Characterization Vol. 224; ISSN 1044-5803

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (35)

The precipitation of γ-hydride plates in zirconium Weatherly, G. C. Acta Metallurgica, Vol. 29, Issue 3 https://doi.org/10.1016/0001-6160(81)90074-2	journal	March 1981
Hydride precipitation in α/β zirconium alloys Perovic, V.; Weatherly, G. C.; Simpson, C. J. Acta Metallurgica, Vol. 31, Issue 9 https://doi.org/10.1016/0001-6160(83)90008-1	journal	September 1983
The orientation of zirconium hydride on grain boundaries in zircaloy-2 Arunachalam, V. S.; Lehtinen, B.; Östberg, G. Journal of Nuclear Materials, Vol. 21, Issue 3 https://doi.org/10.1016/0022-3115(67)90174-2	journal	March 1967
The habit planes of zirconium hydride in zirconium and zircaloy Westlake, D. G. Journal of Nuclear Materials, Vol. 26, Issue 2 https://doi.org/10.1016/0022-3115(68)90072-X	journal	May 1968
Solid state phase equilibria of zircaloy-4 in the temperature range 750–1050°C Miquet, A.; Charquet, D.; Allibert, C. H. Journal of Nuclear Materials, Vol. 105, Issue 2-3 https://doi.org/10.1016/0022-3115(82)90367-1	journal	February 1982
Intergranular δ-hydride nucleation and orientation in zirconium alloys Qin, W.; Kiran Kumar, N. A. P.; Szpunar, J. A. Acta Materialia, Vol. 59, Issue 18 https://doi.org/10.1016/j.actamat.2011.07.054	journal	October 2011
Microstructure and formation mechanisms of δ-hydrides in variable grain size Zircaloy-4 studied by electron backscatter diffraction Wang, Siyang; Giuliani, Finn; Britton, T. Ben Acta Materialia, Vol. 169 https://doi.org/10.1016/j.actamat.2019.02.042	journal	May 2019
On potential core-shell morphologies of δ-hydride precipitates in zircaloy-2: A microstructural characterization approach by electron diffraction and energy-loss spectroscopy Badr, N. N.; Long, F.; Luo, Y. Acta Materialia, Vol. 257 https://doi.org/10.1016/j.actamat.2023.119184	journal	September 2023
On the effects of transformation strain induced by hydride precipitation Taherijam, Masoud; Marashi, Saiedeh; Tondro, Alireza Acta Materialia, Vol. 261 https://doi.org/10.1016/j.actamat.2023.119356	journal	December 2023
Hydrogen in Zircaloy: Mechanism and its impacts Suman, Siddharth; Khan, Mohd. Kaleem; Pathak, Manabendra International Journal of Hydrogen Energy, Vol. 40, Issue 17 https://doi.org/10.1016/j.ijhydene.2015.03.049	journal	May 2015
Investigation of mechanical properties of ε-zirconium hydride using micro- and nano-indentation techniques Xu, Jiujun; Shi, San-Qiang Journal of Nuclear Materials, Vol. 327, Issue 2-3 https://doi.org/10.1016/j.jnucmat.2004.02.004	journal	May 2004
Strain evolution of zirconium hydride embedded in a Zircaloy-2 matrix Kerr, M.; Daymond, M. R.; Holt, R. A. Journal of Nuclear Materials, Vol. 380, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2008.07.004	journal	October 2008
Identification and quantification of hydride phases in Zircaloy-4 cladding using synchrotron X-ray diffraction Daum, R. S.; Chu, Y. S.; Motta, A. T. Journal of Nuclear Materials, Vol. 392, Issue 3 https://doi.org/10.1016/j.jnucmat.2009.04.004	journal	August 2009
Study on the effects of matrix yield strength on hydride phase stability in Zircaloy-2 and Zr 2.5wt% Nb Tulk, E.; Kerr, M.; Daymond, M. R. Journal of Nuclear Materials, Vol. 425, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2011.10.051	journal	June 2012
Effect of He implantation on the microstructure of zircaloy-4 studied using in situ TEM Tunes, M. A.; Harrison, R. W.; Greaves, G. Journal of Nuclear Materials, Vol. 493 https://doi.org/10.1016/j.jnucmat.2017.06.012	journal	September 2017
The effect of cooling rate and grain size on hydride microstructure in Zircaloy-4 Birch, Ruth; Wang, Siyang; Tong, Vivian S. Journal of Nuclear Materials, Vol. 513 https://doi.org/10.1016/j.jnucmat.2018.11.011	journal	January 2019
Effects of hydride rim on the ductility of Zircaloy-4 cladding Kim, Ju-Seong; Kim, Ho-A; Kang, So-Young Journal of Nuclear Materials, Vol. 523 https://doi.org/10.1016/j.jnucmat.2019.06.007	journal	September 2019
Formation and characterization of hydride rim structures in Zircaloy-4 nuclear fuel cladding tubes Kamerman, David; Bachhav, Mukesh; Yao, Tiankai Journal of Nuclear Materials, Vol. 586 https://doi.org/10.1016/j.jnucmat.2023.154675	journal	December 2023
Automated crystal orientation and phase mapping in TEM Rauch, E. F.; Véron, M. Materials Characterization, Vol. 98 https://doi.org/10.1016/j.matchar.2014.08.010	journal	December 2014
Characterization of local deformation around hydrides in Zircaloy-4 using conventional and high angular resolution electron backscatter diffraction Birch, Ruth M.; Douglas, James O.; Britton, T. Ben Materials Characterization, Vol. 202 https://doi.org/10.1016/j.matchar.2023.112988	journal	August 2023
Site specific dependencies of hydrogen concentrations in zirconium hydrides Tunes, Matheus A.; Silva, Chinthaka M.; Edmondson, Philip D. Scripta Materialia, Vol. 158 https://doi.org/10.1016/j.scriptamat.2018.08.044	journal	January 2019
High-resolution elastic strain measurement from electron backscatter diffraction patterns: New levels of sensitivity Wilkinson, Angus J.; Meaden, Graham; Dingley, David J. Ultramicroscopy, Vol. 106, Issue 4-5 https://doi.org/10.1016/j.ultramic.2005.10.001	journal	March 2006
Importance of TEM sample thickness for measuring strain fields Kang, Sangjun; Wang, Di; Kübel, Christian Ultramicroscopy, Vol. 255 https://doi.org/10.1016/j.ultramic.2023.113844	journal	January 2024
py4DSTEM: A Software Package for Four-Dimensional Scanning Transmission Electron Microscopy Data Analysis Savitzky, Benjamin H.; Zeltmann, Steven E.; Hughes, Lauren A. Microscopy and Microanalysis https://doi.org/10.1017/S1431927621000477	journal	May 2021
Miniature all-solid-state heterostructure nanowire Li-ion batteries as a tool for engineering and structural diagnostics of nanoscale electrochemical processes Oleshko, Vladimir P.; Lam, Thomas; Ruzmetov, Dmitry Nanoscale, Vol. 6, Issue 20 https://doi.org/10.1039/C4NR01666A	journal	January 2014
EELS characterization of zirconium hydrides Woo, On Ting; Carpenter, Graham J. C. Microscopy Microanalysis Microstructures, Vol. 3, Issue 1, p. 35-44 https://doi.org/10.1051/mmm:019920030103500	journal	February 1992
Investigation of Hydride Rim Effect on Failure of Zircaloy-4 Cladding with Tube Burst Test Nagase, Fumihisa; Fuketa, Toyoshi Journal of Nuclear Science and Technology, Vol. 42, Issue 1 https://doi.org/10.1080/18811248.2005.9726364	journal	January 2005
Behavior of Pre-hydrided Zircaloy-4 Cladding under Simulated LOCA Conditions Nagase, Fumihisa; Fuketa, Toyoshi Journal of Nuclear Science and Technology, Vol. 42, Issue 2 https://doi.org/10.1080/18811248.2005.9726381	journal	February 2005
Understanding deformation with high angular resolution electron backscatter diffraction (HR-EBSD) Britton, T. B.; Hickey, J. L. R. IOP Conference Series: Materials Science and Engineering, Vol. 304 https://doi.org/10.1088/1757-899X/304/1/012003	journal	January 2018
Solute hydrogen and hydride phase implications on the plasticity of zirconium and titanium alloys: a review and some recent advances Conforto, E.; Guillot, I.; Feaugas, X. Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 375, Issue 2098 https://doi.org/10.1098/rsta.2016.0417	journal	June 2017
More features, more tools, more CrysTBox Klinger, Miloslav Journal of Applied Crystallography, Vol. 50, Issue 4 https://doi.org/10.1107/S1600576717006793	journal	July 2017
Image Contrast And Localized Signal Selection Techniques Howie, A. Journal of Microscopy, Vol. 117, Issue 1 https://doi.org/10.1111/j.1365-2818.1979.tb00228.x	journal	September 1979
Identification and characterization of a new zirconium hydride Zhao, Z.; Morniroli, J. -P.; Legris, A. Journal of Microscopy, Vol. 232, Issue 3 https://doi.org/10.1111/j.1365-2818.2008.02136.x	journal	December 2008
Fabrication of hollow coaxial Al2O3/ZnAl2O4 high aspect ratio freestanding nanotubes based on the Kirkendall effect Shkondin, Evgeniy; Alimadadi, Hossein; Takayama, Osamu Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 38, Issue 1 https://doi.org/10.1116/1.5130176	journal	December 2019
High resolution mapping of strains and rotations using electron backscatter diffraction Wilkinson, A. J.; Meaden, G.; Dingley, D. J. Materials Science and Technology, Vol. 22, Issue 11 https://doi.org/10.1179/174328406X130966	journal	November 2006

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Site-specific nanoscale characterization of zirconium hydrides in the hydride rim structure of hydrogen-charged zircaloy-4 cladding

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