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Title: An electrochemical technique for controlled dissolution of zirconium based components of light water reactors

Abstract

Zircaloy-4 (Zr-4) based liners and getters are the principle functional components of Tritium-Producing Burnable Absorber Rods (TPBARs) in light water nuclear reactors where they reduce tritiated water into tritium gas. Upon tritium exposure, zirconium tritide is formed, which changes the chemical composition, structure and morphology of these materials. Their thermodynamic properties are affected by (i) the hydride phase identity, (ii) radial and spatial tritide/hydride (T/H) distribution, and (iii) the changes in structure and morphology of the material upon T/H-migration, and their comprehensive knowledge is needed to predict performance of these materials. This work demonstrates that controlled potential electrochemistry techniques to be highly efficient for controlled oxidative radial dissolution of Zr-4 based liners (both unloaded and loaded with hydride/deuteride as chemical surrogates for tritium). The electrodissolution is further combined with microscopic techniques to accurately determine the distribution of hydride phases. This work demonstrates a reliable technique for radially etching the liners after irradiation to provide insight into the radial and spatial distribution of tritium within the TPBAR, improving the fundamental understanding of tritium transport and providing a basis for validating predictive models.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [1];  [1];  [1]; ORCiD logo [1];  [1];  [2];  [1]
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  1. Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, USA
  2. Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, USA
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1490768
Alternate Identifier(s):
OSTI ID: 1491720
Report Number(s):
PNNL-SA-140123
Journal ID: ISSN 2046-2069; RSCACL
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Published Article
Journal Name:
RSC Advances
Additional Journal Information:
Journal Name: RSC Advances Journal Volume: 9 Journal Issue: 4; Journal ID: ISSN 2046-2069
Publisher:
Royal Society of Chemistry (RSC)
Country of Publication:
United Kingdom
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Chatterjee, Sayandev, Fujimoto, Meghan S., Canfield, Nathan L., Elmore, Monte R., Olson, Devin W., Buck, Edgar C., Conroy, Michele A., Varga, Tamas, and Senor, David J. An electrochemical technique for controlled dissolution of zirconium based components of light water reactors. United Kingdom: N. p., 2019. Web. doi:10.1039/C8RA08693A.
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Chatterjee, Sayandev, Fujimoto, Meghan S., Canfield, Nathan L., Elmore, Monte R., Olson, Devin W., Buck, Edgar C., Conroy, Michele A., Varga, Tamas, & Senor, David J. An electrochemical technique for controlled dissolution of zirconium based components of light water reactors. United Kingdom. https://doi.org/10.1039/C8RA08693A
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Chatterjee, Sayandev, Fujimoto, Meghan S., Canfield, Nathan L., Elmore, Monte R., Olson, Devin W., Buck, Edgar C., Conroy, Michele A., Varga, Tamas, and Senor, David J. Mon . "An electrochemical technique for controlled dissolution of zirconium based components of light water reactors". United Kingdom. https://doi.org/10.1039/C8RA08693A.
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@article{osti_1490768,
title = {An electrochemical technique for controlled dissolution of zirconium based components of light water reactors},
author = {Chatterjee, Sayandev and Fujimoto, Meghan S. and Canfield, Nathan L. and Elmore, Monte R. and Olson, Devin W. and Buck, Edgar C. and Conroy, Michele A. and Varga, Tamas and Senor, David J.},
abstractNote = {Zircaloy-4 (Zr-4) based liners and getters are the principle functional components of Tritium-Producing Burnable Absorber Rods (TPBARs) in light water nuclear reactors where they reduce tritiated water into tritium gas. Upon tritium exposure, zirconium tritide is formed, which changes the chemical composition, structure and morphology of these materials. Their thermodynamic properties are affected by (i) the hydride phase identity, (ii) radial and spatial tritide/hydride (T/H) distribution, and (iii) the changes in structure and morphology of the material upon T/H-migration, and their comprehensive knowledge is needed to predict performance of these materials. This work demonstrates that controlled potential electrochemistry techniques to be highly efficient for controlled oxidative radial dissolution of Zr-4 based liners (both unloaded and loaded with hydride/deuteride as chemical surrogates for tritium). The electrodissolution is further combined with microscopic techniques to accurately determine the distribution of hydride phases. This work demonstrates a reliable technique for radially etching the liners after irradiation to provide insight into the radial and spatial distribution of tritium within the TPBAR, improving the fundamental understanding of tritium transport and providing a basis for validating predictive models.},
doi = {10.1039/C8RA08693A},
journal = {RSC Advances},
number = 4,
volume = 9,
place = {United Kingdom},
year = {2019},
month = {1}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1039/C8RA08693A
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Figures / Tables:

Fig. 1 Fig. 1: A schematic representation of the TPBAR with its various components. Adapted from Tritium Readiness Subprogram Project Execution Plan 2006.
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