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Title: Trace element migration during UF4 bomb reduction: Implications to metal fuel production, worker health and safety, and nuclear forensics

Abstract

Understanding the migration of trace contaminants during the production of U metal is vital for fabricating advanced nuclear fuels, for managing worker health and safety at foundry and processing facilities, and for advancing nuclear forensic science. A common method used to produce actinide metals is the bomb reduction of suitable U precursors. Here, we report the results of a series of experiments designed to quantitatively track the trace contaminants Th, Ca, and Mg through a bomb reduction of UF4 using a vacuum induction furnace. In this series, UF4 charges were doped with elemental Th at 0 (a blank), 1, 10, 100, and 1000 ppm Th/U. Following reduction, the metal ingot products and the associated slag and crucibles were individually digested and analyzed using inductively coupled plasma-mass spectrometry. The results show that Th fractionation occurred at all concentrations but was most significant, and near quantitative, in samples starting with Th concentrations below 100 ppm. Thorium was found to incorporate into the slag and crucible in roughly equal proportions during reduction. Furthermore, a significant amount of U and Ca migrated into the crucible walls, each correlating positively with the quantities of Mg migrating from the MgO crucible to the U metal product.

Authors:
; ; ; ; ORCiD logo;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1462579
Alternate Identifier(s):
OSTI ID: 1464491
Report Number(s):
PNNL-SA-133845
Journal ID: ISSN 0022-3115; S0022311518305270; PII: S0022311518305270
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Published Article
Journal Name:
Journal of Nuclear Materials
Additional Journal Information:
Journal Name: Journal of Nuclear Materials Journal Volume: 510 Journal Issue: C; Journal ID: ISSN 0022-3115
Publisher:
Elsevier
Country of Publication:
Netherlands
Language:
English
Subject:
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; Nuclear fuel; Uranium; Thorium; Fractionation; Nuclear forensics; Bomb reduction; Metal

Citation Formats

Reilly, Dallas D., Athon, Matthew T., Corbey, Jordan F., Leavy, Ian I., McCoy, Kaylyn M., and Schwantes, Jon M. Trace element migration during UF4 bomb reduction: Implications to metal fuel production, worker health and safety, and nuclear forensics. Netherlands: N. p., 2018. Web. doi:10.1016/j.jnucmat.2018.07.052.
Reilly, Dallas D., Athon, Matthew T., Corbey, Jordan F., Leavy, Ian I., McCoy, Kaylyn M., & Schwantes, Jon M. Trace element migration during UF4 bomb reduction: Implications to metal fuel production, worker health and safety, and nuclear forensics. Netherlands. https://doi.org/10.1016/j.jnucmat.2018.07.052
Reilly, Dallas D., Athon, Matthew T., Corbey, Jordan F., Leavy, Ian I., McCoy, Kaylyn M., and Schwantes, Jon M. Thu . "Trace element migration during UF4 bomb reduction: Implications to metal fuel production, worker health and safety, and nuclear forensics". Netherlands. https://doi.org/10.1016/j.jnucmat.2018.07.052.
@article{osti_1462579,
title = {Trace element migration during UF4 bomb reduction: Implications to metal fuel production, worker health and safety, and nuclear forensics},
author = {Reilly, Dallas D. and Athon, Matthew T. and Corbey, Jordan F. and Leavy, Ian I. and McCoy, Kaylyn M. and Schwantes, Jon M.},
abstractNote = {Understanding the migration of trace contaminants during the production of U metal is vital for fabricating advanced nuclear fuels, for managing worker health and safety at foundry and processing facilities, and for advancing nuclear forensic science. A common method used to produce actinide metals is the bomb reduction of suitable U precursors. Here, we report the results of a series of experiments designed to quantitatively track the trace contaminants Th, Ca, and Mg through a bomb reduction of UF4 using a vacuum induction furnace. In this series, UF4 charges were doped with elemental Th at 0 (a blank), 1, 10, 100, and 1000 ppm Th/U. Following reduction, the metal ingot products and the associated slag and crucibles were individually digested and analyzed using inductively coupled plasma-mass spectrometry. The results show that Th fractionation occurred at all concentrations but was most significant, and near quantitative, in samples starting with Th concentrations below 100 ppm. Thorium was found to incorporate into the slag and crucible in roughly equal proportions during reduction. Furthermore, a significant amount of U and Ca migrated into the crucible walls, each correlating positively with the quantities of Mg migrating from the MgO crucible to the U metal product.},
doi = {10.1016/j.jnucmat.2018.07.052},
journal = {Journal of Nuclear Materials},
number = C,
volume = 510,
place = {Netherlands},
year = {Thu Nov 01 00:00:00 EDT 2018},
month = {Thu Nov 01 00:00:00 EDT 2018}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1016/j.jnucmat.2018.07.052

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Cited by: 7 works
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Works referencing / citing this record:

Atomic spectrometry update: review of advances in the analysis of metals, chemicals and materials
journal, January 2019

  • Carter, Simon; Clough, Robert; Fisher, Andy
  • Journal of Analytical Atomic Spectrometry, Vol. 34, Issue 11
  • DOI: 10.1039/c9ja90058f