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Title: Gas-phase molybdenum-99 separation from uranium dioxide by fluoride volatility using nitrogen trifluoride

Abstract

Production of the important 99mTc medical isotope parent, molybdenum-99 (99Mo), via the fissioning of high- and low-enriched uranium (HEU/LEU) targets followed by target dissolution in acid and solution-phase purification of 99Mo is time-consuming, generates quantities of corrosive radioactive waste, and can result in the release of an array of radionuclides to the atmosphere. An alternative 99Mo purification method has been devised that has the potential to alleviate many of these issues. Herein, we demonstrate the feasibility of a rapid Mo/Tc gas-phase separation from UO2. The results indicate that volatile [99Mo]Mo can be captured downstream of the reacted solid mixture on a column bed (trap) of alumina; the majority of the captured [99Mo]Mo can be subsequently eluted from the alumina trap with a few milliliters of water. >1.0 × 105 single pass decontamination of U and the collected [99Mo]Mo product is demonstrated. This simple thermo-fluorination technique has the potential to provide a rapid methodology for routine 99Mo production.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  2. Flibe Energy, Richland, WA (United States)
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1599144
Report Number(s):
PNNL-SA-148868
Journal ID: ISSN 2046-2069; RSCACL
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Accepted Manuscript
Journal Name:
RSC Advances
Additional Journal Information:
Journal Volume: 10; Journal Issue: 6; Journal ID: ISSN 2046-2069
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

McNamara, Bruce K., O'Hara, Matthew J., Clark, Richard A., Morrison, Samuel S., Soderquist, Chuck Z., and Scheele, Randall D. Gas-phase molybdenum-99 separation from uranium dioxide by fluoride volatility using nitrogen trifluoride. United States: N. p., 2020. Web. doi:10.1039/C9RA10270A.
McNamara, Bruce K., O'Hara, Matthew J., Clark, Richard A., Morrison, Samuel S., Soderquist, Chuck Z., & Scheele, Randall D. Gas-phase molybdenum-99 separation from uranium dioxide by fluoride volatility using nitrogen trifluoride. United States. https://doi.org/10.1039/C9RA10270A
McNamara, Bruce K., O'Hara, Matthew J., Clark, Richard A., Morrison, Samuel S., Soderquist, Chuck Z., and Scheele, Randall D. Tue . "Gas-phase molybdenum-99 separation from uranium dioxide by fluoride volatility using nitrogen trifluoride". United States. https://doi.org/10.1039/C9RA10270A. https://www.osti.gov/servlets/purl/1599144.
@article{osti_1599144,
title = {Gas-phase molybdenum-99 separation from uranium dioxide by fluoride volatility using nitrogen trifluoride},
author = {McNamara, Bruce K. and O'Hara, Matthew J. and Clark, Richard A. and Morrison, Samuel S. and Soderquist, Chuck Z. and Scheele, Randall D.},
abstractNote = {Production of the important 99mTc medical isotope parent, molybdenum-99 (99Mo), via the fissioning of high- and low-enriched uranium (HEU/LEU) targets followed by target dissolution in acid and solution-phase purification of 99Mo is time-consuming, generates quantities of corrosive radioactive waste, and can result in the release of an array of radionuclides to the atmosphere. An alternative 99Mo purification method has been devised that has the potential to alleviate many of these issues. Herein, we demonstrate the feasibility of a rapid Mo/Tc gas-phase separation from UO2. The results indicate that volatile [99Mo]Mo can be captured downstream of the reacted solid mixture on a column bed (trap) of alumina; the majority of the captured [99Mo]Mo can be subsequently eluted from the alumina trap with a few milliliters of water. >1.0 × 105 single pass decontamination of U and the collected [99Mo]Mo product is demonstrated. This simple thermo-fluorination technique has the potential to provide a rapid methodology for routine 99Mo production.},
doi = {10.1039/C9RA10270A},
journal = {RSC Advances},
number = 6,
volume = 10,
place = {United States},
year = {Tue Jan 21 00:00:00 EST 2020},
month = {Tue Jan 21 00:00:00 EST 2020}
}

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Works referenced in this record:

Modification of Targets and Processes for Conversion of 99 Mo Production from High- to Low-Enriched Uranium
journal, September 2000

  • Vandegrift, G. F.; Conner, C.; Hofman, G. L.
  • Industrial & Engineering Chemistry Research, Vol. 39, Issue 9
  • DOI: 10.1021/ie9905815

Adsorption of Molybdenum Hexafluoride on Magnesium Difluoride for Uranium Purification in FLUOREX Reprocessing
journal, December 2011

  • Watanabe, Daisuke; Sasahira, Akira; Hoshino, Kuniyoshi
  • Journal of Nuclear Science and Technology, Vol. 48, Issue 12
  • DOI: 10.1080/18811248.2011.9711834

Fluorination of Uranium Metal to UF 3 and UF 4 by Nitrogen Trifluoride: Evidence for Elusive UF 2
journal, January 2010


On the use of thermal NF3 as the fluorination and oxidation agent in treatment of used nuclear fuels
journal, May 2012


Electron Ionization Mass Spectrum of Tellurium Hexafluoride
journal, April 2015


Separation of plutonium and americium by low-temperature fluorination
journal, October 1994


Synthesis of lower-valent molybdenum oxides in aqueous solutions by reducing Na2MoO4 with NaBH4
journal, January 1997

  • Tsang, Chi Fo; Manthiram, Arumugam
  • Journal of Materials Chemistry, Vol. 7, Issue 6
  • DOI: 10.1039/a606389f

Fluorex reprocessing system for the thermal reactors cycle and future thermal/fast reactors (coexistence) cycle
journal, January 2005

  • Kobayashi, Hiroaki; Amano, Osamu; Kawamura, Fumio
  • Progress in Nuclear Energy, Vol. 47, Issue 1-4, p. 380-388
  • DOI: 10.1016/j.pnucene.2005.05.037

Separation of metallic residues from the dissolution of a high-burnup BWR fuel using nitrogen trifluoride
journal, June 2014


Production of technetium preparations of high radiochemical purity
journal, July 1996

  • Chinenov, P. P.; Rovnyi, S. I.; Ershov, V. V.
  • Atomic Energy, Vol. 81, Issue 1
  • DOI: 10.1007/BF02415728

Commercial rectification facility for deep purification of sublimate uranium hexafluoride
journal, November 2007