Abstract
This work focuses on the polymorphic nature of the UO3 and UO3–H2O system, which are important materials associated with the nuclear fuel cycle. The UO3–water system is complex and has not been fully characterized, even though these species are key fuel cycle materials. Powder X-ray diffraction, and Raman and fluorescence spectroscopies were used to characterize both the several polymorphic forms of UO3 and the certain UO3-hydrolysis products for the purpose of developing predictive capabilities and estimating process history; for example, polymorphic phases of unknown origin. Specifically, we have investigated three industrially relevant production pathways of UO3 and discovered a previously unknown low temperature route to the production of β-UO3. Several phases of UO3, its hydrolysis products, and key starting materials were synthesized and characterized as pure materials to establish optical spectroscopic signatures for these compounds for forensic analysis.
Similar content being viewed by others
References
Benedict M, Pigford TH, Levi HW (1981) Nuclear chemical engineering, 2nd edn. McGraw-Hill, USA
Debets PC (1966) Acta Crystallogr 21:589–593
Wheeler VJ, Dell RM, Wait E (1964) J Inorg Nucl Chem 26(11):1829–1845
Johnson TJ, Profeta LTM, Sams RL, Griffith DWT, Yokelson RL (2010) Vib Spectrosc 53(1):97–102
Sadtler A series of commercially available spectroscopic databases distributed at www.knowitall.com/literature Bio-Rad
Aldrich Library of FT-IR Spectra, 2nd edn, 3-volume set (1997). Sigma-Aldrich Chemical Co., Milwaukee, WI
Johnson TJ, Su Y-F, Jarman KH, Kunkel BM, Birnbaum JC, Joly AG, Stephan EG, Tonkyn RG, Ewing RG, Dunham GC (2012) Int J Spectrosc 2012:297056
Grenthe I, Drożdżyński J, Fujino T, Buck EC, Albrecht-Schmitt TE, Wolf SF (2011) Uranium* the chemistry of the actinide and transactinide elements. In: Morss LR, Edelstein NM, Fuger J (eds). Springer, Netherlands, pp 253-698. doi: 10.1007/978-94-007-0211-0_5
Hoekstra HR, Siegel S (1961) J Inorg Nucl Chem 18:154–165
Cordfunke EHP, Van Der Giessen AA (1963) J Inorg Nucl Chem 25(5):553–555
Eary L, Cathles L (1983) Metall Mater Trans B 14(3):325–334
Hastings EP, Lewis C, FitzPatrick J, Rademacher D, Tandon L (2008) J Radioanal Nucl Chem 276:475–481
Graziani R, Bombieri G, Forsellini E (1972) J Chem Soc, Dalton Trans 19:2059–2061
Weller MT, Light ME, Gelbrich T (2000) Acta Crystallogr Sect B 56(4):577–583
Engmann R, Wolff PMD (1963) Acta Crystallogr 16(10):993
Armstrong DP, Jarabek RJ, Fletcher WH (1989) Appl Spectrosc 43(3):461–468
Taylor P, Wood DD, Duclos AM, Owen DG (1989) J Nucl Mater 168(1–2):70–75
Finch RJ, Hawthorne FC, Ewing RC (1998) Can Mineral 36:831–845
Hoekstra HR, Siegel S (1973) J Inorg Nucl Chem 35(3):761–779
Gal M, Goggin PL, Mink J (1992) Spectrochim Acta, Part A: Mol Spectrosc 48(1):121–132
McGlynn SP, Smith JK (1961) J Mol Spectrosc 6:164–187
Frost RL, Palmer SJ, Reddy BJ (2011) J Raman Spectrosc 42(5):1160–1162
Hoekstra HR (1963) Inorg Chem 2(3):492–495
Frost RL, Weier ML, Čejka J, Ayoko GA (2006) Spectrochim Acta, Part A 65 (3‚Äì4):529–534
Kips AJPR, Houlton MR, Leenaers A, Mace JD, Marie O, Pointurier F, Stefaniak EA, Taylor PDP, Van den Berghe S, Van Espen P, Van Grieken R, Wellum R (2009) Spectrochim Acta, Part B 64:199–207
Gabelnick SD, Reedy GT, Chasanov MG (1973) J Chem Phys 59(12):6397–6404
4.2 Tv (2009) Software for powder X-ray diffraction pattern analysis: Bruker AXS
Burns PC, Hughes KA (2003) Am Mineral 88:1165–1168
Greaves C, Fender BEF (1972) Acta Crystallogr Sect B: Struct Sci 28(DEC15):3609–3614
Kim BH, Lee YB, Prelas MA, Ghosh TK (2012) J Radioanal Nucl Chem 292:1075–1083 Copyright (C) 2012 American Chemical Society (ACS). All Rights Reserved
Hoekstra HR, Siegel S (1958) J Inorg Nucl Chem 7(1–2):174–175
Acknowledgments
This research was supported in part by the National Technical Nuclear Forensics Center (NFNFC, a department of the U.S. Department of Homeland Security), and was co-funded by NA-22 in the National Nuclear Security Administration/Office of Nonproliferation & Verification Research and Development. The work was conducted at the Pacific Northwest National Laboratory, a multiprogram national laboratory operated by Battelle for the U.S. Department of Energy under Contract DE-AC05-76RL01830. We thank our sponsors for their support.
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Sweet, L.E., Blake, T.A., Henager, C.H. et al. Investigation of the polymorphs and hydrolysis of uranium trioxide. J Radioanal Nucl Chem 296, 105–110 (2013). https://doi.org/10.1007/s10967-012-2063-9
Received:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10967-012-2063-9