Comparing results of X-ray diffraction, µ-Raman spectroscopy and neutron diffraction when identifying chemical phases in seized nuclear material, during a comparative nuclear forensics exercise

Rondahl, Stina Holmgren; Pointurier, Fabien; Ahlinder, Linnea; Ramebäck, Henrik; Marie, Olivier; Ravat, Brice; Delaunay, François; Young, Emma; Blagojevic, Ned; Hester, James R.; Thorogood, Gordon; Nelwamondo, Aubrey N.; Ntsoane, Tshepo P.; Roberts, Sarah K.; Holliday, Kiel S.

doi:10.1007/s10967-017-5666-3

Title: Comparing results of X-ray diffraction, µ-Raman spectroscopy and neutron diffraction when identifying chemical phases in seized nuclear material, during a comparative nuclear forensics exercise

Journal Article · Wed Jan 24 00:00:00 EST 2018 · Journal of Radioanalytical and Nuclear Chemistry

DOI:https://doi.org/10.1007/s10967-017-5666-3· OSTI ID:1424108

Rondahl, Stina Holmgren ^[1]; Pointurier, Fabien ^[2]; Ahlinder, Linnea ^[1]; Ramebäck, Henrik ^[3]; Marie, Olivier ^[2]; Ravat, Brice ^[4]; Delaunay, François ^[4]; Young, Emma ^[5]; Blagojevic, Ned ^[5]; Hester, James R. ^[5]; Thorogood, Gordon ^[5]; Nelwamondo, Aubrey N. ^[6]; Ntsoane, Tshepo P. ^[6]; Roberts, Sarah K. ^[7]; Holliday, Kiel S. ^[7]

Swedish Defence Research Agency (FOI), Umea (Sweden). CBRN Defence and Security
DAM, DIF, French Alternative Energies and Atomic Energy Commission (CEA), Arpajon (France)
Swedish Defence Research Agency (FOI), Umea (Sweden). CBRN Defence and Security ; Chalmers University of Technology, Goteborg (Sweden). Department of Chemistry and Chemical Engineering, Nuclear Chemistr
French Alternative Energies and Atomic Energy Commission (CEA), CEA-Centre de Valduc, Is-Sur-Tille (France)
Australian Nuclear Science and Technology Organisation (ANSTO), Lucas Heights (Australia)
South Africa Nuclear Energy Corporation (NECSA) Pelindaba, Pretoria (South Africa)
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

This work presents the results for identification of chemical phases obtained by several laboratories as a part of an international nuclear forensic round-robin exercise. In this work powder X-ray diffraction (p-XRD) is regarded as the reference technique. Neutron diffraction produced a superior high-angle diffraction pattern relative to p-XRD. Requiring only small amounts of sample, µ-Raman spectroscopy was used for the first time in this context as a potentially complementary technique to p-XRD. The chemical phases were identified as pure UO₂ in two materials, and as a mixture of UO₂, U₃O₈ and an intermediate species U₃O₇ in the third material.

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Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 1424108

Report Number(s):: LLNL-JRNL-679185; TRN: US1801905

Journal Information:: Journal of Radioanalytical and Nuclear Chemistry, Vol. 315, Issue 2; ISSN 0236-5731

Publisher:: SpringerCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 6 works

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References (30)

Echidna—the new high-resolution powder diffractometer being built at OPAL Liss, Klaus-Dieter; Hunter, Brett; Hagen, Mark Physica B: Condensed Matter, Vol. 385-386 https://doi.org/10.1016/j.physb.2006.05.322	journal	November 2006
Raman spectra of stoichiometric and hyperstoichiometric uranium dioxide Manara, Dario; Renker, Burkhard Journal of Nuclear Materials, Vol. 321, Issue 2-3 https://doi.org/10.1016/S0022-3115(03)00248-4	journal	September 2003
In situ Raman monitoring of materials under irradiation: study of uranium dioxide alteration by water radiolysis Canizarès, A.; Guimbretière, G.; Tobon, Y. A. Journal of Raman Spectroscopy, Vol. 43, Issue 10 https://doi.org/10.1002/jrs.4088	journal	May 2012
A phase study on the tie line of U3O7PuO2 Nakayama, Yasuyuki Journal of Inorganic and Nuclear Chemistry, Vol. 33, Issue 12 https://doi.org/10.1016/0022-1902(71)80507-9	journal	December 1971
Raman spectrum of U4O9: a new interpretation of damage lines in UO2: Raman spectrum of U4O9 Desgranges, L.; Baldinozzi, G.; Simon, P. Journal of Raman Spectroscopy, Vol. 43, Issue 3 https://doi.org/10.1002/jrs.3054	journal	October 2011
An intelligent background-correction algorithm for highly fluorescent samples in Raman spectroscopy Zhang, Zhi-Min; Chen, Shan; Liang, Yi-Zeng Journal of Raman Spectroscopy, Vol. 41, Issue 6 https://doi.org/10.1002/jrs.2500	journal	October 2009
Identification of the chemical forms of uranium compounds in micrometer-size particles by means of micro-Raman spectrometry and scanning electron microscope Pointurier, F.; Marie, O. Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 65, Issue 9-10 https://doi.org/10.1016/j.sab.2010.06.008	journal	September 2010
The determination of electrochemical reactivity and sustainability on individual hyper-stoichiometric UO2+x grains by Raman microspectroscopy and scanning electrochemical microscopy He, Heming; Ding, Zhifeng; Shoesmith, David W. Electrochemistry Communications, Vol. 11, Issue 8 https://doi.org/10.1016/j.elecom.2009.07.013	journal	August 2009
Surface reactions of uranium oxide powder, thin films and single crystals Idriss, H. Surface Science Reports, Vol. 65, Issue 3 https://doi.org/10.1016/j.surfrep.2010.01.001	journal	March 2010
Oxidation of UO2 fuel pellets in air at 503 and 543 K studied using X-ray photoelectron spectroscopy and X-ray diffraction Tempest, P. A.; Tucker, P. M.; Tyler, J. W. Journal of Nuclear Materials, Vol. 151, Issue 3 https://doi.org/10.1016/0022-3115(88)90019-0	journal	February 1988
Thermal expansion and phase transformations of the U3O8−z phase in air Ackermann, R. J.; Chang, A. T.; Sorrell, Charles A. Journal of Inorganic and Nuclear Chemistry, Vol. 39, Issue 1 https://doi.org/10.1016/0022-1902(77)80436-3	journal	January 1977
Structures of UO2, UO2+x andU4O9 by neutron diffraction Willis, B. T. M. Journal de Physique, Vol. 25, Issue 5 https://doi.org/10.1051/jphys:01964002505043100	journal	January 1964
Raman Microprobe Spectroscopy of Uranium Dioxide Single Crystals and Ion Implanted Polycrystals Graves, P. R. Applied Spectroscopy, Vol. 44, Issue 10 https://doi.org/10.1366/0003702904417472	journal	December 1990
Characterisation of uranium oxides by micro-Raman spectroscopy Allen, Geoffrey C.; Butler, Ian S. Journal of Nuclear Materials, Vol. 144, Issue 1-2 https://doi.org/10.1016/0022-3115(87)90274-1	journal	January 1987
Raman spectroscopy characterization of actinide oxides (U1−yPuy)O2: Resistance to oxidation by the laser beam and examination of defects Jégou, C.; Caraballo, R.; Peuget, S. Journal of Nuclear Materials, Vol. 405, Issue 3 https://doi.org/10.1016/j.jnucmat.2010.08.005	journal	October 2010
Characterization of Uranium Oxides Using in Situ Micro-Raman Spectroscopy Palacios, M. Luisa; Taylor, Stuart H. Applied Spectroscopy, Vol. 54, Issue 9 https://doi.org/10.1366/0003702001951057	journal	September 2000
Determination of uranium metal concentration in irradiated fuel storage basin sludge using selective dissolution Delegard, C. H.; Sinkov, S. I.; Chenault, J. W. Journal of Radioanalytical and Nuclear Chemistry, Vol. 299, Issue 3 https://doi.org/10.1007/s10967-013-2884-1	journal	December 2013
The kinetics of dissolution of UO2 under reducing conditions and the influence of an oxidized surface layer (UO2+x): Application of a continuous flow-through reactor Bruno, Jordi; Casas, Ignasi; Puigdomènech, Ignasi Geochimica et Cosmochimica Acta, Vol. 55, Issue 3 https://doi.org/10.1016/0016-7037(91)90330-8	journal	March 1991
Uranium Speciation As a Function of Depth in Contaminated Hanford Sediments - A Micro-XRF, Micro-XRD, and Micro- And Bulk-XAFS Study Singer, David M.; Zachara, John M.; Brown Jr, Gordon E. Environmental Science & Technology, Vol. 43, Issue 3 https://doi.org/10.1021/es8021045	journal	February 2009
Plutonium–uranium mixed oxide characterization by coupling micro-X-ray diffraction and absorption investigations Degueldre, C.; Martin, M.; Kuri, G. Journal of Nuclear Materials, Vol. 416, Issue 1-2 https://doi.org/10.1016/j.jnucmat.2010.11.096	journal	September 2011
Oxidation states of uranium in depleted uranium particles from Kuwait Salbu, B.; Janssens, K.; Lind, O. C. Journal of Environmental Radioactivity, Vol. 78, Issue 2 https://doi.org/10.1016/j.jenvrad.2004.04.001	journal	January 2005
Investigation of the polymorphs and hydrolysis of uranium trioxide Sweet, Lucas E.; Blake, Thomas A.; Henager, Charles H. Journal of Radioanalytical and Nuclear Chemistry, Vol. 296, Issue 1 https://doi.org/10.1007/s10967-012-2063-9	journal	August 2012
Recognition of uranium oxides in soil particulate matter by means of μ-Raman spectrometry Stefaniak, Elżbieta A.; Alsecz, Anita; Sajó, István E. Journal of Nuclear Materials, Vol. 381, Issue 3 https://doi.org/10.1016/j.jnucmat.2008.08.036	journal	November 2008
Crystallography Open Database (COD): an open-access collection of crystal structures and platform for world-wide collaboration Gražulis, Saulius; Daškevič, Adriana; Merkys, Andrius Nucleic Acids Research, Vol. 40, Issue D1 https://doi.org/10.1093/nar/gkr900	journal	November 2011
The reaction of water on polycrystalline UO2: Pathways to surface and bulk oxidation Senanayake, S. D.; Rousseau, R.; Colegrave, D. Journal of Nuclear Materials, Vol. 342, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2005.04.060	journal	June 2005
Investigation of ammonium diuranate calcination with high-temperature X-ray diffraction Eloirdi, R.; Ho Mer Lin, D.; Mayer, K. Journal of Materials Science, Vol. 49, Issue 24 https://doi.org/10.1007/s10853-014-8553-0	journal	September 2014
Establishing reactor operations from uranium targets used for the production of plutonium Tandon, Lav; Kuhn, Kevin; Martinez, Patrick Journal of Radioanalytical and Nuclear Chemistry, Vol. 282, Issue 2 https://doi.org/10.1007/s10967-009-0297-y	journal	August 2009
Certification of Standard Reference Material 1976B Black, David R.; Windover, Donald; Mendenhall, Marcus H. Powder Diffraction, Vol. 30, Issue 3 https://doi.org/10.1017/S0885715615000445	journal	August 2015
Crystallography Open Database – an open-access collection of crystal structures Gražulis, Saulius; Chateigner, Daniel; Downs, Robert T. Journal of Applied Crystallography, Vol. 42, Issue 4 https://doi.org/10.1107/s0021889809016690	journal	May 2009
Applicability of Raman spectroscopy as a tool in nuclear forensics for analysis of uranium ore concentrates Lin, D. Ho Mer; Manara, D.; Varga, Zs. Radiochimica Acta, Vol. 101, Issue 12 https://doi.org/10.1524/ract.2013.2110	journal	January 2013

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Title: Comparing results of X-ray diffraction, µ-Raman spectroscopy and neutron diffraction when identifying chemical phases in seized nuclear material, during a comparative nuclear forensics exercise

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