Skip to main content
Log in

Quantifying multiple trace elements in uranium ore concentrates: an interlaboratory comparison

  • Published:
Journal of Radioanalytical and Nuclear Chemistry Aims and scope Submit manuscript

Abstract

An intercomparison was organized, with six laboratories tasked to quantify sixty-nine impurities in two uranium materials. The main technique employed for analysis was inductively coupled plasma mass spectrometry in combination with matrix-matched external calibration. The results presented highlight the current state-of-the-practice; lessons learned include previously unaccounted polyatomic interferences, issues related to sample dissolution, blank correction and calibration, and the challenge of estimating measurement uncertainties. The exercise yielded consensus values for the two analysed materials, suitable for use as laboratory standards to partially fill a gap in the availability of uranium reference materials characterized for impurities.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5

Similar content being viewed by others

Notes

  1. The preparation of the U3O8 material was arranged by the Laboratoire Central d’Analyse et de Controle in Grenoble. A large uranium metal billet of industrial origin was molten together with a small uranium ingot carrying the trace elements. It was then converted to U3O8 by ignition under a stream of oxygen. The resulting U3O8 itself was milled, ground, and sieved in order to obtain a 100 mesh grain size powder. The whole batch was then homogenized, and the homogeneity was verified by six laboratories. In 1982 the French Government donated a batch of the resulting material to the IAEA.

  2. Concentrations of Br and Cl impurities, not measured by any of the participating laboratories, remain undetermined.

  3. Technical Meeting on Analysis of Elemental Impurities in Uranium Samples. IAEA, Vienna, 30 May–1 June 2012.

  4. The certified atom (molar) ratios with respective expanded uncertainties (k = 2) are: 234U/238U = 0.00005472(76), 235U/238U = 0.0072568(36). Certified atom ratio 236U/238U is < 2 × 10−8.

  5. Recent measurements at SAL using MTE MC-TIMS yielded the following atom (molar) ratios, traceable to CRM IRMM-184, with respective expanded uncertainties (k = 2): 234U/238U = 0.00005471(21), 235U/238U = 0.0072544(29), and 236U/238U < 5 × 10–9.

  6. Recent measurements at SAL using MTE MC-TIMS yielded atom (molar) ratios traceable to CRM IRMM-184, with respective expanded uncertainties (k = 2): 234U/238U = 0.00005449(23), 235U/238U = 0.0072561(30), and 236U/238U < 1 × 10–8.

References

  1. ASTM C753-04 (2009) Standard specification for nuclear-grade sinterable uranium dioxide powder

  2. ASTM C967-13 (2013) Standard specification for uranium ore concentrate

  3. Keegan E, Richter S, Kelly I, Wong H, Gadd P, Kuehn H, Alonso-Munoz A (2008) The provenance of Australian uranium ore concentrates by elemental and isotopic analysis. Appl Geochem 23:765–777

    Article  CAS  Google Scholar 

  4. Badaut V, Wallenius M, Mayer K (2009) Anion analysis in uranium ore concentrates by ion chromatography. J Radioanal Nucl Chem 280(1):57–61

    Article  CAS  Google Scholar 

  5. Varga Z, Wallenius M, Mayer K, Meppen M (2011) Analysis of uranium ore concentrates for origin assessment. Proc Radiochim Acta 1:1–4

    CAS  Google Scholar 

  6. Keegan E, Wallenius M, Mayer K, Varga Z, Rasmussen G (2012) Attribution of uranium ore concentrates using elemental and anionic data. Appl Geochem 27:1600–1609

    Article  CAS  Google Scholar 

  7. Peńkin MV, Zhao K, Fischer DM, Boulyga SF (2012) Use of rare-earth elemental impurity patterns for origin assessment of uranium materials. In: 9th international conference on methods and applications of radioanalytical chemistry (MARC IX), Kailua-Kona

  8. Button P, Healey G, Chipley D (2013) Change in impurities observed during the refining and conversion processes. ESARDA Symposium, Bruges

    Google Scholar 

  9. Mayer K, Tushingham J, Boulyga S, Aregbe Y (2009) Report on the workshop on measurements of impurities in uranium. ESARDA Bull 43:57–64

    Google Scholar 

  10. Fischer DM (2010) The evolution of environmental sampling for safeguards. In: IAEA symposium on international safeguards, Vienna. IAEA-CN-184/138

  11. Balsley S (2010) Destructive nuclear material analysis for safeguards: importance and future trends. In: IAEA symposium on international safeguards, Vienna. IAEA-CN-184/278

  12. Peńkin M (2012) Safeguards needs for characterization of uranium compounds. In: IAEA technical meet on analysis of elemental impurities in uranium samples, Vienna

  13. De Souza AL, Cotrim MEB, Pires MAF (2013) An overview of spectrometric techniques and sample preparation for the determination of impurities in uranium nuclear fuel grade. Microchem J 106:194–201

    Article  Google Scholar 

  14. Goyal N, Purohit PJ, Dhobale AR, Patel BM, Page AG, Sastry MD (1987) Electrothermal atomisation atomic absorption spectrometric determination of silver, beryllium, calcium, iron, lead and tin in uranium without preliminary separation. J Anal At Spectrom 2:459–461

    Article  CAS  Google Scholar 

  15. Santoliquido PM (1988) Determination of trace-elements in uranium oxide (U3O8) by inductively coupled plasma emission-spectrometry and graphite furnace atomic-absorption spectrometry. J Res Natl Bur Stand 93:452–454

    Article  CAS  Google Scholar 

  16. Premadas A, Srivastava K (2002) Inductively coupled plasma atomic emission spectrometric determination of lanthanides and yttrium in various uranium hydrometallurgical products. J Radioanal Nucl Chem 251(2):233–239

    Article  CAS  Google Scholar 

  17. Dwivedi VN, Mahanta PL, Premadas A (2003) An integrated approach to the complete chemical analysis of magnesium or sodium diuranate (yellow cake) sample. J Radioanal Nucl Chem 258(3):575–581

    Article  CAS  Google Scholar 

  18. Kyser K, Chipley D, Bukata A, Polito P, Fitzpatrick A, Alexandre P (2003) Application of laser ablation and high resolution ICPMS to the analysis of metal contents of three rings, ages of uranium-rich minerals, and Se content in sulphide ores. Can J Anal Sci Spectrosc 48(5):258–268

    CAS  Google Scholar 

  19. Oliveira OP, Sarkis JES (2002) Determination of impurities in uranium oxide by ICPMS by the matrix matching method. J Radioanal Nucl Chem 254(3):519–526

    Article  Google Scholar 

  20. ASTM C1287-10 (2010) Standard test method for determination of impurities in nuclear grade uranium compounds by inductively coupled plasma mass spectrometry

  21. Quemet A, Brennetot R, Chevalier E, Prian E, Laridon AL, Mariet C, Fichet P, Laszak I, Goutelard F (2012) Analysis of twenty five impurities in uranium matrix by ICP-MS with iron measurement optimized by using reaction collision cell, cold plasma or medium resolution. Talanta 99:207–212

    Article  CAS  Google Scholar 

  22. Bürger S, Riciputi LR, Bostick DA (2007) Determination of impurities in uranium matrices by time-of-flight ICP-MS using matrix-matched method. J Radioanal Nucl Chem 274(3):491–505

    Article  Google Scholar 

  23. Švedkauskaitė-LeGore J, Rasmussen G, Abousahl S, Van Belle P (2008) Investigation of the sample characteristics needed for the determination of the origin of uranium-bearing materials. J Radioanal Nucl Chem 278(1):201–209

    Article  Google Scholar 

  24. Varga Z, Katona R, Stefánka Z, Wallenius M, Mayer K, Nicholl A (2010) Determination of rare-earth elements in uranium-bearing materials by inductively coupled plasma mass spectrometry. Talanta 80:1744–1749

    Article  CAS  Google Scholar 

  25. Wolf SF, Bowers DL, Cunnane JC (2005) Analysis of high burnup spent nuclear fuel by ICP-MS. J Radioanal Nucl Chem 263(3):581–586

    Article  CAS  Google Scholar 

  26. Doubek N, Bagliano G, Deron S (1984) Report on intercomparison exercise SR-54. Determination of impurities in U3O8. IAEA, Vienna. IAEA/RL/110

  27. Doubek N, Bagliano G, Deron S (1985) Report on intercomparison exercise SR-64. Determination of impurities in U3O8. IAEA, Vienna. IAEA/RL/116

  28. IAEA (1985) Reference sheet SR-54: impurities in uranium oxide (U3O8)

  29. Granier G, Balsley SD, Bulyha S, Aregbe Y, Roudila D (2012) Round robin “impurities in uranium matrix”: a success for CETAMA and IAEA. Procedia Chem 7:666–672

    Article  CAS  Google Scholar 

  30. Currie LA (1968) Limits for qualitative detection and quantitative determination: application to radiochemistry. Anal Chem 40:586–593

    Article  CAS  Google Scholar 

  31. Currie LA (1995) Nomenclature in evaluation of analytical methods including detection and quantification capabilities (IUPAC recommendations). Pure Appl Chem 87(10):1699–1723

    Google Scholar 

  32. IRMM (1997) Certificate of isotopic composition. Reference number SMS 7267, sample identification # 9064-01-B

  33. ISO 17294-2 (2003) Water quality: application of inductively coupled plasma mass spectrometry. Part 2: determination of 62 elements

  34. DIN 38406-29 (1999) Determination of 61 elements by inductively coupled plasma mass spectrometry (E29)

  35. ASTM C1347-08 (2008) Standard practice for preparation and dissolution of uranium materials for analysis

  36. Link DD, Walter PJ, Kingston HM (1998) Development and validation of the new EPA microwave-assisted leach method 3051A. Environ Sci Technol 32:3623–3628

    Article  Google Scholar 

  37. JCGM 100:2008 (2008) Evaluation of measurement data: guide to the expression of uncertainty in measurement

  38. ISO Guide 35 (1989) Certification of reference materials: general and statistical principles

  39. Bürger S, Mathew KJ, Mason P, Narayanan U (2009) Reference materials characterized for impurities in uranium matrices: an overview and re-evaluation of the NBL CRM 124 series. J Radioanal Nucl Chem 279(2):659–673

    Article  Google Scholar 

  40. Zawisza B, Pytlakowska K, Feist B, Polowniak M, Kita A, Sitko R (2011) Determination of rare earth elements by spectroscopic techniques: a review. J Anal At Spectrom 26:2373–2390

    Article  CAS  Google Scholar 

  41. Varga Z, Wallenius M, Mayer K (2010) Origin assessment of uranium ore concentrates based on their REE impurity pattern. Radiochim Acta 98:771–778

    Article  CAS  Google Scholar 

  42. Riciputi L (2012) Utilization of REE and trace elements in UOC. In: IAEA technical meeting on analysis of elemental impurities in uranium samples, Vienna

  43. Peńkin M (2012) Use of REE patterns in safeguards data evaluations. In: IAEA technical meeting on analysis of elemental impurities in uranium samples, Vienna

  44. CETAMA (2011) Reference materials catalogue

  45. NBL (1991) Certificate of analysis. CRM 123(1–7): uranium (normal) oxide

  46. NBL (1983) Provisional certificate of analysis. CRM 124(1–7): uranium (normal) oxide

  47. CANMET (1988) Certificate of analysis. CUP-2: uranium ore concentrate

Download references

Acknowledgments

Authors are grateful to Mikhail Ryzhinskiy for the in-depth discussions of the quality of analysis results on impurities in uranium samples, which led to the initiation of this interlaboratory comparison, and for his advice regarding the selection of test materials. Also acknowledged is the contribution of Zsolt Varga (ITU) who thoroughly reviewed the manuscript and provided valuable comments.

Author information

Authors and Affiliations

Authors

Corresponding author

Correspondence to M. V. Peńkin.

Additional information

S. Bürger: deceased.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Bürger, S., Boulyga, S.F., Peńkin, M.V. et al. Quantifying multiple trace elements in uranium ore concentrates: an interlaboratory comparison. J Radioanal Nucl Chem 301, 711–729 (2014). https://doi.org/10.1007/s10967-014-3224-9

Download citation

  • Received:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10967-014-3224-9

Keywords

Navigation