Skip to main content
SpringerLink
Log in

Disassembly of old radium sources and conversion of radium sulfate into radium carbonate for subsequent dissolution in acid

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

Abstract

In this work details of safe radium source disassembly which were previously used in brachytherapy are described and different methods for conversion of RaSO4 into aqueous solution are reviewed. The method of choice included three cycles of RaSO4 heating in 1.5 M Na2CO3 up to 85 °C, cooling and subsequent removal of supernatant. X-ray diffraction study showed that the method allows the synthesis of, presumably, amorphous RaCO3, which can be dissolved in mineral acid. Gamma spectrometric measurements showed that most of the initial RaSO4 was converted into solution and that 7 ± 1 % of the initial 210Pb was co-precipitated with RaCO3.

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

Access this article

Log in via an institution

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

Similar content being viewed by others

References

  1. Curie P, Curie MS (1898) Sur une substance nouvelle radioactive, contenue dans la pechblende. CR Acad Sci 127:175–178

    Google Scholar 

  2. Vdovenko V, Dubasov YV (1973) Analytical chemistry of radium. Nauka, Leningrad

    Google Scholar 

  3. Sciaroni G (1918) Radium in the treatment of sarcoma and carcinoma. Int J Orthod 4(12):655–658

    Article  Google Scholar 

  4. Kjellgren O, Ragnhult I (1963) Armamentarium for radium treatment of carcinoma of the uterine cervix. Acta Radiol Ther Phys Biol 1(1):1–22

    Article  Google Scholar 

  5. Decay Data Evaluation Project (DDEP), Laboratoire National Henri Becquerel, France http://www.nucleide.org/DDEP_WG/DDEPdata.htm. Accessed 22 Dec 2015

  6. Karalova Z, Ivanov R, Myasoedov B, Rodionova L, Pyzhova Z, Kalebin S, Gabeskiriya VY (1972) Production of Ac 227 and Th 228 isotopes by irradiation of radium in the SM-2 reactor. At Energy 32(2):133–136

    Article  Google Scholar 

  7. Kuznetsov R, Butkalyuk P, Tarasov V, Baranov AY, Butkalyuk I, Romanov E, Kupriyanov V, Kazakova E (2012) Yields of activation products in 226Ra irradiation in the high-flux SM reactor. Radiochemistry 54(4):383–387

    Article  CAS  Google Scholar 

  8. Bagheri R, Afarideh H, Ghannadi-Maragheh M, Bahrami-Samani A, Shirvani-Arani S (2015) Production of 223Ra from 226Ra in Tehran Research Reactor for treatment of bone metastases. J Radioanal Nucl Chem 304(3):1185–1191

    Article  CAS  Google Scholar 

  9. Kukleva E, Kozempel J, Vlk M, Mičolová P, Vopálka D (2015) Preparation of 227Ac/223Ra by neutron irradiation of 226Ra. J Radioanal Nucl Chem 304(1):263–266

    Article  CAS  Google Scholar 

  10. Nilsson S, Strang P, Aksnes A, Franzèn L, Olivier P, Pecking A, Staffurth J, Vasanthan S, Andersson C, Bruland Ø (2012) A randomized, dose–response, multicenter phase II study of radium-223 chloride for the palliation of painful bone metastases in patients with castration-resistant prostate cancer. Eur J Cancer 48(5):678–686

    Article  CAS  Google Scholar 

  11. Nilsson S, Franzén L, Parker C, Tyrrell C, Blom R, Tennvall J, Lennernäs B, Petersson U, Johannessen DC, Sokal M (2013) Two-year survival follow-up of the randomized, double-blind, placebo-controlled phase II study of radium-223 chloride in patients with castration-resistant prostate cancer and bone metastases. Clin Genitourin Cancer 11(1):20–26

    Article  Google Scholar 

  12. Sartor O, Coleman R, Nilsson S, Heinrich D, Helle SI, O’Sullivan JM, Fosså SD, Chodacki A, Wiechno P, Logue J (2014) Effect of radium-223 dichloride on symptomatic skeletal events in patients with castration-resistant prostate cancer and bone metastases: results from a phase 3, double-blind, randomised trial. Lancet Oncol 15(7):738–746

    Article  CAS  Google Scholar 

  13. Kluetz PG, Pierce W, Maher VE, Zhang H, Tang S, Song P, Liu Q, Haber MT, Leutzinger EE, Al-Hakim A (2014) Radium Ra 223 dichloride injection: US Food and Drug Administration drug approval summary. Clin Cancer Res 20(1):9–14

    Article  CAS  Google Scholar 

  14. Vebersik V (1958) Trennung des Radiums von Platin, Gold und Silber zur Umarbeitung alter klinischer Radiumpräparate. J Prakt Chem 6(1):25–30

    Article  CAS  Google Scholar 

  15. Brown PL, Ekberg C, Ramebäck H, Hedström H, Matyskin A (2015) Solubility of radium and strontium sulfate across the temperature range of 0 to 300° C. In: Uranium-past and future challenges. Springer, International Publishing, pp 553–564

  16. Lind S, Underwood J, Whittemore C (1918) The solubility of pure radium sulfate. 1. J Am Chem Soc 40(3):465–472

    Article  CAS  Google Scholar 

  17. Kuznetsov R, Butkalyuk P, Butkalyuk I (2013) A rapid method for radium regeneration from its sulfate. Radiochemistry 55(1):112–115

    Article  CAS  Google Scholar 

  18. Ebler E, Bender W (1913) Über die Verwendung des Calciumhydrids zur „autogenen Reduktion” der „Rohsulfate” bei der Darstellung des Radiums und Mesothoriums. Z Anorg Allg Chem 83(1):149–158

    Article  Google Scholar 

  19. Whytlaw-Gray R, Ramsay W (1912) The atomic weight of radium. IN: Proceedings of the Royal Society of London series A, containing papers of a mathematical and physical character 86(587):270–290

  20. Bredt OPC (1915) Production of concentrated radium residues and the separation of radium compounds therefrom. Google Patents

  21. Al Abdullah J, Al Masri M, Amin Y (2016) Dissolution of [226Ra] BaSO4 and partial separation of 226Ra from radium/barium sulfate: a new treatment method for NORM waste from petroleum industry. Appl Radiat Isot 107:377–381

    Article  CAS  Google Scholar 

  22. Vebersík V, Horovă K (1958) Trennung des Radiums von Radium D, Radium E und Polonium durch Äthylendiamintetraacetat. Fresen Z Anal Chem 162(6):401–407

    Article  Google Scholar 

  23. Osborn G (1953) Ion-exchange resins in Analytical Chemistry. The application of ion-exchange resins to the analysis of insoluble substances. Analyst 78(925):220–221

    Article  CAS  Google Scholar 

  24. Bok R (1984) A handbook of decomposition methods in analytical chemistry. Khimiya, Moscow

    Google Scholar 

  25. Dedek W (1960) Decomposition of radium sulfate with ion-exchange resin and separation of radium D and polonium from radium. Z Anal Chem 173:399–411

    Article  CAS  Google Scholar 

  26. Curie MS (1910) Traité de radioactivité. Imprimerie Gauthier-Villars, Paris

    Google Scholar 

  27. Kozempel J, Vlk M, Floriánová M, Drtinová B, Němec M (2015) Dissolution of [226Ra]BaSO4 as part of a method for recovery of 226Ra from aged radium sources. J Radioanal Nucl Chem 304(1):337–342

    Article  CAS  Google Scholar 

  28. Annual limilts on intake (ALI) and derived air concentrations (DAC) of radionuclides for occupational exposure; effluent concentrations; concentrations for release to sanitary sewerage. https://labor.ny.gov/workerprotection/safetyhealth/PDFs/RHU/appendix-a-13.pdf. Accessed 22 Dec

  29. Hedström H (2013) Radium sulphate and its co-precipitation behaviour with barium and strontium. Chalmers University of Technology, Gothenburg

    Google Scholar 

  30. Rozenfeld M, Mason E (1969) The plugging of leaks in radium containers. Am J Roentgenol 105(3):689–697

    Article  CAS  Google Scholar 

  31. Langmuir D, Riese AC (1985) The thermodynamic properties of radium. Geochim Cosmochim Acta 49(7):1593–1601

    Article  CAS  Google Scholar 

  32. Koga N, Nakagoe Y, Tanaka H (1998) Crystallization of amorphous calcium carbonate. Thermochim Acta 318(1):239–244

    Article  CAS  Google Scholar 

  33. Ihli J, Wong WC, Noel EH, Kim Y-Y, Kulak AN, Christenson HK, Duer MJ, Meldrum FC (2014) Dehydration and crystallization of amorphous calcium carbonate in solution and in air. Nat Commun 5:3169

    Article  Google Scholar 

  34. Wolf SE, Muller L, Barrea R, Kampf CJ, Leiterer J, Panne U, Hoffmann T, Emmerling F, Tremel W (2011) Carbonate-coordinated metal complexes precede the formation of liquid amorphous mineral emulsions of divalent metal carbonates. Nanoscale 3(3):1158–1165. doi:10.1039/C0NR00761G

    Article  CAS  Google Scholar 

  35. Weigel F, Trinkl A (1973) Zur Kristallchemie des Radiums. Radiochim Acta 19(4):199–202

    CAS  Google Scholar 

  36. Goldschmidt B (1940) A study by means of radioactive elements of fractionation by mixed crystallization. An Chim 13:88–174

    CAS  Google Scholar 

  37. Nelson F, Day R, Kraus K (1960) Anion exchange studies—XXX a number of elements in ethylenediaminetetraacetic acid solutions. J Inorg Nucl Chem 15(1–2):140–150

    Article  CAS  Google Scholar 

  38. Baetsle L, Bengsch E (1962) Ion-exchange characteristics of the radium-ethylene-diaminetetraacetate complex. J Chromatogr A 8:265–273

    Article  CAS  Google Scholar 

  39. Clever HL, Johnston FJ (1980) The solubility of some sparingly soluble lead salts: an evaluation of the solubility in water and aqueous electrolyte solution. J Phys Chem Ref Data 9(3):751–784

    Article  CAS  Google Scholar 

Download references

Acknowledgments

The work was funded by the Swedish Radiation Protection Authority (SSM). The authors gratefully acknowledge Professor Jan John for pointing us in the right direction and, as with all radium work, our thoughts go to Professor Petr Benec. Stellan Holgersson, Vratislav Langer and Mark Foreman are acknowledged for valuable scientific discussions.

Author information

Authors and Affiliations

  1. Nuclear Chemistry and Industrial Materials Recycling Groups, Division of Energy and Materials, Department of Chemistry and Chemical Engineering, Chalmers University of Technology, Kemivägen 4, 412 96, Gothenburg, Sweden

    Artem V. Matyskin, Burçak Ebin, Mikhail Tyumentsev, Stefan Allard, Gunnar Skarnemark, Henrik Ramebäck & Christian Ekberg

  2. Swedish Defence Research Agency (FOI), CBRN Defence and Security, Cementvägen 20, 901 82, Umeå, Sweden

    Henrik Ramebäck

Authors
  1. Artem V. Matyskin
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Burçak Ebin
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Mikhail Tyumentsev
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Stefan Allard
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Gunnar Skarnemark
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Henrik Ramebäck
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Christian Ekberg
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Artem V. Matyskin.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Matyskin, A.V., Ebin, B., Tyumentsev, M. et al. Disassembly of old radium sources and conversion of radium sulfate into radium carbonate for subsequent dissolution in acid. J Radioanal Nucl Chem 310, 589–595 (2016). https://doi.org/10.1007/s10967-016-4927-x

Download citation

  • Received:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10967-016-4927-x

Keywords

Search

Navigation