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Analytical method for determination of 41Ca in radioactive concrete

  • Lee, Yong-Jin (Nuclear Emergency and Environmental Protection Division, Korea Atomic Energy Research Institute) ;
  • Lim, Jong-Myoung (Nuclear Emergency and Environmental Protection Division, Korea Atomic Energy Research Institute) ;
  • Lee, Jin-Hong (Environmental Engineering, Chung-Nam University) ;
  • Hong, Sang-Bum (Decontamination & Decommissioning Research Division, Korea Atomic Energy Research Institute) ;
  • Kim, Hyuncheol (Nuclear Emergency and Environmental Protection Division, Korea Atomic Energy Research Institute)
  • Received : 2020.05.21
  • Accepted : 2020.09.16
  • Published : 2021.04.25

Abstract

The analysis of 41Ca in concrete generated from the nuclear facilities decommissioning is critical for ensuring the safe management of radioactive waste. An analytical method for the determination of 41Ca in concrete is described. 41Ca is a neutron-activated long radionuclide, and hence, for accurate analysis, it is necessary to completely extract Ca from the concrete sample where it exists as the predominant element. The decomposition methods employed were the acid leaching, microwave digestion, and alkali fusion. A comparison of the results indicated that the alkali fusion is the most suitable way for the separation of Ca from the concrete sample. Several processes of hydroxide and carbonate precipitation were employed to separate 41Ca from interferences. The method relies on the differences in the solubility of the generated products. The behavior of Ca and the interfering elements such as Fe, Ni, Co, Eu, Ba, and Sr is examined at each separation step. The purified 41Ca was measured by a liquid scintillation counter, and the quench curve and counting efficiency were determined by using a certified reference material of known 41Ca activity. The recoveries in this study ranged from 56 to 68%, and the minimum detectable activity was 50 mBq g-1 with 0.5 g of concrete sample.

Keywords

Acknowledgement

This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government, Ministry of Science and ICT (No. 2017M2A8A5015143).

References

  1. IAEA, Operational reactors by age, 2020. https://pris.iaea.org/PRIS/WorldStatistics/OperationalByAge.aspx. (Accessed 14 May 2020).
  2. OECD and NEA, R&D and Innovation Needs for Decommissioning of Nuclear Facilities, 2014. NEA No. 7191.
  3. R. Aker, Maine Yankee Decommissioning Experience Report (1997-2004), New Horizon Scientific, LLC, 2005.
  4. KAERI, Nuclear data center at KAERI, 2020. http://atom.kaeri.re.kr. (Accessed 14 May 2020).
  5. IAEA, Radiological Characterization of Shut Down Nuclear Reactors for Decommissioning Purposes, International Atomic Energy Agency, Vienna, 1998. TRS No. 389.
  6. X. Hou, Radiochemical determination of 41Ca in nuclear reactor concrete, Radiochim. Acta 93 (9-10) (2005) 611-617. https://doi.org/10.1524/ract.2005.93.9-10.611
  7. D. Hampe, B. Gleisberg, S. Akhmadaliev, G. Rugel, S. Merchel, Determination of 41Ca with LSC and AMS: method development, modifications and applications, J. Radioanal. Nucl. Chem. 296 (2) (2013) 617-624. https://doi.org/10.1007/s10967-012-2145-8
  8. A.J. Pearson, S. Gaw, N. Hermanspahn, C.N. Glover, Natural and anthropogenic radionuclide activity concentrations in the New Zealand diet, J. Environ. Radioact. 151 (2016) 601-608. https://doi.org/10.1016/j.jenvrad.2015.05.022
  9. P.E. Warwick, I.W. Croudace, D.J. Hillegonds, Effective determination of the long-lived nuclide 41Ca in nuclear reactor bioshield concretes: comparison of liquid scintillation counting and accelerator mass spectrometry, Anal. Chem. 81 (5) (2009) 1901-1906. https://doi.org/10.1021/ac802225a
  10. L. Hoon, L. Jong-Myoung, J. Young-Yong, J. Kun-Ho, K. Mun-Ja, C. Geun-Sik, L. Jin-Hong, Comparison of pretreatment methods for determination of 55Fe and 63Ni activity in nuclear wastes sample, Journal of Nuclear Fuel Cycle and Waste Technology 13 (2) (2015) 113-122. https://doi.org/10.7733/JNFCWT.2015.13.2.113
  11. E. Braysher, B. Russell, S. Woods, M. Garcia-Miranda, P. Ivanov, B. Bouchard, D. Read, Complete dissolution of solid matrices using automated borate fusion in support of nuclear decommissioning and production of reference materials, J. Radioanal. Nucl. Chem. 321 (1) (2019) 183-196. https://doi.org/10.1007/s10967-019-06572-z
  12. B. Russell, M. Garcia-Miranda, P. Ivanov, Development of an optimised method for analysis of 90Sr in decommissioning wastes by triple quadrupole inductively coupled plasma mass spectrometry, Appl. Radiat. Isot. 126 (2017) 35-39. https://doi.org/10.1016/j.apradiso.2017.01.025
  13. Q. Chen, X. Hou, Y. Yu, H. Dahlgaard, S.P. Nielsen, Separation of Sr from Ca, Ba and Ra by means of Ca(OH)2 and Ba(Ra)Cl2 or Ba(Ra)SO4 for the determination of radiostrontium, Anal. Chim. Acta 466 (1) (2002) 109-116. https://doi.org/10.1016/S0003-2670(02)00571-8
  14. J.S. Becker, Mass spectrometry of long-lived radionuclides, Spectrochim. Acta B Atom Spectrosc. 58 (10) (2003) 1757-1784. https://doi.org/10.1016/S0584-8547(03)00156-3
  15. I.W. Croudace, B.C. Russell, P.W. Warwick, Plasma source mass spectrometry for radioactive waste characterisation in support of nuclear decommissioning: a review, J Anal Atom Spectrom 32 (3) (2017) 494-526. https://doi.org/10.1039/C6JA00334F
  16. C.K. Kim, R. Seki, S. Moritat, S.I. Yamasaki, A. Tsumura, Y. Takaku, Y. Igarashi, M. Yamamoto, Application of a high resolution inductively coupled plasma mass spectrometer to the measurement of long-lived radionuclides, J Anal Atom Spectrom 6 (3) (1991) 205-209. https://doi.org/10.1039/JA9910600205
  17. J. Sabine Becker, Recent developments in isotope analysis by advanced mass spectrometric techniques Plenary lecture, J Anal Atom Spectrom 20 (11) (2005) 1173-1184. https://doi.org/10.1039/b508895j
  18. X. Hou, P. Roos, Critical comparison of radiometric and mass spectrometric methods for the determination of radionuclides in environmental, biological and nuclear waste samples, Anal. Chim. Acta 608 (2) (2008) 105-139. https://doi.org/10.1016/j.aca.2007.12.012
  19. L. Zerle, T. Faestermann, K. Knie, G. Korschinek, E. Nolte, J. Beer, U. Schotterer, The 41Ca bomb pulse and atmospheric transport of radionuclides, J. Geophys. Res.: Atmosphere 102 (D16) (1997) 19517-19527. https://doi.org/10.1029/97JD00701
  20. N. Trautmann, G. Passler, K. Wendt, Ultratrace analysis and isotope ratio measurements of long-lived radioisotopes by resonance ionization mass spectrometry (RIMS), Anal. Bioanal. Chem. 378 (2004) 348-355. https://doi.org/10.1007/s00216-003-2183-8
  21. E. Nottoli, D. Bourles, P. Bienvenu, A. Labet, M. Arnold, M. Bertaux, Accurate determination of 41Ca concentrations in spent resins from the nuclear industry by Accelerator Mass Spectrometry, Appl. Radiat. Isot. 82 (2013) 340-346. https://doi.org/10.1016/j.apradiso.2013.09.005
  22. H. Kim, Y. Jung, Y.Y. Ji, J.M. Lim, K.H. Chung, M.J. Kang, Validation of a procedure for the analysis of 226Ra in naturally occurring radioactive materials using a liquid scintillation counter, J. Environ. Radioact. 166 (2017) 188-194. https://doi.org/10.1016/j.jenvrad.2016.05.003
  23. A. Carles, Synergic quenching effects of water and carbon tetrachloride in liquid scintillation gel samples, Appl. Radiat. Isot. 64 (2006) 1505-1509. https://doi.org/10.1016/j.apradiso.2006.02.065
  24. L.A. Currie, Limits for qualitative detection and quantitative determination: application to radiochemistry, Anal. Chem. 40 (3) (1968) 586-593. https://doi.org/10.1021/ac60259a007