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Rapid Screening of Naturally Occurring Radioactive Nuclides (238U, 232Th) in Raw Materials and By-Products Samples Using XRF

  • Park, Ji-Young (Radiation Biotechnology and Applied Radioiostope Science, University of Science & Technology) ;
  • Lim, Jong-Myoung (Korea Atomic Energy Research Institute) ;
  • Ji, Young-Yong (Korea Atomic Energy Research Institute) ;
  • Lim, Chung-Sup (Radiation Biotechnology and Applied Radioiostope Science, University of Science & Technology) ;
  • Jang, Byung-Uck (Korea Institute of Nuclear Safety) ;
  • Chung, Kun Ho (Korea Atomic Energy Research Institute) ;
  • Lee, Wanno (Korea Atomic Energy Research Institute) ;
  • Kang, Mun-Ja (Korea Atomic Energy Research Institute)
  • Received : 2016.03.14
  • Accepted : 2016.09.05
  • Published : 2016.12.31

Abstract

Background: As new legislation has come into force implementing radiation safety management for the use of naturally occurring radioactive materials (NORM), it is necessary to establish a rapid and accurate measurement technique. Measurement of $^{238}U$ and $^{232}Th$ using conventional methods encounter the most significant difficulties for pretreatment (e.g., purification, speciation, and dilution/enrichment) or require time-consuming processes. Therefore, in this study, the applicability of ED-XRF as a non-destructive and rapid screening method was validated for raw materials and by-product samples. Materials and Methods: A series of experiments was conducted to test the applicability for rapid screening of XRF measurement to determine activity of $^{238}U$ and $^{232}Th$ based on certified reference materials (e.g., soil, rock, phosphorus rock, bauxite, zircon, and coal ash) and NORM samples commercially used in Korea. Statistical methods were used to compare the analytical results of ED-XRF to those of certified values of certified reference materials (CRM) and inductively coupled plasma mass spectrometry (ICP-MS). Results and Discussion: Results of the XRF measurement for $^{238}U$ and $^{232}Th$ showed under 20% relative error and standard deviation. The results of the U-test were statistically significant except for the case of U in coal fly ash samples. In addition, analytical results of $^{238}U$ and $^{232}Th$ in the raw material and by-product samples using XRF and the analytical results of those using ICP-MS ($R^2{\geq}0.95$) were consistent with each other. Thus, the analytical results rapidly derived using ED-XRF were fairly reliable. Conclusion: Based on the validation results, it can be concluded that the ED-XRF analysis may be applied to rapid screening of radioactivities ($^{238}U$ and $^{232}Th$) in NORM samples.

Acknowledgement

Grant : Establishment of Technical Basis for Implementation on Safety Management for radiation in the Natural Environment

Supported by : Korea Institute of Nuclear Safety

References

  1. International Commission on Radiological Protection. The 2007 recommendations of the international commission on radiological protection. ICRP Publication 103. 2007;27.
  2. Xhixha G, et al. The worldwide NORM production and a fully automated gamma-ray spectrometer for their characterization. Radioanal. Nucl. Chem. 2013;295:445-457. https://doi.org/10.1007/s10967-012-1791-1
  3. Mas JL, Villa M, Hurtado H, Garcia-Tenorio R. Determination of trace element concentrations and stable lead, uranium and thorium isotope ratios by quadruple-ICP-MS in NORM and NORMpolluted sample leachates. J. Hazard Mater. 2012;205-206:198-207. https://doi.org/10.1016/j.jhazmat.2011.12.058
  4. Baik MH, Kang MJ, Cho YS, Jeong JT. A comparative study for the determination of uranium and uranium isotopes in granitic groundwater. J. Radioanal. Nucl. Chem. 2015;304:9-14. https://doi.org/10.1007/s10967-014-3699-4
  5. L'Annunziata MF. Handbook of radioactivity analysis. 3rd ed. New York, NY. Academic Press. 2012;364-416.
  6. Valkovic V. Radioactivity in environment. 1st ed. New York, NY. Elsevier. 2000;199-204.
  7. Garner J, Cairns J, Read DJ. NORM in the east midlands' oil and gas producing region of the UK. Environ. Radioact. 2015;150:49-56. https://doi.org/10.1016/j.jenvrad.2015.07.016
  8. International Commission on Radiological Protection. Radiation protection and NORM residue management in the titanium dioxide and related industries. Safety Report Series No.76. 2012;53.
  9. Papadopoulos A, Christofides G, Koroneos A, Stoulos S, Papastefanou C. Radioactive secular equilibrium in 238U and 232Th series in granitoids from Greece. Appl. Radiat. Isot. 2013;75:95-104. https://doi.org/10.1016/j.apradiso.2013.02.006
  10. Ji YY, Chung KH, Lim JM, Kim CJ, Jang M, Kang MJ, Park ST. Analytical evaluation of natural radionuclides and their radioactive equilibrium in raw materials and by-products. Appl. Radiat. Isot. 2015;97:1-7. https://doi.org/10.1016/j.apradiso.2014.11.013
  11. Hou X, Roos P. Critical comparison of radiometric and mass spectrometric methods for the determination of radionuclides in environmental, biological and nuclear waste samples. Anal. Chim. Acta. 2008;608:105-139. https://doi.org/10.1016/j.aca.2007.12.012
  12. Becker JS. Mass spectrometry of long-lived radionuclides. Spectrochim. Acta. Part B. 2003;58:1757-1784. https://doi.org/10.1016/S0584-8547(03)00156-3
  13. Verma HR. Atomic and nuclear analytical methods. 1st Ed. New York, NY. Springer. 2006;1-2.
  14. Imanishi Y, BandoA, Komatani S, Wada S. Experimental parameters for XRF analysis of soils. Powder Diffr. 2010;248-255.
  15. Boyle JF. Rapid elemental analysis of sediment samples by isotope source XRF. J. Paleolimnol. 2000;3:213-221.
  16. Trojek T, Cechak T. Detection of terrestrial radionuclides with Xray fluorescence analysis. Radiat. Prot. Dosimetry. 2015;164:529-532. https://doi.org/10.1093/rpd/ncv321
  17. D'Cunha P, Narayana. Comparison of methodologies of gamma ray spectrometer and x-ray fluorescence. Indian. J. Pure Appl. Phys. 2012;50:524-526.
  18. Johnson RL, Durham LA, Rieman GR, Hummel JE. Triad case study: Rattlesnake Creek. Remediation. 2004;15:69-77. https://doi.org/10.1002/rem.20033
  19. International Atomic Energy Agency. IAEA analytical quality in nuclear applications. Series No.32. 2011;12-15.
  20. Thompson M, Wood R. The international harmonized protocol for the proficiency testing of (chemical) analytical laboratories. Pure Appl. Chem. 1993;65:2123-2144. https://doi.org/10.1351/pac199365092123
  21. Feret FR, Hamouche H, Boissonneault Y. Spectral interference in X-ray fluorescence analysis of common materials. Powder Diffr. 2003;46:381-387.
  22. Espen PV, Lemberge P. ED-XRF spectrum evaluation and quantitative analyzing multivariate and nonlinear techniques. Powder Diffr. 2000;43:560-569.
  23. Ramsey MH, Potts PJ, Webb PC, Watkins P, Watson JS, Cloes BJ. An objective assessment of analytical method precision comparison of ICP-AES and XRF for the analysis of silicate rock. Chem. Geol. 1995;124:1-19. https://doi.org/10.1016/0009-2541(95)00020-M
  24. Korea Atomic Energy Research Institute. Development of methods for the determination of 235, 238U, 226Ra, 232Th and 40K in Raw materials or by-products. KAERI-CR-529. 2013;98-101.
  25. Korea Atomic Energy Research Institute. Development of analytical procedures and method validation for quantification of natural radionuclides in raw materials or by-products. KAERICR-576. 2015;63-65.
  26. International Atomic Energy Agency. Radiation protection and NORM residue management in the zircon and zirconia industries. Safety Report series No.51. 2007;119.