Browse > Article
http://dx.doi.org/10.7733/jnfcwt.2021.19.3.367

Overestimation of Radioactivity Concentration of Difficult-To-Measure Radionuclides in Scaling Factor Methodology  

Park, Junghwan (Korea Atomic Energy Research Institute)
Kim, Tae-Hyeong (Korea Atomic Energy Research Institute)
Lee, Jeongmook (Korea Atomic Energy Research Institute)
Kim, Junhyuck (Korea Atomic Energy Research Institute)
Kim, Jong-Yun (Korea Atomic Energy Research Institute)
Lim, Sang Ho (Korea Atomic Energy Research Institute)
Publication Information
Journal of Nuclear Fuel Cycle and Waste Technology(JNFCWT) / v.19, no.3, 2021 , pp. 367-386 More about this Journal
Abstract
The overestimation and underestimation of the radioactivity concentration of difficult-to-measure radionuclides can occur during the implementation of the scaling factor (SF) method because of the uncertainties associated with sampling, radiochemical analysis, and application of SFs. Strict regulations ensure that the SF method as an indirect method does not underestimate the radioactivity of nuclear wastes; however, there are no clear regulatory guidelines regarding the overestimation. This has been leading to the misuse of the SF methodology by stakeholders such as waste disposal licensees and regulatory bodies. Previous studies have reported instances of overestimation in statistical implementation of the SF methodology. The analysis of the two most popular linear models of the SF methodology showed that severe overestimation may occur and radioactivity concentration data must be dealt with care. Since one major source of overestimation is the use of minimum detectable activity (MDA) values as true activity values, a comparative study of instrumental techniques that could reduce the MDAs was also conducted. Thermal ionization mass spectrometry was recommended as a suitable candidate for the trace level analysis of long-lived beta-emitters such as iodine-129. Additionally, the current status of the United States and Korea was reviewed from the perspective of overestimation.
Keywords
Scaling factor; Overestimation; Radioactivity concentration; Minimum detectable activity;
Citations & Related Records
연도 인용수 순위
  • Reference
1 International Atomic Energy Agency. Determination and Use of Scaling Factors for Waste Characterization in Nuclear Power Plants, International Atomic Energy Agency Report, IAEA Nuclear Energy Series NW-T1.18 (2009).
2 K. Il Jung, N.G. Jeong, Y.P. Moon, M.S. Jeong, and J.B. Park, "Prediction of Radionuclide Inventory for the Low- and Intermediate-Level Radioactive Waste Disposal Facility by the Radioactive Waste Classification (in Korean)", J. Nucl. Fuel Cycle Waste Technol., 14(1), 63-78 (2016).   DOI
3 K. Shi, X. Hou, P. Roos, and W. Wu, "Determination of Technetium-99 in Environmental Samples: A Review", Anal. Chim. Acta, 709, 1-20 (2012).   DOI
4 M. Honda, H. Matsuzaki, H. Nagai, and K. Sueki, "Depth Profiles and Mobility of 129I Originating From the Fukushima Dai-ichi Nuclear Power Plant Disaster Under Different Land Uses", Appl. Geochemistry, 85, Part B, 169-179 (2017).   DOI
5 X. Hou, "Radioanalysis of Ultra-Low Level Radionuclides for Environmental Tracer Studies and Decommissioning of Nuclear Facilities", J. Radioanal. Nucl. Chem., 322(3), 1217-1245 (2019).   DOI
6 U.S. Nuclear Regulatory Commission, Standards For Protection Against Radiation, Code of Federal Regulations Title 10 Part 20, United States (2016).
7 U.S. Nuclear Regulatory Commission. Instructions for Completing the U.S. Nuclear Regulatory Commission's Uniform Low-Level Radioactive Waste Manifest, U.S. Nuclear Regulatory Commission Report, NUREG/BR-0204 (1998).
8 M. Kutner, C. Nachtsheim, and J. Neter, Applied Linear Regression Models, 4th ed., Richard D. Irwin. Inc., Homewood (2004).
9 W.T. Best and A.D. Miller. Updated Scaling Factors in Low-Level Radwaste, Electric Power Research Institute Report, EPRI-NP-5077 (1987).
10 L.M. Edwards, Project Number 0800, Revision to NUREG/BR-0204, "Instructions for Completing NRC's Uniform Low-Level Radioactive Waste Manifest", Electric Power Research Institute Letter to U.S. Nuclear Regulatory Commission, ML13260A075 (2013).
11 E.J. Wyse, Inductively Coupled Plasma-Mass Spectrometric (ICP-MS) Analysis, Pacific Northwest National Laboratory Technical Procedure, PNL-ALO-280 (1993).
12 Y.K. Hsieh, T. Wang, L.W. Jian, W.H. Chen, T.L. Tsai, and C.F. Wang, "An Improved Analytical Method for Iodine-129 Determination in Low-Level Radioactive Waste", Radiochim. Acta, 102(12), 1137-1142 (2014).   DOI
13 J. Kim, J.Y. Kim, S.E. Bae, K. Song, and J.H. Park, "Review of the Development in Determination of 129I Amount and the Isotope Ratio of 129I/127I using Mass Spectrometric Measurements", Microchem. J., 169, 106476 (2021).   DOI
14 D.J. Rokop, N.C. Schroeder, and K. Wolfsberg, "Mass Spectrometry of Technetium at the Subpicogram level", Anal. Chem., 62(13), 1271-1274 (1990).   DOI
15 S. Uchida, K. Tagami, W. Ruhm, M. Steiner, and E. Wirth, "Separation of Tc-99 in Soil and Plant Samples Collected Around the Chernobyl Reactor Using a Tc-Selective Chromatographic Resin and Determination of the Nuclide by ICP-MS", Appl. Radiat. Isot., 53(1-2), 69-73 (2000).   DOI
16 T.J. Anderson and R.L. Walker, "Determination of Picogram Amounts of Technetium-99 by Resin Bead Mass Spectrometric Isotope Dilution", Anal. Chem., 52(4), 709-713 (1980).   DOI
17 S.K. Sahoo, Y. Muramatsu, S. Yoshida, H. Matsuzaki, and W. Ruhm, "Determination of 129I and 127I Concentration in Soil Samples From the Chernobyl 30-km Zone by AMS and ICP-MS", J. Radiat. Res., 50(4), 325-332 (2009).   DOI
18 J.M. Gomez-Guzman, S.M. Enamorado-Baez, A.R. Pinto-Gomez, and J.M. Abril-Hernandez, "Microwave-Based Digestion Method for Extraction of 127I and 129I From Solid Material for Measurements by AMS and ICP-MS", Int. J. Mass Spectrom., 303(2-3), 103-108 (2011).   DOI
19 J.E. Olson, M.L. Adamic, D.C. Snyder, J.L. Brookhart, P.A. Hahn, and M.G. Watrous, "Independent Measurements of 129I Content in Environmental Reference Materials Using Accelerator and Thermal Ionization Mass Spectrometry", Nucl. Instrum. Methods Phys. Res. Sect. B Beam Interact. with Mater. Atoms, 438, 84-88 (2019).   DOI
20 D.E. Robertson, C.W. Thomas, S.L. Pratt, E.A. Lepel, and V.W. Thomas. Low-Level Radioactive Waste Classification, Characterization, and Assessment: Waste Streams and Neutron-Activated Metals, U.S. Nuclear Regulatory Commission Report, NUREG/CR-6567, PNNL-11659 (2000).
21 Korea Institute of Nuclear Safety. Technical Review Report on Follow-up Measures for Construction Permit and Operation License of LILW Disposal Facility (in Korean), Korea Institute of Nuclear Safety Report, KINS/AR-1023 (2014).
22 J.L. Mas, K. Tagami, and S. Uchida, "Method for the Detection of Tc in Seaweed Samples Coupling the use of Re as a Chemical Tracer and Isotope Dilution Inductively Coupled Plasma Mass Spectrometry", Anal. Chim. Acta, 509(1), 83-88 (2004).   DOI
23 F.P. Brauer and J.H. Kaye, "Detection Systems for the Low Level Radiochemical Analysis of Iodine-131, Iodine-129 and Natural Iodine in Environmental Samples", IEEE Trans. Nucl. Sci., 21(1), 496-502 (1974).   DOI
24 P. Dixon, D.B. Curtis, J. Musgrave, F. Roensch, J. Roach, and D. Rokop, "Analysis of Naturally Produced Technetium and Plutonium in Geologic Materials", Anal. Chem., 69(9), 1692-1699 (1997).   DOI
25 M.D. Engelmann, L.A. Metz, J.E. Delmore, M. Engelhard, and N.E. Ballou, "Electrodeposition of Technetium on Platinum for Thermal Ionization Mass Spectrometry (TIMS)", J. Radioanal. Nucl. Chem., 276(2), 493-498 (2008).   DOI
26 E.J. Wyse, ICP/MS Determination of 99Tc, Pacific Northwest National Laboratory Technical Procedure, PNL-ALO-281 (1993).
27 L.A. Currie. Lower Limit of Detection: Definition and Elaboration of a Proposed Position for Radiological Effluent and Environmental Measurements, U.S. Nuclear Regulatory Commission Report, NUREG/CR4007 (1984).
28 J.E. Delmore, "Isotopic Analysis of Iodine Using Negative Surface Ionization", Int. J. Mass Spectrom. Ion Phys., 43(4), 273-281 (1982).   DOI
29 B.A. Bergquist, A.A. Marchetti, R.E. Martinelli, J.E. McAninch, G.J. Nimz, I.D. Proctor, J.R. Southon, and J.S. Vogel, "Technetium Measurements by Accelerator Mass Spectrometry at LLNL", Nucl. Instrum. Methods Phys. Res. Sect. B Beam Interact. with Mater. Atoms, 172(1-4), 328-332 (2000).   DOI
30 C.W. Thomas, V.W. Thomas, and D.E. Robertson. Radioanalytical Technology for 10 CFR Part 61 and Other Selected Radionuclides, U.S. Nuclear Regulatory Commission Report, NUREG/CR-6230, PNL-9444 (1996).
31 B. Cox and P. Saunders. Development of Generic Scaling Factors for Technetium-99 and Iodine-129 in Low and Intermediate Level Waste, Electric Power Research Institute Report, 3002005564 (2015).
32 U.S. Nuclear Regulatory Commission, Licensing Requirements for Land Disposal of Radioactive Waste, Code of Federal Regulations Title 10 Part 61, United States (2006).
33 Nuclear Safety and Security Commission, General Acceptance Criteria for Low- and Intermediate-Level Radioactive Waste (in Korean), Nuclear Safety and Security Commission Notice No. 2021-26, Republic of Korea (2021).
34 Nuclear Safety and Security Commission, Regulation on the Criteria for the Classification and Clearance of Radioactive Wastes (in Korean), Nuclear Safety and Security Commission Notice No. 2020-6, Republic of Korea (2020).
35 T.H. Kim, J. Park, J. Lee, J. Kim, J.Y. Kim, and S.H. Lim, "Statistical Methodologies for Scaling Factor Implementation: Part 1. Overview of Current Scaling Factor Method for Radioactive Waste Characterization", J. Nucl. Fuel Cycle Waste Technol., 18(4), 517-536 (2020).   DOI
36 P.S. Mann and C.J. Lacke, Introductory Statistics, 8th ed., Wiley, Hoboken (2012).
37 W.T. Best and A.D. Miller. Radionuclide Correlations in Low-Level Radwaste, Electric Power Research Institute Report, EPRI-NP-4037 (1985).
38 D.W. James and T. Kalinowski. Developing Alternative Low Level Waste Disposal Criteria Per 10 CFR 61.58, Electric Power Research Institute Report, 1019222 (2009).
39 Korea Atomic Energy Research Institute. Chemical Analysis of Radioactive Materials (in Korean), Korea Atomic Energy Research Institute Report, KAERI/RR-4323/2017 (2018).
40 Electric Power Research Institute. Low Level Waste Characterization Guidelines, Electric Power Research Institute Report, TR-107201 (1996).
41 U.S. Nuclear Regulatory Commission, Reporting of H-3, C-14, Tc-99, and I-129 on the Uniform Waste Manifest, U.S. Nuclear Regulatory Commission Regulatory Issue Summary 2015-02 (2015).
42 D.C. Montgomery, E.A. Peck, and G.G. Vining, Introduction to Linear Regression Analysis, 5th ed., Wiley, Hoboken (2012).
43 U.S. Nuclear Regulatory Commission, Low-Level Radioactive Waste Scaling Factors, 10 CFR Part 61, U.S. Nuclear Regulatory Commission Information Notice No. 86-20 (1986).
44 T. Kim, K. Kang, S. Lee, and K. Lee, "Development of Scaling Factor Program for Radioactive Waste (in Korean)", Proc. of Korean Radioactive Waste Society Spring 2006, June 15-16, 2006, Seoul.
45 A.K. Bhattacharyya, R. Janati, and T. Shearer, "Safety Issues Related to Disposal of I-129 in a Low Level Radioactive Waste Repository", Proc. of the 9th Annual DOE Low-level Waste Management Conference, August 27-28, 1987, Denver.
46 International Organization for Standardization, Nuclear Energy - Nuclear Fuel Technology - Scaling Factor Method to Determine the Radioactivity of Low- and Intermediate-Level Radioactive Waste Packages Generated at Nuclear Power Plants, International Organization for Standardization, ISO 21238 (2007).
47 S.F. Fang and T.C. Chu, "Study on Determination of Technetium-99 in Environmental Samples", Proc. of International Congress of the International Radiation Protection Association, May 14-19, 2000, Tokyo.
48 U.S. Department of Energy. Final Environmental Impact Statement for the Disposal of Greater-Than-Class C (GTCC) Low-Level Radioactive Waste and GTCC-Like Waste, U.S. Department of Energy Report, EIS0375 (2016).
49 K. Il Jung, J.H. Kim, N.G. Jeong, and J.B. Park, "Comparison of Radionuclide Inventory Between Predicted and Measured Activity of Dry Active Waste From Korea Nuclear Power Plant (in Korean)", J. Nucl. Fuel Cycle Waste Technol., 15(3), 281-299 (2017).   DOI
50 Korea Institute of Nuclear Safety. Disposal Inspection Report of LILW Disposal Facility (in Korean), Korea Institute of Nuclear Safety Report, KINS/AR-1036 Vol. 23, Issue 1 (2021).
51 S. Bang, "Development and Application Status of LILW Scaling Factor (in Korean)", Proc. of the 18th Nuclear Safety Information Conference, April 14-15, 2015, Daejeon.
52 R.S. Strebin, F.P. Brauer, J.H. Kaye, M.S. Rapids, and J.J. Stoffel, "Neutron Activation and Mass Spectrometric Measurement of 129I", J. Radioanal. Nucl. Chem., 127(1), 59-73 (1988).   DOI
53 F.P. Brauer, "Measurement Methods for Low-Level 129I Determinations", Proc. of the 11th Annual DOE Low-level Waste Management Conference, August 22-24, 1989, Pittsburgh.
54 C.J. Park, H.Y. Choi, M. Boravy, S. Alrawash, J.M. Lee, S.U. Yoo, and H. Han. Radioactive Waste Isotope Characterization Method Development (in Korean), Korea Atomic Energy Research Institute Report, KAERI/CM-2765/2019 (2018).
55 U.S. Nuclear Regulatory Commission. Draft Environmental Impact Statement on 10 CFR Part 61 Licensing Requirements for Land Disposal of Radioactive Waste, U.S. Nuclear Regulatory Commission Report, NUREG-0782 (1981).
56 S. Foti, E. Delucchi, and V. Akamian, "Determination of Picogram Amounts of Technetium in Environmental Samples by Neutron Activation Analysis", Anal. Chim. Acta, 60(2), 269-276 (1972).   DOI
57 M.R. Smith, E.J. Wyse, and D.W. Koppenaal, "Radionuclide Detection by Inductively Coupled Plasma Mass Spectrometry: A Comparison of Atomic and Radiation Detection Methods", J. Radioanal. Nucl. Chem., 160(2), 341-354 (1992).   DOI
58 P. Hepiegne, D. Dall'ava, R. Clement, and J.P. Degros, "The Separation of 99Tc From Low and Medium-Level Radioactive Wastes and Its Determination by Inductively Coupled Plasma Mass Spectrometry", Talanta, 42(6), 803-809 (1995).   DOI
59 J.E. McAninch, A.A. Marchetti, B.A. Bergquist, N.J. Stoyer, G.J. Nimz, M.W. Caffee, R.C. Finkel, K.J. Moody, E. Sideras-Haddad, B.A. Buchholz, B.K. Esser, and I.D. Proctor, "Detection of 99Tc by Accelerator Mass Spectrometry: Preliminary Investigations", J. Radioanal. Nucl. Chem., 234(1-2), 125-129 (1998).   DOI
60 C.K. Kim, R. Seki, S. Morita, S.I. Yamasaki, A. Tsumura, Y. Takaku, Y. Igarashi, and M. Yamamoto, "Application of a High Resolution Inductively Coupled Plasma Mass Spectrometer to the Measurement of Long-Lived Radionuclides", J. Anal. At. Spectrom., 6(3), 205-209 (1991).   DOI
61 T. Kim, "Application of Scaling Factor for Radioactive Waste (in Korean)", Proc. of the 12th Nuclear Safety Information Conference, April 5-6, 2007, Daejeon.
62 U.S. Nuclear Regulatory Commission, Low-Level Waste Licensing Branch Technical Position on Radioactive Waste Classification, U.S. Nuclear Regulatory Commission Branch Technical Position, ML033630755 (1983).
63 J. Olson, M. Adamic, D. Snyder, J. Brookhart, P. Hahn, and M. Watrous, "A Comparative Study of 129I Content in Environmental Standard Materials IAEA-375, NIST SRM 4354 and NIST SRM 4357 by Thermal Ionization Mass Spectrometry and Accelerator Mass Spectrometry", Appl. Radiat. Isot., 126, 54-57 (2017).   DOI
64 S. Chatterjee and A.S. Hadi, "Influential Observations, High Leverage Points, and Outliers in Linear Regression", Stat. Sci., 1(3), 379-393 (1986).   DOI