臺灣博碩士論文加值系統

In this research we established a radionuclide activity absolute counting system which can be the primary standard of the calibration chain for radionuclide activity measurement area in Taiwan. The counting system was composed of a 4π proportional counter, two NaI(Tl) detectors, NIM modules and a personal computer. The proportional counter and the NaI(Tl) detectors respectively detect the charged particles and photons and work with coincidence. That allows researchers to measure the radionuclide activity only by the counts of the counting system and do not need any standard sources. The performance of the counting system was verified by international comparisons and showed that the measurement result of the counting system is equivalent with the Key Comparison Reference Value. The primary standard system was applied to nuclear medicine area and radioactive waste clearance measurement area in this research. In nuclear medicine area, the activity of two radiopharmaceuticals, 67Ga and 188Re, were standardized by the counting system. The standardized radioactive solution of the two nuclides with the standard uncertainties smaller than 0.5% was introduced to calibrate the 4πγ ionization chambers of National Radiation Standard Laboratory, and the Capintec-CRC15R radionuclide activity calibrator which was popularly used in hospitals and radiopharmacies to enhance the accuracy of activity dose received by patients. In radioactive waste clearance measurement area, the standard drums, the calibration techniques of radioactive waste drum counting system and the correction methods of the primal measurement data of the drum counting systems were developed and applied to the proficiency testing study. These techniques improved the proficiency testing pass rate of participants from 20% (primal result of participants) to 70% (corrected result of participants). Details of the primary standard system, the associated techniques and results are described in this report.

本研究建立放射源活度的絕對量測系統，可作為國內放射源活度量測校正鏈之原級標準。此量測系統是由一支4 π比例計數器、2支碘化鈉偵檢器、核儀模組及一部個人電腦所組成，放射源的活度可由此量測系統的計數值直接導出，而無須藉助其他的標準放射源。本量測系統參與多次的國際量測比對活動，其量測結果皆與國際比對參考值達到等同程度，確證了本量測系統的整體性能。在本研究中將此原級標準系統應用於核子醫學領域與放射性廢棄物解除管制量測領域，在核子醫學領域中，本報告以此系統建立67Ga與188Re放射性藥物的放射活度原級標準，其量測不確定度小於0.5％，此活度標準藉由經量測系統標準化後的放射性藥物，傳遞至國家游離輻射標準實驗室所屬的4πγ游離腔與一般醫院及製藥中心常用的Capintec-CRC 15R放射核種校正器上，用以增進病患接受放射性藥物活度劑量的準確度。在放射性廢棄物解除管制量測領域，本研究建立標準校正桶與放射性廢料桶量測儀器的校正技術與數據修正方法，並且將這些技術與方法應用於放射性廢棄物解除管制量測能力試驗的研究上，由能力試驗的結果分析，本研究所建立技術與方法，可將能力試驗參與者的通過率由20％ 提升至70％。關於本研究建立的原級標準量測系統及相關的技術與方法將詳述於本報告中。

Abstract i
摘要 ii
誌謝 iii
Table of Contents iv
List of Figures viii
List of Tables xi
Chapter 1. Introduction 1
Chapter 2. Principles of 4πβ-γ coincidence counting techniques 6
2.1. Corrections related to the counting rate 8
2.1.1. Dead time correction 8
2.1.2. Resolving time correction 10
2.2. Corrections related to the detection efficiency 13
2.3. Linear extrapolation 18
Chapter 3. System implementation and verification 23
3.1. The assembly of 4πβ-γ coincidence counting system 23
3.2. System properties 27
3.2.1. 4? proportional counter 27
3.2.2. Dead time of the system 28
3.2.3. Resolving time of coincidence channels 31
3.3. Uncertainties evaluation of measurement result 35
3.3.1. Counting 36
3.3.2. Dead time and resolving time measurement 37
3.3.3. Background 37
3.3.4. Decay time 38
3.3.5. Weighing 39
3.3.6. Linear extrapolation 41
3.3.7. Combined standard uncertainty 41
3.4. System verification 45
Chapter 4. Absolute counting techniques for radiopharmaceuticals 47
4.1. Absolute counting of 188Re radiopharmaceuticals and the measurement standard dissemination 48
4.1.1. Introduction 48
4.1.2. Methods 49
4.1.3. Result and discussion 51
4.1.4. Conclusions 56
4.2. Primary standardization of 67Ga radiopharmaceuticals and the measurement standard dissemination 57
4.2.1. Introduction 57
4.2.2. Methods 58
4.2.3. Materials 62
4.2.4. Result and discussion 63
4.2.5. Conclusions 69
Chapter 5. Radionuclide activity standard dissemination and comparisons for the clearance measurement of radioactive waste in Taiwan 70
5.1. The calibration and evaluation of a radioactive waste drum counting system 71
5.1.1. Introduction 71
5.1.2. Methods 72
5.1.3. Results and discussion 75
5.1.4. Conclusions 82
5.2. Proficiency testing feasibility study for the measurement of gamma-emitting clearance samples 83
5.2.1. Introduction 83
5.2.2. Methods 84
5.2.3. Results and discussion 91
5.2.4. Conclusions 99
Chapter 6. Conclusions and future works 101
Reference 104
Appendix - Publication list 114

Attie, M. R. P., Koskinas, M. F., Dias, M. S., Fonseca, K. A., 1998. Absolute disintegration rate measurements of Ga-67. Applied Radiation and Isotopes. 49, 1175 - 1177.
Baerg A.P., 1973. The Efficiency Extrapolation Method in Coincidence Counting. Nuclear Instruments and Methods. 112, 143-150
Bé, M.M., Chisté, V., Dulieu, C., Browne, E., Kuzmenko, N., Helmer, R., Nichols, A., Schönfeld, E., Dersch, R. 2004. Table of radionuclides, Monographie BIPM-5, Bureau International Des Poids Et Mesures, Sevres, France.
BIPM, 2006. The International System of Units (SI) 8th edition, Organisation Intergouvernementale de la Convention du Mètre.
BIPM, 2009. Director’s Report on the Activity and Management of the International Bureau of Weights and Measures (1 July 2007 – 30 June 2008). BIPM, France
BIPM, KCDB, 2009. http://kcdb.bipm.org/AppendixB/KCDB_ApB_search.asp.
Bobin, C., 2007. Primary standardization of activity using the coincidence method based on analogue instrumentation. Metrologia. 44, S27-S31.
Bobin, C., Bouchard, J., Hamon, C., Iroulart, M.G., Plagnard, J., 2007. Standardization of 67Ga using a 4??LS)β-γ anti-coincidence system. Applied Radiation and Isotopes. 65, 757-763.
Bombardieri, E., Aktolun C., Baum, R. P., Bishof-Delaloye, A., Buscombe, J., Chatal, J. F., Maffioli, L., Moncayo, R., Mortelmans, L., Reske, S. N., 2003. 67Ga scintigraphy: procedure guidelines for tumour imaging. European Journal of Nuclear Medicine and Molecular Imaging. 30, BP125 - BP131.
Brandi, H. S., and Souza de, T. L., 2009. Metrology infrastructure for sustainable development of the Americas: the role of SIM. Accreditation and Quality Assurance. 14, 567–573.
Brinkman, G.A., Aten, A. H. W. Jr. and Veenboer, J. Th. 1963. Absolute Standardization with a NaI(Tl) Crystal-I. International Journal of Applied Radiation and Isotopes. 14, 153-157
Bruggeman, M., Gerits, J., Carchon, R., 1999. A minimum biased shell-source method for the calibration of rad waste assay systems. Applied Radiation and Isotopes. 51, 255 - 259.
Bryant J., 1963. Coincidence Counting Correction for Dead-time Loss and Accidental Coincidences. International Journal of Applied Radiation and Isotopes. 14, 143-151.
Campion P.J., 1959. The Standardization of Radioisotopes by the Beta-Gamma Coincidence Method Using High Efficiency Detectors. International Journal of Applied Radiation and Isotopes. 4, 232-248.
Capintec, Inc., 1990. Radioisotope dose calibrator owner’s manual. Capintec, Inc. Pittsburgh, PA.
CEC. 1996. TestPoint User’s guide, Capital Equipment Corporation, Billerica, Massachusetts.
Certificate of Compliance, 1992. National Physical Laboratory Certificate of Compliance. Reference R1118. National Physical Laboratory, England.
Chang, T. Y., Chiou, G. S., Chen, W. L., Tsai, C. M., 1980. The absolute counting of complex decay nuclides. INER-0337, Institute of Nuclear Energy Research, Lungtan (in Chiness).
Chou, Y. Y., Chang, T. Y., Chiou, G. S., Tsai, C. M., 1977. 4πβ-γ coincidence countingh. INER-T0569, Institute of Nuclear Energy Research, Lungtan (in Chiness).
Chou, D. P., Wei, Y. H., Chen, W. L., Chiu, K. S., Chiu, C. H., 2002. Direct measurement of 60Co radioactivity bt the 4πβ-γ coincidence method. INER-1113, Institute of Nuclear Energy Research, Lungtan.
Dean, J., 2009. A UK comparison for measurements of low levels of gamma–emitters in waste drums. Applied Radiation and Isotopes. 67, 678 – 682.
Dinescu, L., Vata, I., Cazan, I. L., Macrin, R., Caragheorgheopol, Gh., Rotarescu, Gh., 2002. On the efficiency calibration of a drum waste assay system. Nuclear Instruments and Methods. A478, 661-666.
Early, J. F., Durack, L., Williams, D. and Vanderheyden, J. L., 1990. Consideration for imaging Re-188 and Re-186 isotopes. Clinical Nuclear Medicine. 15, 911-916.
Gandy A. 1962. Absolute Measurement of the Activity of Radionuclides by the Beta-Gamma Coincidence Method Using Detectors of Great Efficiency – Dead Time Corrections. International Journal of Applied Radiation and Isotopes. 13, 501-513.
Grigorescu, L., 1973. Accuracy of coincidence measurements. Nuclear Instruments and Methods. 112, 151-155.
García-Toraño, E., Roteta, M., 2004. Standardization of 67Ga by 4?逽^(NaI) and 4?逽]-γ-coincidence methods. Applied Radiation and Isotopes. 60, 353-356.
Hayward R.W. 1961. On the Determination of Disintegration Rates by the Coincidence Method Using High Efficiency Detectors. International Journal of Applied Radiation and Isotopes. 12, 148-150.
Hafeli, U., Pauer, G., Failing, S. and Tapolsky, G., 2001. Radiolabeling of magnetic particles with rhenium-188 for cancer therapy. Journal of Magnetism and Materials. 225, 73-78.
IAEA, 2004. Application of the concepts of exclusion, exemption and clearance. IAEA Safety Standard Series No. RS-G-1.7, Vienna.
ICRU 52, 1994. Particle Counting in Radioactivity Measurements. International Commission on Radiation Units and Measurements, Bethesda Maryland.
ICRU 60, 1998. Fundamental Qualities and Units for Ionizing Radiation. International Commission on Radiation Units and Measurements, Bethesda Maryland.
ISO Guide 43-1, 1997, Proficiency testing by interlaboratory comparisons – Part 1: Development and operation of proficiency testing schemes.
ISO. 1995. Guide to the Expression of Uncertainty in Measurement, International Organization for Standardization, Switzerland.
Jaffey, A.H., 1954. Solid angle subtended by a circular aperture at point and spread sources: formulas and some tables. Review of Scientific Instruments. 25 (4), 349–354.
Jeong, J. M., Lee, Y. J., Kim, E. H., Chang, Y. S., Kim, Y. J., Son, M., Lee, S. D., Chung, J. K. and Lee, M. C., 2003. Preparation of 188Re-labled paper for treating skin cancer. Applied Radiation and Isotopes. 58, 551-555.
Karam, L. R., 2007. Application of the CIPM MRA to radionuclide metrology. Metrologia. 44, S1-S6.
Kossert, K., Janβen, H., Klein, R., Schneider, M. K. H., Schrader, H., 2006. Activity standardization and nuclear decay data of 109Cd. Applied Radiation and Isotopes. 64, 1031-1035.
Knoll, G. F. 1999. Radiation Detection an Measurement, Chapter 4, John Wiley and Sons , Inc, USA.
Knoll, G. F. 1999. Radiation Detection an Measurement, Chapter 17, John Wiley and Sons , Inc, USA.
Legrand L., Blondel M. and Magnier P. 1973. High Pressure 4? Proportional Counter for Internal Conversion Electron Measurements (139Ce, 109Cd, 99mTc). Nuclear Instruments and Methods. 112, 101-102
Lewis, V. E., Woods, M. J., Goodier, I. W., 1972. The calibration of the 1383A ionization chamber for 67Ga. International Journal of Applied Radiation and Isotopes. 23, 279 - 283.
Liang, J. H., Jiang, S. H., Chou, G. T., 1996. A theoretical investigation of calibration methods for radwaste radioactivity detection systems. Applied Radiation and Isotopes. 47, 669 - 675.
Lin, U. T., Chu, C. H., Hsieh, B.T. and Hwang, W. S., 2004. Dose evaluation and measurement of the 188Re liquid-filled balloon in intravascular brachytherapy. Applied Radiation and Isotopes. 61, 1323-1333
Lin, W. Y., Tsai, S. C., Hsieh, B. T., Lee, T. W., Ting, G. and Wang, S. J., 2000. Evaluation of three rhenium-188 cadidates for intravascular radiation therapy with liquid-filled balloons to prevent restenosis. Journal of Nuclear Cardiology. 7, 37-42.
Müller, J. W. 1973. Dead-time problem, Nuclear Instruments and Methods. 112, 47-57.
Müller, J. W. 1969. Une nouvelle méthode pour la mesure des temps morts, Report BIPM-69/11.
NCRP 58. 1985. A Handbook of Radioactivity Measurements Procedures. National Council on Radiation Protection and Measurements, Bethesda, Maryland.
NE Technology Limited, 1993. Instruction manual for model 288/SA/102 pressurized ion chamber, NE Technology Limited, England.
OIML R111-1. 2004. International recommendation No 111-1: Weights of classes E1, E2, F1, F2, M1,M1-2, M2, M2-3 and M3, Part 1: Metrological and technical requirements, International Organization of Legal Metrology (OIML), Paris, France.
Pate, B. D. and Laffe, L., 1955. A new material and techniques for the fabrication and measurement of very thin films for use in 4π-counting. Canadian Journal of Chemistry, 45, 15-23.
Ratel, G., Michotte, C., Bobin, C., Moune, M., Coursol, N., 2006. Update of the ongoing comparison BIPM.RI(II)-K1.Ga-67 to include the activity measurements of the LNE-LNHB, France. Metrologia, 40, Tech. Suppl., 06008.
Ratel, G., 2007, The Système International de Référence and its application in key comparisons. Metrologia, 44, S7-S16.
Reynen, K., Kockeritz, U., Kropp, J., Wunderlich, G., Knapp, F. F., Schmeisser, A. and Straeesr, R. H., 2004. Intracoronary radiotherapy with a 188rhenium liquid-filled PTCA balloon system in in-stent restenosis: acute and long-term angiographic result, as well as 1-year clinical follow-up. International Journal of cardiology. 95, 29-34.
Phillips H.C., Johansson, L.C., Sephton, J.P., 2010. Standardisationof 85Kr. Applied Radiation and Isotopes. 68, 1335-1339. .
Pommé, S. and Sibbens, G., 2008. Alpha-particle Counting and Spectrometry in a Primary Standardisation Laboratory. Acta Chimica Slovenica. 55, 111–119.
Schotzig, U., Schrader, H., Schonfeld, E., Gunther, E. and Klein, R., 2001. Standardization and decay data of 177Lu and 188Re. Applied Radiation and Isotopes. 55, 89-96.
Silva, M.A.L. da., Poledna, R., Iwahara, A., Silva, C. J. da., Delgado.J. U. and Lopes, R. T., 2006. Standardization and decay data determinations of 125I, 54Mn and 203Hg. Applied Radiation and Isotopes. 65, 1440-1445.
Singh, B., 1990. Nuclear Data Sheets for A=188. Nuclear Data Sheets. 59, 133-262.
Simpson, B.R.S., Ntsoane, T.P., 2000. Decay scheme of 67Ga. Applied Radiation and Isotopes. 52, 551-556.
Smith, D., Stuart, L.E.H., 1975. An extension of the 4???? coincidence technique: two dimensional extrapolation. Metrologia. 11, 67 – 72.
Smith D. 1978. Improve Correction Formulae for Coincidence Counting. Nuclear Instruments and Methods. 152, 505-519.
Spernol A. and Denecke B. 1964. High Precision Absolute Gas Counting of Tritium-I. International Journal of Applied Radiation and Isotopes. 15, 139-149
SPSS Inc., 2002. SigmaPlot 8.0 programming guide, SPSS Inc., Chicago.
Steyn, J., 1973. Special problems involved in liquid scintillation counting – standardization of 87Y and 67Ga. Nuclear Instruments and Methods. 112, 137-141.
Toma, M., Sima, O., Olteanu, C., 2007. Experimental and simulated studies for the calibration of a radioactive waste assay system. Nuclear Instruments and Methods. A580, 391 - 395.
Yeh, C. H., Yuan, M. C.and Chang, B. J., 2008. Calibration and characteristics of gamma-activity monitors used for decommissioning waste. 53rd annual meeting of the health physics society, July 13-17, 2008, Pittsburgh, PA.
Yuan, M. C., Lee, J. H. and Hwang, W. S., 2002. The absolute counting of 166mHo, 58Co and 88Y. Applied Radiation and Isotopes. 56, 429-434.
Yuan, M. C., Pang, H. F. and Wang. C. F., 2006. Absolute counting of 188Re radiopharmaceuticals. Applied Radiation and Isotopes. 64, 1380-1383.
Yuan, M. C., Chen, I. J., Wang, C. F., 2008. Primary standardization of 67Ga radiopharmaceuticals. Applied Radiation and Isotopes. 66, 976–980.
Yuan, M. C., Yeh, C. H., Wang, J. J., Chen, I. J., Wang, C. F., 2009. The calibration and evaluation of a radioactive waste drum counting system. Applied Radiation and Isotopes. 67, 931 – 931.
Yuan, M. C., Yeh, C. H., Yeh, C. Y., Chen, I. J., and Wang, C. F., 2010. Proficiency testing feasibility study for the measurement of gamma-emitting clearance samples. Applied Radiation and Isotopes. 68, 1211-1316.
Yunoki, A., Li, M., Shaha, V. V., Nazaroh, W. M., Yuan, M. C., Nhan, D. D., Park, T. S., Yang, Y., Soodprasert, T., Michotte, C., 2009. APMP comparison of the activity measurements of Ba-133 (APMP.RI(II).K2.Ba-133) and links to the SIR. Metrologia, 46, 06014.
Taylor, J. R. 1982. An Introduction to Error Analysis, Chapter 8, University Science Books, Mill Valley, California.
Wei, H. J., Tsai, T. L., Wang, J. J., Chen, I. J., Wuu, J. L., Wang, T. W., 2009. Clearance measurement of metal scraps for nuclear facility at INER in Taiwan. Applied Radiation and Isotopes. 67, 944 – 949.
Woods, M.J., Keightley, J.D., Ciocanel, M. and Paton Walsh, C., 1998. NPL Second Standard Radionuclide Calibrator: New Calibration Figure for 106Ru, 153Sm, 188Re. Applied Radiation and Isotopes. 49, 1191-1193.
Zimmerman, B. E., Cessna, J. T., Unterweger, M. P., Li, A. N., Whiting, J. S. and Knapp, F. F., 1999. A New Experimental Determination of the Dose Calibrator Setting for 188Re. The Journal of Nuclear Medicine. 40, 1508-1516.
金啟明，2007，台電廢棄物外釋作業規劃, 解除管制量測實務研討會，2007年10月16日， 核能研究所。
行政院衛生署，2010，歷年特定醫療技術檢查檢驗醫療儀器使用人次， http://www.doh.gov.tw/CHT2006/DisplayStatisticFile.aspx?d=68585&s=1