放射化学のテーマの発展 Development of Theme in Radiochemistry
Contents
1. T2. BAT
3. Hk 1 4 2 5
4. 80 100 120 140 22Rn concentration Bq m Fig 16 The Distribution of 22Rn Activity Concentration in 387 Homes in Tokyo No 5 341 7 DS
5. TRIUME 1 3 BU LSS Emax 200 keV cg Emax 200 keV
6. 22 9 Bq 1 1800 Bq 13 1 100 0 1 Bq 1 1 44 5 2 24 48 More than 20 Ba L Sd 15 19 Bg L 10 14 Bg L e 5 9 Bg L Less than 4 Bg L Fig 15 Location of Study Area and Sampling Sites on Part of a Geologic Map of Tokyo Symbols indicate levels of 222Rn activity concentrations 340 Vol 121 2001 ALERT RLERMEFZSE 10 ml LS 8 LS LSS ELF
7. BL LSS 20 LSS 20 LSS LSS LSS
8. Anal Chem 9 100 330 Vol 121 2001 Integral counting rate Pulse height Fig 2 2 3
9. 5 5 1 21 LS Rt ot HE Hd Z7 NG 2 R1 Shakujiigawa River R2 Zenpukujigawa River R3 Kandagawa River R4 Myoshojigawa River Shinjuku Saitama Prefecture Kanagawa Prefecture 20 ml PPO 3 5 LSS SD 30 Fig 15 4
10. SOD superoxide dis mutase No 5 339 FO 10 8 3
11. Bil LS Fig 13 32 o m PO n n n 2 4 2 3 4 3 Fig 14 LSS PPO PPO 444
12. HE LSS T LSS LS Dn LS 2 5 diphenyloxazole PPO MEO MIC W
13. 338 Vol 121 2001 241 PPO BENZENE A 24 3 41 5 C B 6 6 41 3 C PPO O XYLENE A 24 7 21 5 C B 19 5 1 2 C Counts 100s PPO ETHYLBENZENE A 22 9 1 5 C B 23 44 1 2 C C 54 74 0 3 C 24 Lam PPO XYLENE A 24 5 1 5 C B 1 9 1 4 C c 40 44 1 1 C PPO CUMENE A 22 9 41 5 C B 26 5 4 1 1 C C 51 4 41 4 C 200 400 600 800 Relative pulse height Fig 14 Effect of Temperature on Pulse Height Distributions for 241Am in PPO Solutions of Benzene O Xylene M Xylene Ethyl benzene and Cumene aR 4 4 41 HT 1
14. oe 28Po 214Po air luminescence 3 1 o 80 N A second posi tive band system C377 gt B377 N frst negative band system B33 X T LSS MPT R331
15. No 5 331 p Zero detection threshold dpm 20 3 H 15 10 x 10 Integral counting rate cpm ae 10 20 Pulse height keV Fig 3 Determination of the Detection Threshold 2 4 3H C 3S SCa Figs 4 5 0 RUT t Emax 200 keV L
16. O 2 LSS O Fig 2 PPO 3 5 o 4Pb 34Bi 200 keV a B 100 e ZnS Ag
17. liquid scintillation spectrometer LSS liquid scintil lator LS MPT multiplier pho totube wo HS No 5 329 o Ra 1600y a1 4 6017 5 596 ag 4 7844 H 5 71 0 18599 3 28 ce 2 2 Rn 3 824d a 5 4895 99 994 Fig 1 Part of Radioactive Decay Series of Uranium 238 Showing Radium 226 and Daughter Nuclides LSS LSS
18. Te NABA 3 387 18 22 C 31 72 Fig 16 29 2 Bq m 3 16 6 Bq m 3 1 8 Doi 1994 4 9 16 Bq m 3 140 7Bqm 3 if ADEN 22 7 Bgm 3 3 6
19. 328 Vol 121 2001 1 2 3
20. MPT O IH Fig 3 Appl Rad Isot 2 2 2
21. o 3 LS WA eae nee eee No 5 333 6x102 YA 24Db 24Bi Misty Mapapa i Counts 600s ee 500kev pe 14D O lt Ta 1000 Channel Relative pulse height Fig 7 Pulse Height Spectrum of 222Rn LS Sample Measured with an Aloka LSC 3500 Fig 7 LTS
22. 40 Number of observations 0 20 40 60
23. EK 342 Vol 121 2001 17 Homma Y Murase Y Takiue M J REFERENCER Radioanal Nucl Chem Lett 119 457 466 1 Basson J K Steyn J Proc Phy Soc A 1987 67 297 298 1954 18 Dondes S Hartecck P Kunz C Radiat 2 Steyn J Proc Phy Soc A 69 865 867 Res 27 174 210 1966 1955 19 Murase Y Homma Y Takiue M Appl 3 Flynn K F Glendenin L E Phys Rev 116 Radiat Isot 40 295 298 1989 744 748 1959 20 Murase Y Homma Y Takiue M Aburai 4 Goldstein G Nucleonics 23 67 69 1965 T Appl Radiat Isot 40 291 294 1989 5 Horrocks D L Studier M H Anal Chem 21 Homma Y Murase Y Takiue M Aburai 33 615 620 1961 T The Radioecology of Natural and Artifi 6 Homma Y Murakami Y J Radioanal cial Radionuclides ed by Feldt W Verlag Chem 36 173 184 1977 TUV Rheinland GmbH Koln 1989 pp 493 7 Flynn K F Glendenin L E Prodi V Or 498 ganic Scintillators and Liquid Scintillation 22 Homma Y Murase Y Takiue M Aburai Counting ed by Horrocks D L Peng C T Enviromental Radon ed by Shimo M T Academic Press London 1971 pp 687 Tsujimoto
24. 7 Ra 3 2 LS LS LS RY 28Po 24Po Oa 70 Fig 10 TA o 24 Am 210Po 3H MC 35S 72 30 Fig 11 LS RY 218Po 214Po go BimXe
25. TED LSS 9 E
26. RI 25 Horrocks E Fermi a Kurie plot Horrocks S 3H MC 3S SCa LSS Kurie plot 1
27. DED FRY eo 3H C 33S Counting rate No SN y MA KI Pulse height Chemical Quenching Effect on Spectra and Integral Counting Rate Curves MPT 1 detection threshold 1 0 1 5 keV Emax 27200 keV 200keVcutoff Horrocks 1 2 BANZA MPT 1 0 1 5 keV
28. D 1 2 3 4 Ki 2 oe 3 1 4 WOE Wo 3 0 70 12
29. Fig 12 3 COC x103 counts 100s 200 200 600 800 1000 Relative pulse height Fig 10 Pulse Height Spectra for Rn and Its Daughters Measured at a 13 0 C b 65 0 7 C x103 counts 400s x10 counts 400 s 0 00500 1000 Relative pulse height Fig 11 Pulse Height Distributions for 4C and 3H Measured at a 8 8 C b 12 to 11 2 C c 67 to 66 2 C No 5 337 x 03 counts 100s 0 100 200 300 Relative pulse height 0 na x 300 400 500 600 700 800 Relative pulse height Fig 12 Pulse Height Spectra for 31Xe and 241Am Measured at a 13 0 C b 65 0 7 C PPO toluene A Relative fluorescence intensity 0 340 360 380 400 420 440 Wavelength nm u 60 T Pure toluene o 50 a B 6 40 2 oD 30 gt a Se 20 Soa tE o II 0 Pay 6 Mr a 260280 300 320 340 360 380 400 420 Wavelength nm Fig 13 A Fluorescence Spectra of PPO Toluene Solution at a 23 5 C b 20 9 0 9 C c 40 9 0 9 C B Fluorescence Spectra of Pure Toluene a to d and Toluene in Hexane e at a 23 3 C b 3 740 3 C c 20 540 4 C d 59 940 4C e 23 2 C
30. 24Bi 78Po MP 3 gw LSS MCA LS LSS MCA D 2 LS Table 1 2 23 22 ml No 5 335 8ml LS 6 3 LS 10 ml 3 0 22
31. 3H MC 3S SCa Fig 6 LSS 100 0 100 200 Energy keV Fig 6 Kurie Plots for 4C in Liquid Scintillation System 39 i AA CG a 2 6 Kurie plot ec Kurie plot Kurie plot
32. 2 46 ZnS Ag 1 LS co e LSS oe LS 2 3 3H LSS 3H 0 20 keV oe
33. LS Insta gel Emulsifer 6 ml ULS 4g PPO 6ml 2x x CH 2 ni g 226Ra 1m1 3 ml Reales 1 26Ra es Po Po LSS 66 6 66 7 2 LSS 334 Vol 121 2001 Spectral response of photocathode R331 Radiant sensitivity mA W 300 400 Wavelength nm A Bx F N 1 st NEG XI C Tu D 5 N 2 nd Pos A 500 BT B Fig 8 A Spectral Response of a Hamamatsu R331 Photocathode and The Emission Spectra for the N Second Positive Band Sys tem A E and the N First Negative Band Dystem F B Simplified Energy Diag
34. 300 520 nm Fig 8 LSS DA 19 LSS Fig 9 A Aloka LSC 3300 ALAN end point 2 4 keV B Beckman LS5801 end point 18 keV 2 4 keV 18 keV end point 3 11 210Po 238 241Am LSS KE 0 5 ml
35. 332 Vol 121 2001 110 0 E baga Se nina ce a LSS BRERBDERZXO
36. 10 UML a TI LSS KE Argonne D L Hor rocks 2 3 2 2 a L a MeV
37. 2 3 RC DAA
38. pan LS a A 25 26 47 49 3 LS LSS 3 1 5 1 co Po SU Am oc Table 2 Comparison of the Disintegration Rates Obtained by This Method and Conventional Method Sample This method P Conventional method No Ao cpm Ar dpm As dpm A dpm Error 1 80136 90 95488 107 95625 98 95594 98 110612 125 15 7 2 88348 94 95529 1
39. CHS RRO CLF 2 2 1 NG 1 22Rn 2 Ra Hig 1 Kr 14CO GM GM Ek V bM GM
40. 56 57 58 60 61 62 63 64 65 66 67 68 radionuclides ed by Feldt W Verlag TUV Rheinland GmbH Koln 1989 pp 503 508 Takiue M Fujii H Homma Y Appl Radiat Isot 41 195 198 1990 Homma Y Murase Y J Radioanal Nucl Chem Lett 146 205 210 1990 Homma Y Murakami Y Chem Lett 5 449 452 1976 Homma Y Murakami Y Radioisotopes 25 315 322 1976 Homma Y Murakami Y Radioisotopes 26 74 79 1977 Aburai T Homma Y Murakami Y Radioisotopes 26 146 150 1977 Homma Y Murakami Y Bull Chem Soc Japan 50 1251 1256 1977 Homma Y Murakami Y Int J Appl Radiat Isot 28 738 739 1977 Murakami Y Homma Y J Label Comp Radiopharm 13 No 2 1977 Homma Y Kurata K Int J Appl Radiat Isot 30 345 348 1979 Homma Y Murase Y Ishii M Int J Appl Radiat Isot 31 399 403 1980 Homma Y Sugitani Y Matsui Y Matsuura K Kurata K Int J Appl Radiat Isot 31 505 508 1980 Homma Y Murase Y Ishii M J Radioanal Chem 76 283 288 1983 Adams M J Ruth T J Homma Y Pate B D Appl Radiat Isot 36 935 937 1985 Homma Y Murase Y Sonehara K J Radioanal Nucl Chem Lett 105 241 284 1986 Homma Y Murase Y Sonehara K Ishii M J Label Comp Radiopharm 23 791 797 1986 Suwa M Kogawa O Nowatari H Murase Y Homma Y Hashimoto Y J Label
41. T Electron Science Institute Osa 696 ka 1992 pp 333 340 8 Homma Y Murase Y Handa K Appl 23 Homma Y Murase Y Handa K Murakami Radiat Isot 45 341 344 1994 I Abstracts of papers Second International 9 Homma Y Murase Y Handa K J Conference on Isotopes October 12 16 1997 Radioanal Nucl ChemLett 187 367 374 Sydney Australia p 62 1994 24 Homma Y Murase Y Murakami I Handa 10 Homma Y Murase Y Handa K Liquid K Horiuchi K Radon and Thron in the Scintillation Spectrometry 1992 ed by Human Environment ed by Katase A Shi Noaks J Polach H Schonhofer F mo M World Scientific River Edge NJ RADIOCARBON Tucson Arizona 1993 1998 pp 61 65 pp 59 62 25 Murase Y Homma Y Takiue M The 11 Homma Y Murase Y Handa K Appl Radioecology of Natural and Artificial Radiat Isot 45 699 702 1994 Radionuclides ed by Feldt W Verlag TUV 12 Homma Y Murase Y Handa K Rheinland GmbH Koln 1989 pp 509 513 Atomospheric Radon Families and Environ 26 Morita Murase Y Homma Y Isotope mental Radioactivity III ed by Research Production and Applications in the 21st Cen Committee on Atomospheric Radon Families tury ed by Stevenson N R World Scien The Atomic Energy Society of Japan 1995 tific River Edge NJ 1999 pp 112 116 pp 47 50 27 Homma Y Murase Y Handa K Koyama 13 Homma Y Murakami Y Bunsekikiki 15 S S
42. Y Murakami I Homma Y The 8th Symposium of Atomic Energy Research Center Murase Y Homma Y Murakami I Handa K Appl Radiat Isot 49 861 865 1998 Morishima H Koga T Kawai H Kondo S ed by Shimo M Tsujimoto T Electron Science Institute Osa ka 1992 pp 428 437 Homma Y Murase Y Handa K Koyama Enviromental Radon S Suzuki N Liquid Scintillation Spectro metry 1994 ed by Cook T Harkeness D D RADIOCARBON Tucson 1996 pp 111 116 Murase Y Homma Y Murakami I Handa K Horiuchi K Appl Radiat Isot 50 561 565 1999 Morita Murase Y Murakami I Homma Y Chem Lett 10 1158 1159 2000 Doi M Fujimoto K Kobayashi S Health Phys 66 43 49 1994 Homma Y Murase Y Handa K In Liquid Scintillation Spectrometry 1992 ed by Noaks J Polach H Schonhofer F RADIOCARBON Tucson Arizona 1993 pp 63 67 Takiue M Ishikawa H Nucl Instrum Methods 159 139 1979 Birks J B Conte J C Proc Royal Soc Ser A 303 85 1968 Georghio S Munto I H In Organic Scin Arizona tillators and Liquid Scintillation Counting Proc Int Conf 1970 ed by Horrocks D L Peng C T Academic Press 1971 p 339 Morita Murase Y Murakami I Homma Y Chem Lett 3 238 239 2001 Takiue M Fujii H Homma Y The Radioecology of Natural and Artificial 48 49 50 51 52 53 54 55
43. ml ml gaseous liquid aqueous m space scintillator solution 1 18 1 4 0 27 3 72 4 0 3 2 14 1 8 0 12 8 87 0 0 2 3 10 1 12 0 6 5 93 3 0 2 4 6 1 16 0 3 1 96 8 0 1 1 ml of 226RaCl solution LSS IC MPT 2325 26 2 2 Jy CH HTO TO HIRE 3H LSS
44. 15 95548 98 95410 98 101423 109 6 3 3 93016 96 96704 100 97075 99 96664 98 99553 103 1 3 0 4 92504 96 941464 98 94491 97 94082 97 95402 99 1 4 Calculated based on 100 47 A A Ao the observed counting rate Ar the sum of the disintegration rates A the sum of the disintegration rates ob tained by subtracting the air luminescence counts graphically A the standardized sum of the disintegration rates determined based on known amounts of 226Ra Art the sum of the disintegration rates determined by the conventional method Vol 121 2001 2 WRK 26Ra 226Ra 222Rn 30 60 3 5 Ra
45. AF ORK B CENA MC 8 LSS 7 Zero detection threshold 7 Zero detection threshold 10 Integral counting rate cpm Pulse height keV Fig 4 Method for Obtaining the Disintegration Rate of Quenched 3H and 4C Samples by Extrapolating the Integral Pulse Height Spectra to the Detection Threshold Zero detection threshold z Zero detection threshold 5 D 5 30 dpm 35g 20 dpm 45C a H YA D A YA c D 3 a LE 6 Lc 20 z9 15 Hs Kr E G vi F 5 b unG H Pi H mng o ag KY l
46. Comp Radiopharm 31 349 354 1992 Ishiwata K Saito N Yanagawa K Furuta R Ishii S Kiyosawa M Homma Y Ishii K Suzuki F Sennda M Nucl Med Biol 23 285 290 1996 Kawamura K Ishiwata K Tajima H Ishii S Shimada Y Matsuno K Homma Y Sen da M Nucl Med Biol 26 915 922 1999 Kawamura K Ishiwata K Futatsubashi S Ishii Y Ouchi Y Homma Y Senda M 344 Vol 121 2001 69 Appl Radiat Isot 52 225 228 2000 Kawarura K Ishiwata K Tajima H Ishii S Matsuno K Homma Y Senda M Nucl Med Biol 27 255 261 2000 70 Kawamura K Ishiwata K Shimada Y Kimura Y Kobayashi T Matsuno K Hom ma Y Senda M Ann Nucl Med 14 285 292 2000
47. YAKUGAKU ZASSHI 121 5 327 344 2001 327 Reviews 105 8512 1 5 30 Development of Theme in Radiochemistry Yoshio HOMMA and Yuko MORITA MURASE Laboratory for Radiopharmaceutical Chemistry Kyoritsu College of Pharmacy 1 5 30 Shibakoen Minato ku Tokyo 105 8512 Japan Received February 9 2001 The disintegration rates of Rn and its daughters in natural water were determined successfully by the use of the in tegral counting method with a liquid scintillation spectrometer A significant advantage of this method is its freedom from the quenching effect Moreover when plural a and emitters are present their total amounts can be determined The simple extrapolation of integral counting curve to zero pulse height however do not give the true disintegration rate for the soft B emitters Emax lt 200 keV because the liquid scintillator LS has a relatively high detection threshold Therefore the zero detection threshold of the liquid scintillation spectrometer was determined by measuring standard 3H samples and a modified integral counting method which extrapolates the integral counting curve to the zero detection threshold was proposed The method has been successfully applied to various 6 emitters Rn samples and coloured samples of emitters giving more accurate absolute d
48. isintegration rate than the conventional integral count ing method and the efficiency tracing method In the course of the study determining 222Rn by liquid scintillation count ing we observed unexpected phenomena the air luminescence from gaseous space above LS and the temperature de pendence of pulse height spectra As for the former phenomenon we proposed a method for correcting errors due to air luminescence a method for determining a emitters by the air luminescence and a rapid calibration method for Rn de tectors As for the latter phenomenon we observed that the pulse height spectra for a and f emitters in LS are shifted toward higher pulse height with decreasing temperature We found that the fluorescence intensities of the solvent of LS toluene is promoted at lower temperatures and that not only toluene but also the fluorescence intensity of a number of aromatic hydrocarbons and aliphatic hydrocarbons show the same effect as toluene Other unexpected results are exis tence of metals in number of enzymes and discrepancies between the experimental value for Kurie plot of allowed emitters and the value which would be expected according to Fermi s theory the results of which would affect the trans mission probability of potential barrier for a particles Key words modified integral counting method air luminescence Rn temperature dependence of fluorescence aromatic hydrocarbon 1
49. ml 20ml LS LS LS 18 20 ml 19 2224 3 1 4 a MPT ae LSS Nal TD NG a KABA AH MPT o MC LSS LSS EK Table 1 Distribution of Rn and the Daughters among the Gaseous Space the Liquid Scintillator and the Aqueous So lution Perfect of Rn and Volume Volume of of the daughters in Sample gaseous liquid No space scintillator _ the the the
50. o 10 0 2 4 6 8 10 9 2 4 6 8 10 Pulse height kev Fig 5 Method for Obtaining the Disintegration Rate of Quenched 35S and Ca Samples by Extrapolating the Integral Pulse Height Spectra to the Detection Threshold a 10 1242 LS LS MPT KE
51. rams Showing the N Second Positive and N First Negative Transition N x102 Counts 6005 A Nn 8 Ng w C 3 a O orn 1000 TO 500 Channel Channel B Relative pulse height Fig 9 Pulse Height Spectra of the Air Sample 22Rn Measured with A an Aloka LSC 3500 Liquid Scintillation Spectrometer B a Beckman LS 5801 Liquid Scintillation Spectrometer MPT D 3 12 LS LS 10 ml BBW 78Po 214Po co LSPS RY OR 3 1 3 1 Fig 7 23Pb
52. uzuki N Horiuchi K Atomospheric 227 232 1977 Radon Families and Environmental Radioac 14 Homma Y Murase Y Sonehara K J tivity III ed Research Committee on Radioanal Nucl ChemLett 105 241 284 Atomospheric Radon Families The Atomic 1986 Energy Society of Japan 1995 pp 18 21 15 Homma Y Morita Murase Y Handa K 28 Homma Y Murase Y Handa K Koyama Abstracts of papers The 39th Symposium on S Suzuki N Horiuchi K Liquid Scintilla Radiochemistry Niigata University October tion Spectrometry 1994 ed by Noaks J 3 1995 pp 217 218 Polach H RADIOCARBON Tucson Arizo 16 Homma Y Morita Murase Y Handa K na 1996 pp 115 120 Abstracts of papers The 40th Symposium on 29 Morita Murase Y Murakami I Homma Y Radiochemistry The Institute of Physical and Chem Lett 10 1158 1159 2000 Chemical Research October 22 1996 p 280 30 Homma Y Murase Y Ishii M J No 343 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 Radioanal Nucl Chem Lett 95 263 270 1985 Homma Y Murase Y J Radioanal Nucl Chem Lett 119 355 366 1987 Homma Y Murase Y Ishii M J Radioanal Nucl Chem Lett 95 281 290 1985 Homma Y Murase Y Sonehara K Appl Radiat Isot 38 91 98 1987 Murase Y Homma Y J Radioanal Nucl ChemLett 146 215 222 1990 Ohara K Morita Murase
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