Institut für Radioökologie und Strahlenschutz Leibniz Universität Hannover Iodine-129 and Iodine-127 in the European Environment Rolf Michel R. Michel, IRS, Leibniz Universität Hannover Institut für Radioökologie und Strahlenschutz Leibniz Universität Hannover Th. Ernst, A. Daraoui, M. Gorny, K. Gückel, J. Handl, D. Jakob, J. Korntheuer, R. Sachse, A. Schmidt, Ch. Schnabel, S. Szidat, L. Tosch Zentrum für Strahlenschutz und Radioökologie, Leibniz Universität Hannover V. Alfimov, H.-A. Synal Ion Beam Physics, Paul Scherrer Institut und ETH Zürich H. Nies, J. Herrmann, I. Goroncy Bundesamt für Seeschifffahrt und Hydrographie, Hamburg R. Michel, IRS, Leibniz Universität Hannover 1 Content Sellafield Iodine-129: characteristics and occurrence Analytical techniques and state of knowledge I-129 in the North Sea and elsewhere I-129 and I-127 in Northern Germany: From the sea to the continent I-129 and I-127 in animals and humans Retrospective dosimetry Conclusions and perspectives La Hague R. Michel, IRS, Leibniz Universität Hannover http://rapidfire.sci.gsfc.nasa.gov/gallery/ Relevant Iodine-Isotopes R. Michel, IRS, Leibniz Universität Hannover 2 I-129 (T1/2 = 15.7 Ma ) 129Xe 129I E,max = 0.2 MeV, E = 39.58 keV, I = 7.52 % Production in nature Cosmic ray induced spallation reactions on Xenon Spontaneous fission of Uranium Natural equilibrium isotopic ratio = (0.3 - 3.0) 10-12 model calculations 129I/127I = 1.5 10-12 marine hydrosphere 129I/127I = 0.2 10-12 terrestrial biosphere 129I/127I R. Michel, IRS, Leibniz Universität Hannover Fission Yields in 235U(n th,f) fission yield in % Y(129I) = 0.74 % 129I/127I 131I/129I = 6.06 = 3.82 239Pu(n ,f): th Y(129I) = 1.6 % Mass number R. Michel, IRS, Leibniz Universität Hannover 3 I-129 in the Environment total natural I-129 inventory of the Earth: 50 000 kg (327 TBq) emissions from atmospheric test explosions: 43 kg – 150 kg Chernobyl: 2 kg – 6 kg anthropogenic I-129 emissions from European reprocessing plants until 2005 liquid total free natural I-129 inventory of atmosphere, hydrosphere, pedosphere, and biosphere 263 kg 129I/127I aerial 4720 kg 251 kg isotopic ratios in environmental compartments ? ~ 10-12 up to ? ~ 10-12 R. Michel, IRS, Leibniz Universität Hannover World-wide nuclear reprocessing facilities WAK Karlsruhe Nach Santschi (2005) Goldsmith Conference R. Michel, IRS, Leibniz Universität Hannover 4 Annual 129I Emissions from Sellafield and La Hague Sellafield I-129 Emissionen in Bq a-1 1E+13 1E+12 liquid total emissions until 2005: flüssig liquid 31 TBq; gaseous 1,7 TBq 1E+11 gaseous luftgetragen 1E+10 1950 1960 1970 1980 1990 2000 2010 Jahr La Hague R. Michel, IRS, Leibniz Universität Hannover Liquid I-129 Discharges to the Sea 1E+13 Sellafield emission in Bq a-1 1E+12 1E+11 1E+10 1E+09 1E+08 1950 1960 1970 1980 1990 2000 2010 year total liquid La Hague liquid Sellafield liquid La Hague R. Michel, IRS, Leibniz Universität Hannover 5 Gaseous I-129 Discharges Sellafield emission in Bq a-1 1E+11 1E+10 1E+09 1E+08 1950 1960 1970 1980 1990 2000 2010 year total gaseous La Hague gaseous Sellafield gaseous La Hague R. Michel, IRS, Leibniz Universität Hannover Early Investigations of I-129 by RNAA R. Michel, IRS, Leibniz Universität Hannover 6 I-129/I-127 Isotopic Ratios in U.S. Environmental Materials measured by RNAA 10-3 10-6 10 10-9 Brauer, 1974 R. Michel, IRS, Leibniz Universität Hannover Tandem accelerator at ETH Zürich in the PSI/ETH-AMS-Laboratory R. Michel, IRS, Leibniz Universität Hannover 7 (129I/127I = 4,7 · 10-10) TOF-Spectrum of a Standard and of a Blank in an AMS measurement (129I/127I = 5 · 10-14) Wagner, 1995 R. Michel, IRS, Leibniz Universität Hannover „Small“ AMS Maschine 500 kV – 1 MV A universal AMS System for Be-10, C-14, Al-26, Ca-41, I-129, Actinides Charge state +1 R. Michel, IRS, Leibniz Universität Hannover 8 I-129 in a soil column from Nemirovka/Ukraine, zone III (137Cs: 185 - 555 kBq/m2) R. Michel, IRS, Leibniz Universität Hannover What is normal? Depth-Profile of the 129I/127I ratio for two sediment cores from the continental slope NE of Cape Hatteras Fehn et al., 1986 R. Michel, IRS, Leibniz Universität Hannover 9 Pre-nuclear 129I/127I isotopic ratios 129I/127I isotopic ratios in 10-13 Iodid/Iodat-Sublimat 1918 a+b 2,23 ± 0,22 Iodtinktur 1918 a 2,38 ± 0,19 Iodtinktur 1918 b 1,28 ± 0,311) Diiodtryosin 1935 2,09 ± 0,75 Geometric mean 2,00 · 1,39 ±1 R. Michel, IRS, Leibniz Universität Hannover I-129/I-127 in soil profiles from Bavaria and Chile 1E+06 I/ 129 127 I in 10-12 1E+05 1E+04 1E+03 1E+02 1E+01 1E+00 1E-01 0 Wald-Kraiburg Lado Pinguinera Costal Cordillera 10 20 Untereichet 1 Lado Base Easter Island 1 30 40 50 depth in cm Untereichet 2 Curinanco Alto Easter Island 2 60 Salzburghofer Curinanco Bajo 1 70 80 Petting Curinanco Bajo 2 R. Michel, IRS, Leibniz Universität Hannover 10 Annual Fall-Out of Cl-36 and I-129 in Switzerland Iodine-129 in mBq m-2 a-1 1E+01 Chlorine-36 in mBq m-2 a-1 1E-02 Cl-36 1E-03 1E-04 Fiescherhorn/Ch 1E+00 I-129 1E-01 1E-02 1940 1E-05 Zurich/Ch 1950 1960 1970 1980 1990 2000 Year 1E-06 1940 1950 1960 1970 1980 1990 Fiescherhorn Glacier / Ch Year Synal et al., 1990; Wagner et al., 1996; Schnabel et al., 2001 R. Michel, IRS, Leibniz Universität Hannover I-129/I-127 isotopic iatios (in units of 10-10) in water and seaweed sampled between 1984 and 1992 Yiou et al., 1994 our work, 1999-2000: 129/127 = 16 500 · 10-10 R. Michel, IRS, Leibniz Universität Hannover 11 Project StSch 4481 Mapping of Tc-99, I-129 and I-127 in surface water of the North Sea Sellafield La Hague R. Michel, IRS, Leibniz Universität Hannover Bailly du Bois and Dumas (2005) R. Michel, IRS, Leibniz Universität Hannover 12 Sampling from the North Atlantic by the Polarstern and AWI: Sampling with FS „Gauss“ Spitzbergen CTD St. 280 Seawater pump CTD St. 339 Seawater pump Seawater pump Seawater pump Seawater pump Seawater pump 78°56.87'N 11°51.64'E 78°49.74'N 5°01.44'E 78°22.50'N 8°02.84'E 78°49.98'N 4°20.04'W 76°49.13'N 8°49.15'W 74°48.39'N 1°58.84'E 69°39.71'N 11°37.09'E 64°57.73'N 6°15.82'E 59°50.52'N 4°13.40'E 05.09.2005; ~9m, 13m 26.08.2005 12:04; 2m, 200m 28.08.2005 13:11; 11m 06.09.2005 19:45; 10m, 200m 10.09.2005 18:14; 11m 11.09.2005 12:20; 11m 13.09.2005 11:20; 11m 14.09.2005 19:11; 11m 16.09.2005 03:42; 11m Sampling from the Irish Sea by the Endeavour and by ZSR: Oban Maror Ullapool Stn. 32 Stn. 41 Stn. 33 Stn. 43 56o25’21’’N 56o58’03’’N 57o54’18’’N 54o15’00’’N 54o35’07’’N 54o25’00’’N 54o38’00’’N 05o29’06’'W 05o50’42’’W 05o10’40’’W 03o30’00’’W 03o43’06’’W 03o34’00’’W 03o50’00’’W 1. cruise: German Bight 2. cruise: North Sea 3. cruise: German Bight 4. cruise: German Bight 30.07.2006 13:20 01.08.2006 13:29 06.08.2006 15:15 23.06.2006 16:22 24.06.2006 22:00 24.06.2006 08:10 25.06.2006 10:00 25.05. – 05.06.2005 10.08. – 28.08.2005 29.08. – 05.09.2005 18.11. – 28.11.2005 R. Michel, IRS, Leibniz Universität Hannover I-129/I-127 in 10-8 129I/127I in 10-8 R. Michel, IRS, Leibniz Universität Hannover 13 I-129 in mBq m-3 129I in mBq m-3 R. Michel, IRS, Leibniz Universität Hannover I-129/I-127 in 10-9 129I/127I in 10-9 R. Michel, IRS, Leibniz Universität Hannover 14 I-129 in mBq m-3 129I in mBq m-3 R. Michel, IRS, Leibniz Universität Hannover 1E-05 tideland, German coast I-129 / I-127 1E-06 1E-07 1E-08 Baltic Sea & Elbe estuary Le Gurp/France Garonne estuary 1E-09 1E-10 1E-10 1E-09 1E-08 1E-07 1E-06 1E-05 1E-04 I-127 in g/g sea w ater,R1 Pacific Maui Indian Ocean German Bight V/2005 North Sea VIII/2005 North Atlantic VIII/2005 Baltic Sea German Bight IX/2005 German Bight XI/2005 Irish Sea 2005 Le Gurp, France, 2001 R. Michel, IRS, Leibniz Universität Hannover 15 1E-05 I-129 / I-127 1E-06 tideland, German coast 1E-07 Baltic Sea & Elbe estuary 1E-08 Le Gurp/France Garonne estuary 1E-09 1E-10 1E-18 1E-17 1E-16 1E-15 1E-14 1E-13 1E-12 I-129 in g/g sea w ater,R1 Pacific Maui Indian Ocean German Bight V/2005 North Sea VIII/2005 North Atlantic VIII/2005 Baltic Sea German Bight IX/2005 German Bight XI/2005 Irish Sea 2005 Le Gurp, France, 2001 R. Michel, IRS, Leibniz Universität Hannover From sea to land R. Michel, IRS, Leibniz Universität Hannover 16 selective filters lmpactor Sampled mass in g Iodine isotopes in air at Föhr local aerosol (maritime) global aerosol mean particle diameter in m R. Michel, IRS, Leibniz Universität Hannover Speciation of air-borne iodine at Föhr 127I 127I 129I 129I 129I 129I/127I-ratio in ng m-3 in % fg m-3 nBq m-3 in % 10-7 Bound to particles > 0,1 m 1,9 ± 0,4 15 1,7 ± 0,2 11,1 ± 1,3 18 8,4 ± 1,8 Organic 5,1 ± 0,8 40 1,6 ± 0,2 10,5 ± 1,3 40 3,1 ± 0,4 Inorganic < 0,1 m 5,8 ± 0,9 45 0,7 ± 0,1 4,6 ± 0,7 43 1,2 ± 0,2 Sum 12,8 ± 1,2 100 4,0 ± 0,3 26,1 ± 2,0 100 - R. Michel, IRS, Leibniz Universität Hannover 17 129I in European Natural Waters R. Michel, IRS, Leibniz Universität Hannover 129I/127I isotopic ratios in quarterly precipitation in Northern Germany I-129/I-127 in 10 -8 1000 100 10 Norderney (Freiland) Buer (Freiland) Buer (durchfallend) Siemen (Freiland) 1 Jan. 97 Jan. 98 Jan. 99 Jan. 00 Jan. 01 Jan. 02 Jan. 03 Jan. 04 Jan. 05 Jan. 06 Mitte des vierteljährlichen Probenahmeintervalls R. Michel, IRS, Leibniz Universität Hannover 18 Quarterly 129I Deposition Rates in Northern Germany 100,0 Norderney (Freiland) Buer (Freiland) Buer (durchfallend) Siemen (Freiland) I-129 in mBq m -2 through-fall precipitation 10,0 1,0 open-field precipitation 0,1 Jan. 97 Jan. 98 Jan. 99 Jan. 00 Jan. 01 Jan. 02 Jan. 03 Jan. 04 Jan. 05 Jan. 06 Mitte des vierteljährlichen Probenhameintervalls R. Michel, IRS, Leibniz Universität Hannover Quarterly 127I Deposition Rates in Northern Germany 10,00 I-127 vierteljährliche Deposition in mg m -2 through-fall precipitation 1,00 0,10 open-field precipitation Norderney (Freiland) Buer (Freiland) Buer (durchfallend) Siemen (Freiland) 0,01 Jan. 97 Jan. 98 Jan. 99 Jan. 00 Jan. 01 Jan. 02 Jan. 03 Jan. 04 Jan. 05 Jan. 06 Mitte des vierteljährlichen Probenahmeintervalls R. Michel, IRS, Leibniz Universität Hannover 19 Annual deposition densities of 129I in Switzerland (1950–1986) and Germany (1988–2009) 1E+01 -2 I-129 Fallout in mBq m a -1 1E+02 1E+00 1E-01 Fiescherhorn/Ch Deutschland Siemen (Freiland) Buer (durchfallend) 1E-02 Mappenberg Norderney (Freiland) Buer (Freiland) 1E-03 1950 1960 1970 1980 1990 2000 2010 Jahr R. Michel, IRS, Leibniz Universität Hannover 1E+03 1E+01 1E+02 1E+00 1E-01 1E+01 total annual release in kg -2 I-129 deposition rate in mBq m a -1 1E+02 1E-02 1E-03 1950 1960 1970 1980 1990 2000 1E+00 2010 year Fiescherhorn/Ch Norderney (open-field) Buer (through-falling) Mappenberg Siemen (open-field) gaseous releases Hannover Buer (open-field) liquid releases R. Michel, IRS, Leibniz Universität Hannover 20 129I and 127I in soils R. Michel, IRS, Leibniz Universität Hannover 129I, 127I, and 129I/127I Ratios in a Soil Profile from Groß Lobke/Lower Saxony/Germany I-129 in mBq/m² ; I-127 in g/m² I-129/I-127 in 1E-10 1000,0 I-129 I-127 I-129/I-127 100,0 10,0 1,0 0,1 0 20 40 60 80 100 120 140 160 180 200 220 depth in cm Ernst et al., Kerntechnik 68, 155-167 (2003). R. Michel, IRS, Leibniz Universität Hannover 21 Depth dependence of I-129/I-127 isotopic ratios in soil profiles from Christinowka, Dowigij-Lis and Schurba (Ukraine, Zone II) 1E-06 isotopic ratio I-129/I-127 Dowgij-Lis Shurba Christinowka 1E-07 1E-08 1E-09 1E-10 0 50 100 150 200 250 depth in cm R. Michel, IRS, Leibniz Universität Hannover I-127 in g m-2 1E+01 127I inventories and 129I/127I Isotope Ratios in Soils from Lower Saxony/Germany 1E+00 1E-01 1E-02 0 50 100 150 200 127I mean annual deposition rate: 4.0 1.21 mg m-2 a-1 mean total inventory: 3,500 1.6±1 mg m-2 I-129/ I-127 isotopic ratio in 10 -10 Surface of individual depth increment in cm 1E+03 1E+02 1E+01 1E+00 1E-01 0 50 100 150 Average depth in cm 200 250 R. Michel, IRS, Leibniz Universität Hannover 22 Balance of 129I and 127I in Region III of Lower Saxony / Germany Surface-projected concentrations Geometric mean and standard deviation 127I 129I in mg m–2 in mBq m–2 3.500 × 1,61 168 × 1,51 Pre-nuclear < 0,08 Annual deposition densities through-falling precipitation Geometric mean and standard deviation 127I 129I in mg m-2 a-1 in mBq m-2 a-1 4,0 × 1,21 11 × 1,31 R. Michel, IRS, Leibniz Universität Hannover 1E-05 seawater 1E-06 I-129 / I-127 Rain 1E-07 Surface soils Surface water 1E-08 1E-09 Groundwater 1E-10 1E-10 1E-09 235U(n,f): 129I/127I 1E-08 1E-07 I-127 in g/g 1E-06 = 6.06 1E-05 1E-04 updated 23.06.2007 R. Michel, IRS, Leibniz Universität Hannover 23 1E-05 Seawater 1E-06 I-129 / I-127 Rain 1E-07 1E-08 1E-09 Surface soils Surface water Ground -water 235U(n,f): 129I/127I = 6.06 1E-10 1E-19 1E-18 1E-17 1E-16 1E-15 1E-14 I-129 in g/g 1E-13 1E-12 updated 23.06.2007 R. Michel, IRS, Leibniz Universität Hannover A first conclusion I-129 and I-127 in precipitation in Lower Saxony (Germany) can be completely explained by the liquid releases into the sea from Sellafield and La Hague. There is no evidence for a significant influence of the atmospheric releases of the reprocessing plants on the iodine in precipitation in Lower Saxony. R. Michel, IRS, Leibniz Universität Hannover 24 Transfer through the food chain and the biospheric response R. Michel, IRS, Leibniz Universität Hannover 1E-05 I-129/I-127 1E-06 1E-07 1E-08 1E-09 1975 Animal thyroid glands 1980 1985 1990 1995 2000 2005 year ren- und Roedeer Sweden sheep Danmark bovine Germany bovine Netherlands bovine Austria bovine Belgium bovine Italy deer Germany bovine Germany sheep Germany pig Germany precipitation deer Germany R. Hou Michel, IRS, Leibniz Universität Hannover Data for Danmark: et al. (2003) 25 1E-05 129I/127I I-129/I-127 1E-06 in European human thyroid glands Human thyroid glands remote from reprocessing plants 1E-07 Hthyroid = 6 nSv a-1 for adults 1E-08 1E-09 1975 1980 1985 1990 1995 2000 2005 year Data for Belarus: Hou et al. (2003) human Hannover human Hamburg human Germany human Belarus precipitation R. Michel, IRS, Leibniz Universität Hannover Institut für Radioökologie und Strahlenschutz Leibniz Universität Hannover Retrospective dosimetry of the I-131 exposure in Northern Ukraine after the Chernobyl accident via AMS-measurements of I-129 in soils R. Michel, IRS, Leibniz Universität Hannover 26 Thryroid Cancer in Children under 15 Years Old until 1998 100 total: 1036 cases 90 number of cases 80 70 Belarus 60 Russ. Fed. 50 Ukraine 40 30 20 10 0 1986 1988 1990 1992 1994 1996 1998 year UNSCEAR (2000) R. Michel, IRS, Leibniz Universität Hannover Mean thyroid doses (Sv) of children and adolescents in April/May 1986 in 1034 villages contaminated by the Chernobyl accident in Belarus and Ukraine. Shown are villages with 10 measurements of the 131I activity in the human thyroid (Jacob et al. 2006). R. Michel, IRS, Leibniz Universität Hannover 27 One of those towns … Narodici, 75 km away from the Chernobyl NPP R. Michel, IRS, Leibniz Universität Hannover Ambient dose rates measured in Narodici 27.4. – 2.5.1986 3 R/h = 30 mSv/h 1,7 R/h = 17 mSv/h 0,6 R/h = 6 mSv/h R. Michel, IRS, Leibniz Universität Hannover 28 Retrospective dosimetry of I-131 via I-129 (T1/2 = 15,7 Ma) R. Michel, IRS, Leibniz Universität Hannover Retrospective Dosimetry of I-131 Exposures Using I-129 H thyr D (129 I ) Dpre Ch. (129 I ) A131 DF (131 I) f ( t ) A129 Hthyr: thyroid equivalent dose due to 131I in Sv D(129I): measured 129I deposition density in Bq m-2 Dpre-Ch.(129I) = 44 24 mBq m-2 pre-Chernobyl deposition density in Bq m-2 129I/131I: isotopic ratio in the Chernobyl fall-out 12 ± 3 A(131I)/A(129I) = 5,9 107 activity ratio DF(131I): aggregated dose coefficient for 131I in Sv per Bq m-2 f(t): correction factor for the time of arrival etc. R. Michel, IRS, Leibniz Universität Hannover 29 1E+04 D(129I) in mBq m-2 Survey on al measurements in Belarus and Ukraine as of 2005 1E+03 Lower Saxony Decision threshold 1E+02 Pre-Chernobyl deposition 555 kBq m-2 Zone II 185 kBq m-2 1E+01 1E+00 1E+01 1E+02 1E+03 1E+04 1E+05 D(137Cs) in kBq m-2 Straume et al. (1996), Mironov et al. (2002), Michel et al. (2005) R. Michel, IRS, Leibniz Universität Hannover 129I/131I atomic ratios for the Chernobyl accident as of 26.4.1986 material origin sampling date 129I/131I atomic ratio 26.4.1986 reference sewage sludge Berlin/D May 1986 34.3 ± 2.8 this work bovine and deer thyroid glands Ulm/D, Bad Hall/A May - June 1986 27 ± 10 VanMiddlesworth and Handl (1997) rain Munich/D end of April 1986 19 ± 5 Kutschera et al. (1988) rain Israel 5. May 1986 15 ± 3 Paul et al. (1987) soil Belarus May - June 1986 15 ± 5 Mironov et al. (2002) soil Belarus May 1986 12 ± 3 Straume et al. (1996) theoretical estimate - - 11 - 15 Ermilov (1993) theoretical estimate - - 22.8 Kirchner and Noack (1988) R. Michel, IRS, Leibniz Universität Hannover 30 131I Aggregated Dose Coefficients in Sv per Bq m-2 Pietrzak-Flis et al. (2003) with CLRP (Krajewski, 1996) 5-years-old 2,5 10-7 children 10-years-old 1,7 10-7 children 5,9 10-8 adults R. Michel, IRS, Leibniz Universität Hannover E D (129 I) exp( 2 2) Ort Expectations of deposition densities and committed thyroid doses E(Dcorr(I-129)) E(D(I-131)) in Bq m-2 in 106 Bq m-2 Thyroid dose Hthyroid in Gy 5-years-old 10-years-old adults Medium contaminated area (Zone III) near Korosten Nemirovka 0.122 6.41 1.6 1.1 0.38 Woronewo 0.124 6.50 1.6 1.1 0.38 Kupetsch 0.119 6.25 1.5 1.0 0.37 Tschigiri 0.078 4.10 1.0 0.7 0.24 Highly contaminated area (Zone II) near Narodici Nosdrischtsche 1.060 55.7 14 9.3 3.3 Novo Scharno 0.962 50.5 13 8.4 3.0 Christinovka 0.824 43.3 11 7.2 2.6 R. Michel, IRS, Leibniz Universität Hannover 31 A second investigation: Validation of the Retrospective Dosimetry R. Michel, IRS, Leibniz Universität Hannover Mean thyroid doses (0,1 mGy) of children and adolescents R. Michel, IRS, Leibniz Universität Hannover 32 Sampling Locations: 2nd campaign 75 km Sampling in 62 villages, Mixed soils 40 cm deep, 5 samples per village Plus three 2 m deep depth profiles. R. Michel, IRS, Leibniz Universität Hannover 98 290 129I in mBq m-2 120 62 236 67 48 100 88 96 92 74 123 131 144 258 67 135 110 144 146 153 105 98 2060 418 1281 108 748 524 323 182 578 126 225 407 124 94 380 120 184 421 90 Geometric means of the 5 soil samples taken in the individual villages in Ukraine for I-129 analysis 33 111 70 151 80 62 54 107 149 69 83 82 66 47 129 R. Michel, IRS, Leibniz Universität Hannover 33 Geometric means and standard deviations for all 62 villages 10000 100 129I in mBq m-2 1000 10 10 100 1000 137Cs 10000 100000 in kBq m-2 R. Michel, IRS, Leibniz Universität Hannover Individual doses acc. to measurements of I-131 activities in thyroid glands and calculated mean doses (histogram) for the Ukrainian village Rudka Likhtarev et al., Rad. Envir. Biophys. 33 (1994) 149 R. Michel, IRS, Leibniz Universität Hannover 34 1,4 4,3 Hthyr in Gy Hthyroid in Sv 3,5 1,1 0,10 1,5 1,2 1,8 1,9 2,1 3,8 1,0 2,0 1,6 2,1 2,1 2,3 1,5 1,1 30,3 6,2 18,9 1,3 1,4 1,4 1,3 0,9 0,8 1,0 0,7 1,0 1,2 1,2 1,0 11,0 7,7 1,1 2,7 1,9 1,9 3,3 6,0 2,2 2,7 4,8 8,5 2,3 1,4 5,6 1,8 6,2 Thyroid doses due to I-131 calculated from I-129 deposition densities for 5-years-old children 0,5 1,6 1,0 2,2 0,7 1,6 R. Michel, IRS, Leibniz Universität Hannover Thyroid doses derived from I-129 versus doses derived from direct measurements of I-131 in thyroid glands for 5-years-old children thyroid dose in Gy from I-129 100,0 10,0 1,0 Corrected for pre-Chernobyl I-129 0,1 0,1 1,0 10,0 100,0 thyroid dose in Gy directly measured Corrected for pre-Chernobyl background R. Michel, IRS, Leibniz Universität Hannover 35 Thyroid doses derived from I-129 versus doses derived from direct measurements of I-131 in thyroid glands for 10-years-old children thyroid dose in Gy from I-129 100,0 10,0 Corrected for pre-Chernobyl I-129 1,0 0,1 0,1 1,0 10,0 100,0 thyroid dose in Gy directly measured Corrected for pre-Chernobyl background R. Michel, IRS, Leibniz Universität Hannover Retrospective dosimetry The feasibility of retrospective dosimetry of I-131 exposures via I-129 has been demonstrated. The method was validated by comparison with measured thyroid doses. The retrospective dosimetry is applicable only in the highly contamination zones depending on the pre-accident background. Our retrospective dosimetry in the Northern Ukraine tends to underestimate the thyroid doses. The aggregated dose coefficients appear to be too low. This needs further investigations. The reasons could be individual local situations (pasture and watering conditions of cattle and others conditions), conditions of I-131 deposition (dry or wet), and time of arrival of the I-131. R. Michel, IRS, Leibniz Universität Hannover 36 Conclusions The natural abundances of 129I in the environment were changed by man in a sustainable manner. In Europa these changes are going on. The releases from reprocessing plants are predominantely into the sea. The 129I/127I system is in an extreme disequilibrium. Though 129I is presently not of radiological relevance, the development of ist environmental abundances should be closely monitored. is a radioactive tracer for enviromental processes and its potential should be used. 129I 129I is an indicator for the long term human impact on the environment. R. Michel, IRS, Leibniz Universität Hannover Prospects In order to understand the natural iodine cycle and the development of man-made changes, we need: A systematic description of the ecological pathways of 129I from sources to sinks including a continuous surveillance of key release points in Europe and worldwide. A detailed bookkeeping of the stable iodine cycle in all relevant environmental compartments. Further investigations of the physical, chemical and biochemical behavior of the iodine isotopes in atmosphere, hydrosphere and pedosphere. A complete (radio)ecology of 129I and 127I . R. Michel, IRS, Leibniz Universität Hannover 37 The End R. Michel, IRS, Leibniz Universität Hannover 38
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