Iodine-129 in the European Environment MICHEL (Presentation... · Iodine-129 in the European...
Transcript of Iodine-129 in the European Environment MICHEL (Presentation... · Iodine-129 in the European...
R. Michel, IRS, Leibniz Universität Hannover
Iodine-129 in the European Environment
Rolf Michel
Institut für Radioökologie und Strahlenschutz
Leibniz Universität Hannover
R. Michel, IRS, Leibniz Universität Hannover
L. Tosch, A. Daraoui, M. Gorny, D. Jakob
Institut für Radioökologie und Strahlenschutz,
Leibniz Universität Hannover
V. Alfimov, H.-A. Synal
Labor für Ionenstrahlphysik,
ETH Hönggerberg, Zürich, Schweiz
H. Nies, J. Herrmann, I. Goroncy
Bundesamt für Seeschifffahrt und Hydrographie, Hamburg
Institut für Radioökologie und Strahlenschutz
Leibniz Universität Hannover
R. Michel, IRS, Leibniz Universität Hannover
Content
Iodine-129: characteristics and sources
Analytical techniques and state of knowledge
Iodine in the environment
I-129 in the North Sea and elsewhere
I-129 and I-127 in Northern Germany
I-129 and I-127 in animals and humans
Conclusions and perspectives
Sellafield
La Hague
http://rapidfire.sci.gsfc.nasa.gov/gallery/
R. Michel, IRS, Leibniz Universität Hannover
Relevant Iodine-Isotopes
R. Michel, IRS, Leibniz Universität Hannover
I-129 (T1/2 = 15.7 Ma )
- 129I 129Xe
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
129I/127I = (0.3 - 3.0) 10-12 model calculations
129I/127I = 1.5 10-12 marine hydrosphere
129I/127I = 0.2 10-12 terrestrial biosphere
R. Michel, IRS, Leibniz Universität Hannover
Fission yields for 235U(nth,f)
Massenzahl
S
palt
au
sb
eu
te in
%
Y(129I) = 0.74 %
129I/127I = 6.06 131I/129I = 3.82
239Pu(nth,f):
Y(129I) = 1.6 %
R. Michel, IRS, Leibniz Universität Hannover
I-129 in the Environment
~ 10-12
129I/127I isotopic ratios in environmental compartments ?
~ 10-12 up to ?
total free natural I-129 inventory
of atmosphere, hydrosphere,
pedosphere, and biosphere
anthropogenic I-129 emissions
from European reprocessing
plants until 2005
aerial
liquid
263 kg 251 kg
4720 kg
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
R. Michel, IRS, Leibniz Universität Hannover
World-wide nuclear reprocessing facilities
Acc. to Santschi (2005) Goldsmith Conference
WAK
Karlsruhe
R. Michel, IRS, Leibniz Universität Hannover
Annual 129I Emissions from Sellafield and La Hague
Sellafield
La Hague
1E+10
1E+11
1E+12
1E+13
1950 1960 1970 1980 1990 2000 2010
Jahr
I-129 E
mis
sio
nen
in
Bq
a-1
flüssig
luftgetragen
liquid
gaseous
total emissions until 2005:
liquid 31 TBq; gaseous 1,7 TBq
R. Michel, IRS, Leibniz Universität Hannover
Liquid I-129 Discharges to the Sea
Sellafield
La Hague
1E+08
1E+09
1E+10
1E+11
1E+12
1E+13
1950 1960 1970 1980 1990 2000 2010
year
em
issio
n i
n B
q a
-1
total liquid La Hague liquid Sellafield liquid
R. Michel, IRS, Leibniz Universität Hannover
Aerial I-129 Discharges
Sellafield
La Hague
1E+08
1E+09
1E+10
1E+11
1950 1960 1970 1980 1990 2000 2010
year
em
issio
n i
n B
q a
-1
total gaseous La Hague gaseous Sellafield gaseous
R. Michel, IRS, Leibniz Universität Hannover
Early Investigations by RNAA
R. Michel, IRS, Leibniz Universität Hannover
I-129/I-127 Isotopic Ratios in U.S. Environmental Materials
Brauer, 1974
10
10-9
10-6
10-3
R. Michel, IRS, Leibniz Universität Hannover
Tandem accelerator at ETH Zürich in the PSI/ETH-AMS-Laboratory
R. Michel, IRS, Leibniz Universität Hannover
(129I/127I = 4,7 · 10-10)
(129I/127I = 5 · 10-14)
TOF-Spectrum of a Standard and of a Blank
in an AMS measurement
Wagner, 1995
R. Michel, IRS, Leibniz Universität Hannover
„Small“ AMS Maschine 500 kV – 1 MV
Charge state +1
A universal AMS System for Be-10, C-14, Al-26, Ca-41, I-129, Actinides
R. Michel, IRS, Leibniz Universität Hannover
I-129 in a soil column from Nemirovka/Ukraine, zone III (1885 – 555 kBq/m2 137Cs)
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
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
Annual Fall-Out of Cl-36 and I-129 in Switzerland
1E-06
1E-05
1E-04
1E-03
1E-02
1940 1950 1960 1970 1980 1990
Ch
lori
ne
-36 in
mB
q m
-2 a
-1
Year
1E-02
1E-01
1E+00
1E+01
1940 1950 1960 1970 1980 1990 2000
Iodin
e-1
29
in m
Bq m
-2 a
-1
Year
Fiescherhorn/Ch Zurich/Ch
Synal et al., 1990; Wagner et al., 1996; Schnabel et al., 2001
Cl-36 I-129
Fiescherhorn Glacier / Ch
R. Michel, IRS, Leibniz Universität Hannover
I-129/I-127 Isotopic Ratios in Water and Seaweed Measured in
1992/93
Impact of the Columbia River
Kilius et al., 1994
I-129/I-127 in units
of 10-11
R. Michel, IRS, Leibniz Universität Hannover
I-129/I-127 Isotopic Ratios
(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
Iodine is biophilic !
Santschi (2005) Goldsmith Conference
Iodine concentrations in seaweed 20 – 250 ppm
Iodine is enriched in organic materials in rivers
with enrichment factors of up to 105 l/kg
Large amounts of I-127 and I-129 in freshwater,
estuaries and oceanic surface water are
associated with macromolecular organic matter
R. Michel, IRS, Leibniz Universität Hannover
Distribution of Iodine & Chlorine in the Earth Crust (Muramatsu und Wedepohl, 1996)
Muramatsu, NRC 6 (2004)
0.8 %
68 %
28 %
0.6 %
2.7 %
R. Michel, IRS, Leibniz Universität Hannover
Iodine Speciation
atmosphere
photic zone (< 100 m)
deep waters
sediments
photochemical oxidation
organic matter
bacterial, phytoplankton
chemical reduction
small amount of release of I- from POC
bacterial decomposition
H2S
I-, IO, HOI, IO3-
R-I
I2
HOI
RI
CH3I
IO3- I-
I2
HOI
O2 O3 H2O2
I- R* +
(IO3- dominates)
IO3- is thermodyn. stable species
?
Acc. to Santschi (2005)
R. Michel, IRS, Leibniz Universität Hannover
Pathways of Iodine through the Environment
Muramatsu, NRC 6 (2004)
R. Michel, IRS, Leibniz Universität Hannover
Iodine-Isotopes in the North-Sea
1E+03
1E+04
1E+05
Jun- 99 Dez- 99 Jun- 00 Dez- 00 Jun- 01 Dez- 01 Jun- 02
12
9I/
12
7I in
10
-10
Datum
Yiou et al. (1994) 129I/127I < 460 10-10
Amrum Meerseite
Amrum Wattseite
Amrum
Meerseite
Amrum
Wattseite
R. Michel, IRS, Leibniz Universität Hannover
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
Sampling with FS „Gauss“
1. cruise: German Bight 25.05. – 05.06.2005
2. cruise: North Sea 10.08. – 28.08.2005
3. cruise: German Bight 29.08. – 05.09.2005
4. cruise: German Bight 18.11. – 28.11.2005
Sampling from the North Atlantiv by the Polarstern and AWI:
Spitzbergen 78°56.87'N 11°51.64'E 05.09.2005; ~9m, 13m
CTD St. 280 78°49.74'N 5°01.44'E 26.08.2005 12:04; 2m, 200m
Seawater pump 78°22.50'N 8°02.84'E 28.08.2005 13:11; 11m
CTD St. 339 78°49.98'N 4°20.04'W 06.09.2005 19:45; 10m, 200m
Seawater pump 76°49.13'N 8°49.15'W 10.09.2005 18:14; 11m
Seawater pump 74°48.39'N 1°58.84'E 11.09.2005 12:20; 11m
Seawater pump 69°39.71'N 11°37.09'E 13.09.2005 11:20; 11m
Seawater pump 64°57.73'N 6°15.82'E 14.09.2005 19:11; 11m
Seawater pump 59°50.52'N 4°13.40'E 16.09.2005 03:42; 11m
Sampling by the Endeavour and by ZSR:
Oban 56o25’21’’N 05o29’06’'W 30.07.2006 13:20
Maror 56o58’03’’N 05o50’42’’W 01.08.2006 13:29
Ullapool 57o54’18’’N 05o10’40’’W 06.08.2006 15:15
Stn. 32 54o15’00’’N 03o30’00’’W 23.06.2006 16:22
Stn. 41 54o35’07’’N 03o43’06’’W 24.06.2006 22:00
Stn. 33 54o25’00’’N 03o34’00’’W 24.06.2006 08:10
Stn. 43 54o38’00’’N 03o50’00’’W 25.06.2006 10:00
R. Michel, IRS, Leibniz Universität Hannover
I-129/I-127 in 10-8
129I/127I in 10-8
R. Michel, IRS, Leibniz Universität Hannover
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
I-129
in mBq m-3 129I
in mBq m-3
R. Michel, IRS, Leibniz Universität Hannover
1E-10
1E-09
1E-08
1E-07
1E-06
1E-05
1E-10 1E-09 1E-08 1E-07 1E-06 1E-05 1E-04
I-127 in g/g
I-129 / I-1
27
sea w ater,R1 Pacif ic 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
Baltic Sea &
Elbe estuary
tideland,
German coast
Le Gurp/France
Garonne estuary
R. Michel, IRS, Leibniz Universität Hannover
1E-10
1E-09
1E-08
1E-07
1E-06
1E-05
1E-18 1E-17 1E-16 1E-15 1E-14 1E-13 1E-12
I-129 in g/g
I-129 / I-1
27
sea w ater,R1 Pacif ic 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
Baltic Sea &
Elbe estuary
tideland,
German coast
Le Gurp/France
Garonne estuary
R. Michel, IRS, Leibniz Universität Hannover
From Sea to Land
R. Michel, IRS, Leibniz Universität Hannover
Iodine isotopes in air at Föhr
Sam
ple
d m
ass in
g
selective filters lmpactor
mean particle diameter in m
global
aerosol
local aerosol
(maritime)
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
129I in European
Natural Waters
R. Michel, IRS, Leibniz Universität Hannover
129I/127I isotopic ratios in quarterly precipitation in Northern Germany
1
10
100
1000
Jan. 97 Jan. 98 Jan. 99 Jan. 00 Jan. 01 Jan. 02 Jan. 03 Jan. 04 Jan. 05 Jan. 06
Mitte des vierteljährlichen Probenahmeintervalls
I-129/I-1
27 in
10
-8
Norderney (Freiland) Buer (Freiland)
Buer (durchfallend) Siemen (Freiland)
R. Michel, IRS, Leibniz Universität Hannover
Quarterly 129I Deposition Rates in Northern Germany
0,1
1,0
10,0
100,0
Jan. 97 Jan. 98 Jan. 99 Jan. 00 Jan. 01 Jan. 02 Jan. 03 Jan. 04 Jan. 05 Jan. 06
Mitte des vierteljährlichen Probenhameintervalls
I-129 in
mB
q m
-2
Norderney (Freiland) Buer (Freiland)
Buer (durchfallend) Siemen (Freiland)
through-fall precipitation
open-field precipitation
R. Michel, IRS, Leibniz Universität Hannover
Quarterly 127I Deposition Rates in Northern Germany
0,01
0,10
1,00
10,00
Jan. 97 Jan. 98 Jan. 99 Jan. 00 Jan. 01 Jan. 02 Jan. 03 Jan. 04 Jan. 05 Jan. 06
Mitte des vierteljährlichen Probenahmeintervalls
I-127 v
iert
eljäh
rlic
he D
ep
osit
ion
in
mg
m-2
Norderney (Freiland) Buer (Freiland)
Buer (durchfallend) Siemen (Freiland)
through-fall precipitation
open-field precipitation
R. Michel, IRS, Leibniz Universität Hannover
Annual deposition densities of 129I in Switzerland (1950–1986) and Germany (1988–2009)
1E-03
1E-02
1E-01
1E+00
1E+01
1E+02
1950 1960 1970 1980 1990 2000 2010
Jahr
I-129 F
all
ou
t in
mB
q m
-2 a
-1
Fiescherhorn/Ch Mappenberg
Deutschland Norderney (Freiland)
Siemen (Freiland) Buer (Freiland)
Buer (durchfallend)
R. Michel, IRS, Leibniz Universität Hannover
1E-03
1E-02
1E-01
1E+00
1E+01
1E+02
1950 1960 1970 1980 1990 2000 2010
year
I-129 d
ep
osit
ion
rate
in
mB
q m
-2 a
-1
1E+00
1E+01
1E+02
1E+03
tota
l an
nu
al
rele
ase i
n k
g
Fiescherhorn/Ch Mappenberg Hannover
Norderney (open-field) Siemen (open-field) Buer (open-field)
Buer (through-falling) gaseous releases liquid releases
R. Michel, IRS, Leibniz Universität Hannover
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
0.1
1.0
10.0
100.0
1000.0
0 20 40 60 80 100 120 140 160 180 200 220
I-1
29
in
mB
q/m
² ;
I-1
27
in
g/m
² I-
12
9/I
-12
7 i
n 1
E-1
0
depth in cm
I-129 I-127 I-129/I-127
Ernst et al., Kerntechnik 68, 155-167 (2003).
R. Michel, IRS, Leibniz Universität Hannover
127I-127 inventories and 129I/127I Isotope Ratios in Soils from Lower Saxony/Germany
1E-02
1E-01
1E+00
1E+01
0 50 100 150 200
I-127 in
g m
-2
Surface of individual depth increment in cm
1E-01
1E+00
1E+01
1E+02
1E+03
0 50 100 150 200 250
I-129/
I-1
27 iso
top
ic r
atio
in
10 -1
0
Average depth in cm
R. Michel, IRS, Leibniz Universität Hannover
Balance of 129I and 127I in Region III of Lower Saxony / Germany
Surface-projected
concentrations
127I
in mg m–2
129I
in mBq m–2
Geometric mean and
standard deviation 3.500 × 1,61 168 × 1,51
Pre-nuclear < 0,08
Annual deposition densities
through-falling precipitation
127I
in mg m-2 a-1
129I
in mBq m-2 a-1
Geometric mean and
standard deviation 4,0 × 1,21 11 × 1,31
R. Michel, IRS, Leibniz Universität Hannover
1E-10
1E-09
1E-08
1E-07
1E-06
1E-05
1E-10 1E-09 1E-08 1E-07 1E-06 1E-05 1E-04
I-127 in g/g
I-1
29
/ I-1
27
updated 23.06.2007
Stand Mai 2007
Surfce soils
seawater
Rain
Groundwater
Surface water
235U(n,f): 129I/127I = 6.06
R. Michel, IRS, Leibniz Universität Hannover
1E-10
1E-09
1E-08
1E-07
1E-06
1E-05
1E-19 1E-18 1E-17 1E-16 1E-15 1E-14 1E-13 1E-12
I-129 in g/g
I-1
29
/ I-1
27
updated 23.06.2007
Stand Mai 2007
235U(n,f): 129I/127I = 6.06
Surface soils
Seawater
Rain
Ground-water
Surface water
R. Michel, IRS, Leibniz Universität Hannover
1st Conclusion
I-129 and I-127 in precipitation in Northern Germany can completely be explained by the liquid releases of I-129 from Sellafield and La Hague.
There is no evidence of significant immissions from the atmospheric releases from the reprocessing plants.
R. Michel, IRS, Leibniz Universität Hannover
Transfer through the food chain
and the biospheric response
R. Michel, IRS, Leibniz Universität Hannover
1E-09
1E-08
1E-07
1E-06
1E-05
1975 1980 1985 1990 1995 2000 2005
I-129/I
-127
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
Animal thyroid glands
Data for Danmark: Hou et al. (2003)
R. Michel, IRS, Leibniz Universität Hannover
129I/127I in European human thyroid glands remote from reprocessing plants
1E-09
1E-08
1E-07
1E-06
1E-05
1975 1980 1985 1990 1995 2000 2005
I-129/I-1
27
year
human Hannover human Hamburg human Germany human Belarus precipitation
Human thyroid glands
Hthyroid = 6 nSv a-1 for adults
Data for Belarus: Hou et al. (2003)
R. Michel, IRS, Leibniz Universität Hannover
Total Diet from the mensa academica of the Universität Hannover
Probenahme-
datum
127I 129I 129I/127I
in 10–10 in g g–1 in fg g–1
09. 04. 2002 0,19 < 0,78 < 40
10. 04. 2002 0,12 < 0,55 < 46
11. 04. 2002 0,20 < 0,82 < 41
12. 04. 2002 0,12 < 0,72 < 58
12. 08. 2002 0,092 < 0,78 < 83
13. 08. 2002 0,16 < 0,70 < 44
14. 08. 2002 0,11 < 0,66 < 58
15. 08. 2002 0,12 < 1,4 < 120
16. 08. 2002 0,090 9,6 1 050
Daily 127I intake
180 - 400 g d–1
WHO
recommended
150 g d–1
R. Michel, IRS, Leibniz Universität Hannover
Iodinated table salts
Sample I-127 con-
centration
in g g-1
I-129 con-
centration
in fg g-1
129I/127I
atomic ratio
in 10-12
Esco european
salt company,
Bernburg > 14.8 < 0.021 < 1
Südsalz GmbH,
Bad Friedrichshall > 14.8 0.22 1.1
Südsalz GmbH,
Bad Reichenhall 14.8 – 24.9 < 0.2 < 9.8
R. Michel, IRS, Leibniz Universität Hannover
Iodine pills
Sample Iodine
content
in mg
I-129
content
in fg
129I/127I
atomic ratio
in 10-12
Naturreform Iod-Tablette,
VIVA GmbH 0.092 < 0.17 < 1.9
Jodetten® depot,
Henning, Berlin 1.53 2.1 1.3
Iod-Prophylaxe-Tabletten,
Lannacher Heilmittel
GmbH 49.7 16 0.32
R. Michel, IRS, Leibniz Universität Hannover
Drinking water
Sample I-127
concentration
in g kg-1
I-129
concentration
in fg kg-1
129I/127I
atomic ratio
in 10-10
Hamburg-
Eimsbüttel 9.8 2.4 1.3 0.4 1.4 0.5
Hannover-
Buchholz 5.7 2.2 30 1.0 52 20
Hannover-
Gleidingen 0.92 0.36 45 1.4 480 190
R. Michel, IRS, Leibniz Universität Hannover
Conclusions The natural environmental abundances of 129I have been
changed by man in a sustainable way.
In Europe, these changes are going on.
The dominant releases from the nuclear reprocessing
plants are into the sea.
The 129I/127I system is widely in disequilibrium.
In spite of the fact that presently 129I is radiologically not
relevant, the development should be carefully monitored.
129I is a radioactive tracer for environmental processes
which offers a wide range of applications in environmental
sciences.
129I is an indicator for the long-term human impact on the
environment.
R. Michel, IRS, Leibniz Universität Hannover
In order to understand the natural system of the iodine
isotopes and the development of the man-made changes
we need:
A systematic description of the ecological pathways of 129I
from the sources to the sinks and a continuous
surveillance of the release points in Europe and worldwide.
A detailed book keeping of the environmental cycles of the
stable iodine in all relevant environmental compartments.
Further investigations of the physical, chemical and
biochemical behaviour of the iodine isotopes in
atmosphere, hydrosphere and pedosphäre.
A complete (radio)ecology of 129I and 127I .
Perspective
R. Michel, IRS, Leibniz Universität Hannover
The End