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

L. Tosch, A. Daraoui, M. Gorny, D. Jakob

Institut für Radioökologie und Strahlenschutz,

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

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/

Relevant Iodine-Isotopes

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

Fission yields for 235U(nth,f)

Massenzahl

Y(129I) = 0.74 %

129I/127I = 6.06 131I/129I = 3.82

239Pu(nth,f):

Y(129I) = 1.6 %

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

World-wide nuclear reprocessing facilities

Acc. to Santschi (2005) Goldsmith Conference

Karlsruhe

Annual 129I Emissions from Sellafield and La Hague

Sellafield

La Hague

1950 1960 1970 1980 1990 2000 2010

I-129 E

flüssig

luftgetragen

liquid

gaseous

total emissions until 2005:

liquid 31 TBq; gaseous 1,7 TBq

Liquid I-129 Discharges to the Sea

Sellafield

La Hague

1950 1960 1970 1980 1990 2000 2010

total liquid La Hague liquid Sellafield liquid

Aerial I-129 Discharges

Sellafield

La Hague

1950 1960 1970 1980 1990 2000 2010

total gaseous La Hague gaseous Sellafield gaseous

Early Investigations by RNAA

I-129/I-127 Isotopic Ratios in U.S. Environmental Materials

Brauer, 1974

Tandem accelerator at ETH Zürich in the PSI/ETH-AMS-Laboratory

(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

„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

I-129 in a soil column from Nemirovka/Ukraine, zone III (1885 – 555 kBq/m2 137Cs)

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

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

Annual Fall-Out of Cl-36 and I-129 in Switzerland

1940 1950 1960 1970 1980 1990

-36 in

1940 1950 1960 1970 1980 1990 2000

Fiescherhorn/Ch Zurich/Ch

Synal et al., 1990; Wagner et al., 1996; Schnabel et al., 2001

Cl-36 I-129

Fiescherhorn Glacier / Ch

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

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

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

Distribution of Iodine & Chlorine in the Earth Crust (Muramatsu und Wedepohl, 1996)

Muramatsu, NRC 6 (2004)

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

I-, IO, HOI, IO3-

IO3- I-

O2 O3 H2O2

I- R* +

(IO3- dominates)

IO3- is thermodyn. stable species

Acc. to Santschi (2005)

Pathways of Iodine through the Environment

Muramatsu, NRC 6 (2004)

Iodine-Isotopes in the North-Sea

Jun- 99 Dez- 99 Jun- 00 Dez- 00 Jun- 01 Dez- 01 Jun- 02

Yiou et al. (1994) 129I/127I < 460 10-10

Amrum Meerseite

Amrum Wattseite

Meerseite

Wattseite

Project StSch 4481

Mapping of Tc-99, I-129 and I-127 in surface water of the

North Sea

Sellafield

La Hague

Sampling with FS „Gauss“

1. cruise: German Bight 25.05. – 05.06.2005

2. cruise: North Sea 10.08. – 28.08.2005

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

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

I-129/I-127 in 10-8

129I/127I in 10-8

in mBq m-3

I-129/I-127 in 10-9

129I/127I

in 10-9

in mBq m-3 129I

in mBq m-3

1E-10 1E-09 1E-08 1E-07 1E-06 1E-05 1E-04

I-127 in g/g

I-129 / I-1

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

1E-18 1E-17 1E-16 1E-15 1E-14 1E-13 1E-12

I-129 in g/g

I-129 / I-1

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

From Sea to Land

Iodine isotopes in air at Föhr

ass in

selective filters lmpactor

mean particle diameter in m

global

aerosol

local aerosol

(maritime)

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 -

129I in European

Natural Waters

129I/127I isotopic ratios in quarterly precipitation in Northern Germany

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

Norderney (Freiland) Buer (Freiland)

Buer (durchfallend) Siemen (Freiland)

Quarterly 129I Deposition Rates in Northern Germany

Mitte des vierteljährlichen Probenhameintervalls

I-129 in

through-fall precipitation

open-field precipitation

Quarterly 127I Deposition Rates in Northern Germany

Mitte des vierteljährlichen Probenahmeintervalls

I-127 v

eljäh

through-fall precipitation

open-field precipitation

Annual deposition densities of 129I in Switzerland (1950–1986) and Germany (1988–2009)

1950 1960 1970 1980 1990 2000 2010

I-129 F

Fiescherhorn/Ch Mappenberg

Deutschland Norderney (Freiland)

Siemen (Freiland) Buer (Freiland)

Buer (durchfallend)

1950 1960 1970 1980 1990 2000 2010

I-129 d

Fiescherhorn/Ch Mappenberg Hannover

Norderney (open-field) Siemen (open-field) Buer (open-field)

Buer (through-falling) gaseous releases liquid releases

129I and 127I in soils

129I, 127I, and 129I/127I Ratios in a Soil Profile from Groß Lobke/Lower Saxony/Germany

1000.0

0 20 40 60 80 100 120 140 160 180 200 220

depth in cm

I-129 I-127 I-129/I-127

Ernst et al., Kerntechnik 68, 155-167 (2003).

127I-127 inventories and 129I/127I Isotope Ratios in Soils from Lower Saxony/Germany

0 50 100 150 200

I-127 in

Surface of individual depth increment in cm

0 50 100 150 200 250

I-129/

27 iso

Average depth in cm

Balance of 129I and 127I in Region III of Lower Saxony / Germany

Surface-projected

concentrations

in mg m–2

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

in mg m-2 a-1

in mBq m-2 a-1

Geometric mean and

standard deviation 4,0 × 1,21 11 × 1,31

1E-10 1E-09 1E-08 1E-07 1E-06 1E-05 1E-04

I-127 in g/g

updated 23.06.2007

Stand Mai 2007

Surfce soils

seawater

Groundwater

Surface water

235U(n,f): 129I/127I = 6.06

1E-19 1E-18 1E-17 1E-16 1E-15 1E-14 1E-13 1E-12

I-129 in g/g

updated 23.06.2007

Stand Mai 2007

235U(n,f): 129I/127I = 6.06

Surface soils

Seawater

Ground-water

Surface water

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.

Transfer through the food chain

and the biospheric response

1975 1980 1985 1990 1995 2000 2005

I-129/I

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)

129I/127I in European human thyroid glands remote from reprocessing plants

1975 1980 1985 1990 1995 2000 2005

I-129/I-1

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)

Total Diet from the mensa academica of the Universität Hannover

Probenahme-

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

recommended

150 g d–1

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

Iodine pills

Sample Iodine

content

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

Drinking water

Sample I-127

concentration

in g kg-1

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

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.

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

The End

Iodine-129 in the European Environment MICHEL (Presentation... · Iodine-129 in the European...

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