Application of ICPICP-MS and AMS for
determination of PuPu- and UU-isotope
ratios for source identification
Lindis Skipperud,
Norwegian University of Life Sciences
www.umb.no
ISOTOPE LABORATORY DEP
PARTMENT PLANT AND ENVIRONMENTAL SCIENCES
NORWEGIAN UNIVERSITY OF
O LIFE SCIENCES
Why are the transuranics so
important?
Long lived (T1/2 up to 8x107 y)
Man-made sources
– weapon production (Pu
(Pu-239),
239),
– nuclear fuel cycle
– satellite battery (Pu-238),
– fire alarms (Am-241),
Alfa-emitters;
– high radiological toxicity
– bone seekers.
Multi valence
– gives complicated
environmental chemistry and
biochemistry
1
ISOTOPE LABORATORY DEP
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Isotope ratios
and sources
Actinides have source
related isotope
composition.
composition
Isotope ratios can act
as ”fingerprint” in the
environment
Uranium: Natural, Enriched, Depleted,
Reprocessed
– U-234, U-235, U236, U-238
Plutonium: Weapon production, nuclear weapon
tests, reactor type and ”burn up”
– Pu-238, Pu-239, Pu-240, Pu-241, Pu-242
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Key Question
Can the plutonium isotopic
signatures be used effectively in
complex environmental systems to
define the relative contributions
from potential sources?
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Canberra 7401 Mixer/router
1501, α-spectrometry
Perkin Elmer Elan
6000, ICP-MS
NORWEGIAN UNIVERSITY OF
O LIFE SCIENCES
ISOTOPE LABORATORY DEP
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Isotope Laboratory, UMB
THE 14UD TANDEM
ACCELERATOR
Dept. Nuclear Physics
Australian National
University
NORWEGIAN UNIVERSITY OF
O LIFE SCIENCES
ISOTOPE LABORATORY DEP
PARTMENT PLANT AND ENVIRONMENTAL SCIENCES
AMS
3
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240
Measuring isotope ratios in water and sediment
- Objectives
Different sources often exhibit characteristic uranium or
plutonium isotope ratios and these ratios can be used to
– identify the origin of contamination,
– calculate inventories,
– or follow the migration of contaminated sediments and
waters
Weapons-grade plutonium is characterized by a low
content of the 240Pu isotope
–
240Pu/239Pu
isotope
p ratio < 0.05.
– global weapons fallout and spent nuclear fuel
from civil reactors have higher 240Pu/239Pu isotope ratios.
Different sources – different Pu isotope ratios
0.6
Pu powered
reactors
Pu/239Pu
05
0.5
Civil reactor waste
0.4
0.3
02
0.2
0.1
Global fallout
Weapons
grade Pu
0.1
Naval reactors (235U
enriched)
0.2
0.3
0.4
0.5
0.6
238
Pu/240,239Pu
4
0.7
Pu--238/Pu-239+140 (activity rattio)
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Kara Sea, Novaya Zemlya fjords
Sources – isotope ratios
Abrosimov
0.6
Stepovogo
0.5
Ob
Yenisey
0.4
Open Kara
Kara Gate
0.3
0.2
0.1
GF
0
0
0.05
0.1
0.15
0.2
0.25
0.3
0.35
0.4
Pu-240/Pu-239 (atom ratio)
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Pu in Mayak PA area
Background
Mayak PA was
established 1948
to produce Pu for
Soviets atom
weapon program
Routine and
accidental
releases of
radioactive waste
have caused
severe
contamination to
the surrounding
areas.
5
Oughton, DH., Fifield, LK., Day, JP., Cresswell,
RC., Salbu, B., Skipperud, L., Strand, P., Drozhco,
E., and Mokrov, Y., (2000) Env. Sci. Tech.
238/239+240 (activity ratio)
10
1
0.1
Asanov (1949-1951)
Techa
River
EURT (1957)
Karachay (1951-)
0 01
0.01
Res. 10 (1952-)
Res. 11 (1964-)
0.001
0.01
0.1
240/239 (atom ratio)
1
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Isotope ratios in the Mayak Reservoir 10
sediments
0,6
0,5
Pu-240/Pu-239
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Pu isotope ratios in
Techa River
0,4
0,3
0,2
0,1
0
0 00
0,00
0 20
0,20
0 40
0,40
0 60
0,60
0 80
0,80
1 00
1,00
1 20
1,20
1 40
1,40
1 60
1,60
1 80
1,80
2 00
2,00
Pu-238/Pu-239, 240
Core1, 0-10cm
Core1, 10-20cm
Core 1, 20-25cm
Core2, 0-10cm
Core2, 10-20cm
Core3, 0-10cm
Core3, 10-20cm
Core3, 20-30cm
Core4, 0-2cm
Core4, 2-4cm
Core4, 4-6cm
Core4, 6-8cm
Core4, 8-10
Core4, 10-15cm
Core4, 15-20cm
Core4, 20-25cm
Core5, 0-2cm
Core5, 2-4cm
Core5, 4-6cm
Core5, 6-8cm
Core5, 8-10cm
Core5, 10-15cm
Core6, 0-5cm
Skipperud, L., Oughton, DH., Salbu, B., Strand, P., Drozcho, E., and Mokrov, Y., (2004)
“Plutonium contamination in soils and sediments at Mayak PA, Russia” Health Physics
6
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”New” and ”old” sources
Calculated
amount
Weapon
source
Civil
source
25 %
Isotope ratio
Isotope ratio
240Pu/
P /239Pu
P
238Pu/
239 240Pu
P /239,240
P
0.06
0.04
Up to 0.60
Up to 1.6
(10 TBq)
75 %
(30 TBq)
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Ob and Yenisey
Estuaries
Some of the sampling
sites in Ob and
Yenisey estuaries
(below), with sources
of weapons related
contamination (left)
7
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Pu isotope ratios in surface sediments in Ob
River compared to the Yenisey
240Pu/239Pu
atom ratios
= 0.16, n=2
(Skipperud
et al., 2004)
240Pu/239Pu
atom
ratios
0.16-0.18,
n=7
(Skipperud
et al.,
2004)
Estuary
240Pu/239Pu
atom ratios
0.09-0.13, n=8
(Skipperud et
al., 2004)
River
0.05- 0.12
n=8 (Skipperud et al.,
2004)
240Pu/239Pu:
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Size fractionation and source identification in Yenisey
estuary water
8
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Trace of weapon grade Pu found in colloidal
phase all the way into Kara Sea
Pycnocline
24,3 psu
8
41
51
Near
6
bottom 21
32,9 psu
31 36
36
31
33
33
P a rtic ulate (>0,45 u m )
C o llo id al (8 kD a-0,45u m )
L M M (< 8kD a )
61
61
68
82
70
73
Pycnocline
28 psu
Surface
41
19
11
13 9
78
72
4
Surface
0 psu
52
52
19 29
19
29
8
32 23,8 psu
32
7
7
19
52 29
Pycnocline
28 psu
Surface
25 45 0,1 psu
30
16 Near bottom
0 psu
36
48
Lind, OC., Oughton, DH., Salbu, B., Skipperud, L., et. al., (2006)
Earth and Planetary Science Letters
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Trace of weapon grade Pu found in
colloidal phase all the way into Kara Sea
Lind, OC., Oughton, DH., Salbu, B., Skipperud, L., et. al., (2006)
Earth and Planetary Science Letters
9
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This study has shown
The movement of Pu contamination from the KMCIC
installations has been detected almost 3000 km downstream
from the plant both in sediments and water.
It has
h now reached
h d th
the coastt off K
Kara S
Sea.
Pu-isotopes ratios in various Mayak samples has identified the
presence of different sources and confirmed recent reports of
civil reprocessing at Mayak
240Pu/ 239Pu
and 238Pu/ 239, 240Pu isotope ratios in discharges
from Mayak have increased with time.
between 30 and 70 % of Pu further down River Techa (50
(50-100
100
km) can originate from other sources than the early weapon
production
Using isotope ratios is an useful technique in identification of
Pu sources
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And…
ICP-MS has proven to be a good tool
together with traditional α-spectrometry
α spectrometry
when it comes to analysing uranium and
plutonium and its isotope ratios in
contaminated areas and hot particles.
Accelerator mass spectrometry has proved
to be a powerful method for measuring lowlow
level U- and Pu activity concentrations and
U- and Pu isotope ratios.
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Thank you!
www.umb.no
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