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Journal of Environmental Radioactivity 135 (2014) 128e134

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Journal of Environmental Radioactivity


journal homepage: www.elsevier.com/locate/jenvrad

Characteristic of pollution with groundwater inflow 90Sr natural


waters and terrestrial ecosystems near a radioactive waste storageq
G.V. Lavrentyeva*
Candidate of Biological Sciences, Department of Ecology, Obninsk Institute for Nuclear Power Engineering, Branch of the National Research Nuclear
University MEPhI, Studgorodok, 1, 249040 Obninsk, Kaluga Region, Russian Federation

a r t i c l e i n f o a b s t r a c t

Article history: The studies were conducted in the territory contaminated by 90Sr with groundwater inflow as a result of
Received 21 July 2013 leakage from the near-surface trench-type radioactive waste storage. The vertical soil 90Sr distribution up
Received in revised form to the depth of 2e3 m is analyzed. The area of radioactive contamination to be calculated with a value
18 April 2014
which exceeds the minimum significant activity 1 kBq/kg for the tested soil layers: the contaminated
Accepted 22 April 2014
Available online 13 May 2014
area for the 0e5 cm soil layer amounted to 1800  85 m2, for the 5e10 cm soil layer amounted to
300  12 m2, for the 10e15 cm soil layer amounted to 180  10 m2. It is found that 90Sr accumulation
proceeds in a natural sorption geochemical barrier of the marshy terrace near flood plain. The exposure
Keywords:
Storage of radioactive waste
doses for terrestrial mollusks Bradybaena fruticum are presented. The excess 90Sr interference level was
90
Sr registered both in the ground and surface water during winter and summer low-water periods and
Migration in soil autumn heavy rains.
Water Ó 2014 Elsevier Ltd. All rights reserved.
Terrestrial molluscs

1. Introduction polluted by technogenic radionuclides (IAEA Safety Standards


Series, 2005).
Now the emission of technogenic radionuclides into the envi- The article is aimed at the researching of characteristic of natural
ronment is under a rigorous control of atomic power enterprises, waters and terrestrial ecosystems pollution with groundwater
however, the problem of ecological safety of radioactive waste inflow 90Sr.
(RAW) storage sites created in the second half of the last century is Despite a body of information on the features of technogenic
unsolved yet. It must be borne in mind that the RAW storage are in radionuclide migration in natural habitats as a result of accidental
operation for 35e55 years and do not meet the current regulation releases from RAW storages (Roudak et al., 2011; Monastyrskaya
requirements to a long-term radioactive waste storage (IAEA Safety et al., 2012; Simakov et al., 2008; Shandala et al., 2008; Sneve
Standards Series, 2011; SR, 2003). Proceeding from their forecasted et al., 2007; Lavrentyeva et al., 2012a; Lavrentyeva, G.V., 2013), it
conditions, the break of tightness and radionuclide ingress in the should be considered that the radionuclide behavior will be highly
environment are expected and this may result in the additional dependent on the specific geomorphological, landscape, natural-
exposure source for population and ecosystem as a whole. As a climatic and other characteristic of the ecosystem. Studies of
result of such emergency situations, practically all feasible mea- radionuclide migration features depending on local conditions will
sures aimed at security assurance are to be carried out, including allow the methodical basis of radioecological territory monitoring
those on the abatement of radionuclide migration in natural hab- at a regional level to be expanded.
itats. In turn, it is possible with regular monitoring of territories The paper presents radioecological studies in the territory of a
regional RAW storage. This object had been put into operation in
the 50e70s of the last century. Now the object is a closure. There
are 4 trench storage facility (N  1, 2, 3 and 4) (Fig. 1) for solid RAW
q This research was conducted with financial support from Rosatom State Cor-
in the object territory. The total waste volume is about 2500 m3.
poration (State Agreement No, 1054 This research was conducted with financial
There is also a reinforced concrete container (N  5) of 330 m3 in
support from Rosatom State Corporation (State Agreement No. H.4b.43.9B.14.1054) volume for liquid RAW collection and storage (Vasiljeva et al.,
and the Grant of the President of the Russian Federation (Agreement No.14.125.13. 2007). The territory under studies is situated in the middle of the
368-MK). river Protva basin in the terrace above flood- plain within the actual
* Tel.: þ7 961 122 71 06.
elevation 131e145 m. The distance to the river is 1000e1200 m. The
E-mail address: Lavrentyeva_G@list.ru.

http://dx.doi.org/10.1016/j.jenvrad.2014.04.013
0265-931X/Ó 2014 Elsevier Ltd. All rights reserved.
G.V. Lavrentyeva / Journal of Environmental Radioactivity 135 (2014) 128e134 129

oxide. Strontium carrier solution (50 mg of metal) and 5 M HNO3 of


200e300 cm3 in volume were added in a glass with annealed soil.
The soil/solution mixture was boiled in a sand-bath during half an
hour. A solution was separated from a solid phase by filtration. Solid
soil was twice treated by boiling in 4e5 M HNO3 during half an
hour. After filtration the solid soil sediment had been washed three
times with distilled water in a filter. After filtration the solutions
were combined and evaporated to 100 cm3.
A version of oxalate precipitation was used to separate stron-
tium from other radionuclides and chemical elements and to
concentrate it. Ethanedioic acid solution (95 g/l H4C2O2) in the
quantity of about 100 cm3 was added to the solution obtained after
desalinization and evaporation. pH ¼ 4 in a solution was set by
deacidification with an aqua ammonium solution. The solution
with an oxalate precipitate was stayed for 4 h, further a precipitate
was elutriated and washed twice with hot distilled water in a filter.
A precipitate and a filter were dried and then annealed at 7500S in
a muffle furnace during an hour. Hereafter a precipitate was put
into a glass and dissolved in 3e4 M HNO3, the solution acidity was
set at 3.0 M/l (the solution volume is preferably made up to 5e
10 cm3). When the accompanying components were separated, 90Sr
was cleaned by extraction. Nitric-acid solution was put in a sepa-
rating funnel of 50e100 cm3, poured with chloroform in a 2:1 ratio
of the aqueous and organic phases, shaked up and phased. After
phase separation, the aqueous solution was added by 5e10 cm3
dicyclohexane-18-crown-6 in 0.2 M of a chloroform solution and
extracted by shaking up during 30 s. The organic phase was washed
with two portions of 2M HNO3 solution in a 1:1 ratio; the aqueous
phase was rejected. The extract (organic phase) or its aliquot part
was put on a target and dried under an infrared lamp. Dry matter b-
activity on the target was measured.
Fig. 1. Diagram of sampling points at the RAW storage site and the adjacent territory.
2.2. Plant sample analysis

storage facilities are put in well-drained, mainly sand deposits. The Plant e great nettle (Urtíca dióica) e samples were collected at
flood plain begins at a 100 m distance from the RAW storage. The the same sites (Fig. 1). Before analysis, fresh crude plant samples
soil is generally soddy-podzolic formed on deluvial and moraine were washed from dust and soil first with tap water, then with
loam. The soil texture is loamy and heavy clay loamy. In 1998e1999 distilled water. Then the plant mass was dried up in desiccators at
the increased specific activity of 90Sr had been revealed in the 80e850S. A dried plant sample was milled. The optimal size of
surveying wells and in the following this was stipulated by surface plant fragments had to be about 1e5 mm. Plant mineralization was
water penetration in one of the facility (N  4). Storage facility N  4 realized by dry ashing. After digestion a sample had undergone acid
has size: 21.5  10 m and a depth of 3 m. In reservoir overfilling, 90Sr treatment according to the above procedure (Instruction, 1994).
and 137Cs radionuclide exposed water escaped outside. Multi-year Analysis of radionuclide content in the studied soils was conducted
studies allowed one to establish that 90Sr contributes much to by comparison with the regional background of radionuclide con-
radioactive contamination on the territory near the storage and in tent in the soils within the 30-km radius of the Obninsk reactors, as
the adjacent territory (Vasiljeva et al., 2007; Lavrentyeva, 2013). well as levels of global fall-outs resulting from technogenic emis-
sions and the disaster at the Chernobyl Nuclear Power Plant. The
90
2. Materials and methods Sr value amounted to 1.2e1.8 Bq/kg. (Vasiljeva et al., 2007; YB,
2011; Ivanov et al., 1999).
2.1. Soil sample analysis
2.3. Mollusk sample analysis
Soil samples are collected by a special sampler with a set of
Edelman hand soil drills (Eijkelkamp Firm, Netherlands). Layer-by- Terrestrial mollusks Bradybaena fruticum were collected from
layer sampling had been carried out in a 5 cm increment to 50 cm plants (great nettle (Urtíca dióica)) and soil under plants at the tested
and a 10 cm increment up to 2e3 m at controlled sites noted in the sites (Fig. 1). At least 10 specimens were chosen in each mollusk
Fig. 1. Soil sample preparation for assessing 90Sr content had been sample. First soft tissues were removed from shells. Shells were
realized according to the (Instruction, 1994). grinded in a mortar, hereafter the direct 90Sr activity measurements
Soil mass of 1 kg was counter balance weighed and uniformly were performed. Samples had been incinerated in a muffle furnace
distributed on a stainless steel griddle in the layer of 20e30 mm in at 450  C during 6 h. Radiochemical separation and 90Sr content
thickness. To dehumidify, the griddle with samples had been kept assessment were realized according to the above procedure.
in a drying box at 110  C during 5e7 h. Dried samples were dis-
integrated and mixed in a mortar to the grain size of 2e3 mm. Then 2.4. Water sample analysis
the mean average sample (mass 50e300 g) of air-dried soil was
analytical balance weighed. The sample had been annealed in a Well and hole water was sampled according to the state stan-
muffle furnace at 700e750  C to transform the basic mass into dard (SS, 2000). Water samples were collected from the following
130 G.V. Lavrentyeva / Journal of Environmental Radioactivity 135 (2014) 128e134

objects (Fig. 1): the surveying well C4 located near an emergency sandy deposits (Table 1). The moraine loam depth is low and it can
storage; the creek in the storage area on the marshy terrace near not be a reliable barrier under emergency situations. The first
flood plain primarily supplied by groundwater (top water); the reliable aquitard represented by almost a 20-meter continuous clay
marshy territory appeared for a time after heavy rains and snow soil is found at the depth from 23 m in the storage top to about 18 m
melting near site 7d. in its lower part.
Water samples were acidified with nitric acid to pH ¼ 1e2 in the The characteristic of a geomorphological territory structure also
universal indicator paper. For that purpose the carriers in a form of contribute to the surface and internal soil radionuclide migration
nitric-acid solutions were added to the water solution: 10e20 mg (Vasiljeva et al., 2007). In this case the surface runoff 90Sr migration
strontium (in terms of metal) and 20 mg/l calcium. The carrier, i.e. is stipulated by the following factors. Surface slopes of about 10-150
alkaline-earth element (AEE) was precipitated as carbonates for promotes to surface erosion. The low-thickness (not more than 1 m
strontium radionuclide concentration. at the bottom of the slope) deluvial formation is the redeposited
The activity of 40K, 90Sr and 137Cs was measured in a scintillation clay loam. The presence of almost rectilinear hollows along the
b-spectrometer «BETA-01S» according to the standard procedure maximum gradient lines is indicative of the low erosion soil
for assessing 90Sr concentration from b-radiation of its daughter 90Y stability.
radionuclide in environmental objects (Instruction, 1994). The flushing water conditions in the aeration zone, light soil
texture, significant slope of territory are reason of the active in-
2.5. Calculation of annual exposure doses for mollusks ternal soil migration of 90Sr. At the depth of 6 m in the centre of the
terrace slope and at about 3 m in its lower part the sand is underlain
The annual doses of external b-exposure of mollusk tissues due by loam which serves a confining layer for top water; in the lower
to 90Sr and it daughter 90Y radionuclide contained in shells were slope part it crops out and groundwater is discharged here.
calculated with software package ERICA Tool (Brown et al., 2008; We must note that texture of the soil (silt, clay) of the adjacent
Garnier-Laplace, Gilbin, 2006). territory contribute to minimization of the 90Sr migration processes
(Table 2). It offers the expected formation of a natural geochemical
barrier at the sites 6a, 10e and 11 where this radionuclide is accu-
3. Results and discussion
mulated. During eight years, the 90Sr specific activity at the sam-
90 pling points of that area has increased on average by 1.7e2 times.
3.1. Pattern of soil contamination with Sr at the RAW storage site
The 90Sr maximum specific activity in soil exceeding 1 kBq/kg was
and the adjacent area
recorded in 2012 at the sampling points 6a (1,7  0,3 kBq/kg), 10f
(1,1  0,2 kBq/kg) and 11 (1,6  0,2 kBq/kg) outside the storage site
The analysis of long-term data (2004e2007) on the 90Sr radio-
(Fig. 1).
nuclide content in the soil of the studied site and the continued
Due to significant irregularity of contamination of the studied
experimental work (2010e2013) allowed us to establish the
site with 90Sr, we took separate measurements of the radionuclide
following. A 1.5e2-fold reduction of the specific 90Sr activity in soil
specific activity from various soil sublayers in the sampling points.
near the studied object had been observed from 2005 to 2012
The data analysis of radionuclide vertical distribution in the soil
(Fig. 2); this reduction may be stipulated by self-cleaning of
behind the site allowed us to establish the following characteristics.
ecosystem from radioactive contamination including radioactive
Relatively similar dependence of radionuclide specific activity at
decay, secondary dispersal, soil and plant radioisotope distribution,
depths was discovered for soddy glay soil of back marsh (points 6a,
formed natural geochemical barriers and technogenic measures.
10f and 11) (Fig. 3). The 90Sr maximum specific activity of 1.7 kBq/
We shall not forget about active horizontal displacement of radio-
kg was recorded in the upper 2-cm layer, which may be caused by
nuclides that occurs in flood plains, as a result of surface runoff after
few factors. First, the soil samples collected in the upper layer that
heavy rains or land loss during snowmelt runoff.
concentrate 90Sr represent clay loam, which contributes to reduc-
The increase was observed of 90Sr concentration gradient from
tion of radionuclide migration processes due to its active sorption.
the contamination source (emergency storage) to the sampling
Second, a drift of silt from contaminated areas may occur during
sites 6a, 10e and 11 located beyond the object territory. In turn, it
flood, as well as runoff from a contaminated RAW storage site.
may be also was determined by lithological and geomorphological
Third, active fixation of 90Sr by soil organic fraction may occur.
characteristic of the territory.
In spite of the fact that, in the next soil layers, we can observe a
The description of a lithological structure in the object territory
trend of drastic decrease of radionuclide activity (3e8 times),
shows that storage facility are put into well-drained, primarily
which may be related to predominance of sand deposits, 90Sr mi-
grates to the deeper layers; even at the 2-meter depth, it reaches a
value that exceeds value (1.2e1.8 Bq/kg) by 80e100 times.
55 sampling site 1 A slightly different picture of radionuclide distribution in soils is
Specific Sr-90 acƟvity, Bq/kg

sampling site 2c observed at the RAW storage site (Fig. 3). A relatively uniform 90Sr
45 distribution through immature soddy soil profile may be caused by
biogeochemical and technogenic factors. First, the processes of
35

Table 1
25
Description of the lithological basis of the territory of the RAW storage (Vasiljeva
et al., 2007).
15
Depth, meter Soil characteristics

5 0e0.5 Backfill soil


2005 2010 2011 2012 0.5e8.8 Alluvial consertal sandstone
8.8e11.7 Alluvial fine low-loamy sand
Year
11.7e13.5 Moraine loam with a high gravel and pebble concentration
90 13.5e15.7 Fluvioglacial consertal sandstone with gravel and pebble
Fig. 2. Change in the specific activity of Sr in soils of the territory of the RAW storage
15.7e16.8 Gravel-pebble and sandy fluvioglacial deposites
(error is a confidence interval).
G.V. Lavrentyeva / Journal of Environmental Radioactivity 135 (2014) 128e134 131

Table 2
Dose rate of terrestrial mollusc external exposure to the b e particles and characteristic of sampling points.
90 137 40
Sampling Characteristic of sampling points Dose rate on Sr, Dose rate on Cs, Dose rate on K,
points mGy/year mGy/year mGy/year

1b Fluvioglacial and alluvial sandy sediments, disturbed soil. Herb-grass vegetation. 84.0  6.0 14.0  2.0 1.0  1$101
1 76.0  8.0 28.0  3.0 94$102  8$102
2a 346.0  5.0 57.0  5.0 99$102  7$102
2c Fluvioglacial and alluvial sandy sediments, disturbed soil. Buried diluvial loam 46.0  7.0 1$102  1$103 83$102  9$102
2b soil (redeposited covering loam) closed 40 cm thick layer of sand deposits. 653.0  13.0 12.0  2.0 2.0  1.0
Herb-grass vegetation.
3 The surface is not swamped, covered with diluvial loam. Reclaimed turf medium 35.0  3.0 1$102  1$103 94$102  7$102
loamy soils. Raspberry, filbert, in a grassy nettle tier dominates.
4 The surface is not swamped, covered with diluvial loam. Reclaimed turf with signs 56.0  5.0 2$102  1$103 82$102  9$102
podzolization medium loamy soils. Raspberries in a grassy tier dominates nettle, hops.
6 Swampy surface, covered with silt (depht of 2e10 cm) with the inclusion of weakly 134.0  24.0 e e
6a decomposed plant residues. Alder, aspen, nettle. 281.0  31.0 5$102  3$103 69$102  8$102
7b Swampy surface, covered with silt (depht of 2e10 cm) with the inclusion of weakly 62.0  12.0 2$102  1$103 1.0  1$101
7d decomposed plant residues and sand. Alder, aspen, nettle, hops. 89.0  17.0 e e
10 Swampy surface, covered with silt (depht of 2e5 cm) with the inclusion of weakly 537.0  37.0 3$102  1$103 1.0  8$101
decomposed plant residues, sand. Alder, willow, aspen, bulrush.
10a Swampy surface, covered with silt (depht of 2e5 cm) with the inclusion of weakly 182.0  27.0 1$102  2$103 1.0  9$101
10b decomposed plant residues and sand. Alder, aspen, nettle. 74.0  4.0 12.0  3.0 1.0  7$101
10c 50.0  13.0 17.0  4.0 1.0  7$102
10d Swampy surface, covered with (depht of 2e5 cm) with the inclusion of weakly 47.0  7.0 27$102  2$102 1.0  5$102
decomposed plant residues and sand. Alder, aspen, nettle, hops.
10e Swampy surface, covered with (depht of 2e5 cm) with the inclusion of weakly 77.0  7.0 28.0  5.0 1.0  8$102
decomposed plant residues and sand. Alder, aspen, nettle.

 Confidence interval.

subsoil inflow of radionuclides and their penetration into upper that, the 90Sr specific activity at different depths exceeds the
layers mostly occur due to filtration and capillary rise of contami- background value by 50e120 times.
nated waters. Second, the absence of scrub and tree vegetation at The obtained data allowed the area of radioactive contamination
the site near the sampling point leads to minimization of radio- to be calculated with a value which exceeds the minimum signifi-
nuclide fixation in the upper layer. The third factor is technogenic e cant activity 1 kBq/kg for the tested soil layers: the contaminated
performance of overburden work after intake of radionuclides in area for the 0e5 cm soil layer amounted to 1800  85 m2, for the 5e
groundwater, and mixing the soil layers with various activity. At 10 cm soil layer amounted to 300  12 m2, for the 10e15 cm soil

Fig. 3. Vertical distribution of 90Sr in soils inside (sampling points 2a, 2c and 2d) and outside (sampling points 6a, 10e and 11) the RAW storage site (error is a confidence interval).
132 G.V. Lavrentyeva / Journal of Environmental Radioactivity 135 (2014) 128e134

layer amounted to 180  10 m2 (SR, 2002). These data may be of and the start-up of spring snow melting and heavy rains. The
service in developing the program of 90Sr contaminated soil reha- period of spring heavy rains and active snow melting was observed
bilitation at the stage of RAW storage decommissioning. from 20 March to 18 June. During this period the main bulk of the
slope runoff (288  17 mm), consisting of melt-water
3.2. Biota exposure dose in the RAW storage area (121  15 mm) and spring heavy rain (167  14 mm) enters sub-
terraneous horizons and the river valley. The summer drought
Terrestrial mollusks Bradybaena fruticum have been chosen as period, i.e. dry hot summer with rare short rains, had come from 18
reference species most properly reflecting the ecosystem 90Sr ef- June. The groundwater recharge and surface runoff had practically
fect. Some papers (Khmeleva et al., 1993; Frantsevich et al., 1995; ceased. The amount of precipitations during two summer months
Gudkov et al., 2009) have stated that practically the whole was as little as 20  4 mm. The summer drought period had
amount of radioactive strontium is concentrated in a mollusk shell. completed on the 20th of August. Heavy rains had started and
In addition, the content of 90Sr in mollusk shells is primarily gov- persisted practically continuously till 4 September, then inter-
erned by the ground contamination level and undergoes insignifi- ruptedly up to frosts. The amount of precipitations compared with
cant seasonal and taxonomic variations. the summer months had doubled and 20 October (the last date of
In view of ICRP recommendations on a step-by-step approach to activity measurements) it corresponded to 39  12 mm.
the radioecological situation analysis, this paper presents results of Groundwater contamination near the old RAW storage from
the first stage which involves the screening analysis to reveal monitoring results of 2010 is illustrated by the calendar data of
obvious situations not requiring further consideration (ICRP, 2009). Table 3.
The screening value meant for the initial biota safety assessment is The water activity concentration in a sample taken from the well
taken equal to 10 mGy/h. It should be noted that this value is taken N  4 changes slightly with hydrological seasons. The groundwater
90
as a safe biota exposure limit within the European PROTECT project Sr activity value of 34 Bq/l was registered in the late winter low-
(Kryshev, Sazykina, 2013). Taking the foregoing into account, water period and the early period of snow melting and spring rains.
further studies of radioecological conditions are not efficient at the The water sample, collected on the 15th of June, characterizes the
local sites, where the is not target of exceeding. Hence, the next end of spring snow melting. The analyzed water had demonstrated
stage of these radioecological studies intended for a more detailed a positive reducing trend of this radionuclide activity concentration
analysis in view of local ecosystem contamination conditions apparently due to the residual groundwater dilution by rain pre-
should be carried out at the sites with consideration of the safe cipitations. The value of 90Sr activity in groundwater during the dry
biota exposure limit (Table 2). hot summer period is similar to 90Sr content in the sample collected
in the winter low-water period. The a slight increase in activity of
90
3.3. 90Sr content in surface and underground waters at the RAW Sr to 38 Bq/l in a well was observed in the early autumn heavy
storage site and the adjacent area rain period as a result of the winter runoff front registered. In
addition, the groundwater radionuclide concentration in different
In 2010, the 90Sr volumetric activity was measured in water hydrological seasons exceeded the pollution standard (5 Bq/l) by a
samples collected each season from inspection wells and controlled factor of 6e8 (RSS, 2009).
water bodies where the highest radionuclide activity was recorded Surface water contamination near the RAW storage based on the
earlier (Lavrentyeva et al., 2012b): in the surveying well; in the results of monitoring in 2010 is illustrated in Table 3.
creek; and in the marsh (Fig. 1). The activity concentration of 90Sr in the creek water after
In the context of hydrology, the year 2010 had no significant flooding was 5 Bq/l. This very day the activity concentration in the
deviations from the average many-year characteristics. The steady marsh located in this brook valley was 1.5 Bq/l. In the summer low-
negative winter temperature in 2009e2010 had begun from 6 water period of a drought season the activity of 90Sr in a brook
December, 2009 and lasted until 20 March, 2010. Snow had fallen sample had increased up to 34 Bq/l and in a marsh sample it
on the thawed ground and did not melt in winter months. About dropped to 0.75 Bq/l. It is clear that rain precipitations had diluted
121  15 mm of snow had precipitated during this period. Thus, the initial 90Sr concentration in June. Autumn rains which enriched
snow melting in 2010 took place under the conditions of the active the surface runoff of 90Sr accumulated in trench stagnant water
snow water discharge through the thawed ground into the un- during the drought summer period began on the 19th of 2010.
derground horizons. Spring flood under such conditions was Strontium-90 concentration in brook water was 7e8 times higher
characterized by low water and weak inversion feed of surface than the standard of water pollution (4.9 Bq/l) during summer
water into the underground water-bearing layers. drought low-water and autumn heavy rains, respectively.
The transition to stable positive temperature was registered on The analysis of the results of long-term monitoring of 90Sr in
the 20th of March. This date is the end of a winter low-water period surface and underground waters allows us to note that, within

Table 3
90
Activity concentration of Sr in groundwater surface water near the RAW storage.

Object Date Activity concentration, Bq/l Precipitation mm Air temperature, 0C Hydrological season

The surveying well C4 15.03.10 34  5 1  5$101 7  5$101 Winter low-water period


15.06.10 29  3 7 4 14  1 After flooding
22.07.10 34  6 0 29  2 Summer drought period
20.10.10 38  7 5 1 3  1 Autumn heavy rains
The creek 15.06.10 5  1 7 4 14  1 After flooding
22.07.10 34  5 0 29  2 Summer drought period
20.10.10 38  7 5 2 3  1 Autumn heavy rains
The marsh 15.06.10 2  1 7 4 14  2 After flooding
22.07.10 1  8$101 0 29  1 Summer drought period
20.10.10 5$101  3$101 5 2 3  6$101 Autumn heavy rains

 Confidence interval.
G.V. Lavrentyeva / Journal of Environmental Radioactivity 135 (2014) 128e134 133

140 250
The surveying well
A

Volumetric acƟvity of Sr-90, Bq/l


PrecipitaƟons
120

PrecipitaƟons/month, mm
200
100

150
80

60
100

40
50
20

0 0

08.1999

07.2005
10.1998
12.1998
02.1999
04.1999
06.1999

12.1999
02.2000
04.2000
06.2000
08.2000
03.2001
07.2001
12.2001
04.2002
07.2002
02.2003
05.2003
10.2003
03.2005

11.2005
08.2006
03.2010
07.2010
Sampling Ɵme (month.year)

12 B The marsh 250


Volumetric acƟvity of Sr-90, Bq/l

PrecipitaƟons

PrecipitaƟons/month, mm
10
The creek 200

8
150
6
100
4

50
2

0 0

Sampling Ɵme (month. year)


90
Fig. 4. Results of Sr monitoring in underground (A) and surface (B) waters in the area of the RAW storage.

twelve years of monitoring the RAW storage, the 90Sr concentration The repeated spike of radioactivity in subterranean waters was
in water bodies repeatedly changed (Fig. 4). The most drastic recorded in the 2000 year. In the period required for radionuclide to
changes in strontium radioactivity can be seen in water samples migrate from the trench to the well, the increase of water radio-
collected from the well C4 (Fig. 4 A). During the period from activity in the inspection well was delayed from the date of pre-
December 1998 to August 1999, we recorded stable high radionu- cipitation. The water activity level in this period slightly decreased
clide content practically independent of the precipitation amount. regardless the amount of precipitation, which can be explained by
A sudden decrease in 90Sr activity in subterranean waters of the partial sorption of 90Sr by a bergmeal shield. Upon saturation of
well occurred in summer 1999. Starting from this period and until bergmeal barrier, the water activity level began to gradually in-
August 2010, the graphs of strontium activity and amount of pre- crease, and the activity once again became synchronous with rain
cipitation are synchronous. During the period from December 1999 precipitation. It should be noted that the observations of activity in
to July 2002, a relative shift in maximum values in graphs was the date range of October 1999 to November 2005 showed a good
observed. After that, until November 2005, we see graph syn- correlation with rainfall. The correlation coefficient is 0.53. Activity
chronism once again; in 2006 and 2010, complete divergence be- is directly proportional to the amount of precipitation with aspect
tween graphs. Despite uneven changes in the 90Sr activity, we can ratio 0.706. The reliability of this factor (p-value) is equal to 1.5e7.
note a slight decrease in water radioactivity. In the last interval of the graph that covers years 2005e2010,
The analysis of long-term dynamics of the 90Sr emission from radioactivity of subterranean waters has decreased, and its relation
the RAW storage allows us to state that the first of the above- to meteorological conditions became uncertain.
mentioned periods is defined by transit carryover of radionuclide
under conditions of sealing failure in the trenches with radioactive 4. Conclusions
waste. Radioactive subterranean waters that filled the trench
evenly discharged into the aquifer, which was recorded after water The review of previous studies of radionuclide migration in the
sampling from the C4 well. Change in activity in the aquifer natural environment has shown that these problems are thor-
occurred in summer 1999, when waterproofing of trenches has oughly understood, however, practically all efforts are aimed at
undergone repairs (Vasiljeva et al., 2007). Supposedly, after repair, investigating the radionuclide behavior in a soil-plant cover and
the strontium discharge from the trench temporarily stopped, and aquatic ecosystems in aerial contamination. In this case radioactive
the soil of trench bunds where significant amount of radionuclide substances enter into the soil-plant cover surface, often together
has collected became the main source of 90Sr. with hardly soluble particles and stay in the upper soil profile for
134 G.V. Lavrentyeva / Journal of Environmental Radioactivity 135 (2014) 128e134

years. The radionuclide behavior and characteristic of their vertical Instruction: Procedure of radiochemical strontium-90 assessment in soil and plant
samples, 1994. Instruction of Rosleskhoz of Russia from 05.09.1994 N  192.
and lateral migration, their impact on biota with groundwater
Moscow (in Russian).
inflow are studied poorly. Our research considers just this way of Ivanov, V.K., Tsyb, A.F., Ivanov, S.I., 1999. Liquidators of the Chernobyl Disaster:
radioactive contamination and it is very important for assessing the Radiological and Epidemiological Analysis of the Health Consequences, p. 312.
radioactive waste storage impact on adjacent territory in case of the Moscow, (in Russian).
Khmeleva, N.N., Golubev, A.P., Plenin, A.E., 1993. Radiation resistance of mollusk
multi-barrier protection fault. populations from water bodies with different levels of radioactive contamina-
It is found that 90Sr accumulation proceeds in a natural sorption tion. Reports Acad. Sci. RF 329 (5), 677e679 (in Russian).
geochemical barrier of the marshy terrace near flood plain. The data Kryshev, I.I., Sazykina, T.G., 2013. Radiation safety of the environment: request for
harmonization of Russian and international regulation documents with
analyzed on the vertical soil radionuclide distribution in the object consideration of Federal laws and new International Basic Safety Standards.
and adjacent territories allowed one to establish the following. The Radiat. Risk Bull. Natl. Radiat. Epidemiol. Registry) 22 (1), 47e61 (in Russian).
maximum specific activity of 90Sr was recorded in the upper hori- Lavrentyeva, G.V., 2013. Radioecological analysis of the area of the storage of
radioactive waste. Bezopasnost’ v tekhnosfere 2 (6), 14e19. http://dx.doi.org/
zon of 2 cm in depth and amounted to 1.7 kBq/kg in the object 10.12737/2156.
territory. There is a relatively uniform radionuclide distribution Lavrentyeva, G.V., Bakhvalov, A.V., Synzynys, B.I., Mullayarova, R.R., 2012a. Envi-
over a soil profile in the RAW storage territory and it does not ronmental risk assessment technology for terrestrial ecosystem under condi-
tions of chronic radioactive pollution. Problem Risk Anal. 9 (5), 30e43 (in
exceed 250 Bq/kg. Screening analysis of biota conditions during Russian).
radioecological studies has shown that this contamination is local Lavrentyeva, G.V., Silin, I.I., Koz’min, G.V., Vasilieva, A.N., Synzynys, B.I.,
in character. Therefore further studies in the territory should be Glushkov, YuM., Momot, O.A., 2012b. Dynamics of the 90Sr seasonal behavior in
surface and underground waters of the area of radioactive waste repository.
conducted in accordance with local contamination conditions at
Water: Chem. Ecol. (12), 26e31 (in Russian).
certain sites. Monastyrskaya, S.G., Kochetkov, O.A., Barchukov, V.G., Kuznetsova, L.I., 2012.
Results of natural water monitoring near the RAW storage Problems of regulation safety of radioactive waste management in Russia.
enabled to establish the most dynamic periods of 90Sr activity Occup. Med. Ind. Ecol. (10), 44e48.
Publication ICRP e International Commission on Radiological Protection, 2009.
concentration variations to which greater attention is to be paid. Environmental Protection: Transfer Parameters for Reference Animals and
The excess 90Sr interference level was registered in ground water as Plants, 114. Annals of the ICRP, p. 111.
well as surface water during winter and summer low-water periods Roudak, S.F., Sneve, M.K., Kiselev, M.F., Shandala, N.K., 2011. Progress Report on the
Regulatory Cooperation Program Between the Norwegian Radiation Protection
and autumn heavy rains. Authority and the Federal Medical Biological Agency of Russia, 8. Norwegian
In view of the foregoing, it may be concluded that acute radio- Radiation Protection Authority, Østerås, p. 52. Final report of projects and other
ecological problems in the RAW storage territory have not been activities completed in 2008e2009 and plans for 2010e2011.
StrålevernRapport.
revealed for the present. However, the places of 90Sr accumulation RSS, 2009. Radiation Safety Standards. RSS e 99/2009. Moscow, (in Russian.
can act as a secondary source of radioactive contamination and this Shandala, N.K., Sneve, M.K., Smith, G.M., Kiselev, M.F., Kochetkov, O.A., Savkin, M.N.,
requires continued radioecological studies of the territory. Simakov, A.V., Novikova, N.Y., Titov, A.V., Romanov, V.V., Seregin, V.A.,
Filonova, A.V., Semenova, M.P., 2008. Regulatory supervision of sites for spent
fuel and radioactive waste storage in the Russian northwest. J. Radiol. Prot. 28,
453e465.
Simakov, A.V., Sneve, M.K., Abramov, Y.V., Kochetkov, O.A., Smith, G.M.,
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