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Article

Reconstruction of the Long-Term Dynamics of Particulate Concentrations and Solid–Liquid Distribution of Radiocesium in Three Severely Contaminated Water Bodies of the Chernobyl Exclusion Zone Based on Current Depth Distribution in Bottom Sediments

1
Institute of Environmental Radioactivity, Fukushima University, Kanayagawa 1, Fukushima 960-1296, Japan
2
Ukrainian Hydrometeorological Institute, Nauki Av., 37, 03028 Kyiv, Ukraine
3
Chernobyl Ecocentre, State Agency of Ukraine on Exclusion Zone Management, 07270 Chernobyl, Ukraine
*
Author to whom correspondence should be addressed.
Land 2022, 11(1), 29; https://doi.org/10.3390/land11010029
Submission received: 26 October 2021 / Revised: 1 December 2021 / Accepted: 21 December 2021 / Published: 24 December 2021
(This article belongs to the Topic Fate and Transport of Artificial Radionuclides in Soil-Water Environment)
(This article belongs to the Section Soil-Sediment-Water Systems)

Abstract

:
Given the importance of understanding long-term dynamics of radionuclides in the environment in general, and major gaps in the knowledge of 137Cs particulate forms in Chernobyl exclusion zone water bodies, three heavily contaminated water bodies (Lakes Glubokoe, Azbuchin, and Chernobyl NPP Cooling Pond) were studied to reconstruct time changes in particulate concentrations of 137Cs and its apparent distribution coefficient Kd, based on 137Cs depth distributions in bottom sediments. Bottom sediment cores collected from deep-water sites of the above water bodies were sliced into 2 cm layers to obtain 137Cs vertical profile. Assuming negligible sediment mixing and allowing for 137Cs strong binding to sediment, each layer of the core was attributed to a specific year of profile formation. Using this method, temporal trends for particulate 137Cs concentrations in the studied water bodies were derived for the first time and they were generally consistent with the semiempirical diffusional model. Based on the back-calculated particulate 137Cs concentrations, and the available long-term monitoring data for dissolved 137Cs, the dynamics of 137Cs solid–liquid distribution were reconstructed. Importantly, just a single sediment core collected from a lake or pond many years after a nuclear accident seems to be sufficient to retrieve long-term dynamics of contamination.

1. Introduction

Thirty-five years after the Chernobyl nuclear power plant (ChNPP) accident, studies of radioactive contamination of water bodies continue to be of importance and relevance due to the need to understand long-term processes and dynamics. Closed and semi-closed lakes and ponds were found to be most sensitive to radioactive contamination, as evidenced by numerous studies conducted in the Chernobyl contaminated areas [1,2,3,4,5] and the Fukushima Dai-ichi nuclear power plant zone [6,7,8,9,10], as well as in the PA Mayak area [11,12,13] and in the USA including Savannah River site [14,15,16]. Despite a vast number of studies of radionuclide behavior in such water bodies, most of them lacked broad temporal coverage and did not deal with long-term changes in radionuclide concentrations. This is especially true for particulate concentrations in the Chernobyl zone water bodies, with the monitoring system primarily focused on dissolved concentrations as being the most important in terms of radionuclide mobility and bioavailability [17,18]. In our work, particulate concentration as a function of time is reconstructed from radionuclide depth distribution in bottom sediments, assuming certain conditions are satisfied for sediment column formation. Such thinking was previously used for Chernobyl-derived 137Cs profiles in the bottom sediments of Shchekino dam reservoir on Upa River [19,20] and for Fukushima-derived 137Cs in bottom sediments of Ogaki dam on Ukedo River [21] to estimate radionuclide concentrations in rivers. This study, to our knowledge, is the first attempt to apply the approach for lakes and artificial pond.
Immediately after the accident, the primary pathway of radioactive contamination for water bodies is atmospheric fallout directly on the water surface [5,22]. The main long-term source of sediments and sediment-associated radionuclides in lakes is surface runoff from the contaminated catchment [5,23,24,25], with suspended particles delivered from the topsoil layer on the catchment. Numerous studies of wash-off of different origin contaminants have shown that the effective soil layer depth interacting with surface runoff is only the top several millimeters (up to 1 cm) [26,27,28,29,30,31]. The radionuclide concentration in the “contact” topsoil layer decreases with time due to radioactive decay and vertical migration to deeper layers [32,33,34,35,36]. As a consequence, the particulate concentration of radionuclides in lakes and ponds decreases, and, accordingly, the dissolved concentration also decreases. Suspended particles settle continuously on the bottom, and thereby the depth profile of sediment-associated 137Cs is formed in bottom sediments. The highest concentrations of radionuclide in the sediment profile can be attributed to the initial period or the first year after the accident. This holds true, however, provided mixing of particles in the bottom sediment column is negligible and the radionuclide is strongly bound by sediments.
The ability of suspended sediments to bind a radionuclide is usually characterized by the apparent distribution coefficient Kd, which, by definition, is the ratio of radionuclide particulate concentration cp to its dissolved concentration cd at equilibrium or steady-state condition [37,38,39]:
K d = c p c d
The requirement of radionuclide strong binding to sediments is fulfilled when Kd > 104 L/kg [19,20,21].
When mixing of sediments in the bottom depth profile is insignificant and radionuclides are strongly bound to sediments, the maximum radionuclide concentration in its depth distribution should be well marked with a sharp front below. Reasoning from this, many authors conducted dating of bottom sediments and determined average sedimentation rates in lakes [40,41,42,43]. Determination of the sedimentation rate based on the position of the radionuclide concentration peak in the sediment profile is common practice. Such studies, however, are focused on sediments and their dating exclusively and do not relate the radionuclide depth profile in bottom sediments to temporal changes in radioactive contamination of the water body. In our work, we use 137Cs depth distribution in bottom sediments to reconstruct activity concentrations in water as a function of time in lakes and ponds, which have not been attempted before.
The sediment profile formed since the accident shows how the particulate concentration of 137Cs in the water body changed with time, given the highest 137Cs concentration in the depth profile corresponds to its particulate concentration in the initial period after the accident, and 137Cs concentration in the top sediment layer represents the current particulate 137Cs concentration in the water column. Changes in the particulate 137Cs concentration with time can be reconstructed from the profile above the peak, given data on annual average sedimentation rate are available or, as a first approximation, assuming this parameter to be constant over the time after the accident [19,21].
Long-term dynamics of 137Cs concentrations in water bodies can be described using the earlier proposed semi-empirical diffusional model [44,45]. According to the model, for water bodies, where a major source of suspended material is the top layer of catchment soil, the long-term dynamics of 137Cs particulate concentration cp and dissolved concentration cd can be described by the following equations:
c p ( t ) = σ ρ π D e f f t e λ t = c p 0 e λ t t ;                 c p 0   = σ ρ π D e f f
c d ( t ) = σ ρ K d π D e f f t e λ t = c d 0 e λ t t ;       c d 0   = σ ρ K d π D e f f
where σ is the catchment averaged 137Cs deposition (Bq/m2); ρ is the catchment averaged bulk density of the topsoil layer (g/m3); Deff is the catchment averaged effective coefficient of 137Cs dispersion in the topsoil layer (m2/y); λ is the rate constant of 137Cs radioactive decay equal to 0.023 y−1; Kd is the 137Cs apparent distribution coefficient in the suspended sediment–water system in the water body (m3/g) and t is the time since the Chernobyl accident (y).
This model enables predicting particulate and dissolved 137Cs concentrations in lakes and ponds for the mid- and long-term phases after a nuclear accident, using, besides 137Cs deposition, two key physicochemical parameters of 137Cs dispersion and distribution in the sediment–water system. The particulate 137Cs concentration is determined by the effective dispersion coefficient Deff in the catchment topsoil, depending on 137Cs speciation, sorption, and fixation ability of catchment soil, and climatic conditions (e.g., mean annual rainfall, mean annual air temperature, etc.) [31,32,33,34,35,36], whereas the dissolved 137Cs concentration, along with Deff, is controlled by the distribution coefficient Kd in the sediment–water system [3,45].
The present study aims (1) to reconstruct 137Cs particulate concentrations in severely contaminated water bodies in the Chernobyl exclusion zone (ChEZ), using the 137Cs depth distributions in the bottom sediment cores collected; (2) to estimate time dependence of 137Cs apparent distribution coefficient in these water bodies; and (3) to test the applicability of semi-empirical diffusional model to describe long-term dynamics of particulate and dissolved 137Cs in heavily contaminated water bodies.

2. Materials and Methods

2.1. Study Sites

For study purposes, the three most heavily contaminated water bodies in the ChNPP exclusion zone were selected: Typical eutrophic oxbow lakes of the Pripyat River floodplain, namely, Glubokoe (left bank of the Pripyat River) and Azbuchin (right bank of the Pripyat River), and a man-made reservoir, the Chernobyl NPP cooling pond (Figure 1). Table 1 includes the main characteristics of the studied water bodies.
The soils in the studied catchments are mainly alluvial-soddy-meadow and soddy- weakly podzolic soils with a sandy easily permeable bedrock. Part of the Glubokoe catchment is occupied by man-made plantations of deciduous trees. The depth of groundwater occurrence is 1.5–2.0 m depending on the season since the lakes are hydraulically connected to the Pripyat River channel. Bottom sediments are made of black sandy mud, and a layer of dense sandy-gley parental C-subsoil occurs at the core bottom.

2.2. Sampling

The soil cores from Lakes Glubokoe and Azbuchin catchments 68 to 102 cm long were collected to determine 137Cs inventories using a DIK-110C liner soil sampler (DAIKI, Japan) with a plastic cylinder insert of 5 cm in diameter. The soil cores were sliced into 2 cm layers. Bottom sediment cores were collected in August 2018 using a gravity sampler designed by Ukrainian Hydrometeorological Institute (UHMI). Sampling was conducted at the deepmost places where sediments could potentially accumulate and where horizontal water flows are minimal. Depth was determined by echo sounding of the bottom using FishElite 480 (Eagle, USA). Water temperature and dissolved oxygen (DO) in water bodies were measured using submersible multitester U-52 (HORIBA, Japan). In the cooling pond (CP), the location of bottom sediment core sampling was tied to a small old floodplain no-name lake, and its coordinates were taken from a military topographic map from 1926, well before the construction of the CP.

2.3. Sample Analysis

The water samples were filtered in situ through sandwich-type Petryanov filters (with a pore size of 0.5 µm) to separate suspended material from solution [48]. Dissolved 137Cs was immobilized by two sequential cartridges of cellulose-based and iron hexacyanoferrate-impregnated ANFEZH sorbent (EKSORB Ltd., Ekaterinburg, Russia) [10,49,50]. Alternatively, the filtrate was collected into plastic containers and 1 mL of 6M nitric acid was added for direct determination of activity. Gamma spectrometry with GMX-40-LB (Ortec, USA) high purity germanium detector (HPGe) was used to determine 137Cs activity concentration in soil and bottom sediment samples, filtrate, and suspended material, as well as 241Am in the soil and bottom sediment samples [51]. Detector calibration was implemented using NIST-, IAEA-, and NPL UK-certified reference materials. Corrections were made for the effect of self-absorption of low energy g-rays within the sample matrix using mass-attenuation parameters determined by the method reported in [52], considering actual composition of the sediment matrix (CaCO3, mineral and organic matter). All measurements were performed in the analytical laboratories of the UHMI (Kyiv) and Ecocentre (Chernobyl). The reported uncertainty of analytical results, presented as expanded uncertainty calculated from combined standard uncertainty using a coverage factor k = 2 at level of confidence of 95%, did not exceed ±10%. Most contribution to combined standard uncertainty comes from spectral peak statistics, calibration curve fitting, and reported uncertainty of calibration standards.

3. Results

The characteristics of bottom sediment cores collected from the three water bodies for successive analysis are provided in Table 2. Depth distributions for 137Cs and 241Am in bottom sediments in the accumulation zones are shown in Figure 2. 137Cs and 241Am in the investigated water bodies are strongly bound by solid soil and sediment particles, and the values of their solid–liquid distribution coefficient in suspended matter–water system Kd > 104 L/kg [37].
As shown in Figure 2, the 137Cs and 241Am profiles have a pronounced sharp maximum from below. Presumably, the activity peak for these radionuclides was formed in the first year after the accident when radioactive particles fell out and settled on the bottom. Right below the peak, the137Cs and 241Am activity concentrations in the profile are about an order of magnitude lower, which suggests that the suspended material deposited on the bottom did not mix with the underlying layers of the bottom sediments, and the dispersion of radionuclides through interstitial water in the sediments is rather insignificant. Lack of mixing in the deep-water zones of the lakes was also supported by numerous measurements, showing the deficit of DO there, to the point of its total absence. In the absence of oxygen, vital activity of biota is minimized and as a result bioturbation, as one of bottom sediment mixing drivers, does not occur. We admit that horizontal redistribution of sediments is possible, to some extent, along the bottom surface after their sedimentation. This, however, will not change the general vertical profile of radionuclides formed over many years.
It should be noted that in the following discussion we use only data on 137Cs distribution in bottom sediments. Results of 241Am measurements and their comparison with 137Cs were provided exclusively to illustrate that the vertical distribution of 137Cs in bottom sediments is determined by settling of carrier particles. Absolute values of activity concentrations for these two radionuclides differ for more than one order of magnitude. Nevertheless, the profiles of 137Cs and 241Am in relative units appeared to be very similar. Both radionuclides are strongly bound by sediments for solute transport to play negligible role in their vertical distribution in bottom sediments, though 241Am is even more strongly bound by sediments than 137Cs [37]. In this context, vertical distributions of 137Cs in bottom sediment cores collected in 2018 may represent the time dependence of 137Cs activity concentrations in suspended sediments deposited on the bottom after the accident.

4. Discussion

4.1. Reconstruction of Long-Term Dynamics of Particulate 137Cs Activity Concentrations in Studied Water Bodies

The 137Cs activity concentration in the sediment core layers above the peak slowly declines up to the surface sediment layer, as can be seen from Figure 2, which reflects temporal changes in particulate concentrations in the water column after the accident. Some minor deviations can be noticed for Lake Azbuchin and CP, yet not contradicting the general trend. There are also secondary maxima in the 137Cs activity concentrations, which are likely to be associated with water level manipulation and other remediation activities, as well as changes in the ChNPP operational mode [18].
The obtained 137Cs core profiles provided a basis for reconstructing long-term dependence of its particulate activity concentration in the water column. This is especially important since throughout the years after the accident, this crucial characteristic of radioactive contamination was not monitored on a regular basis but measured only occasionally in selected water bodies within some projects [18,44,45,53].
For reconstruction, the whole 137Cs profile from the peak to the sediment surface is split into layers, representing sediments deposited on the bottom over a respective time interval. It can be assumed that the sediments accumulate evenly in a timewise manner, i.e., about the same amount of sediments depositing on the bottom each year. Even though this is an approximation, ample corroborating data can be found in the literature. For example, studies on bottom sediments dating in Brno dam reservoir (Czech Republic) for over almost 70 years (from 1939 to 2007) showed that the sedimentation rate there was quite stable, varying in a narrow range from 3.1 to 3.4 cm/y [43].
Given the differences in bottom sediment density with depth, it seems reasonable to use the dependence of 137Cs activity concentration on mass depth in kg/m2 rather than depth in cm. The mean annual sedimentation rates for the studied water bodies both in kg/m2y and in cm/y, calculated by the position of the 137Cs peak attributed to the first year after the accident (1986–1987), are presented in Table 2.
When reconstructing the time dependence of 137Cs activity in suspended sediments, we corrected for 137Cs radioactive decay over the time elapsed since the sediment deposition on the bottom. The 137Cs activity in the profile peak decreased by approximately a factor of two over 32 years since sediment deposition, given the half-life of 137Cs is 30.2 years. For decay correction, we multiplied the measured activity in the sediment layer, as of the sampling date in 2018 by e λ ( 2018 t ) , where t is the reconstructed year for the given sediment layer, and λ = 0.023 y−1 is the 137Cs radioactive decay rate constant. The decay corrected 137Cs profiles for the bottom sediments in the studied water bodies are shown in Figure 3 versus uncorrected profiles (i.e., the depth profiles of 137Cs activity concentrations as of the core sampling date).
The reconstructed time dependences of 137Cs particulate activity concentration in the three studied water bodies since the accident are shown in Figure 4. The significance of this data is that it seems to be the first and, so far, the only estimate of long-term dependence of 137Cs particulate concentration in the heavily contaminated water bodies of the ChNPP exclusion zone. Knowing 137Cs particulate concentrations is necessary not only for a better understanding of the radionuclide behavior in the soil–water system, but also for assessment of radionuclide transfer to biota and food chain migration.
The reconstructed data, in addition, can be used for testing the semi-empirical diffusional model (Equation (2)) accounting for dynamics of particulate 137Cs concentrations in water bodies [44,45]. The obtained data help to ascertain that the processes and mechanisms described by this model really occur in the studied water bodies and therefore the model can be used for prediction purposes. The 137Cs particulate concentrations as a function of time in the water bodies, calculated by the model at c p 0   = 3000 Bq∙(y)1/2g−1, are shown in Figure 4 (dashed line).
In the calculations of c p 0 , we used the 137Cs effective dispersion coefficient in soil 0.1 cm2/y, which corresponds to the lower bound of the range of Deff values in the ChEZ soils [33,36,54]. The low value of Deff was taken since 137Cs deposited on these catchments was incorporated in persistent fuel particles characterized by slow disintegration and low mobility [18,55,56].

4.2. Reconstruction of Long-Term Dynamics of Apparent 137Cs Distribution Coefficient Kd (137Cs) in Studied Water Bodies

Based on the reconstructed 137Cs particulate concentrations and dissolved 137Cs concentrations obtained by monitoring [17,18] we estimated Kd for the time period from 1986 to 2018. The results for the three water bodies are shown in Figure 5. Earlier studies of the Chernobyl rivers revealed no time trend in the annual average Kd (137Cs) in the suspended matter–water system after the accident [44,45]. As shown in Figure 5, this is true for Lakes Glubokoe and Azbuchin, for which the multi-year average values for Kd (137Cs) are (3.5 ± 0.7) × 104 L/kg and (5.5 ± 2.1) × 104 L/kg, respectively. However, the picture is different for the CP, in which the apparent Kd (137Cs) increased from 5.5 × 104 L/kg in 1986–87 to 3 × 105 L/kg in 1997, and reached a plateau afterwards.
The obtained Kd (137Cs) time dependence for the cooling pond is most likely to be due to CP maintenance features. The mode of ChNPP operations changed significantly and consequently the circulation, thermal, hydrological, and hydro-chemical conditions in CP changed too. In the years following the initial phase, the Kd (137Cs) value in the suspended matter–water system of CP was approximately an order of magnitude higher than those typical of other water bodies in the ChNPP zone [18].
With Kd (137Cs) time dependence reconstructed, it became possible to calculate temporal changes in dissolved 137Cs in the studied water bodies using the semi-empirical diffusional model (Equation (3)). Figure 6 shows available monitoring data on dissolved 137Cs activity concentrations over time in the studied water bodies [17,18] versus calculations by the diffusional model. In model calculations of the dissolved 137Cs concentrations, Kd (137Cs) was taken to be constant and equal to 3.5 × 104 L/kg for Lake Glubokoe and 5.5 × 104 L/kg for Lake Azbuchin. For the CP, long-term monitoring data show an abnormally quick reduction in the dissolved 137Cs concentration from 1986 to 1997 [18], which is possibly associated with a sharp increase in 137Cs apparent distribution coefficient, as supported by Figure 5. When modeling the dissolved 137Cs concentration time dependence, we therefore assume Kd (137Cs) in CP to grow from 5.5 × 104 L/kg (the value typical for Lake Azbuchin located nearby and groundwater connected with CP) in 1986–1987 to 3.0 × 105 L/kg in 1997, remaining constant since then. The results of our calculations of dissolved 137Cs activity concentrations time dependences by the diffusional model are consistent with the available monitoring data (Figure 6).
We admit that certain assumptions were used in our reconstruction of long-term dynamics of 137Cs concentrations, leading to uncertainty in results. Specifically, it is required that sediments settling on the bottom should not mix in the course of sediment profile formation throughout the time, and the other condition is that the radionuclide be strongly bound to sediments. In using the proposed approach, it is essential to make sure that these conditions are satisfied. Even though such requirements are constraints of the method, evidence from experience suggests that it is also so in reality. It is also worth pointing out that our study is concerned with temporal trends of sedimentation based on using mean annual values, which results in smoothing over variations in sedimentation rate within a specific year. Actually, the effect of variation smoothing was demonstrated for a number of lakes across the world with relatively non-uniform distribution of precipitation within a year [40,43,57]. We supposed that the same would be true for ChEZ water bodies under study and the obtained reconstruction results were not contrary to what we expected.
Strictly speaking, the accuracy of the proposed reconstruction method can be improved in the future by accounting for annual precipitation variations from year to year. For the ChEZ, however, annual precipitation generally differs from the mean annual precipitation by not more than 15–20%, and therefore the assumption in our reconstruction that the sedimentation rate does not change much from year to year seems very reasonable. Parameterization of mean annual sedimentation rate through rainfall erosivity factor R, based on Universal Soil Loss Equation (USLE) [58], can help to obtain an even more realistic sedimentation history. Use of such a parameterization of sedimentation rate time dependence would reduce uncertainty in reconstruction results. At this stage it is important for us to set out the concept underlying our method, and in future it can be further developed and improved.
The proposed method, when used jointly with the diffusional model, enables not only reconstructing dynamics of contamination in the past, but also predicting future trends in contamination.

5. Conclusions

The 137Cs depth distribution in bottom sediment cores collected more than 30 years after the Chernobyl accident in deep parts of heavily contaminated Lakes Glubokoe and Azbuchin and the cooling pond was used to reconstruct particulate 137Cs concentrations as a function of time. To our knowledge, the obtained estimates of particulate 137Cs concentrations and their temporal trends in these heavily contaminated water bodies are the first of its kind for the Chernobyl exclusion zone. Knowing 137Cs particulate concentrations is necessary not only for better understanding and prediction of the radionuclide behavior in the soil–water system, but also for assessment of radionuclide transfer to biota and food chain migration.
Reconstruction of temporal changes in particulate 137Cs concentration was based on the understanding that each bottom sediment layer can be taken as representing suspended sediments deposited on the bottom during a certain time interval after the accident. Just a single sediment core collected in the deep–water accumulation zone of lake or pond many years after a nuclear accident appears to be sufficient to retrieve long-term dynamics of contamination.
The apparent distribution coefficient Kd (137Cs) in the suspended matter–water system, derived using reconstructed 137Cs particulate concentrations and available monitoring data for dissolved 137Cs, was found to remain quite constant with time for Lakes Glubokoe and Azbuchin. On the other hand, Kd (137Cs) in the cooling pond increased from 5.5 × 104 to 3.0 × 105 L∙kg−1 during the first 10 years after the accident, but afterwards remained constant until very recently. This means that in the long-term 137Cs mobility and bioavailability in Lakes Glubokoe and Azbuchin can be expected to be much higher than in the cooling pond.
The proposed method enables, based on cesium distribution profile in bottom sediments, reconstructing temporal changes in water-body radioactive contamination for the years following the accident, which is particularly important when regular monitoring data are not available. We admit that the proposed method involves certain assumptions leading to uncertainty in results. It is required that, as the sediment column is formed, sediments settling on the bottom in different time intervals should not mix, and the other condition is that the radionuclide is strongly bound to sediments. These assumptions, however, seem to be quite realistic. Even though these requirements are constraints on the method, it is important that they are satisfied in performing analysis and calculations.

Author Contributions

Conceptualization, A.K. and G.L.; methodology, A.K. and G.L.; software, H.L.; validation, A.K., G.L. and V.P.; formal analysis, A.K.; investigation, H.D., K.K., Y.I. and D.S.; resources, K.N. and S.K.; data curation, A.K. and G.L.; writing—original draft preparation, A.K.; writing—review and editing, G.L. and Y.I.; visualization, H.L.; supervision, K.N. and S.K.; project administration, Y.I.; funding acquisition, K.N. and A.K. All authors have read and agreed to the published version of the manuscript.

Funding

This research was partially funded by the Science and Technology Research Partnership for Sustainable Development, the Japan Science and Technology Agency/Japan International Cooperation Agency (SATREPS), grant number JPMJSA1603; the Japan Society for the Promotion of Science, Grant-in-aid for Scientific Research (KAKENHI B), grant number 18H03389; and by the Environment Research and Technology Development Fund of the Environmental Restoration and Conservation Agency of Japan, grant number JPMEERF20211R03.

Institutional Review Board Statement

Not applicable.

Informed Consent Statement

Not applicable.

Data Availability Statement

The data presented in this study are available on request from the corresponding author.

Acknowledgments

The authors are grateful to Dyvak T.I. and Derkach A.N. from UHMI for the analytical support.

Conflicts of Interest

The authors declare no conflict of interest. The funders had no role in the design of the study; in the collection, analyses, or interpretation of data; in the writing of the manuscript, or in the decision to publish the results.

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Figure 1. Location of the studied water bodies in the Chernobyl exclusion zone on the map of land use: 1—Lake Glubokoe; 2—Lake Azbuchin; 3—Chernobyl NPP cooling pond.
Figure 1. Location of the studied water bodies in the Chernobyl exclusion zone on the map of land use: 1—Lake Glubokoe; 2—Lake Azbuchin; 3—Chernobyl NPP cooling pond.
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Figure 2. 137Cs (●) and 241Am () depth distributions in the bottom sediment cores collected in the studied water bodies: (a)—Lake Glubokoe, (b)—Lake Azbuchin, (c)—Chernobyl NPP cooling pond.
Figure 2. 137Cs (●) and 241Am () depth distributions in the bottom sediment cores collected in the studied water bodies: (a)—Lake Glubokoe, (b)—Lake Azbuchin, (c)—Chernobyl NPP cooling pond.
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Figure 3. 137Cs activity concentration profiles corrected for radioactive decay over the time since deposition as a function of mass depth of bottom sediments versus uncorrected profiles, as of the sampling date in 2018.
Figure 3. 137Cs activity concentration profiles corrected for radioactive decay over the time since deposition as a function of mass depth of bottom sediments versus uncorrected profiles, as of the sampling date in 2018.
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Figure 4. Time dependence of particulate 137Cs activity concentrations in Lakes Glubokoe, Lake Azbuchin, and Cooling Pond after the accident in 1986, back calculated from the 137Cs depth distribution in the bottom sediments collected in 2018 in deep-water zones. Dashed line—calculation by the semiempirical diffusional model (Equation (2)) at c p 0   = 3000 Bq∙(y)1/2g−1.
Figure 4. Time dependence of particulate 137Cs activity concentrations in Lakes Glubokoe, Lake Azbuchin, and Cooling Pond after the accident in 1986, back calculated from the 137Cs depth distribution in the bottom sediments collected in 2018 in deep-water zones. Dashed line—calculation by the semiempirical diffusional model (Equation (2)) at c p 0   = 3000 Bq∙(y)1/2g−1.
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Figure 5. Time changes in the 137Cs apparent distribution coefficient Kd (137Cs) estimated from reconstructed particulate 137Cs concentrations and data of long-term monitoring of dissolved 137Cs in the studied water bodies.
Figure 5. Time changes in the 137Cs apparent distribution coefficient Kd (137Cs) estimated from reconstructed particulate 137Cs concentrations and data of long-term monitoring of dissolved 137Cs in the studied water bodies.
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Figure 6. Time dependence of annual averaged monitoring data on dissolved 137Cs activity concentrations in the studied water bodies (black circles) versus calculations by the semiempirical diffusional model (dashed lines): (a)—Lake Glubokoe, (b)—Lake Azbuchin, and (c)—ChNPP cooling pond. In model calculations Kd (137Cs) was taken to be constant and equal to 3.5 × 104 L/kg for Lake Glubokoe and 5.5 × 104 L/kg for Lake Azbuchin. Kd (137Cs) in the cooling pond was assumed to increase from 5.5 × 104 L/kg in 1986–1987 to 3.0 × 105 L/kg in 1997, remaining constant since then. Deff was taken to be 0.1 cm2/y for all three water bodies.
Figure 6. Time dependence of annual averaged monitoring data on dissolved 137Cs activity concentrations in the studied water bodies (black circles) versus calculations by the semiempirical diffusional model (dashed lines): (a)—Lake Glubokoe, (b)—Lake Azbuchin, and (c)—ChNPP cooling pond. In model calculations Kd (137Cs) was taken to be constant and equal to 3.5 × 104 L/kg for Lake Glubokoe and 5.5 × 104 L/kg for Lake Azbuchin. Kd (137Cs) in the cooling pond was assumed to increase from 5.5 × 104 L/kg in 1986–1987 to 3.0 × 105 L/kg in 1997, remaining constant since then. Deff was taken to be 0.1 cm2/y for all three water bodies.
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Table 1. Characteristics of the studied water bodies in the Chernobyl exclusion zone.
Table 1. Characteristics of the studied water bodies in the Chernobyl exclusion zone.
Water BodyLake GlubokoeLake AzbuchinCooling Pond
Coordinates51.444° N 30.065° E51.406° N 30.117° E51.354° N 30.166° E
137Cs mean deposition, MBq/m211 ± 5 a7.6 ± 3.2 a4.2 ± 1.3 b
Water surface area, km20.170.2322.6
Maximum depth, m7.15.517.0
Average depth, m3.02.56.2
Reference[46][47][18]
a Data of this work for 2018; b Middle part (dyke).
Table 2. Characterization of the bottom sediment cores.
Table 2. Characterization of the bottom sediment cores.
Water BodyLake GlubokoeLake AzbuchinCooling Pond
Sampling date25.07.201824.07.201805.06.2018
Sampling location coordinatesN51.34583 E30.16242N51.4057 E30.1119N51.3458 E30.1624
Depth at sampling location, m6.34.28.6
Core length, cm416268
Mean sedimentation rate a,
kg/m2y (cm/y)
1.65 (1.1)1.2 (1.4)3.2 (1.7)
137Cs inventory b, MBq/m218 ± 3.617 ± 3.463 ± 12
241Am inventory b, MBq/m20.8 ± 0.160.5 ± 0.11.7 ± 0.35
a Determined by position of the 137Cs peak attributed to the first year after the accident 1986–1987; b Expanded uncertainty at coverage factor k = 2 and level of confidence of 95%.
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Konoplev, A.; Laptev, G.; Igarashi, Y.; Derkach, H.; Protsak, V.; Lisovyi, H.; Korychenskyi, K.; Kirieiev, S.; Samoilov, D.; Nanba, K. Reconstruction of the Long-Term Dynamics of Particulate Concentrations and Solid–Liquid Distribution of Radiocesium in Three Severely Contaminated Water Bodies of the Chernobyl Exclusion Zone Based on Current Depth Distribution in Bottom Sediments. Land 2022, 11, 29. https://doi.org/10.3390/land11010029

AMA Style

Konoplev A, Laptev G, Igarashi Y, Derkach H, Protsak V, Lisovyi H, Korychenskyi K, Kirieiev S, Samoilov D, Nanba K. Reconstruction of the Long-Term Dynamics of Particulate Concentrations and Solid–Liquid Distribution of Radiocesium in Three Severely Contaminated Water Bodies of the Chernobyl Exclusion Zone Based on Current Depth Distribution in Bottom Sediments. Land. 2022; 11(1):29. https://doi.org/10.3390/land11010029

Chicago/Turabian Style

Konoplev, Alexei, Gennady Laptev, Yasunori Igarashi, Hrigoryi Derkach, Valentin Protsak, Hlib Lisovyi, Kyrylo Korychenskyi, Serhii Kirieiev, Dmitry Samoilov, and Kenji Nanba. 2022. "Reconstruction of the Long-Term Dynamics of Particulate Concentrations and Solid–Liquid Distribution of Radiocesium in Three Severely Contaminated Water Bodies of the Chernobyl Exclusion Zone Based on Current Depth Distribution in Bottom Sediments" Land 11, no. 1: 29. https://doi.org/10.3390/land11010029

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