Natural attenuation processes control groundwater contamination in the Chernobyl exclusion zone: evidence from 35 years of radiological monitoring.

The Chernobyl Exclusion Zone (CEZ) contains the vast majority of radionuclides released by the accident in nuclear fuel particle form. We present and analyze groundwater measurements collected from the monitoring network in CEZ covering key aquifers over 35 years since the accident. These new data, together with a comprehensive analysis of historical data shows that 90Sr remains mobile in the subsurface environment, while groundwater concentrations of 137Cs, Pu isotopes and 241Am are relatively low, and are not of radiological concern. During the last two decades, 90Sr and 137Cs levels have declined or remained stable over time in the majority of monitoring locations. This is due to natural attenuation driven by gradual exhaustion of the fuel particle source, geochemical evolution of groundwater downstream from waste dumps and radionuclide retention in surface soil due to absorption and bio-cycling. Decommissioning of the cooling pond and construction of the 'New safe confinement' over Unit 4 (damaged reactor) also favored better protection of groundwater close to the Chernobyl plant site. Data from confined and unconfined aquifers, as well as rivers, evidence low radiological risks from groundwater contamination both outside the CEZ and to onsite "self-settlers". Though several groundwater contamination "hot spots" remain in the vicinity of Unit 4, "Red Forest" waste trenches and surface water bodies with contaminated bottom sediments, the findings of this study support a monitored natural attenuation approach to groundwater management in the CEZ.

Simulating dissolved 90Sr concentrations within a small catchment in the Chernobyl Exclusion Zone using a parametric hydrochemical model.

Strontium-90 (90Sr) is the major long-lived radionuclide derived from the Chernobyl accident, and is still being detected in the heavily contaminated catchments of the Chernobyl Exclusion Zone. This study examines the long-term decrease in the dissolved-phase 90Sr concentration and the concentration-discharge (90Sr-Q) relationship in stream water since the accident. We show that the slow decline in 90Sr follows a double-exponential function, and that there is a clear relationship between 90Sr and Q. This study is the first to reveal that the log(90Sr)-log(Q) slope has been gradually decreasing since the accident. This trend persists after decay correction. Thus, it is not caused by the physical decay of 90Sr and environmental diffusion, but implies that the concentration formation processes in stream water have been changing over a long period. We propose a hydrochemical model to explain the time-dependency of the 90Sr-Q relationship. This paper presents a mathematical implementation of the new concept and describes the model assumptions. Our model accurately represents both the long-term 90Sr trend in stream water and the time-dependency of the 90Sr-Q relationship. Although this paper considers a small catchment in Chernobyl, the conceptual model is shown to be applicable to other accidental releases of radionuclides.

Solid-liquid distribution coefficients (Kd-s) of geological deposits at the Chernobyl Nuclear Power Plant site with respect to Sr, Cs and Pu radionuclides: A short review.

A review is presented of data on solid-liquid distribution coefficients (Kd-s) of the main radiologically important radionuclides of the Chernobyl release within geological deposits at the Chernobyl Nuclear Power Plant (ChNPP) Site. The Kd values for Sr, Cs and Pu for Quaternary sandy deposits that form sedimentary cover at Chernobyl fall within the range of parameters reported in international sorption databases. In agreement with general knowledge on radionuclide geochemical behavior and affinity to soils, Kd-s increase in the sequence: Sr < Cs < Pu. Alluvial and fluvioglacial sandy deposits are characterized by larger Kd values then deposits of eolian genesis due to higher content of clay minerals in fine fractions. For Sr, laboratory batch tests have given Kd values that are in a reasonable agreement with in situ measurements. At the same time, the 90Sr Kd-s obtained from groundwater transport model calibrations were noticeably lower than experimentally determined values, thus showing potential limitations of the Kd-approach. Monitoring data on mobility of 90Sr, 137Cs and 239,240Pu in groundwater in the Chernobyl zone on a whole are consistent with the radionuclide Kd-s summarized in this article. The highest concentrations in groundwater (based on data for 2012-2014) were observed for 90Sr, while orders of magnitude lower concentrations were observed for 137Cs and 239,240Pu. At the same time, detection of 137Cs and 239,240Pu in groundwater at sites with a relatively deep groundwater table suggests the possibility of facilitated transport of small amounts of these radionuclides in the form of non-retarded colloids or complexes.

High (36)Cl/Cl ratios in Chernobyl groundwater.

After the explosion of the Chernobyl Nuclear Power Plant in April 1986, contaminated material was buried in shallow trenches within the exclusion zone. A (90)Sr plume was evidenced downgradient of one of these trenches, trench T22. Due to its conservative properties, (36)Cl is investigated here as a potential tracer to determine the maximal extent of the contamination plume from the trench in groundwater. (36)Cl/Cl ratios measured in groundwater, trench soil water and leaf leachates are 1-5 orders of magnitude higher than the theoretical natural (36)Cl/Cl ratio. This contamination occurred after the Chernobyl explosion and currently persists. Trench T22 acts as an obvious modern point source of (36)Cl, however other sources have to be involved to explain such contamination. (36)Cl contamination of groundwater can be explained by dilution of trench soil water by uncontaminated water (rainwater or deep groundwater). With a plume extending further than that of (90)Sr, radionuclide which is impacted by retention and decay processes, (36)Cl can be considered as a suitable tracer of contamination from the trench in groundwater provided that modern release processes of (36)Cl from trench soil are better characterized.

The effective source area of 90Sr for a stream near Chernobyl, Ukraine.

Remediation of streams impacted by non-point source contaminants requires an understanding of both the areas within a watershed that are contributing contamination to streams and the pathways of contaminant migration to streams. From 1998 to 2002, we studied the migration of 90Sr in the Borschi watershed, a small (8.5 km2) catchment three km south of the Chernobyl Nuclear Power Plant, Ukraine. Fuel particles, distributed in a heterogeneous pattern across the watershed, are weathering and releasing 90Sr from the fuel matrix. Depletion of (90)Sr, evaluated in comparison to the immobile fission product europium-154, is occurring in the channel and wetland sediment. Channel sediments are uniformly depleted in 90Sr with depth. In wetland sediments, there is a zone of depletion in the top 10 cm and a zone of accumulation at depths from 10 to 25 cm. Estimates of 90Sr depletion are used to map the effective source area that has contributed (90)Sr loading to the main channel. The effective source area includes channel bottom sediments, a wetland in the central region of the watershed, and periodically flooded soils surrounding the wetland. The total depletion from the effective source area is estimated to be 36 +/- 7 x 10(10) Bq. Based on observations of stream flow rate and water quality in 1999-2001, the annual 90Sr removal rate from the watershed is estimated to be 1.4 +/-0.2 x 10(10) or 1.5% of the inventory per year. When extrapolated over a 15-year period following the Chernobyl accident, the last value is in reasonable agreement with the estimated depletion of the source area based on 90Sr/154Eu ratios. The 90Sr yearly leaching rate considering the whole watershed is 0.2% while the 90Sr leaching rate considering the effective source area is an order of magnitude higher. Most of the 90Sr release in the watershed has originated from an effective source area of 0.62 km2, or 7% of the watershed area.