What cooling pond sediments can reveal about 14C in nuclear power plant liquid effluents: Case study Lake Druksiai, Ignalina nuclear power plant cooling pond.

The vertical distribution of radiocarbon (14C) was examined in two bottom sediment cores, taken from Lake Druksiai which had been used as a cooling pond for the Ignalina nuclear power plant (INPP) with two RBMK type reactors. The aim of this work was to reconstruct 14C amounts in the lake ecosystem during an 8-year period after the INPP was closed, as any official monitoring of 14C in liquid releases from the INPP was not performed. The possibility of comparing the variation of the 14C specific activity in the corresponding layers of the same period of 3 different cores (one taken in 2013 and two in 2019) revealed the variability of the determined values of liquid radiocarbon discharges from the INPP into the lake. Cores taken in 2019 showed a permament14C release rate of 0.76±0.06 GBq/y all eight years after the closure of the INPP. The 14C release rate established from radiocarbon measurements in both cores did not differ by more than 0.8 GBq/y. However, including data from the core taken several years ago, the estimated radiocarbon release rate values varied within 1.3 GBq/y.

Analysis of the vertical distribution of 137Cs and 239,240Pu in waterlogged and non-boggy soils by the sequential extraction method.

Mobile capabilities of 137Cs, 239,240Pu and some stable element physicochemical forms were studied in soil layers at a depth of 6-8 cm (maximum concentrations of radionuclides) of non-boggy and waterlogged soil cores sampled on the shores of Lake Bedugnis (Lithuania). Soil samples were acidic with small amount of clay (muscovite). The radionuclide activity concentrations were about 2.5 times higher in non-boggy soil. It was explained by different conditions of deposition of radioactive fallout at these sampling sites and density of the soil samples. The value of the exchangeable fraction of radionuclides is shown to be an indicator of their migration capabilities in the soil. Under anaerobic conditions in waterlogged soil (stagnant pore water conditions) and due to the presence of clay admixture, ∼90% of 137Cs was concentrated in the residual fraction and its mobility was low. 239,240Pu was concentrated mainly in organic matter with rather large exchangeable fractions (∼9.6-∼13.9%). Under oxidizing conditions in non-boggy soil (dynamic pore water conditions in the case of rain), 239,240Pu was mostly concentrated in the oxide fraction. Its exchangeable fractions were less than those in waterlogged soil and, respectively, its mobility was lower. In non-boggy soils, exchangeable fractions of 137Cs were large and varied in the range of 10.1-12.2%, which indicated its high mobility. In the case, 137Cs adsorption by clay materials was reduced and its residual fraction did not exceed 71.3%. The obtained data show that in the area of Lake Bedugnis, the migration capabilities of 137Cs and 239,240Pu change in antiphase.

Impact of soil organic matter on Pu migration in five Lithuanian surface soils.

Pu distribution coefficient Kd variation was experimentally determined and examined in natural soil samples considering the type of soil, particle size, pH, the concentration of macroelements and organic matter content. This research was carried out with sand, silty sand, peat, clayey sand and clayey loam samples by applying 236Pu tracer in flow-through column tests. Due to relatively short contact time of 0.5-40 h the tests are considered as have not reached equilibrium state and represent the fast-moving contaminants retardation processes closer to field conditions. Every soil sample was fractionated into two particle size fractions: ≤0.25 mm and 0.25 ÷ 0.5 mm. Analysis revealed that Kd of Pu is higher for the smaller soil particle fraction (≤0.25 mm). The experimental study with 1.6, 4, 6 and 9 pH tracer solution revealed a tendency of elevated Kd when 4 pH and 6 pH solutions were applied, but obtained Kd values were not correlated with initial soil pH due to high buffering capacity of soils. This study shows a very significant influence (r = 0.98) of organic matter content on the Pu distribution coefficient. The Kd of Pu for the fine fraction of peat soil with high organic matter content (67%) reached maximum values of 6597 L/kg and 6200 L/kg when tracer solution was applied of pH = 4 and pH = 6, respectively. In comparison, the minimum Kd value of 3.9 L/kg was obtained for the coarse silty sand fraction with the lowest organic matter content of 1.3% at tracer pH = 1.6. A statistically reliable high correlations of r = 0.95 and 0.94 were also observed between Kd and specific soil elements Mg and Pb content in soils, respectively. The content of Fe in soils was significantly correlated (r = 0.67) with the Kd values of plutonium as well. However, the organic matter content in soils appeared to be the governing factor determining good correlations and causing the highest Kd of Pu values.

Distribution of radiocarbon in sediments of the cooling pond of RBMK type Ignalina Nuclear Power Plant in Lithuania.

The vertical distribution of radiocarbon (14C) was examined in the bottom sediment core, taken from Lake Druksiai, which has served as a cooling pond since 1983 for the 26 years of the Ignalina Nuclear Power Plant (INPP) operation using two RBMK-1500 reactors (Russian acronym for"Channelized Large Power Reactor"). 14C specific activity was measured in alkali-soluble and -insoluble fractions of the sediment layers. Complementary measurements of the 210Pb and 137Cs activity of the samples provided the possibility to evaluate the date of every layer formation, covering the 1947-2013 period. In addition, 14C distribution was examined in the scales of pelagic fish caught between 1980 and 2012. Our measurements reveal that, during the period 1947-1999, the radiocarbon specific activity in both fractions exhibits a parallel course with a difference of 5 ± 1 pMC (percent of modern carbon) being higher in alkali-soluble fraction, although 14C specific activity in both fractions increased by 11.4-13.6 pMC during the first 15 years of plant operation. However, during the 2000-2009 period, other than previously seen, a dissolved inorganic carbon (DIC) → aquatic primary producers → sediments 14C incorporation pattern occurred, as the radiocarbon specific activity difference between alkali-soluble and -insoluble fractions reached 94, 25, and 20 pMC in 2000, 2006, and 2008, respectively. Measurements in different sediment fractions allowed us to identify the unexpected organic nature of 14C contained in liquid effluences from the INPP in 2000-2009. The discrepancy between 14C specific activity in fish scales samples and DIC after 2000 also confirmed the possibility of organic 14C contamination. Possible reasons for this phenomenon might be industrial processes introduced at the INPP, such as the start of operation of the cementation facility for spent ion exchange resins, decontamination procedures, and various maintenance activities of reactor aging systems and equipment.

Experimental and modelling studies of radiocesium sorption/desorption processes in the fixed-bed moss column.

The experimental and modelling studies of the fixed-bed column filled with inanimate mosses Ptilium crista-castrensis containing background levels of 137Cs, flushed with the distilled water are presented. Fitting of the experimental results by Langmuir and Freundlich sorption models gave significant deviations. A more sophisticated two kinetic site model created for the case of non-equilibrium transport of the radiocesium solute through porous media was more suitable to describe the experimental data. It has been shown that theoretically the two site sorption model can be simplified to the conventional one kinetic site model with time dependent parameters. The radiocesium transport equation included the terms taking into account advection, dispersion and decay. General analytical solution was derived for two types of the border conditions: 1) when a constant flux of the material on the surface layer of the absorbent is known (i.e. a Cauchy type border condition); 2) a border condition with constant initial material concentrations. The mathematical solution was derived using the Laplace transformation method. In such a way, the obtained simulated profile of the radionuclide concentration distribution within the fixed-bed column with inanimate mosses showed the best-fitting to the experimental results.

Risk of hematological malignancies among Chernobyl liquidators.

A case-control study of hematological malignancies was conducted among Chernobyl liquidators (accident recovery workers) from Belarus, Russia and Baltic countries to assess the effect of low- to medium-dose protracted radiation exposures on the relative risk of these diseases. The study was nested within cohorts of liquidators who had worked around the Chernobyl plant in 1986-1987. A total of 117 cases [69 leukemia, 34 non-Hodgkin lymphoma (NHL) and 14 other malignancies of lymphoid and hematopoietic tissue] and 481 matched controls were included in the study. Individual dose to the bone marrow and uncertainties were estimated for each subject. The main analyses were restricted to 70 cases (40 leukemia, 20 NHL and 10 other) and their 287 matched controls with reliable information on work in the Chernobyl area. Most subjects received very low doses (median 13 mGy). For all diagnoses combined, a significantly elevated OR was seen at doses of 200 mGy and above. The excess relative risk (ERR) per 100 mGy was 0.60 [90% confidence interval (CI) -0.02, 2.35]. The corresponding estimate for leukemia excluding chronic lymphoid leukemia (CLL) was 0.50 (90% CI -0.38, 5.7). It is slightly higher than but statistically compatible with those estimated from A-bomb survivors and recent low-dose-rate studies. Although sensitivity analyses showed generally similar results, we cannot rule out the possibility that biases and uncertainties could have led to over- or underestimation of the risk in this study.

Risk of thyroid cancer among chernobyl liquidators.

After the Chernobyl accident in 1986, the "liquidators" or clean-up workers were among those who received the highest radiation doses to the thyroid from external radiation. Some were also exposed to radioiodines through inhalation or ingestion. A collaborative case-control study nested within cohorts of Belarusian, Russian and Baltic liquidators was conducted to evaluate the radiation-induced risk of thyroid cancer. The study included 107 cases and 423 controls. Individual doses to the thyroid from external radiation and from iodine-131 ((131)I) were estimated for each subject. Most subjects received low doses (median 69 mGy). A statistically significant dose-response relationship was found with total thyroid dose. The Excess Relative Risk (ERR) per 100 mGy was 0.38 [95% confidence interval (CI): 0.10, 1.09]. The risk estimates were similar when doses from (131)I and external radiation were considered separately, although for external radiation the ERR was not statistically significantly elevated. The ERR was similar for micro carcinomas and larger size tumors, and for tumors with and without lymph node involvement. Although recall bias and uncertainties in doses could have affected the magnitude of the risk estimates, the findings of this study contribute to a better characterization the risk of thyroid cancer after radiation exposure in adulthood.

Reconstruction of radiation doses in a case-control study of thyroid cancer following the Chernobyl accident.

A population-based case-control study of thyroid cancer was carried out in contaminated regions of Belarus and Russia among persons who were exposed during childhood and adolescence to fallout from the Chernobyl accident. For each study subject, individual thyroid doses were reconstructed for the following pathways of exposure: (1) intake of 131I via inhalation and ingestion; (2) intake of short-lived radioiodines (132I, 133I, and 135I) and radiotelluriums (131mTe, 132Te) via inhalation and ingestion; (3) external dose from radionuclides deposited on the ground; and (4) ingestion of 134Cs and 137Cs. A series of intercomparison exercises validated the models used for reconstruction of average doses to populations of specific age groups as well as of individual doses. Median thyroid doses from all factors for study subjects were estimated to be 0.37 and 0.034 Gy in Belarus and Russia, respectively. The highest individual thyroid doses among the subjects were 10.2 Gy in Belarus and 5.3 Gy in Russia. Iodine-131 intake was the main pathway for thyroid exposure. Estimated doses from short-lived radioiodines and radiotelluriums ranged up to 0.53 Gy. Reconstructed individual thyroid doses from external exposure ranged up to 0.1 Gy, while those from internal exposure due to ingested cesium did not exceed 0.05 Gy. The uncertainty of the reconstructed individual thyroid doses, characterized by the geometric standard deviation, varies from 1.7 to 4.0 with a median of 2.2.

Radrue method for reconstruction of external photon doses for Chernobyl liquidators in epidemiological studies.

Between 1986 and 1990, several hundred thousand workers, called "liquidators" or "clean-up workers," took part in decontamination and recovery activities within the 30-km zone around the Chernobyl nuclear power plant in Ukraine, where a major accident occurred in April 1986. The Chernobyl liquidators were mainly exposed to external ionizing radiation levels that depended primarily on their work locations and the time after the accident when the work was performed. Because individual doses were often monitored inadequately or were not monitored at all for the majority of liquidators, a new method of photon (i.e., gamma and x rays) dose assessment, called "RADRUE" (Realistic Analytical Dose Reconstruction with Uncertainty Estimation), was developed to obtain unbiased and reasonably accurate estimates for use in three epidemiologic studies of hematological malignancies and thyroid cancer among liquidators. The RADRUE program implements a time-and-motion dose-reconstruction method that is flexible and conceptually easy to understand. It includes a large exposure rate database and interpolation and extrapolation techniques to calculate exposure rates at places where liquidators lived and worked within approximately 70 km of the destroyed reactor. The RADRUE technique relies on data collected from subjects' interviews conducted by trained interviewers, and on expert dosimetrists to interpret the information and provide supplementary information, when necessary, based upon their own Chernobyl experience. The RADRUE technique was used to estimate doses from external irradiation, as well as uncertainties, to the bone marrow for 929 subjects and to the thyroid gland for 530 subjects enrolled in epidemiologic studies. Individual bone marrow dose estimates were found to range from less than one muGy to 3,300 mGy, with an arithmetic mean of 71 mGy. Individual thyroid dose estimates were lower and ranged from 20 muGy to 507 mGy, with an arithmetic mean of 29 mGy. The uncertainties, expressed in terms of geometric standard deviations, ranged from 1.1 to 5.8, with an arithmetic mean of 1.9.

Risk of thyroid cancer after exposure to 131I in childhood.

BACKGROUND: After the Chernobyl nuclear power plant accident in April 1986, a large increase in the incidence of childhood thyroid cancer was reported in contaminated areas. Most of the radiation exposure to the thyroid was from iodine isotopes, especially 131I. We carried out a population-based case-control study of thyroid cancer in Belarus and the Russian Federation to evaluate the risk of thyroid cancer after exposure to radioactive iodine in childhood and to investigate environmental and host factors that may modify this risk. METHODS: We studied 276 case patients with thyroid cancer through 1998 and 1300 matched control subjects, all aged younger than 15 years at the time of the accident. Individual doses were estimated for each subject based on their whereabouts and dietary habits at the time of the accident and in following days, weeks, and years; their likely stable iodine status at the time of the accident was also evaluated. Data were analyzed by conditional logistic regression using several different models. All statistical tests were two-sided. RESULTS: A strong dose-response relationship was observed between radiation dose to the thyroid received in childhood and thyroid cancer risk (P<.001). For a dose of 1 Gy, the estimated odds ratio of thyroid cancer varied from 5.5 (95% confidence interval [CI] = 3.1 to 9.5) to 8.4 (95% CI = 4.1 to 17.3), depending on the risk model. A linear dose-response relationship was observed up to 1.5-2 Gy. The risk of radiation-related thyroid cancer was three times higher in iodine-deficient areas (relative risk [RR]= 3.2, 95% CI = 1.9 to 5.5) than elsewhere. Administration of potassium iodide as a dietary supplement reduced this risk of radiation-related thyroid cancer by a factor of 3 (RR = 0.34, 95% CI = 0.1 to 0.9, for consumption of potassium iodide versus no consumption). CONCLUSION: Exposure to (131)I in childhood is associated with an increased risk of thyroid cancer. Both iodine deficiency and iodine supplementation appear to modify this risk. These results have important public health implications: stable iodine supplementation in iodine-deficient populations may substantially reduce the risk of thyroid cancer related to radioactive iodines in case of exposure to radioactive iodines in childhood that may occur after radiation accidents or during medical diagnostic and therapeutic procedures.