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Environmental Monitoring of Radionuclide Pollutants in Black Sea Sediments A

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Environmental Monitoring of Radionuclide Pollutants in Black Sea Sediments A 1 ENVIRONMENTAL MONITORING OF RADIONUCLIDE POLLUTANTS IN BLACK SEA SEDIMENTS A. STREZOV, Tz. NONOVA, T. STOILOVA Bulgarian Academy of Sciences Institute for Nuclear Research and Nuclear Energy Sofia 1784, blvd. Tzarigradsko shosse № 72 ABSTRACT Sediment samples from the Bulgarian Black Sea shelf were analyzed for radionuclide content in the period 1991 - 2002 from 26 locations. Sediment samples were taken also from greater depths – 56, 109, 130, 150 and 2040 m and data were compared with near-shore ones. The distribution of anthropogenic 137Cs, 134Cs and natural 238U, 232Th, 226Ra radionuclide content in Black Sea bottom sediments - slime, silt and sandy is measured by low level gamma spectroscopy. The obtained data show that radionuclides concentrations strongly depend on the sediment nature - results for sandy sediments are within close range, while higher concentrations are measured in slime and silt shelf samples. 137Cs is found to be strongly bound by slime sediments and also disequilibrium between natural nuclides is observed. The deep sediment matrixes seem to accumulate higher radionuclide concentrations compared to the near-shore ones. The dependencies of radionuclide concentration on sampling year and location are evaluated showing that natural nuclides in slime sediments are considerably constant during the years, while Cs content decreases while the opposite trend is observed for silt sediments. Nuclide content is rather constant in sand sediments that can be attributed to the nature of sediment matrix. Statistical treatment of the obtained data is performed showing correlations between sediment nature depending on sampling year and location. A comprehensive database for the nuclide concentration values for near-shore and deep-sea sediments is created to enable the modeling of radionuclide transfer, accumulation and influence on the Black Sea marine ecosystems. INTRODUCTION Radionuclides are part of hazardous anthropogenic pollutants in the Black Sea marine ecosystems. After the Chernobyl accident a considerable increase occurred in nuclides quantity in the environment [1, 2, 3, 4, 5, 6]. The Black Sea being near to the reactor accepted a great quantity of direct atmospheric radionuclide fallout. Additionally, Chernobyl nuclides entered the marine environment in the northwest corner of the Black Sea carried by the big rivers - Dnyepr, Dnester, Danube [7] plus massive amounts of industrial effluents. The association of radionuclides with sediments in coastal and estuary areas makes sediments a large reservoir for radionuclides affecting significantly specific marine ecosystems. As the seawater is constantly in contact with organic and inorganic matter from sea shelf, the first necessary step in the estimation of radionuclide migration is the measurement of radionuclide content in sea bed sediments and setting up a radioecological data base. The coast of Bulgaria, extending 270 km is mainly soft sedimentary limestone or sandstone, overlaid in many areas with beach or wind-blown sand. In the northern part, suspended material from the Danube delta has settled, carrying a lot of intertidal mud. A monitoring program has been utilized since 1991 measuring technogenic and natural radionuclide content in marine environmental samples from the Bulgarian Black Sea coast. The aim of the present work is to provide data for nuclide accumulation in Black Sea bottom sediments in the period 1991 2002 and compare their concentration variations along the whole coast. 2 MATERIALS AND METHODS Near-shore sediment samples from 26 reference locations (7-15 m depth,) and sediments from eight deep-sea marine sites (150-2040 m depth) were collected in the period 1991 – 2003 at along the Bulgarian Black Sea coast (Fig. 1) from the north - Romanian border (Duran Kulak) to the South - Turkish border (Rezovo). ROMANIA ↑ Durankulak • N Shabla • Tulenovo Kamen Briag •• Kavarna • •Kaliakra Balchik••Tuzlata Albena • • Golden Sands Varna • Kamchia • BLACK SEA Bjala • Sunny Beach • • Nessebar Pomorie • Burgas • Sozopol Chernomoretz • • Primorsko • • Tzarevo Ahtopol • Sinemoretz Rezovo•• TURKEY Figure 1. Diagram of Bulgarian Black Sea coast (sampling location). Near-shore samples were collected from the upper sediment layer (approximately 1 m2 up to 2-3 cm depth, acquiring about 2-3 kg sediment), while deep sediment samples were taken by a submarine belonging to the Oceanographic Institute in Varna. All samples were dried at 105oC to constant weight and homogenized. One liter of every sediment sample was enclosed hermetically in Marinelli containers for a period of at least three weeks before the γ spectrometry measurements. Technogenic and natural radionuclide content was determined by low level gamma spectroscopy - the γ spectrometry measurements were carried out using HPGe detector (Ortec type) with 35 % counting efficiency and energy resolution 1.8 KeV (at 1332 KeV) with measuring time between 12 - 48 hours. The evaluation of natural nuclides was done using the recommendations of Murray [8]. The lowest limit of detection (LLD) for the different nuclides in sediments assuming 24 hours measurement time are estimated as follows: 137Cs and 134Cs - 0.1 Bq; 238U - 3 Bq/kg; 232Th and 226Ra - 0.2 Bq. RESULTS AND DISCUSSION The obtained results for Black Sea sediment samples show that radionuclide concentrations strongly depend on the nature of the sea bed sediments, because the data 3 obtained for sand sediments are within a close range while those for silt and slime ones are higher and vary to a much greater extent. The nuclide content in sand sediment samples from 15 locations along the Black Sea coast are given on Fig. 2. Figure 2. Nuclide content in sand sediments along the Bulgarian coast The beach matrix and the near shore sediments at these locations are mainly sand and 137Cs data are within a close range: Sunny Beach - 3.2 - 5.6 Bq/kg, Golden Sands – 1.8 – 6.9 Bq/kg, Albena - 3.4 – 7.3 Bq/kg, Tulenovo 4.0-7.1 Bq/kg, Kamen Briag - 4.4-6.6 Bq/kg, Balchik - 4.6 - 7.8 Bq/kg, Primorsko 4.0 - 5.6 Bq/kg, Sinemoretz – 3.6 – 7.8 Bq/kg. It should be noted that all sand sediment data fall within 8 Bq/kg level except Albena, Golden sands, Ravda, Burgas and Sozopol where nuclide content is higher. The highest measured cesium content (Fig. 3) on the Bulgarian Black Sea coast is at the north locations with slime sediments – Kaliakra (mean 89 Bq/kg), Kavarna (mean 30 Bq/kg) and central Ravda - 2 (mean 65 Bq/kg). Figure 3. Nuclide content in silt and slime sediments along the Bulgarian coast 4 The increase in 137Cs concentration in slime sediments and sorption on fine particles leads to cesium scavenging and occurrence at greater depths, which can be explained by physico-chemical interaction processes of the soluble Cs forms with the surrounding media. In sand and sandy sediments Cs content does not change greatly while the process of 137Cs accumulation is observed in slime and silt sediments. Due to such a process, sea bottom sediments play a major role in radionuclide redistribution between different components in the ecosystems, which change the concentration of 137Cs in the water as radiocaesium is accumulated more in the sediments. The observed dependence of radionuclide content on sediment type is valid also for the natural nuclides in sediments. The lowest concentrations of natural nuclides in sand sediments are at the north locations – Duran Kulak, Shabla, Tulenovo and Kamen briag 238U (4.0 - 10) Bq/kg, 232Th (3.4 - 10) Bq/kg, and 226Ra (3.6 - 9) Bq/kg as well as Primorsko and Sunny beach 238U (3 – 8) Bq/kg, 232Th (4.4 - 8) Bq/kg, and 226Ra (3.5 – 6.2) Bq/kg (Fig 2 and 3). The highest values for natural nuclides content (similarly to Cs) are obtained for the slime sediments - the obtained results for 238U vary in different years from 238U-(5 - 50) Bq/kg, 232Th - (4.0 - 35 Bq/kg), 226Ra - (9 - 50 Bq/kg). The mean values of 238U, 232Th and 226Ra specific activities for slime sampling locations are presented on Fig. 3 and these values show the maximum natural nuclide content at the Bulgarian Black Sea coast. There is one exception at Rossenetz where the operation of near-by copper mine led to the contamination of the surrounding environment, including the river and the sea bay with radionuclides from 238U series (238U – up to 2300 Bk/kg, 226Ra up to 5200 Bq/kg). The obtained values for silt sediments are between sand and slime ones with exception of Bjala, whose values 238U (14 - 77 Bq/kg); 232Th (12- 110 Bq/kg); 226Ra (10 - 77 Bq/kg) are the highest from the silt and slime locations. The data on Fig. 3 show that all natural nuclide content in slime sediments varies around 30 Bq/kg (except 232Th at Kavarna) showing some uniformity of natural nuclide concentrations along the whole coast. The radionuclide content variations during the investigation period 1991 – 2002 was done by taking only the most upper part of the bottom layers and away from the influence of the surf. It has been estimated that for sand sediments, the changes during different years are small (Fig. 4) and the nuclide concentration variations are within close limits. Figure 4. Nuclide content in sand sediments during the period 1991 – 2002 The variation of Cs content during the years shows a weak decrease with time, which can be attributed to the sinking of Cs nuclides in the sediments and also due to the more 5 strongly bounding with the sediment matrix especially in slime sediments. It is clear that sorption behavior of Cs is linked with the types of minerals that form the sediment nature and the probability of Cs to enter the crystalline structure of sediment matrix. The mean nuclide content in sand sediments during different years is considerably low and in a narrow range: for 238U 10 – 11 Bq/kg, in the period 1991 – 1999 while in the next years the content is lower 6 – 8 Bq/kg.
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