137Cs and plutonium isotopes accumulation/retention in bottom sediments and soil in Lithuania: A case study of the activity concentration of anthropogenic radionuclides and their provenance before the start of operation of the Belarusian Nuclear Power Plant (NPP).

Knowledge of the background activity concentrations of anthropogenic radionuclides before the start of operations of the new nuclear facilities in Belarus is of great value worldwide. Inland water bodies in Lithuania (specifically the Neris River, the Nemunas River and the Curonian Lagoon) are near the site of the Belarusian NPP under construction and, for this reason, sediments and flooded soils from these sensitive areas were analysed for radiocesium and plutonium isotopes (macrophytes were analysed only for 137Cs) in 2011-2012. The 137Cs and 239+240Pu activity concentrations in bottom sediments from the Nemunas River, sampled in 1995-1996 and re-calculated to the year 2016, were compared with those of 2011-2012. The obtained activity of 137Cs in bottom sediments of the Nemunas River and Curonian Lagoon varied from 1 Bq/kg to 47.0 Bq/kg. The activity of 137Cs in the tested soils ranged from 5.3 B g/kg to 32.9 Bq/kg. The 239+240Pu activity in bottom sediments of the studied sampling sites varied between 0.016 and 0.34 Bq/kg and in flooded soils from 0.064 to 0.55 Bq/kg. The 238Pu activity values were very low or lower than the detection limit. The activity of 137Cs in macrophytes varied from values lower than the detection limit to 6 Bq/kg. A strong positive linear correlation for bottom sediments was calculated between: 239+240Pu and total organic carbon (TOC), r = 0.86, p-value 0.01; 239+240Pu and silt, r = 0.80, p-value 0.029; 137Cs and silt, r = 0.78, p-value 0.04; and 137Cs and TOC, r = 0.85, p-value 0.015. The similar peculiarities of 137Cs and 239+240Pu accumulation in bottom sediments and flooded soil allow us to assume that 137Cs can be used as a tracer for 239+240Pu in the initial stage of searching for radionuclide accumulation zones. A remaining impact of the Chernobyl fallout in average comprised: in the Lower Nemunas River and Curonian Lagoon sediments - 51%, in the Middle Nemunas River -90% and in the floodplains of the Nemunas River - 59%, while the provenance of plutonium in studied bottom sediments and flooded soil was the global fallout.

The assessment of ionising radiation impact on the cooling pond freshwater ecosystem non-human biota from the Ignalina NPP operation beginning to shut down and initial decommissioning.

The radiological doses to non-human biota of freshwater ecosystem in the Ignalina NPP cooling pond - Lake Druksiai were evaluated for several cases including the plant's operation period and initial decommissioning activities, using the ERICA 1.2 code with IAEA SRS-19 models integrated approach and tool. Among the Lake Druksiai freshwater ecosystem reference organisms investigated the highest exposure dose rate was determined for bottom fauna - benthic organisms (mollusc-bivalves, crustaceans, mollusc-gastropods, insect larvae), and among the other reference organisms - for vascular plants. The mean and maximum total dose rate values due to anthropogenic radionuclide ionising radiation impact in all investigated cases were lower than the ERICA screening dose rate value of 10 µGy/h. The main exposure of reference organisms as a result of Ignalina NPP former effluent to Lake Druksiai is due to ionizing radiation of radionuclides (60)Co and (137)Cs, of predicted releases to Lake Druksiai during initial decommissioning period - due to radionuclides (60)Co, (134)Cs and (137)Cs, and as a result of predicted releases to Lake Druksiai from low- and intermediate-level short-lived radioactive waste disposal site in 30-100 year period - due to radionuclides (99)Tc and (3)H. The risk quotient expected values in all investigated cases were <1, and therefore the risk to non-human biota can be considered negligible with the exception of a conservative risk quotient for insect larvae. Radiological protection of non-human biota in Lake Druksiai, the Ignalina NPP cooling pond, is both feasible and acceptable.

Anthropogenic radionuclide fluxes and distribution in bottom sediments of the cooling basin of the Ignalina Nuclear Power Plant.

Based on γ-ray emitting artificial radionuclide spectrometric measurements, an assessment of areal and vertical distribution of (137)Cs, (60)Co and (54)Mn activity concentrations in bottom sediments of Lake Druksiai was performed. Samples of bottom sediments from seven monitoring stations within the cooling basin were collected in 1988-1996 and 2007-2010 (in July-August). For radionuclide areal distribution analysis, samples from the surface 0-5 cm layer were used. Multi sample cores sliced 2 cm, 3 cm or 5 cm thick were used to study the vertical distribution of radionuclides. The lowest (137)Cs activity concentrations were obtained for two stations that were situated close to channels with radionuclide discharges, but with sediments that had a significantly smaller fraction of organic matter related to finest particles and consequently smaller radionuclide retention potential. The (137)Cs activity concentration was distributed quite evenly in the bottom sediments from other investigated monitoring stations. The highest (137)Cs activity concentrations in the bottom sediments of Lake Druksiai were measured in the period of 1988-1989; in 1990, the (137)Cs activity concentrations slightly decreased and they varied insignificantly over the investigation period. The obtained (238)Pu/(239,240)Pu activity ratio values in the bottom sediments of Lake Druksiai represented radioactive pollution with plutonium from nuclear weapon tests. Higher (60)Co and (54)Mn activity concentrations were observed in the monitoring stations that were close to the impact zones of the technical water outlet channel and industrial rain drainage system channel. (60)Co and (54)Mn activity concentrations in the bottom sediments of Lake Druksiai significantly decreased when operations at both INPP reactor units were stopped. The vertical distribution of radionuclides in bottom sediments revealed complicated sedimentation features, which may have been affected by a number of natural and anthropogenic factors resulting in mixing, resuspension and remobilization of sediments and radionuclides. The associated with particles (137)Cs flux was 129 Bq/(m(2) year). The (137)Cs transfer rate from water into bottom sediments was 14.3 year(-1) (or, the removal time was 25 days). The Kd value for (137)Cs in situ estimated from trap material was 80 m(3)/kg. The associated with particles (60)Co flux was 21 Bq/(m(2) year), when (60)Co activity concentration in sediment trap particles was 15.7 ± 5 Bq/kg. (60)Co activity concentration in soluble form was less than the minimum detectable activity (MDA = 1.3 Bq/m(3)). Then, the conservatively derived Kd value for (60)Co was >90 m(3)/kg.