Spatial patterns and ratios of ¹³7Cs, 9°Sr, and Pu isotopes in the top layer of undisturbed meadow soils as indicators for contamination origin.

Spatial distribution of activity concentrations of (137)Cs, (90)Sr, and (239,240)Pu in the top layer of undisturbed meadow soils was compared between two regional transects across Lithuania: one in the SW region, more affected by the Chernobyl radioactive fallout, and the other in the NE region. Radiochemical, γ-, α-, ß-, and mass spectrometric methods were used to determine the radionuclide activity. Our results validate that higher activity concentrations in the top soil layer were present in the SW region, despite the fact that sampling was performed after 22 years of the Chernobyl Nuclear Power Plant (NPP) accident. Using the activity concentration ratio (137)Cs/(239,240)Puglobal, the contribution of the Chernobyl NPP accident to the total radiocesium activity concentrations in these meadow soils was evaluated and found to be in the range of 6.5-59.1%. Meanwhile, the activity concentration ratio (238)Pu/(239,240)Pu showed that Chernobyl-derived Pu occurred at almost half of the sampling sites. The locations with maximal values of 47% of Chernobyl-derived Pu material were close to northeastern Poland, where deposition of most of non-volatile radioisotopes from the Chernobyl plume was determined.

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.

Development of graphitization method for low carbon aerosol filter samples with Automated Graphitization System AGE-3.

The wide applications of the radiocarbon (14C) approach in environmental, archeological, and geological research often necessitates the analysis of microgram-sized samples. The ability to measure low carbon samples is particularly relevant for aerosol particle filters, especially for samples from pristine environments. For this purpose, we investigated the sample dilution method for graphitization of low-carbon samples (20-200 µg C) with an Automated Graphitization System (AGE-3), and applied a mass balance equation for the calculation of 14C values. Materials with known 14C values (standards NIST-OXII and IAEA-C7) were diluted with 14C-free phthalic anhydride (PhA) until sufficient mass (500 µg C) for graphitization with the AGE-3 system was acquired. Reliable 14C values were obtained for samples with carbon amount in the range of 40-200 µg. Next, we adapted the dilution method for estimation of aerosol sample 14C values. Using it, we attained a precision of 0.71 ± 0.83 pMC for 14C measurements of aerosol samples containing 40-200 µg C. A shift of radiocarbon values to 5.07 pMC (average 3.08 ± 1.7 pMC) was observed for samples with low carbon content (<20 µg C). We determined that a precision of 2-3 pMC is acceptable for aerosol particle source apportionment studies. Using the sample dilution method, graphitization with AGE-3 of aerosol samples with carbon content >40 µg becomes a viable and efficient way of sample preparation for 14C analysis.

The elemental composition of small mammals in a commercial orchard-meadow system.

We analyze concentrations of various elements in small mammals from commercial orchards and berry plantations and test differences between them depending on species, individual body mass, age, gender, type and age of crop and intensity of applied agricultural measures. Skinned front legs (muscle and bones) were used to register the presence and concentration of Ca, Cd, Mo, Ni, Se, Ag, As, Be, Bi, Co, Cr, Cu, Fe, Ga, Mg, Mn, Pb, Sr, U, V and Zn. The most abundant species were common vole (Microtus arvalis), yellow-necked (Apodemus flavicollis) and striped field (A. agrarius) mice. The maximum recorded concentrations exceeded the minimums by 1.7-7.7 times in Mg, Zn, Cu, Ga, Ni and Ca, and 11.0-23.2 times in Mn, Be, Mo, Co, Sr, V, Pb and As. The hypothesis that the use of fertilization and pesticides in commercial orchards should induce differences in the elemental concentrations between crop areas and control habitats was confirmed by the higher concentrations of Cu, Mn, Bi, Co, Cr, Fe, Ni, Sr and Pb in rodents from the crop areas. Spatially controlled generalized linear mixed model confirmed the cumulative influence of species and crop, explaining 30-80% of the distribution of Ca, Ni, Co, Cu, Ga, Mn, Pb and U. The effect of species and the age of the individual was significant for Ni, Co, Cu, Fe, Ga, Mn and Pb, while effect of gender was not expressed. Depletion of Cu in older individuals was found in all three species. With species as a grouping factor, the effect of crop type and the intensity of agricultural practices were significant factors in the accumulation of Ca, Ni, Co, Cu, Ga, Mn and Pb, while effect of crop age was not expressed. The obtained elemental concentrations in rodents indicated orchards to be cleaner than heavy polluted areas.

Stable Isotopes Reveal the Dominant Species to Have the Widest Trophic Niche of Three Syntopic Microtus Voles.

Diets and trophic positions of co-occurring animals are fundamental issues in their ecology, and these issues in syntopic rodents have been studied insufficiently. Using carbon (δ13C) and nitrogen (δ15N) stable isotope ratios from hair samples, we analysed the trophic niches of common (Microtus arvalis), field (M. agrestis), and root (M. oeconomus) voles co-occurring in orchards, berry plantations, and nearby meadows (as control habitat to orchards and plantations). We tested if the niche of the dominant common vole was the widest, whether its width depended on the presence of other vole species, and whether there were intraspecific differences. Results suggest stability in the trophic niches of all three Microtus species, as season explained only 2% of the variance. The widest trophic niche was a characteristic of the dominant common vole, the range of δ13C values exceeding the other two species by 1.6, the range of δ15N values exceeding the other two species by 1.9, and the total area of niche exceeding that of the other voles by 2.3-3 times. In the meadows and apple orchards, co-occurring vole species were separated according to δ13C (highest values in the dominant common vole), but they maintained similar δ15N values. Results give new insights into the trophic ecology small herbivores, showing the impact of species co-occurrence.

Isotopic Niche of Syntopic Granivores in Commercial Orchards and Meadows.

In agricultural habitats, diets and trophic positions of syntopic granivorous small mammals are not known sufficiently. Agroecosystems may be quite complex isotopically and the most complex situation concerns the nitrogen-15 isotope as δ15N values are influenced by many internal and external fluxes. We analysed the isotopic niches of striped field (Apodemus agrarius), yellow-necked (Apodemus flavicollis), and harvest (Micromys minutus) mice living sympatrically and syntopically in apple and plum orchards, raspberry and currant plantations, and nearby meadows that were used as control habitats. Carbon (δ13C) and nitrogen (δ15N) stable isotope ratios from hair samples were used as a proxy for their diet. As the main hypothesis, we expected differences in the isotopic niches of these three species, minimising interspecific competition. All species were fully separated according to δ15N values, presuming different amounts of food of animal origin in their diet. The separation of species according to δ13C was not expressed in all habitats. The core dietary niches of these species were fully separated in the apple orchards and raspberry plantations. Intraspecific differences of the isotopic niche were not present in any of the three species: that is, resources were equally used by males and females, adults, subadults, and juveniles.

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.

Seasonal Variation in Stable Isotope Ratios of Cow Milk in Vilnius Region, Lithuania.

Various studies have shown that stable isotope analysis has the potential to verify the geographic origin of foods and drinks. However, stable isotope composition is not always constant in the environment and can even change in the same area. Dairy products are of particular interest as a group of foods that play an important role in feeding the population. The composition of milk is fundamentally dependent on the feeding of the cows, and thereby on a particular environment. To better understand the amount of variation in δ18O, δ13C, and δ15N values in the milk from the same area, we measured stable isotope ratios in cow milk water, artesian water, and precipitation (δ18O) as well as in bulk milk samples (δ13C and δ15N) collected in 2014⁻2016. Different water and food sources were available during the winter (artesian water only and dry grass) and summer (artesian water and fresh grass), and spring and autumn seasons reflected transitional periods. Oxygen stable isotope ratios in milk water were relatively lower in winter and transitional seasons and higher in summer, showing the dependence on the main water source. δ13C values reflected particular food sources. This study shows the applicability of the stable isotope ratio method in linking cow milk to specific environments and reveals the amount of variation in stable isotope ratios in the same area. These results could be valuable for other studies on geographical origin determination of dairy products.

Aerosol source (biomass, traffic and coal emission) apportionment in Lithuania using stable carbon and radiocarbon analysis.

In the present study, a combination of the stable carbon isotope ratio (13C/12C) with radiocarbon data (14C) allowed us to perform the aerosol source apportionment. Filter samples of PM1 were collected during the warm and cold periods in rural and urban sites in Lithuania. The 14C/12C ratio of total carbon (TC) was measured using the single stage accelerator mass spectrometer quantifying of fossil and non-fossil derived aerosol emissions. The δ13C value was measured using an elemental analyser interfaced with an isotope ratio mass spectrometer. We have found that the highest fraction of contemporary carbon (fc = 0.82) was measured during a warm period in a rural location. A higher fraction of fossil fuel-derived carbon was observed for air masses transported from highly industrialized Western European regions during both seasons. Isotope mass balance calculations revealed that the traffic emissions composed 15 and 25 % in rural and urban sites, respectively, and did not change during either season. Input from coal-derived aerosol particles was estimated to be 15 % at an urban site during the cold period. The combination of the stable carbon isotope ratio with the radiocarbon data allowed us to distinguish coal, liquid fossil fuel combustion, and non-fossil derived aerosol particle emissions.

Yeast-assisted synthesis of polypyrrole: Quantification and influence on the mechanical properties of the cell wall.

In this study, the metabolism of yeast cells (Saccharomyces cerevisiae) was utilized for the synthesis of the conducting polymer - polypyrrole (Ppy).Yeast cells were modified in situ by synthesized Ppy. The Ppy was formed in the cell wall by redox-cycling of [Fe(CN)6]3-/4-, performed by the yeast cells. Fluorescence microscopy, enzymatic digestions, atomic force microscopy and isotope ratio mass spectroscopy were applied to determine both the polymerization reaction itself and the polymer location in yeast cells. Ppy formation resulted in enhanced resistance to lytic enzymes, significant increase of elasticity and alteration of other mechanical cell wall properties evaluated by atomic force microscopy (AFM). The suggested method of polymer synthesis allows the introduction of polypyrrole structures within the cell wall, which is build up from polymers consisting of carbohydrates. This cell wall modification strategy could increase the usefulness of yeast as an alternative energy source in biofuel cells, and in cell based biosensors.

Uncertainty of determination of 158Tb in the RBMK nuclear reactor waste.

The activity of 158Tb was measured in waste samples from the Ignalina NPP Unit I RBMK-1500 reactor using gamma-ray spectrometry. The origin of 158Tb and the other observed gamma-ray emitters has been studied by using SCALE 6.1 modeling and comparing radionuclide ratios in the RBMK-1500 radioactive waste. The results of the calculation of the massic activity of gamma-ray emitters were used for interpretation of the total gamma-ray spectrum and the determination of 158Tb massic activity uncertainty in the waste of RBMK-1500.

Rapid analysis method for the determination of 14C specific activity in irradiated graphite.

14C is one of the limiting radionuclides used in the categorization of radioactive graphite waste; this categorization is crucial in selecting the appropriate graphite treatment/disposal method. We propose a rapid analysis method for 14C specific activity determination in small graphite samples in the 1-100 µg range. The method applies an oxidation procedure to the sample, which extracts 14C from the different carbonaceous matrices in a controlled manner. Because this method enables fast online measurement and 14C specific activity evaluation, it can be especially useful for characterizing 14C in irradiated graphite when dismantling graphite moderator and reflector parts, or when sorting radioactive graphite waste from decommissioned nuclear power plants. The proposed rapid method is based on graphite combustion and the subsequent measurement of both CO2 and 14C, using a commercial elemental analyser and the semiconductor detector, respectively. The method was verified using the liquid scintillation counting (LSC) technique. The uncertainty of this rapid method is within the acceptable range for radioactive waste characterization purposes. The 14C specific activity determination procedure proposed in this study takes approximately ten minutes, comparing favorably to the more complicated and time consuming LSC method. This method can be potentially used to radiologically characterize radioactive waste or used in biomedical applications when dealing with the specific activity determination of 14C in the sample.

Stable isotope ratio method for the characterisation of the poultry house environment.

Stable isotope analysis was applied to describe the poultry house environment. The poultry house indoor environment was selected for this study due to the relevant health problems in animals and their caretakers. Air quality parameters including temperature, relative humidity, airflow rate, NH3, CO2 and total suspended particles, as well as mean levels of total airborne bacteria and fungi count, were measured. Carbon isotope ratios (13C/12C) were obtained in size-segregated aerosol particles. The carbon (13C/12C) and nitrogen (15N/14N) isotope ratios were measured in feed, litter, scrapings from the ventilation system, feathers and eggs. Additionally, the distribution of δ13C and δ15N values in different tissues of the chicken was examined. The airborne bacteria and fungi extracted from the air filters collected from poultry farms were grown in the laboratory in media with known isotope values and measured for stable isotope ratios. Analysis of isotope fractionation between microorganisms and their media indicated the applicability of stable isotope analysis in bulk samples for the identification of source material. The analysed examples imply that stable isotope analysis can be used to examine the indoor environment along with its biology and ecology, and serve as an informative bioanalytical tool.

The impact of Great Cormorants on biogenic pollution of land ecosystems: Stable isotope signatures in small mammals.

Studying the isotopic composition of the hair of two rodent species trapped in the territories of Great Cormorant colonies, we aimed to show that Great Cormorants transfer biogens from aquatic ecosystems to terrestrial ecosystems, and that these substances reach small mammals through the trophic cascade, thus influencing the nutrient balance in the terrestrial ecosystem. Analysis of δ(13)C and δ(15)N was performed on two dominant species of small mammals, Apodemus flavicollis and Myodes glareolus, inhabiting the territories of the colonies. For both species, the values of δ(13)C and δ(15)N were higher in the animals trapped in the territories of the colonies than those in control territories. In the hair of A. flavicollis and M. glareolus, the highest values of δ(15)N (16.31±3.01‰ and 17.86±2.76‰, respectively) were determined in those animals trapped in the biggest Great Cormorant colony. δ(15)N values were age dependent, highest in adult A. flavicollis and M. glareolus and lowest in juvenile animals. For δ(13)C values, age-dependent differences were not registered. δ(15)N values in both small mammal species from the biggest Great Cormorant colony show direct dependence on the intensity of influence. Biogenic pollution is at its strongest in the territories of the colonies with nests, significantly diminishing in the ecotones of the colonies and further in the control zones, where the influence of birds is negligible. Thus, Great Cormorant colonies alter ecosystem functioning by enrichment with biogens, with stable isotope values in small mammals significantly higher in the affected territories.

Stable isotopes measurements reveal dual carbon pools contributing to organic matter enrichment in marine aerosol.

Stable carbon isotope ratios in marine aerosol collected over the Southern Indian Ocean revealed δ13C values ranging from -20.0‰ to -28.2‰. The isotope ratios exhibited a strong correlation with the fractional organic matter (OM) enrichment in sea spray aerosol. The base-level isotope ratio of -20.0‰ is characteristic of an aged Dissolved Organic Matter (DOM) pool contributing a relatively homogeneous background level of DOM to oceanic waters. The range of isotope ratios, extending down to -28.2‰, is characteristic of more variable, stronger, and fresher Particulate Organic Matter (POM) pool driven by trophic level interactions. We present a conceptual dual-pool POM-DOM model which comprises a 'young' and variable POM pool which dominates enrichment in sea-spray and an 'aged' but invariant DOM pool which is, ultimately, an aged end-product of processed 'fresh' POM. This model is harmonious with the preferential enrichment of fresh colloidal and nano-gel lipid-like particulate matter in sea spray particles and the observed depleted δ13C ratio resulting from isotope equilibrium fractionation coupled with enhanced plankton photosynthesis in cold water (-2 °C to +8 °C). These results re-assert the hypothesis that OM enrichment in sea-spray is directly linked to primary production and, consequently, can have implications for climate-aerosol-cloud feedback systems.

Effect of microorganisms on the plutonium oxidation states.

Particular microbes from substrates at the low-level radioactive waste repository in the Ignalina NPP territory were exposed to (239)Pu (IV) at low pH under aerobic conditions. Pu(III) and Pu(IV) were separated and quantitatively evaluated using the modified anion exchange method and alpha spectrometry. Tested bacteria Bacillus mycoides and Serratia marcescens were more effective in Pu reduction than Rhodococcus fascians. Fungi Paecillomyces lilacinus and Absidia spinosa var. spinosa as well as bacterium Rhodococcus fascians did not alter the plutonium oxidation state.