Reinvestigation of airborne 210Pb, 137Cs and 207Bi in Vienna (Austria) after atmospheric nuclear weapons tests

Reconstruction of atmospheric 210Pb and 137Cs activity concentrations occurring in Vienna immediately after the atmospheric nuclear weapons tests shall answer the question, whether artificial 210Pb has been produced by fusion devices using lead materials. If so, 207Bi also can be expected. In 1962, weekly average values for 210Pb were between 0.08 +/- 0.02 and 1.31 +/- 0.30 mBq/m2, 137Cs amounts up to 5.1 +/- 0.6 mBq/m3. 207Bi remains below the detection limit, viz. < 0.5 mBq/m3. Bimonthly averages for the periods 1962-1964 and 1974-1975 show 137Cs activity concentrations with typical springtime maxima occurring together with low 210Pb values and 207Bi < 0.02 mBq/m3. Annual averages of 210Pb are varying between 0.27 and 0.53 mBq/m3, independent of whether atmospheric tests have been performed or not. Comparison of the activity ratios 207Bi/210Pb, 207Bi/137Cs and 210Pb/137Cs with published data, leads to the conclusion that no evidence exists for a significant production of 210Pb by nuclear explosions, neither after the Soviet tests in 1961-1962 nor after the Chinese tests in 1973-1976.     

A note on 207Bi in environmental samples

Traces of the radionuclide (207)Bi were identified in soil and cryoconite (glacier sediment) samples from Alpine regions of Austria. This nuclide has been produced in thermonuclear explosions mainly in the early 1960s and subsequently dispersed in the atmosphere. Activity concentrations up to 22 Bq/kg d.m. have been found. The ratio (207)Bi:(137)Cs(global fallout) equals (1.70+/-0.12)10(-3), which is in accordance with literature data. When low levels of (207)Bi are assessed by gamma spectrometry, corrections must be made for a gamma line produced in the lead shield by neutron activation due to cosmic neutrons.     

Accumulation of anthropogenic radionuclides in cryoconites on Alpine glaciers

Cryoconites are airborne sediments which accumulate on the surface of glaciers. In samples of cryoconites a temperate Austrian glacier high activity concentrations of anthropogenic radionuclides were found, which stem from global and Chernobyl fallouts. Radionuclides identified were ¹³⁷Cs, ¹³⁴Cs, ²³⁸Pu, ^239+240Pu, ⁹⁰Sr, ²⁴¹Am, ⁶⁰Co, ¹⁵⁴Eu, ²⁰⁷Bi, and ¹²⁵Sb.     

Geochronology of anthropogenic radionuclides in Ribeira Bay sediments, Rio de Janeiro, Brazil

Ribeira Bay is located approximately 130 km south of the city of Rio de Janeiro and receives discharges of liquid effluent from the Angra dos Reis nuclear power plant (NPP) site, where two pressurized water reactors are located. To test whether the presence of anthropogenic radionuclides in sediments in Ribeira Bay could be correlated to the NPP operations, we sampled seven sediment cores and determined accumulation rates and chronologies. Only one sediment core did not exhibit a superficial mixing layer; this sample was used for dating purposes. Cesium-137 and ²⁰⁷Bi were observed in this sediment profile, but their presence was associated with atmospheric fall-out rather than the nearby NPP. The exponential decay of ²¹⁰Pb concentration with sediment layer depth was verified below a superficial mixing layer for all other sediment cores. Calculated accumulation rates ranged from 1.2 mm y⁻¹ in the inner bay to 6.2 mm y⁻¹ close to its entrance.     

Level and origin of 129I and 137Cs in lichen samples (Cladonia alpestris) in central Sweden

Lichen is a symbiosis between algae and fungi. They have for decades been used as bioindicators for atmospheric deposition of heavy metals, organic compounds and radioactive elements. Especially the species Cladonia alpestris and Cladonia rangiferina are important for the food chain lichen-reindeer-man.The concentration of ¹²⁹I was determined in lichen samples (Cladonia alpestris) contaminated by fallout from atmospheric nuclear tests explosions and the Chernobyl accident. The samples were collected at Lake Rogen District (62.3°N, 12.4°E) in central Sweden in the periods 1961-1975 and 1987-1998, and analysed with accelerator mass spectrometry (AMS) at CNA (Seville) to study its distribution in different layers. Data on the ¹³⁷Cs activity measured previously were also included in this study. The ¹²⁹I concentration ranged from (0.95 ± 0.13) × 10⁸ at g⁻¹ in 1961 in the uppermost layer to (14.2 ± 0.5) × 10⁸ at g⁻¹ in 1987 in deepest layer. The ¹²⁹I/¹³⁷Cs atom ratio ranged between 0.12 and 0.27 for lichen samples collected in the period 1961-1975, indicating weapons tests fallout. For lichen samples collected between 1987 and 1998 the behaviour of ¹³⁷Cs concentrations reflected Chernobyl fallout. The concentrations of the two radionuclides followed each other quite well in the profile, reflecting the same origin for both.From the point of view of the spatial distribution in the lichen, it appears that ¹²⁹I was predominantly accumulated in the lowest layer, the opposite to ¹³⁷Cs for which the highest amounts were detected systematically in the topmost layer of lichen. This vertical distribution is important for radioecology because lichen is the initial link in the food chain lichen-reindeer-man, and reindeer only graze the upper parts of lichen carpets.     

Po-210 and Pb-210 as atmospheric tracers and global atmospheric Pb-210 fallout: a review

Over the past ∼5 decades, the distribution of ²²²Rn and its progenies (mainly ²¹⁰Pb, ²¹⁰Bi and ²¹⁰Po) have provided a wealth of information as tracers to quantify several atmospheric processes that include: i) source tracking and transport time scales of air masses; ii) the stability and vertical movement of air masses iii) removal rate constants and residence times of aerosols; iv) chemical behavior of analog species; and v) washout ratios and deposition velocities of aerosols. Most of these applications require that the sources and sink terms of these nuclides are well characterized.Utility of ²¹⁰Pb, ²¹⁰Bi and ²¹⁰Po as atmospheric tracers requires that data on the ²²²Rn emanation rates is well documented. Due to low concentrations of ²²⁶Ra in surface waters, the ²²²Rn emanation rates from the continent is about two orders of magnitude higher than that of the ocean. This has led to distinctly higher ²¹⁰Pb concentrations in continental air masses compared to oceanic air masses. The highly varying concentrations of ²¹⁰Pb in air as well the depositional fluxes have yielded insight on the sources and transit times of aerosols. In an ideal enclosed air mass (closed system with respect to these nuclides), the residence times of aerosols obtained from the activity ratios of ²¹⁰Pb/²²²Rn, ²¹⁰Bi/²¹⁰Pb, and ²¹⁰Po/²¹⁰Pb are expected to agree with each other, but a large number of studies have indicated discordance between the residence times obtained from these three pairs. Recent results from the distribution of these nuclides in size-fractionated aerosols appear to yield consistent residence time in smaller-size aerosols, possibly suggesting that larger size aerosols are derived from resuspended dust. The residence times calculated from the ²¹⁰Pb/²²²Rn, ²¹⁰Bi/²¹⁰Pb, and ²¹⁰Po/²¹⁰Pb activity ratios published from 1970’s are compared to those data obtained in size-fractionated aerosols in this decade and possible reasons for the discordance is discussed with some key recommendations for future studies.The existing global atmospheric inventory data of ²¹⁰Pb is re-evaluated and a ‘global curve’ for the depositional fluxes of ²¹⁰Pb is established. A current global budget for atmospheric ²¹⁰Po and ²¹⁰Pb is also established. The relative importance of dry fallout of ²¹⁰Po and ²¹⁰Pb at different latitudes is evaluated. The global values for the deposition velocities of aerosols using ²¹⁰Po and ²¹⁰Pb are synthesized.     

Occurrence and behaviour of radionuclides in the Moselle River—Part I: Entry of natural and artificial radionuclides

Various sources contribute to the radioactive contamination of the Moselle River, among which the French NPP Cattenom with four units of 1300 M We represents the most important. Appropriate operational precautions were taken in order to monitor the nuclide transfer on different pathways under normal and accidental conditions and the effectiveness of these measures has been tested using natural (²¹⁴Pb/²¹⁴Bi, ⁷Be, ⁴⁰K) and artificial radionuclides. (³H, ⁵⁸Co, ⁶⁰Co, ¹³¹I, ¹³⁷Cs) as tracers. Measurements of suspended matter have revealed that the inputs of natural nuclides exceed the discharges of the NPP Cattenom. In 1992 the annual loads of ⁷Be and ⁴⁰K in suspended matter at Palzem amounted to 21 and 130 GBq year⁻¹, whereas the emission rates of ⁶⁰Co and ¹³⁷Cs were about 2.6 and 1.0 GBq year⁻¹. The total nuclide load of ¹³⁷Cs at Palzem reached 6.2 GBq year⁻¹, which is about six times the quantity emitted by the NPP Cattenom in the same year. This excess is due to the accident at Chernobyl and to a lesser extent to prior atmospheric weapons tests.     

A study of radionuclides, metals and stable lead isotope ratios in sediments and soils in the vicinity of natural U-mineralisation areas in the Northern Territory

Australian guidelines recommend that tailings materials from uranium (U) mining and milling be contained without any detrimental impact on the environment for at least 1000 years. Natural analogue sites are being investigated to determine if they can provide data on the rates of natural erosion processes which occur over these timescales, for input into predictive geomorphic computer models. This paper presents radionuclide, metal and stable lead (Pb) isotope data from sediment cores and surface soils in the vicinity of two mineralised areas in the Alligator Rivers Region.Surface scrapes from the natural Anomaly #2, south of the Ranger mineral lease, exhibit radiogenic ²⁰⁶Pb/²⁰⁷Pb and ²⁰⁸Pb/²⁰⁷Pb ratios, and elevated U and metal concentrations typical for a near surface U anomaly. In contrast, samples taken from the Koongarra mineral lease (KML) show radionuclide activity and metal concentrations similar to natural areas elsewhere in the Alligator Rivers Region and Pb isotope ratios are closer to present day average crustal ratios (PDAC), as the orebodies at KML are covered by surficial sand. A sediment core collected from Anbangbang Billabong, downstream of KML, exhibits small variations in Pb isotope ratios that indicate that approximately 1% of the upper sediments in the sediment core may be derived from material originating from the U anomaly at Koongarra.     

Estimating the effect of nitrogen fertilizer on the greenhouse gas balance of soils in Wales under current and future climate

The Welsh Government is committed to reduce greenhouse gas (GHG) emissions from agricultural systems and combat the effects of future climate change. In this study, the ECOSSE model was applied spatially to estimate GHG and soil organic carbon (SOC) fluxes from three major land uses (grass, arable and forest) in Wales. The aims of the simulations were: (1) to estimate the annual net GHG balance for Wales; (2) to investigate the efficiency of the reduced nitrogen (N) fertilizer goal of the sustainable land management scheme (Glastir), through which the Welsh Government offers financial support to farmers and land managers on GHG flux reduction; and (3) to investigate the effects of future climate change on the emissions of GHG and plant net primary production (NPP). Three climate scenarios were studied: baseline (1961–1990) and low and high emission climate scenarios (2015–2050). Results reveal that grassland and cropland are the major nitrous oxide (N₂O) emitters and consequently emit more GHG to the atmosphere than forests. The overall average simulated annual net GHG balance for Wales under baseline climate (1961–1990) is equivalent to 0.2 t CO₂e ha^?1 y^?1 which gives an estimate of total annual net flux for Wales of 0.34 Mt CO₂e y^?1. Reducing N fertilizer by 20 and 40 % could reduce annual net GHG fluxes by 7 and 25 %, respectively. If the current N fertilizer application rate continues, predicted climate change by the year 2050 would not significantly affect GHG emissions or NPP from soils in Wales.     

Pre-concentration of naturally occurring radionuclides and the determination of (212)Pb from fresh waters

A novel technique has been developed for determining the ²¹²Pb activity of fresh waters. This is of interest to environmental monitoring programmes that utilise gross α-activity methods to screen for anthropogenic radionuclides. The contribution from ²¹²Pb varies, and is difficult to experimentally measure due to its relatively short half-life (t_½ = 10.6 h) and low environmental activity (<0.1 Bq l⁻¹). The use of a three-stage technique that encompasses a unique form of pre-concentration, separation and analysis by liquid scintillation counting allows a lower detection limit of 0.006 Bq l⁻¹ with a chemical yield of 92.5 ± 5.6%. The measurement can be obtained within 7 h of sample collection, and is calculated using the radioactive decay of ²¹²Bi. Other naturally occurring radionuclides may also be extracted using the pre-concentration stage of the technique, with efficiencies above 90% at a range of pH values.     

Trends in food production and nitrous oxide emissions from the agriculture sector in India: environmental implications

We studied trends in food production and nitrous oxide emissions from India's agricultural sector between 1961 and 2000. Data from Food and Agricultural Statistics (FAO) have been gathered covering production, consumption, fertilizer use and livestock details. IPCC 1996 revised guidelines were followed in studying the variations in N₂O-N emissions. Results suggest that total N₂O-N emissions (direct, animal waste and indirect sources) increased ~6.1 times from ~0.048 to ~0.294 Tg N₂O-N, over 40 years. Source-wise breakdown of emissions from 1961–2000 indicated that during 1961 most of the N₂O-N inputs were from crop residues (61%) and biological nitrogen fixation (25%), while during 2000 the main sources were synthetic fertilizer (~48%) and crop residues (19%). Direct emissions increased from ~0.031 to ~0.183 Tg. It is estimated that ~3.1% of global N₂O-N emissions comes from India. Trends in food production, primarily cereals (rice, wheat and coarse grains) and pulses, and fertilizer consumption from 1961–2000 suggest that food production (cereals and pulses) increased only 3.7 times, while nitrogenous fertilizer consumption increased ~43 times over this period, leading to extensive release of nitrogen to the atmosphere. From this study, we infer that the challenge for Indian agriculture lies not only in increasing production but also in achieving production stability while minimizing the impact to the environment, through various management and mitigation options.     

Solar-driven technology for freshwater production from atmospheric air by using the composite desiccant material “CaCl<Subscript>2</Subscript>/floral foam”

In this communication, experiments have been performed to check the capability of the newly formed composite desiccant material (CaCl₂/floral) for the extraction of freshwater from atmospheric air. Three numbers of solar glass desiccant box type system (SGDBS) with a captured area of 0.36 m² each, have been used. The design parameters for the water production are height of glass from desiccant bed at 0.22 m, inclination in angle as 30°, the effective thickness of glass as 3 mm and number of glazing as single. The maximum yield by the new composite desiccant material is 0.35 ml/cm³/day. The efficiency of the system SGDBS with 37 % concentration of CaCl₂ is 76.44 %.     

Selection of an effective sludge dewatering system for a small wastewater treatment plant

The Jahra Plant was commissioned in 1981 as a secondary treatment plant employing the extended aeration process. The plant has been upgraded since that time by constructing additional tertiary filtration units to improve effluent quality. The plant has a design capacity of 66 000 m³/d. At present, the daily inflow to the plant is about 47 000 m³/d of domestic sewage. The sludge produced at the Jahra Plant can be classified as excess activated sludge which combines the primary and secondary solids. At present, there are 30 drying beds receiving about 100 m³ of sludge dally. Sewage-sludge production represents about 0.5% of the total flow treated at the plant and is increasing yearly with increases in population and water consumption. Present dewatering systems are not adequate to cope with expansion in sewage treatment. Increasing the capacity of the existing plant would require more drying beds that could exacerbate existing odor problems. Some dewatering systems, such as the belt filter press and the centrifuge, have been tested to determine the most effective one under local conditions. Appropriate polymer doses for thickening have been determined. This paper describes present sludge dewatering units and operating techniques which have been developed during the operation of this facility.     

Radon measurements in 12,000 Swedish homes

Radon daughter levels have been monitored in 12,000 Swedish dwellings during the last two years. In 1979 the Swedish Government introduced temporary limits for the radon daughter concentration in dwellings. For existing buildings this limit is 400 Bq/m³ (0.11 WL). Two different methods were used to monitor the radon daughter concentration. The majority of the houses presented in this paper were monitored using a track-etch detector; some houses were tested using a filter sampling technique while the ventilation rate was determined. Close to 15% of the investigated houses have a radon daughter concentration higher than 400 Bq/m³. The majority of these houses were one-family houses. Almost 10% of this group has a concentration above 1000 Bq/m³ (0.27 WL). The results from this study show that the two most important sources for radon in buildings are building materials and the ground.     

How changes in diet and trade patterns have shaped the N cycle at the national scale: Spain (1961–2009)

During the last five decades (1961–2009), Spain has experienced a considerable expansion in the nutrient cycle of its agricultural sector and, in particular, a threefold increase in anthropogenic reactive nitrogen inputs, from 536 Gg N year^?1 in 1961–1965 to 1673 Gg N year^?1 in 2005–2009. Import of feed (soybean, cereals, and cakes) from America and Europe to supply a growing livestock population constitutes the largest share of this increase, along with intensification of synthetic fertilizer use. While in the early 1960s, Spain was nearly self-sufficient in terms of food and feed supply, the net import of agricultural products presently equals domestic crop production, when expressed in terms of nitrogen content (ca. 650 Gg N year^?1). The most important driver of this shift appears to be the rapid change in domestic consumption patterns, which evolved from a typical Mediterranean diet to an animal-protein-rich diet similar to the North European and American diets. Besides livestock production mostly for national consumption, the Spanish agricultural system has specialized in vegetal products with low N content such as olive oil, wine, vegetables, and citrus fruit, which are for the most part exported. The nitrogen load exported outside the Spanish borders by rivers is very low (6.5 % of the total net N input). As a result of the high import and low export of reactive nitrogen, the Spanish mainland is suffering from considerable pollution by local emissions of reactive nitrogen forms to air and water.     

The sources and fate of 210Po in the urban air: A review

The origin of ²¹⁰Po activity and its fluctuations in the air are discussed in this paper. In the case of atmospheric aerosol samples, a comparison of the ²¹⁰Po/²¹⁰Pb and ²¹⁰Bi/²¹⁰Pb activity ratios makes it possible not only to determine aerosol residence times but also to appraise the contribution of the unsupported ²¹⁰Po coming from other sources than ²²²Rn decay, such as human industrial activities, especially coal combustion. A simple mathematical method makes it possible to observe the seasonal fluctuations of the anthropogenic excess of ²¹⁰Po in the urban air. The average doses of ²¹⁰Po intake with food (including drinking water) and inhalation of urban aerosols are usually lower than those from ²¹⁰Po intake by cigarette smokers and negligible in comparison to total natural radiation exposure.     

Psychrophilic and Psychrotolerant Heterotrophic Microorganisms of Middle Siberian Karst Cavities

The natural microflora of Middle Siberian karst cavities, which comprises psychrotolerant bacteria and fungi capable of growing at 3–15 and 3...+28°C, respectively, has been studied. Bacteria are ubiquitous in caves, their count varying from 10³ to 10⁷ cells/g ground. The bacteria have been identified as Pseudomonas, Arthrobacter, Bacillus, and coryneform bacteria. Fungi have been found in places exposed to increased anthropogenic impact, their count being as large as 10⁶ to 10⁷ cells/g ground. Mucor, Penicillium, and Chrysosporium were dominant fungal genera.     

Natural and anthropogenic radionuclides in airborne particulate samples collected in Barcelona (Spain)

Results for naturally occurring ⁷Be, ²¹⁰Pb, ⁴⁰K, ²¹⁴Bi, ²¹⁴Pb, ²¹²Pb, ²²⁸Ac and ²⁰⁸Tl and anthropogenic ¹³⁷Cs in airborne particulate matter in the Barcelona area during the period from January 2001 to December 2005 are presented and discussed. The ²¹²Pb and ²⁰⁸Tl, ²¹⁴Bi and ²¹⁴Pb, ⁷Be and ²¹⁰Pb radionuclide levels showed a significant correlation with each other, with correlation coefficients of 0.99, 0.78 and 0.69, respectively, suggesting similar origin/behaviour of these radionuclides in the air. Caessium-137 and Potassium-40 were transported to the air as resuspended particle from the soil. The ⁷Be and ²¹⁰Pb concentrations showed similar seasonal variations, with a tendency for maximum concentrations during the summer months. An inverse relationship was observed between the ⁷Be, ²¹⁰Pb, ⁴⁰K and ¹³⁷Cs concentrations and weekly rainfall, indicating washout of atmospheric aerosols carrying these radionuclides.     

Aspects on the analysis of 210Po

There has been little development regarding analysis of polonium (Po) in environmental samples since the 1960ies. This is due to the straightforward spontaneous deposition of this element on silver (Ag), nickel (Ni) or copper (Cu) without any radiochemical separation. For many years, no radiochemical yield determinant was used and it was generally supposed that the yield was 100% after two depositions. Counting was often done using ZnS scintillation counter coupled to a photomultiplier tube. However, the use of the yield determinants ²⁰⁸Po and ²⁰⁹Po and the development of alpha spectrometry showed that the yield was lower. Furthermore, the tendency of Po to volatilize at low temperatures constrains the sample preparation techniques; dry-ashing cannot be used. But during the wet-ashing procedure, there are still some losses.The aim of this study was to evaluate the Po losses during wet-ashing by the use of a double-tracer technique. We have found that the losses were about 30% when open glass beakers were used and about 17% when the samples were digested in microwave oven. When long-necked bottles (Kjeldahl flasks) were used, a loss of about 20% was registered.It has also been observed that ²¹⁰Pb to some extent is plating out together with its daughter nuclide Po during the electrochemical deposition. This will result in a systematic error since an unknown amount of supported ²¹⁰Po will be produced from the ²¹⁰Pb decay depending on the fraction of ²¹⁰Pb being deposited on the disc and the waiting time between deposition and measurement of the sample. A further consequence of this is that in the assessment of the ²¹⁰Pb content in the sample, very often the remaining liquid is stored after deposition for build-up of ²¹⁰Po. Since some ²¹⁰Pb is lost on the disc, the result for ²¹⁰Pb will be too low. Both these systematic errors give rise to a too high ²¹⁰Po/²¹⁰Pb ratio. The fraction of ²¹⁰Pb which is plating out has been assessed in this study for different matrices and is about 50-90%. During the measurement by solid state Si-detectors, some Po is evaporated in the vacuum conditions contaminating the detectors. Experiments have here been done by heating the discs after deposition which indicate that less Po is evaporated from Ag than from Ni. The losses from Ag are less than that from the other metals probably due to a deeper penetration into the surface of Po. We conclude that in most aspects, Ag is better to use than the other plating metals.     

Isotope tracing of submarine groundwater discharge offshore Ubatuba, Brazil: results of the IAEA–UNESCO SGD project

Results of groundwater and seawater analyses for radioactive (³H, ²²²Rn, ²²³Ra, ²²⁴Ra, ²²⁶Ra, and ²²⁸Ra) and stable (D and ¹⁸O) isotopes are presented together with in situ spatial mapping and time series ²²²Rn measurements in seawater, direct seepage measurements using manual and automated seepage meters, pore water investigations using different tracers and piezometric techniques, and geoelectric surveys probing the coast. This study represents first time that such a new complex arsenal of radioactive and non-radioactive tracer techniques and geophysical methods have been used for simultaneous submarine groundwater discharge (SGD) investigations. Large fluctuations of SGD fluxes were observed at sites situated only a few meters apart (from 0 cm d⁻¹ to 360 cm d⁻¹; the unit represents cm³/cm²/day), as well as during a few hours (from 0 cm d⁻¹ to 110 cm d⁻¹), strongly depending on the tidal fluctuations. The average SGD flux estimated from continuous ²²²Rn measurements is 17 ± 10 cm d⁻¹. Integrated coastal SGD flux estimated for the Ubatuba coast using radium isotopes is about 7 × 10³ m³ d⁻¹ per km of the coast. The isotopic composition (δD and δ¹⁸O) of submarine waters was characterised by significant variability and heavy isotope enrichment, indicating that the contribution of groundwater in submarine waters varied from a small percentage to 20%. However, this contribution with increasing offshore distance became negligible. Automated seepage meters and time series measurements of ²²²Rn activity concentration showed a negative correlation between the SGD rates and tidal stage. This is likely caused by sea level changes as tidal effects induce variations of hydraulic gradients. The geoelectric probing and piezometric measurements contributed to better understanding of the spatial distribution of different water masses present along the coast. The radium isotope data showed scattered distributions with offshore distance, which imply that seawater in a complex coast with many small bays and islands was influenced by local currents and groundwater/seawater mixing. This has also been confirmed by a relatively short residence time of 1–2 weeks for water within 25 km offshore, as obtained by short-lived radium isotopes. The irregular distribution of SGD seen at Ubatuba is a characteristic of fractured rock aquifers, fed by coastal groundwater and recirculated seawater with small admixtures of groundwater, which is of potential environmental concern and has implications on the management of freshwater resources in the region.