Distribution,cycling and mean residence time of 226Ra, 210Pb and 210Po in the Tagus estuary

Results for dissolved and particulate ²²⁶Ra, ²¹⁰Pb and ²¹⁰Po in the Tagus river, estuary and coastal sea system show different distribution and chemical behaviour patterns for these radionuclides in the three aquatic environments. ²²⁶Ra from riverborne particles dissolves in the estuary and contributes to increased concentrations of dissolved ²²⁶Ra in estuarine water. In the estuary, dissolved ²¹⁰Pb and ²¹⁰Po from river discharge and atmospheric deposition are scavenged by suspended matter, which in turn becomes enriched in these nuclides in comparison with riverborne particles. As a result of these processes, the estuarine water flowing into the coastal sea contains enhanced concentrations of dissolved ²²⁶Ra, but is depleted in dissolved ²¹⁰Pb and ²¹⁰Po. Under average river flow conditions, mass balance calculations for dissolved ²¹⁰Po and ²¹⁰Pb in the estuary allowed their mean residence times to be estimated as 18 and 30 days, respectively. Due to the rapid sorption of these radionuclides on to settling particles, bottom sediments in the estuary represent a sink for ²¹⁰Pb and ²¹⁰Po from both natural sources and industrial waste releases. Results also suggest that partial re-dissolution of these radionuclides from bottom sediments and intertidal mudflats is likely to occur in the mid- and low-estuary zones. Nevertheless, box-model computations indicate that the discharge of ²¹⁰Pb and ²¹⁰Po into the coastal sea takes place mainly with the transport of sediment, whereas the discharge in the dissolved fraction can only account for one third of the activities entering the estuary in the soluble phase. Implications of these results to the cycling of radionuclides in phosphate waste releases into estuarine environments are discussed.     

210Po and 210Pb cycling in a hydrothermal vent zone in the coastal Aegean sea.

To quantify the potential enhancement of naturally-occurring 210Po and 210Pb that may result from the high sulfur-reducing and sulfur-oxidizing regimes associated with hydrothermal vents, sinking particles from both inside and outside vent areas and benthic molluscs grazing on or living near bacterial mats in the vent zone were collected off Milos Island (Aegean Sea) and analyzed for their 210Po and 210Pb content. There was no significant difference in the range of 210Po specific activities measured in particulate material collected by sediment traps in a control area and in the vent area; the resultant 210Po levels were of the same order of magnitude as literature values reported for other Mediterranean coastal areas. 211Pb levels in sinking particles from the control site tended to be higher than those measured in the vent zone, as demonstrated by the lower 210Po/210Pb ratios observed in particles from the control site. Nevertheless, these 210Pb levels were also comparable with similar 210Pb data reported for the northwestern Mediterranean Sea. The 210Po and 210Pb vertical particulate fluxes were, on average, higher in the vent zone as a consequence of the higher particle flux. This observation indicates that vents can indirectly control the flux of these natural radionuclides by affecting the types and amount of particles produced in hydrothermal areas. The 210Po levels measured in a gastropod and a bivalve living on or near the microbial mat in the vent zone were higher than values reported for non-vent gastropods and bivalves from the NW Mediterranean Sea, an observation which suggests that an enhanced food chain transfer of 210Po may occur in the vicinity of vents off Milos Island. Nevertheless, the lack of a general enhancement of 210Po and 210Pb in the marine particulate samples collected indicates that any input of these radionuclides through venting activity may have a minimal effect in the surrounding environment.     

(210)Po and (210)Pb in the tissues of the deep-sea hydrothermal vent mussel Bathymodiolus azoricus from the Menez Gwen field (Mid-Atlantic Ridge)

The hydrothermal deep-sea vent fauna is naturally exposed to a highly specific environment enriched in potentially toxic species such as sulfides, metals and natural radionuclides due to the convective seawater circulation inside the oceanic crust and its interaction with basaltic or ultramafic host rocks. However, data on radionuclides in biota from such environment are very limited. An investigation was carried out on tissue partitioning of ²¹⁰Po and ²¹⁰Pb, two natural radionuclides within the ²³⁸U decay chain, in Bathymodiolus azoricus specimens from the Mid-Atlantic Ridge (Menez Gwen field). These two elements showed different distributions with high ²¹⁰Pb levels in gills and high ²¹⁰Po levels in both gills and especially in the remaining parts of the body tissue (including the digestive gland). Various factors that may explain such partitioning are discussed. However, ²¹⁰Po levels encountered in B. azoricus were not exceptionally high, leading to weighted internal dose rate in the range 3 to 4 μGy h^− 1. These levels are slightly higher than levels characterizing coastal mussels (~ 1 μGy h^− 1).     

Natural radionuclides in mineral waters

Concentration levels of natural radionuclides in mineral waters have been studied in several European countries. In the Federal Republic of Germany in recent years a nationwide investigation was carried out by several institutions.The concentrations of ²²⁶Ra, uranium isotopes, ²¹⁰Pb and ²¹⁰Po found are similar to those in other European countries. While for adults the health risk from drinking mineral water is comparable to the risk from terrestrial radiation, special consideration has to be given to the risk of infants when mineral water is used for preparing their food.     

Determination of 210Po in various foodstuffs and its annual effective dose to inhabitants of Qena City, Egypt

The concentration of ²¹⁰Po was determined in different foodstuffs of plant origin purchased from markets in Qena City, Upper Egypt. Measurement of ²¹⁰Po has been carried out using alpha spectrometry technique in different food categories such as vegetables, fruits, cereals beverages and herbs. The general range of ²¹⁰Po activity levels ranged widely from < 0.010-18.6 ± 0.910 mBq g^− 1, with minimum being in cereal samples and maximum being in beverage samples. Tea samples recorded highest activity concentrations of ²¹⁰Po with lowest value of 10 ± 0.54 mBq g⁻¹ for Crown tea and highest value of 18.6 ± 0.910 mBq g⁻¹ for El maabad tea. The daily intake of ²¹⁰Po from food consumption reveals that vegetables are the biggest contributors, while beverages are the lowest. The effective ingestion dose has been estimated for Qena City residents and it was found in the range 0.008-38.3 μSv y⁻¹.     

Spatial distribution of radionuclides in soil around a coal-fired power plant: 210Pb, 210Po, 226Ra, 232Th, 40K emitted with the fly ash and 137Cs from the worldwide weapon testing fallout

To determine the effect of airborne emissions of radionuclides from coal-fired power plants on the environment, the concentrations of the most important radionuclides were measured in soil samples from the local environments (0.4–5.2 km) as well as in fly ash. The spatial distribution of the radionuclides in the soil did not indicate any significantly increased concentrations in the area downwind of the plant compared to other areas; the ratios ²¹⁰Pb/²²⁶Ra and ²¹⁰Po/²²⁶Ra were within the range observed for unaffected soils. The emissions from the plant, though present, are obviously too small to significantly change the natural local distribution pattern of the radionuclides in the soil. A highly significant correlation between ⁴⁰K and ²³²Th was observed which was independent of the different types of soils found in this area. The concentration of ¹³⁷Cs in topsoil, which is the result of worldwide fallout from nuclear weapons testing, varied at some places even within a small distance (～ 2 km) by up to one order of magnitude. Furthermore, it was observed that the concentration of ¹³⁷Cs in soils from cropland was on average a factor of 2 less than in those from grassland. This variability has to be considered in planning monitoring programs around nuclear power plants, which may also release this radionuclide.     

Unusually high (210)Po activities in the surface water of the Zhubi Coral Reef Lagoon in the South China Sea

Recent researches revealed the exciting application of ²¹⁰Po in tracing carbon and nitrogen cycling in the coral reef system. In order to quantify the recycling of particulate organic nitrogen (PON), both ²¹⁰Po and ²¹⁰Pb were examined at both high and low tides in the Zhubi Coral Reef lagoon, the South China Sea. Unusually, much higher ²¹⁰Po activities and ²¹⁰Po/²¹⁰Pb ratios, in comparison with those found in the open seawater and the lagoon subsurface water, showed additional input of ²¹⁰Po besides production from in situ²¹⁰Pb in the lagoon surface water. Statistical analysis identified that the reef flat seawater was the additional ²¹⁰Po source. Based on a mass balance model, the input rates of ²¹⁰Po varied from 0.04 Bq m⁻³ year⁻¹ to 8.41 Bq m⁻³ year⁻¹. On average, the additional ²¹⁰Po contributed more than 60% of the total ²¹⁰Po. The particulate ²¹⁰Po significantly correlated with the concentrations of PON, indicating that diffusion of ²¹⁰Po from sediment could be used to quantify the recycling of nitrogen. The average input rate of nitrogen was 16 mmol m⁻³ year⁻¹, which can support up to 11% of the primary production rate. These results suggested that the unusual behavior of ²¹⁰Po could provide new insight into the nitrogen recycling in the coral reef system.     

Distribution and biokinetic analysis of Pb and Po in poultry due to ingestion of dicalcium phosphate

Dicalcium phosphate (DCP) is used as a calcium supplement for food producing animals (i.e., cattle, poultry and pig). When DCP is produced via wet acid digestion of the phosphate rock and depending on the acid used in the industrial process, the final product can result in enhanced ²¹⁰Pb and ²¹⁰Po specific activities (∼ 2000 Bq·kg⁻¹). Both ²¹⁰Pb and ²¹⁰Po are of great interest because their contribution to the dose received by ingestion is potentially large. The aims of this work are to examine the accumulation of ²¹⁰Pb and ²¹⁰Po in chicken tissues during the first 42 days of life and to build a suitable single-compartment biokinetic model to understand the behavior of both radionuclides within the entire animal using the experimental results. Three commercial corn-soybean-based diets containing different amounts and sources of DCP were fed to broilers during a period of 42 days. The results show that diets containing enhanced concentrations of ²¹⁰Pb and ²¹⁰Po lead to larger specific accumulation in broiler tissues compared to the blank diet. Radionuclides do not accumulate homogeneously within the animal body: ²¹⁰Pb follows the calcium pathways to some extent and accumulates largely in bones, while ²¹⁰Po accumulates to a large extent in liver and kidneys. However, the total amount of radionuclide accumulation in tissues is small compared to the amounts excreted in feces. The single-compartment non-linear biokinetic model proposed here for ²¹⁰Pb and ²¹⁰Po in the whole animal takes into account the size evolution and is self-consistent in that no fitting parameterization of intake and excretions rates is required.     

Distribution of (210)Pb and (210)Po in boreal forest soil

Vertical distribution and activity contents of ²¹⁰Pb and ²¹⁰Po were investigated in forest soils of Scots pine-dominated (Pinus sylvestris L.) stands from seven different locations in Finland. The mean total inventory in the soil profile, up to 20 cm, of ²¹⁰Pb was 4.0 kBq m^− 2 (range 3.1-5.0 kBq m^− 2) and ²¹⁰Po 5.5 kBq m^− 2 (range 4.0-7.4 kBq m^− 2), the organic soil layer containing 45% of the total inventory of both nuclides. In both the organic and the mineral layers the ²¹⁰Po/²¹⁰Pb ratio was close to unity indicating a radioactive equilibrium between them. In the litter layer there was, however, a clear excess of ²¹⁰Po suggesting that polonium is recycled via root uptake from the root zone to the ground surface. The activity concentration (Bq kg^− 1) of ²¹⁰Pb clearly correlated with organic matter and the Fe, Al and Mn concentrations in soil indicating that radioactive lead is associated both with humic substances and the oxides of iron, aluminium and manganese. Radioactive lead was also seen to follow the behavior of stable lead. No systematic correlation between polonium and soil properties was seen.     

Estimated dose to man from uranium millling via the beef/milk food-chain pathway

One of the major pathways of radiological exposure to man from uranium milling operations is through the beef/milk food chain. Studies by various investigators have shown the extent of uptake and distribution of ²³⁸U, ²³⁴U, ²³⁰Th, ²²⁶Ra, ²¹⁰Pb, and ²¹⁰Po in plants and cattle. These long0lived natural radioisotopes, all nuclides of the uranium decay series, are found in concentrated amounts in uranium mill tailings. In this paper, data from these investigations are used to estimate the dose to man from consumption of beef and milk from cattle that have fed on forage contaminated with the tailings. The estimated doses from this technologically enhanced source are compared with those resulting from average dietary intake of these radionuclides from natural sources.     

Lead-210 and polonium-210 concentrations in some species of marine molluscs.

Data are presented for 210Pb and 210Po concentrations in three species of molluscs collected in the intertidal region of the coast of Rio de Janeiro, Brazil. Lead-210 activity in the soft tissue of the edible mussel Perna perna was 20 times higher than that found in its shell. The visceral mass contained the largest activity for both radionuclides, which is attributed to the feeding habits of the molluscs. Animals collected from Ponta Negra beach (open sea) showed higher concentrations of isotopes than those collected from Boa Viagem beach (within Guanabara Bay).     

Uptake of 210Pb and 210Po by Brazilian Bunodosoma caissarum Corrêa, 1964 (cnidaria, actinidae)

Bunodosoma caissarum, a carnivorous marine species exclusive to the Brazilian southern coast, recognized as a sensitive bioindicator of artificial radioactive pollution, also shows a great capacity for concentrating natural alpha-emitters. The authors have measured the alpha-emitters 210Po and its precursor 210Pb in this animal. The average concentrations found are greater (by a factor of 4.6) for 210Po measured in samples gathered on Ponta Negra Beach (protected outer coast) than the values obtained in specimens collected on Boa Viagem Beach (closed bay) along the Rio de Janeiro coast, Brazil. The same was also found for 210Pb (a factor of 2.5).     

Distribution of Pb and Po concentrations in wild berries and mushrooms in boreal forest ecosystems

The activity concentrations and distribution of ²¹⁰Pb and ²¹⁰Po in wild berries and edible mushrooms were investigated in Finnish forests. The main study areas were located in Scots pine (Pinus sylvestris L.) forests in southern and northern Finland. The activity concentrations of ²¹⁰Pb and ²¹⁰Po in blueberry (Vaccinium myrtillus L.) and lingonberry (Vaccinium vitis-idaea L.) samples decreased in the order: stems > leaves > berries (i.e. fruits). The activity ratios of ²¹⁰Po/²¹⁰Pb in the wild berry samples were mainly higher than one, indicating elevated activity concentrations of polonium in the samples. In mushrooms the activity concentrations of ²¹⁰Pb and especially ²¹⁰Po were higher than in fruits of the wild berries. The highest activity concentration of ²¹⁰Pb was detected in Cortinarius armillatus L. (16.2 Bq kg^− 1 d.w.) and the lowest in Leccinum vulpinum L. (1.38 Bq kg^− 1 d.w.). The ²¹⁰Po activity concentrations of the whole fruiting bodies ranged from 7.14 Bq kg^− 1 d.w. (Russula paludosa L.) to 1174 Bq kg^− 1 d.w. (L. vulpinum L.). In general, the highest activity concentrations of ²¹⁰Po were recorded in boletes. The caps of mushrooms of the Boletaceae family showed higher activity concentrations of ²¹⁰Po compared to the stipes. In most of the mushrooms analyzed, the activity concentrations of ²¹⁰Po were higher than those of ²¹⁰Pb. ²¹⁰Po and ²¹⁰Pb dominate the radiation doses received via ingestion of wild berries and mushrooms in northern Finland, while in southern Finland the ingested dose is dominated by ¹³⁷Cs from the Chernobyl fallout.     

Sedimentation rates in Western Nipigon Bay,Lake Superior using the 210Pb method

²¹⁰Pb, ²²⁶Ra and ¹³⁷Cs profiles have been measured for sediment cores from three locations in western Nipigon Bay, Lake Superior, Canada. Compaction of the sediment with depth of burial was taken into account in calculating recent sedimentation rates and age profiles at these locations from the excess ²¹⁰Pb profiles. The rates at two of the locations were 0.85±0.03 mmy^?1 (16.7 mg cm^?2 y^?1) and 1.39±0.12 mmy^?1 (29.5 mg cm^?2 y^?1). The third core had an anomaly in the ²¹⁰Pb profile below a depth of 3.5 cm corresponding to the time that the outfall of a nearby pulp mill was relocated. The ¹³⁷Cs profiles of the two undisturbed cores were in accord with the corresponding age/depth curves derived from the ²¹⁰Pb measurements.     

Contamination and restoration of an estuary affected by phosphogypsum releases

The Huelva Estuary in Huelva, Spain, has been one of the most studied environmental compartments in the past years from the point of view of naturally occurring radioactive material (NORM) releases. It has been historically affected by waste releases, enriched in radionuclides from the U-decay series, from factories located in the area devoted to the production of phosphoric acid and phosphate fertilizers.Nevertheless, changes in national regulations forced a new waste management practice in 1998, prohibiting releases of phosphogypsum into the rivers. The input of natural radionuclides from phosphate factories to rivers was drastically reduced. Because of this there was a unique opportunity for the study of the response of a contaminated environmental compartment, specifically an estuary affected by tidal influences, after the cessation of the contaminant releases to, in this case, the Huelva Estuary (henceforth referred to as the Estuary).To investigate the environmental response to this new discharge regime, the specific activities of radionuclides ²²⁶Ra and ²¹⁰Pb in water and sediment samples collected in four campaigns (from 1999 to 2005) were determined and compared with pre-1998 values.From this study it is possible to infer the most effective mechanisms of decontamination for the Estuary. Decontamination rates of ²¹⁰Pb and ²²⁶Ra in the sediments and water have been calculated using exponential fittings and corresponding half-lives have been deduced from them. The cleaning half-life in the whole area of the Estuary is about 6 and 3.5 years for ²²⁶Ra and ²¹⁰Pb respectively.The observed trend clearly shows that contamination of the Estuary by natural radionuclides is now decreasing and radioactive levels in waters and sediments are approaching the natural background references. This work attempts to evaluate whether it can be expected that the decontamination of the enhanced levels of natural radioactivity in the Estuary can be performed via natural processes.     

Recent sedimentation rates and 210Pb fluxes in Georgian Bay and Lake Huron

The ²¹⁰Pb and ¹³⁷Cs profiles are determined at five locations in Georgian Bay and Lake Huron. Compaction-corrected recent sedimentation rates are derived for all locations using the ²¹⁰Pb data. The rates range from 0.13 ± 0.03 mm y^?1 (2.2 ± 0.4 mg cm^?2 y^?1) to 0.78 ± 0.06 mm y^?1 (14.5 ± 1.1 mg cm^?2 y^?1). Except for one location, the rates show marginal to good agreement with those estimated from palynological measurements at four of the five study locations. ¹³⁷Cs profiles at study locations suggest that the top portions of the sediment cores were satisfactorily retrieved during coring and sectioning operations. However, considerable downward migration of ¹³Cs is noted at three locations. The fluxes of excess ²¹⁰Pb vary between 0.06 and 0.27 pCi cm^?2 y^?1. The average depositional flux is found to be considerably lower than the flux of atmospheric ²¹⁰Pb. It is postulated that the deposition of atmospheric ²¹⁰Pb in Lake Huron and Georgian Bay sediments is limited by the supply of scavenging particulates.     

Anthropogenic and natural radionuclides in caribou and muskoxen in the western Alaskan Arctic and marine fish in the Aleutian Islands in the first half of 2000s

A number of caribou and muskoxen samples from the western Alaskan Arctic and fish samples from the Aleutian Islands were collected between 1998 and 2006 and analyzed for anthropogenic (⁹⁰Sr and ¹³⁷Cs) and natural radionculides (⁴⁰ K, ²¹⁰Pb and ²²⁶Ra), as part of the radiological assessment for the regional subsistence hunting communities in the first half of 2000s. We examined the relationship between the activities of these nuclides with the size of the fish. In caribou samples, concentration of ⁹⁰Sr in muscle was below the detection limit of 0.14 Bq kg^− 1 and ¹³⁷Cs concentration in bones was below the detection limit of 0.15 Bq kg^− 1.¹³⁷Cs activity varied over an order of magnitude in caribou muscle samples with an average value of 2.5 Bq/kg wet wt. Average ¹³⁷Cs activity in muskoxen muscle was found to be 9.7 Bq/kg wet wt. However, there were a little variation (less than 60%) in ²¹⁰Pb, ⁴⁰ K, and ²²⁶Ra in both muscle and bone of both caribou and muskoxen. The activities of total ²¹⁰Pb in caribou and muskox bones were found to be 1-2 orders of magnitude higher than that of parent-supported ²¹⁰Pb indicating the potential for dating of bones of terrestrial mammals (time elapsed since the death of the animal) based on the excess ²¹⁰Pb method exists. In fish muscle samples, ¹³⁷Cs activity varied from below detection limit to 154 mBq/kg wet wt. and its content increased with the size of the fish due to its transfer through the food chain. Among the seven fish species investigated, ²¹⁰Pb activities varied almost an order of magnitude; however, ⁴⁰K and ²²⁶Ra activities varied less than a factor of two. Total annual effective dose due to ⁹⁰Sr and ¹³⁷Cs from the ingestion of those terrestrial and marine meats was estimated to be negligible (ca. 9 μSV/a) compared to the natural radionuclides present thus posing negligible radiological threat to humans.     

210Pb in di-calcium phosphate consumed by dairy cows

In the semiarid region of the Brazilian state of Pernambuco, the feedstuffs for dairy cattle contain the mineral supplement of di-calcium phosphate (DCP). This study was carried out to determine the concentration of ²¹⁰Pb in samples of di-calcium phosphate (DCP: CaHPO₄) consumed by dairy cows in Pedra and Venturosa. ²¹⁰Pb concentrations ranged from 17 to 256 Bq.kg^?1, and although they are below the concentrations reported in Spain (up to 2260 Bq.kg^?1), they also could be considered to represent a potential risk of chemical toxicity in dairy cows.     

Pb and stable lead content in fungi: Its transfer from soil

The uptake and transfer of natural radionuclides, other than ⁴⁰K, from soil to mushrooms has been somewhat overlooked in the literature. Their contribution to the dose due to the consumption of mushrooms was considered negligible. But the contribution of ²¹⁰Pb in areas unaffected by any recent radioactive fallout has been found to be significant, up to 35% of the annual dose commitment in Spain. More than 30 species of mushrooms were analyzed, and the ²¹⁰Pb detected was in the range of 0.75-202 Bq/kg d.w. A slight difference was observed between species with different nutritional mechanisms (saprophytes ≥ mycorrhizae). The ²¹⁰Pb content was correlated with the stable lead content, but not with its predecessor in the uranium radioactive series, ²²⁶Ra. This suggested that ²¹⁰Pb was taken up from the soil by the same pathway as stable lead. The bioavailability of ²¹⁰Pb in soil was determined by means of a sequential extraction procedure (NH₄OAc, 1M HCl, 6M HCl, and residue). About 30% of the ²¹⁰Pb present in the soil was available for transfer to mushrooms, more than other natural radionuclides in the same ecosystem. Lycoperdon perlatum, Hebeloma cylindrosporum, and Amanita curtipes presented the highest values of the available transfer factor, ATF. As reflected in their ATF values, the transfer from soil to mushroom of some natural and anthropogenic radionuclides was in the following order:

^228,230,232Th ≈ ⁴⁰K ≥ ¹³⁷Cs ≥ ^234,238U ≈ ²²⁶Ra ≥ ⁹⁰Sr ≥ ²¹⁰Pb ≈ ^239 + 240Pu ≈ ²⁴¹Am.     

Pb and 210Pb in a tropical river environment

The Periyar River in south India receives the major share of Pb and ²¹⁰Pb from effluents released by factories along its bank that process monazite ore and rock phosphate. Their distribution in the river system is influenced by the rains during the monsoon and by salinity during the non-monsoon period. The concentration of both Pb and ²¹⁰Pb in the sediments from the backwater zone was observed to increase during the monsoon due to sediment transport from the upstream industrial zone. The water in the backwater zone showed increased levels of Pb and ²¹⁰Pb in the non-monsoon period, due possibly to solubilization from the sediments as a result of salinity changes. The levels of Pb and ²¹⁰Pb in the river water are much lower than the international standards for safe limits in drinking water. No significant concentration of Pb and ²¹⁰Pb above a background level was observed in fish obtained from the river.