210Po in the marine environment with emphasis on its behaviour within the biosphere

The distribution and behaviour of the natural-series alpha-emitter polonium-210 in the marine environment has been under study for many years primarily due to its enhanced bioaccumulation, its strong affinity for binding with certain internal tissues, and its importance as a contributor to the natural radiation dose received by marine biota as well as humans consuming seafoods. Results from studies spanning nearly 5 decades show that ²¹⁰Po concentrations in organisms vary widely among the different phylogenic groups as well as between the different tissues of a given species. Such variation results in ²¹⁰Po concentration factors ranging from approximately 10³ to over 10⁶ depending upon the organism or tissue considered. ²¹⁰Po/²¹⁰Pb ratios in marine species are generally greater than unity and tend to increase up the food chain indicating that ²¹⁰Po is preferentially taken up by organisms compared to its progenitor ²¹⁰Pb. The effective transfer of ²¹⁰Po up the food chain is primarily due to the high degree of assimilation of the radionuclide from ingested food and its subsequent strong retention in the organisms. In some cases this mechanism may lead to an apparent biomagnification of ²¹⁰Po at the higher trophic level. Various pelagic species release ²¹⁰Po and ²¹⁰Pb packaged in organic biodetrital particles that sink and remove these radionuclides from the upper water column, a biogeochemical process which, coupled with scavenging rates of this radionuclide pair, is being examined as a possible proxy for estimating downward organic carbon fluxes in the sea. Data related to preferential bioaccumulation in various organisms, their tissues, resultant radiation doses to these species, and the processes by which ²¹⁰Po is transferred and recycled through the food web are discussed. In addition, the main gaps in our present knowledge and proposed areas for future studies on the biogeochemical behaviour of ²¹⁰Po and its use as a tracer of oceanographic processes are highlighted in this review.     

Study of 210Po and 210Pb in the riverine environments of coastal Karnataka

Activity of ²¹⁰Po and ²¹⁰Pb were measured in soil and sediment samples collected from the major rivers Kali, Sharavathi and Netravathi of Coastal Karnataka. The activity of these two radionuclides were determined by radiochemical separation of ²¹⁰Po and counting the activity using a ZnS(Ag) Alpha counter. The activity of ²¹⁰Pb was higher than that of ²¹⁰Po in the riverine environs. The ²¹⁰Po and ²¹⁰Pb content in sediment was found to increase with silt/clay and organic matter contents. However no significant correlation was found between the activity ²¹⁰Po and ²¹⁰Pb with pH in sediments. The activity of ²¹⁰Po and ²¹⁰Pb and influence of physico-chemical parameters on these radionuclides were studied and discussed in this paper.     

Activities of Po and Pb in the water column at Kuala Selangor, Malaysia

Natural radionuclides, such as ²¹⁰Po and ²¹⁰Pb were measured in the water samples collected from six stations at Kuala Selangor, Malaysia. Results for ²¹⁰Po and ²¹⁰Pb in dissolved and particulate phases have showed the difference in distribution and chemical behavior. The fluctuation activities of ²¹⁰Po and ²¹⁰Pb depend on wave action, geology and degree of fresh water input occurring at study areas and probably due to different sampling dates. The distribution coefficient, K_d, values of ²¹⁰Po and ²¹⁰Pb ranged from 2.0 × 10³ l g⁻¹ to 265.15 × 10⁵ l g⁻¹, and from 3.0 × 10³ l g⁻¹ to 558.16 × 10⁵ l g⁻¹, respectively. High K_d values of ²¹⁰Po and ²¹⁰Pb indicated that a strong adsorption of ²¹⁰Po and ²¹⁰Pb onto suspended particles, and the sinking of both nuclides on the seabed at study locations were controlled by the characteristics of suspended particles.     

Lead-210 and Beryllium-7 fallout rates on the southeastern coast of Brazil

Total ²¹⁰Pb and ⁷Be fallout rates were measured on the coastal region of Niteroi, Brazil. The monthly depositional flux of ²¹⁰Pb and ⁷Be varied by a factor of 26, from 1.7 to 43.3 mBq cm⁻² year⁻¹ and ∼27, from 7.5 to 203.5 mBq cm⁻² year⁻¹, respectively. The relatively large oscillations in the depositional flux of ²¹⁰Pb at this study site were likely due to variations in air mass sources, while the ⁷Be fluctuations may be driven by a combination of weather conditions. Local geology could support the periodic high fluxes of ²¹⁰Pb from continental air masses, as shifting oceanic wind sources were affirmed by the uncorrelated ²¹⁰Pb and ⁷Be fallout activities and ⁷Be/²¹⁰Pb ratios. The ²¹⁰Pb atmospheric deposition was found to be in agreement with local sediment inventories, an important consideration in geochemical studies that estimate sedimentation processes.     

210Pb as a tool for establishing sediment chronologies: examples of potentials and limitations of conventional dating models

For aquatic sediments, the use of ²¹⁰Pb originating from the decay of atmospheric ²²²Rn is a well-established methodology to estimate sediment ages and sedimentation rates. Traditionally, the measurement of ²¹⁰Pb in soils and sediments involved laborious and time-consuming radiochemical separation procedures. Due to the recent development of advanced planar (‘n-type’) semi-conductors with high efficiencies in the low-energy range which enable the gamma-spectrometric analysis of the 46.5 keV decay line of ²¹⁰Pb, sediment dating using this radionuclide has gained renewed interest.In this contribution, potentials and limitations of the ²¹⁰Pb methodology and of the models used for estimating sediment ages and sedimentation rates are discussed and illustrated by examples of freshwater and marine sediments. Comparison with the use of ¹³⁷Cs shows that the information which may be gained by these two tracers is complementary. As a consequence, both radionuclides should be used in combination for dating of recent sediments. It is shown that for various sedimentation regimes additional information from other sources (e.g. sediment lithology) may be needed to establish a reliable chronology. A strategy for sediment dating using ²¹⁰Pb is recommended.     

210Pb deposition in the far East Asia: controlling factors of its spatial and temporal variations

In order to better understand the behavior of ²¹⁰Pb deposition in Far East Asia, comprehensive data of monthly ²¹⁰Pb deposition, which includes several time-series and spatial distribution data at 14 stations in Japan and 2 stations in Taiwan, were analyzed. Pb-210 deposition at most of the sites exhibited a typical seasonal change with higher values in winter and lower values in summer; especially, the greatest ²¹⁰Pb deposition in the world occurred in winter at sites beside the Japan Sea. The deposition behavior of ²¹⁰Pb in Far East Asia differed between winter and summer. The meteorological phenomenon peculiar to winter of the Japan Sea side, i.e., formation of the Japan Sea convergence zone, might cause the high ²¹⁰Pb concentration in rainwater, as may heavy snowfall. The ²¹⁰Pb concentration in rainwater showed long-term variability, although this differed between winter and summer. This long-term variability may be related to climatological factors such as El Niño.     

Transfer factors of Polonium from soil to parsley and mint

Transfer factors of ²¹⁰Po from soil to parsley and mint have been determined. Artificial polonium isotope (²⁰⁸Po) was used as a tracer to determine transfer factor of Po from soil to plant in pot experiments. Two plant growing systems were used for this study namely, an outdoor system and a sheltered system by a polyethylene tent. ²⁰⁸Po and ²¹⁰Po were determined in soil and different parts of the studied plants (stem and leaf), using alpha spectroscopy. The results have shown that there was a clear uptake of ²⁰⁸Po by roots to leaves and stems of both plants. Higher values of transfer factors using the ²¹⁰Po activity concentrations than the ²⁰⁸Po activity concentration were observed. Transfer factors of ²¹⁰Po from soil to parsley varied between 20 × 10⁻² and 50 × 10⁻² and 22 × 10⁻³ and 67 × 10⁻³ in mint, while ²⁰⁸Po transfer factors varied between 4 × 10⁻² and 12 × 10⁻² for parsley and 10 × 10⁻² and 22 × 10⁻² in mint. Transfer factors of Po were higher in those plants grown in the sheltered system than in the open system; about 75% of Po was transferred from atmosphere to parsley parts using the two systems. Ratios of transferred Po from soil to mint stem and leaf in the sheltered system were higher by 2 times from those in the open system.     

Increase of 210Po levels in human semen fluid after mussel ingestion

Polonium-210 (²¹⁰Po) radioactive concentrations were determined in human semen fluid of vasectomized non-smoker volunteers. The ²¹⁰Po levels ranged from 0.10 to 0.39 mBq g⁻¹ (mean: 0.23 ± 0.08 mBq g⁻¹). This value decreased to 0.10 ± 0.02 mBq g⁻¹ (range from 0.07 to 0.13 mBq g⁻¹) after two weeks of a controlled diet, excluding fish and seafood. Then, volunteers ate during a single meal 200 g of the cooked mussel Perna perna L., and ²¹⁰Po levels were determined again, during ten days, in semen fluid samples collected every morning. Volunteers continued with the controlled diet and maintained sexual abstinence through the period of the experiment. A 300% increase of ²¹⁰Po level was observed the day following mussel consumption, with a later reduction, such that the level returned to near baseline by day 4.     

Distribution of radionuclides in the guano sediments of Xisha Islands, South China Sea and its implication

Several natural and anthropogenic radionuclides (²¹⁰Pb, ²²⁶Ra and ¹³⁷Cs) in guano-phosphatic coral sediments and pure guano particles collected from Ganquan, Guangjin, Jinqing and Jinyin Islands of the Xisha archipelago, South China Sea, were analyzed. The Constant Initial Concentration (CIC) model and the Constant Rate of Supply (CRS) model were applied for age calculation. The average supply rate of ²¹⁰Pb was 126 Bq m⁻² a⁻¹, very close to the flux of northern hemisphere average (125 Bq m⁻² a⁻¹). The activities of anthropogenic radionuclides in the sediments were very low, indicating that human nuclear tests did not notably impact this region. The main source of radionuclides in the sediments was from atmospheric precipitation, and the organic matter derived from plant and produced by nutrient-rich guano could further enhance them.     

Recent atmospheric lead deposition recorded in an ombrotrophic peat bog of Great Hinggan Mountains, Northeast China, from Pb and Cs dating

Radioactive markers are useful in dating lead deposition patterns from industrialization in peat archive. Peat cores were collected in an ombrotrophic peat bog in the Great Hinggan Mountains in Northeast China in September 2008 and dated using ²¹⁰Pb and ¹³⁷Cs radiometric techniques. The mosses in both cores were examined systematically for dry bulk density, water and ash content. Lead also was measured using atomic emission spectroscopy with inductively coupled plasma (ICP-AES). Both patterned peat profiles were preserved well without evident anthropogenic disturbance. Unsupported ²¹⁰Pb and ¹³⁷Cs decreased with the depth in both of the two sample cores. The ²¹⁰Pb chronologies were established using the constant rate of supply model (CRS) and are in good agreement with the ¹³⁷Cs time marker. Recent atmospheric ²¹⁰Pb flux in Great Hinggan Mountains peat bog was estimated to be 337 Bq m⁻² y⁻¹, which is consistent with published data for the region. Lead deposition rate in this region was also derived from these two peat cores and ranged from 24.6 to 55.8 mg m⁻² y⁻¹ with a range of Pb concentration of 14-262 μg g⁻¹. The Pb deposition patterns were consistent with increasing industrialization over the last 135-170 y, with a peak of production and coal burning in the last 50 y in Northeast China. This work presents a first estimation of atmospheric Pb deposition rate in peatlands in China and suggests an increasing trend of environmental pollution due to anthropogenic contaminants in the atmosphere. More attention should be paid to current local pollution problems, and society should take actions to seek a balance between economic development and environmental protection.     

Ra–Po–Pb isotope systematics in waters of Sambhar Salt Lake,Rajasthan (India): geochemical characterization and particulate reactivity

The Sambhar Salt Lake hydrological system, including river waters, groundwaters, evaporating pans and sub-surface brines, has been analyzed for the salt content (TDS) and naturally occurring radionuclides (²¹⁰Po, ²¹⁰Pb and ^226,228Ra). The abundance of these radionuclides and their activity ratios show a wide variation in different hydrological regimes, which helps to geochemically characterize the lake system. A significantly lower Ra to total dissolved solids (TDS) ratio in the brines (by two to three orders of magnitude), when compared to the groundwaters and river waters, suggests removal of dissolved Ra by co-precipitation with Ca–Mg minerals at an early stage of the brine evolution. The concentration of Ra in evaporating lake/pan waters saturates at a value of about 35 Bq L⁻¹ over the salinity range of 100–370 g L⁻¹; attributable to its equilibration with the clay minerals. The two distinct regimes, saline lake system (lake water, evaporating pans and sub-surface brines) and groundwaters have been identified based on their differences in the distribution of ^226,228Ra isotopes. This observation points to the conclusion that the groundwaters and the lake brines are not intimately coupled in terms of their origin and evolution. The abundances of ²¹⁰Po and ²¹⁰Pb along with their activity ratios (²¹⁰Po/²¹⁰Pb) are markedly different among the surface lake waters/evaporating pans, sub-surface lake brines and groundwaters. These differences are explained in terms of different geochemical behaviour of these nuclides in presence of algae and organic matter present in these water regimes.     

Recent Cs deposition in sediments of Admiralty Bay, Antarctica

Cesium-137, radium-226 and lead-210 profiles of a 25 cm sediment core give an indication of recent changes in land-ocean interactions at a polar coastal environment (Admiralty Bay, King George Island, Antarctica). The linear sedimentation accumulation rate at the study site calculated from the unsupported ²¹⁰Pb profile was 6.7 mm/year from 1965 to 2005. A 3.5-fold increase in ¹³⁷Cs concentrations was observed in the top layer of this sediment core. This sharp increase seems to indicate a recent redistribution of fallout radionuclides previously deposited on soil, vegetation and snow. These results imply enhanced land-ocean interactions at this site likely as a result of climate change. Because our results are based on a single core, additional investigations are needed to confirm our observations.     

The effect of air mass origin on the ambient concentrations of Be and Pb in Islamabad, Pakistan

Concentration of radionuclides ²¹⁰Pb and ⁷Be, having half lives of 22.3 years and 53.29 days, respectively, in the surface air samples of Islamabad (33.38° N, 73.10° E and Altitude ∼536 m asl.) are measured. The non-destructive technique of gamma-spectrometry, with a high purity germanium HPGe detector, was employed for the analysis of all samples. The annual average concentrations of ²¹⁰Pb and ⁷Be in the surface air samples were determined as 0.284 ± 0.15 and 3.171 ± 1.14 mBq m⁻³, respectively. Our results have shown a seasonal variation of the concentration of ⁷Be in air samples with high values for the spring season. High concentrations for ²¹⁰Pb are obtained when air masses originate from plain areas of Pothohar region, located in the South-West, West and North West of Islamabad. Our values of concentrations show a nice agreement with the relevant reported results.     

Recent changes in Red Lake (Romania) sedimentation rate determined from depth profiles of Pb and Cs radioisotopes

This work presents a first estimation of the sedimentation rate for the Red Lake (Romania). The sediment accumulation rates were determined by two well-known methods for recent sediment dating: ²¹⁰Pb and ¹³⁷Cs methods. Both techniques implied used the gamma emission of the above-mentioned radionuclides. The ²¹⁰Pb and ¹³⁷Cs concentrations in the sediment were measured using a gamma spectrometer with a HpGe detector, Gamma-X type. Activities ranging from 41 ± 7 to 135 ± 34 Bq/kg were found for ²¹⁰Pb and from 3 ± 0.5 to 1054 ± 150 Bq/kg for ¹³⁷Cs. The sediment profile indicates acceleration in sedimentation rate in the last 18 years. Thus, the sedimentation process for the Red Lake can be divided in two periods, the last 18 years, and respectively, the period before that. Using the Constant Rate of ²¹⁰Pb Supply method values between 0.18 ± 0.04 and 1.85 ± 0.5 g/cm² year (0.32 ± 0.08 and 2.83 ± 0.7 cm/year) were obtained. Considering both periods, an average sedimentation rate of 0.87 ± 0.17 g/cm² year (1.17 cm/year) was calculated. Considering an average depth of 5.41 m for the lake and the sedimentation rate estimated for the last 18 years, it could be estimated that the lake will disappear in 195 years.     

Concentrations of U,U, U,Th, Th,Th, Ra,Ra, Ra,Po, Pb and Pb in drinking water in Italy: reconciling safety standards based on measurements of gross α and β

Some important naturally occurring α- and β-radionuclides in drinking water samples collected in Italy were determined and the radiological quality evaluated. The mean activity concentrations (mBq L⁻¹) of the radionuclides in the water samples were almost in the order: 26 ± 36 (²³⁴U) > 21 ± 30 (²³⁸U) > 8.9 ± 15 (²²⁶Ra) > 4.8 ± 6.3 (²²⁸Ra) > 4.0 ± 4.1 (²¹⁰Pb) > 3.2 ± 3.7 (²¹⁰Po) > 2.7 ± 1.2 (²¹²Pb) > 1.4 ± 1.8 (²²⁴Ra) > 1.1 ± 1.3 (²³⁵U) > 0.26 ± 0.39 (²²⁸Th) > 0.0023 ± 0.0009 (²³⁰Th) > 0.0013 ± 0.0006 (²³²Th). The mean estimated dose (μSv yr⁻¹) to an adult from the water intake was in this order: 2.8 ± 3.3 (²¹⁰Po) > 2.4 ± 3.2 (²²⁸Ra) > 2.1 ± 2.1 (²¹⁰Pb) > 1.8 ± 3.1 (²²⁶Ra) > 0.94 ± 1.30 (²³⁴U) > 0.70 ± 0.98 (²³⁸U) > 0.069 ± 0.087 (²²⁴Ra) > 0.036 ± 0.044 (²³⁵U) > 0.014 ± 0.021 (²²⁸Th) > 0.012 ± 0.005 (²¹²Pb) > 0.00035 ± 0.00029 (²³⁰Th) > 0.00022 ± 0.00009 (²³²Th). It is obvious that ²¹⁰Po, ²²⁸Ra, ²¹⁰Pb and ²²⁶Ra are the most important dose contributors in the drinking water intake. As far as the seventeen brands of analysed drinking water were concerned, the committed effective doses were in the range of 2.81–38.5 μSv yr⁻¹, all well below the reference level of the committed effective dose (100 μSv yr⁻¹) recommended by the WHO. These data throw some light on the scale of the radiological impact on the public from some naturally occurring radionuclides in drinking water, and can also serve as a comparison for the dose contribution from artificial radionuclides released to the environment as a result of human practices. Based on the radionuclide composition in the analysed waters, comment was made on the new screening level for gross α activity in guidelines for drinking-water quality recommended by the WHO, 2004.     

Comparative trends and seasonal variation of ⁷Be, ²¹⁰Pb and ¹³⁷Cs at two altitude sites in the central part of France

The atmospheric concentrations of ¹³⁷Cs, ²¹⁰Pb, and ⁷Be were measured over a three-year period at two research stations located less than 12 km apart and at different altitudes (puy de Dôme, 1465 m a.s.l. and Opme, 660 m a.s.l., France). Seasonal trends in all radionuclides were observed at both stations, with high concentration measured during the summer and low concentrations during the winter. The ²¹⁰Pb concentrations at both stations were similar to each other. Higher concentrations of both ⁷Be and ¹³⁷Cs were measured at puy de Dôme than at Opme. These observations can be explained by the stratospheric and upper tropospheric sources of ⁷Be and the long-range transportation of ¹³⁷Cs at high altitudes. Air mass origins during sampling periods were classified into several groups by their route to the stations (marine, marine modified, continental and mediterranean). We observed that ⁷Be concentrations were constant regardless of the air mass origins, unlike ¹³⁷Cs and ²¹⁰Pb concentrations that increased when influenced by continental air masses. Higher ⁷Be concentrations were observed when air masses were arriving from the upper troposphere than from the boundary layer, the opposite was observed for ¹³⁷Cs. The temporal trend in concentrations of ⁷Be shows good agreement with previous modelling studies suggesting that there is a good understanding of its sources and the atmospheric vertical mixing of this radionuclide. The sources and mixing of ²¹⁰Pb, however, seem to be more complex than it appeared to be in previous modelling studies.     

Radium and radium-daughter nuclides in carbonates: a brief overview of strategies for determining chronologies

Radium isotopes have been used extensively to trace the movement of groundwater as well as oceanic water masses, but these radionuclides (and their daughters) are also useful chronometers for the determination of the time scales of other Earth and environmental processes. The purpose of this overview is to present the application of Ra and Ra daughters in the dating of carbonates. We show that the choice of dating method (decay of excess radionuclide or ingrowth of daughter) depends strongly on the parent/daughter activity ratios in the water in which the carbonate was precipitated. Thus freshly precipitated carbonates uniformly show excesses of ²²⁶Ra relative to its parent ²³⁰Th, and ²²⁶Ra decay can provide ages of carbonates over Holocene time scales. In contrast, carbonates are precipitated in waters of greatly varying ²¹⁰Pb/²²⁶Ra. Corals, deep-sea hydrothermal vent clams and the shelled cephalopod Nautilus live in waters with significant dissolved ²¹⁰Pb and all show excesses of ²¹⁰Pb in their carbonate. Bivalve molluscs from nearshore and coastal waters, and carbonates deposited from groundwater environments (e.g. travertines) in which ²¹⁰Pb is efficiently scavenged from solution, show deficiencies of ²¹⁰Pb relative to ²²⁶Ra. In contrast, fish otoliths strongly discriminate against ²¹⁰Pb regardless of the environment in which the fish lives. Deficiencies of ²²⁸Th relative to ²²⁸Ra are common in all carbonates. Useful time ranges for the ²¹⁰Pb/²²⁶Ra and ²²⁸Th/²²⁸Ra chronometers are ∼100 y and ∼10 y, respectively.     

Observations and modelling of thoron and its progeny in the soil-atmosphere-plant system

Samples of pasture vegetation, mainly Trifolium pratensis, were collected at the Botanic Garden of the University of Bologna during the period 1998-2000 and measured by gamma-spectrometry for determining thoron progeny. Concentrations of ²¹²Pb were between 1.5 and 20 Bq m⁻², with individual peaks up to 70 Bq m⁻². Soil samples were collected at the same location and physically characterised. Their chemical composition (particularly Th and U) was determined by X-ray fluorescence spectroscopy. Lead-212 on plants mainly originates from dry and wet deposition of this isotope generated in the lower atmosphere by the decay of its short-lived precursor ²²⁰Rn, which is produced in the upper soil layers as a member of the natural thorium decay chain and exhales into the atmosphere. Concentrations of ²²⁰Rn in the atmosphere depend on (1) the amount of Th present in soil, (2) the radon fraction which escapes from the soil minerals into the soil pore space, (3) its transport into the atmosphere, and (4) its redistribution within the atmosphere. The mobility of radon in soil pore space can vary by orders of magnitude depending on the soil water content, thus being the main factor for varying concentrations of ²²⁰Rn and ²¹²Pb in the atmosphere. We present a simple model to predict concentrations of thoron in air and its progeny deposited from the atmosphere, which takes into account varying soil moisture contents calculated by the OPUS code. Results of this model show close agreement with our observations.     

Inventories of Pu, Cs, and excess Pb in sediments from freshwater and brackish lakes in Rokkasho, Japan, adjacent to a spent nuclear fuel reprocessing plant

We investigated the vertical profiles of ^239+240Pu, ¹³⁷Cs, and excess ²¹⁰Pb (²¹⁰Pb_ex) in sediment core samples obtained from two freshwater lakes and two brackish lakes situated near the first commercial spent nuclear fuel reprocessing plant in Rokkasho, Japan, before the final test of the plant using actual spent nuclear fuel. The inventory of ^239+240Pu in those lakes was larger than that in soil in Rokkasho, which indicated the inflow of ^239+240Pu from the catchment area in addition to direct deposition on the lake surfaces. The ¹³⁷Cs inventory in sediments of the brackish lakes was lower than that in the soil, which showed that part of the ¹³⁷Cs was removed from the sediments by the brackish water or that it was not deposited into the sediments, because of the high solubility of Cs in brackish water. The ¹³⁷Cs inventory in sediments of the freshwater lakes was higher than that of the brackish lakes, and comparable with that in soil except for one core sample out of four. The ^239+240Pu/¹³⁷Cs ratio in freshwater lake sediments was higher than that in soil, and that indicated that part of the ¹³⁷Cs was lost from the sediments. The low inventory of ¹³⁷Cs may be attributable to competition for absorption sites in sediments with ammonium ions formed in the reducing environment which occurs from summer to fall in the sediments. Those data will be used as background data on the artificial radionuclides in the lakes to assess the effect of released radionuclides on their concentrations.