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Journal of Environmental Radioactivity 102 (2011) 420e429

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Journal of Environmental Radioactivity


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Polonium-210 and lead-210 in the terrestrial environment: a historical review


Bertil R.R. Persson a, *, Elis Holm b
a b

Dept. of Medical Radiation Physics, Lund University, Barngatan 2, SE-221 85 Lund, Sweden Norwegian Radiation Protection Authority, sters, Norway

a r t i c l e i n f o
Article history: Received 19 December 2010 Accepted 21 January 2011 Available online 5 March 2011 Keywords: Po-210 Pb-210 Moss Lichen Reindeer Man

a b s t r a c t
The radionuclides 210Po and 210Pb widely present in the terrestrial environment are the nal long-lived radionuclides in the decay of 238U in the earths crust. Their presence in the atmosphere is due to the decay of 222Rn diffusing from the ground. The range of activity concentrations in ground level air for 210 Po is 0.03e0.3 Bq m3 and for 210Pb 0.2e1.5 Bq m3. In drinking water from private wells the activity concentration of 210Po is in the order of 7e48 mBq l1 and for 210Pb around 11e40 mBq l1. From water works, however, the activity concentration for both 210 Po and 210Pb is only in the order of 3 mBq l1. Mosses, lichens and peat have a high efciency in capturing 210Po and 210Pb from atmospheric fallout and exhibit an inventory of both 210Po and 210Pb in the order of 0.5e5 kBq m2 in mosses and in lichens around 0.6 kBq m2. The activity concentrations in lichens lies around 250 Bq kg1, dry mass. Reindeer and caribou graze lichen which results in an activity concentration of 210Po and 210Pb of about 1e15 Bq kg1 in meat from these animals. The food chain lichen-reindeer or caribou, and Man constitutes a unique model for studying the uptake and retention of 210Po and 210Pb in humans. The effective annual dose due to 210Po and 210Pb in people with high consumption of reindeer/caribou meat is estimated to be around 260 and 132 mSv a1 respectively. In soils, 210Po is adsorbed to clay and organic colloids and the activity concentration varies with soil type and also correlates with the amount of atmospheric precipitation. The average activity concentration levels of 210Po in various soils are in the range of 20e240 Bq kg1. Plants become contaminated with radioactive nuclides both by absorption from the soil (supported Po) and by deposition of radioactive fallout on the plants directly (unsupported Po). In fresh leafy plants the level of 210Po is particularly high as the result of the direct deposition of 222Rn daughters from atmospheric deposition. Tobacco is a terrestrial product with high activity concentrations of 210Po and 210Pb. The overall average activity concentration of 210Po is 13 2 Bq kg1. It is rather constant over time and by geographical origin. The average median daily dietary intakes of 210Po and 210Pb for the adult world population was estimated to 160 mBq day1 and 110 mBq day1, corresponding to annual effective doses of 70 mSv a1 and 28 mSv a1, respectively. The dietary intakes of 210Po and 210Pb from vegetarian food was estimated to only 70 mBq day1 and 40 mBq day1 corresponding to annual effective doses of 30.6 mSv a1 and 10 mSv a1, respectively. Since the activity concentration of 210Po and 210Pb in seafood is signicantly higher than in vegetarian food the effective dose to populations consuming a lot of seafood might be 5 e15 fold higher. 2011 Elsevier Ltd. All rights reserved.

1.

210

Po and

210 210

Pb in the terrestrial environment


210

1.1. Origin of

Po and

Pb in the terrestrial environment

* Corresponding author. Tel.: 46 17 31 10, 46708 27 80 87(mobile); fax: 46 46 13 61 56. E-mail address: bertil_r.persson@med.lu.se (B.R.R. Persson). 0265-931X/$ e see front matter 2011 Elsevier Ltd. All rights reserved. doi:10.1016/j.jenvrad.2011.01.005

Polonium-210 occurs widely in the terrestrial environment and as an a-emitter, it is an important component of Mans natural radiation background. Its presence in deep soils and minerals may be traced to the decay of radionuclides of the 238U decay chain:

B.R.R. Persson, E. Holm / Journal of Environmental Radioactivity 102 (2011) 420e429


238

421

U>

234

Th >

234

Pa >

234

U>

230

Th >

226

Ra >

222

Rn >

Radon-222 originates from the decay of uranium-238 in the earths crust and diffuses from soil to the atmosphere where its concentration decreases monotonously with height. With a halflife of 3.82 days, 222Rn decays to the short-lived radon daughters: > 218Po (RaA 3.10 min) > 214Pb (RaB 26.8 min) > 214Bi (RaC 19.9 min) > 214Po(RaC164.3 ms). These decay products attach to airborne particles and deposit as dry and wet deposition on the earths surface. The rst daughter 218 Po (RaA 3.10 min) is in radioactive equilibrium with 222Rn at about 5 m above the surface. This is followed by 214Pb (RaB 26.8 min) > 214Bi (RaC 19.9 min) > 214Po(RaC164.3 ms), which are in radioactive equilibrium with 222Rn at about 50 m. The activity concentration of 222Rn and its short-lived decay products at the earths surface (1e10 m) is about 7e2 Bq m3 (Jacobi, 1963). The decay products following 214Po are long-lived radionuclides such as:
210

the mean atmospheric 210Po ux over several decades have been made using cumulative deposits in selected soil cores. Simplied models of the evolution of the vertical distribution of 222Rn, 210Pb and their daughter products 210Bi and 210Po in a vertical column of air moving over the Earths surface have been developed and used to model geographical variations in the 210Po ux long-range transport, which is of major importance when modelling atmospheric fallout in regional domains. As a result of a build-up of 222 Rn concentrations in the atmosphere due to the transport of air masses from west to east over the intervening land surface, there is a corresponding increase in 210Pb fallout within the major continents at northern mid-latitudes. (Appleby, 2008). And modelling suggests that 210Pb concentrations in the Northern Hemisphere are about an order of magnitude higher than in the Southern Hemisphere (Henderson and Maier-Reimer, 2002). 1.3.
210

Po and

210

Pb in ground water and drinking water

>

210

Pb (RaD 22.20 a) > 210Bi (RaE 5.01 d) Po(RaF 138.4 d) > 206Pb(stable).

The natural ground air levels of 210Po varies in the range of 0.03e0.3 Bq m3 and for 210Pb in the range of 0.2e1.5 Bq m3 (Jacobi, 1963; Porstendorfer et al., 1990). The activity concentrations of these long-lived radionuclides increase with height and reach in the stratosphere a maximum estimated to 1.1 Bq m3 for 210Pb, and 1.9 Bq m3 for 210Po (Jacobi, 1963). Atmospheric fallout of these decay products result in the contamination of plants and the top layer of soil with 210Pb, 210Bi and 210Po. Most of the natural radioactivity content in wild leafy plants is 210Po as the result of the direct deposition of 222Rn daughters from atmospheric precipitation (Hill, 1960). The activity ratio of 210Pb/222Rn in ground air is in the order of 104 and the activity ratio of 210Po/210Pb is in the order of 0.05e0.2 (Baskaran and Shaw, 2001; McNeary and Baskaran, 2007). Anthropogenic sources, such as coal or peat combustion and nuclear explosions, have been estimated to contribute less than 1% of 222Rn and 210Pb in the atmosphere (UNSCEAR, 1988). 1.2. Atmospheric fallout of
210

Po and

210

Pb

Since late 1950ies observations of 210Bi/210Pb and 210Po/210Pb activity ratios have been widely used in studying the mean residence time of natural aerosols in the troposphere (Lambert and Nezami, 1965; Papastefanou, 2006; Piliposian and Appleby, 2003; Rastogi and Sarin, 2008). The atmospheric residence time of 210Po varies between 15 and 75 days with a mean value in the order of 26 3 days. Pb-210 is continuously deposited from the atmosphere in association with aerosols at a rate of about 55 Bq m2 a1 over Scandinavia (ElDaoushy and Garcia-Tenorio, 1988). Generally, atmospheric 210Pb concentrations are related to whether the underlying surface is primarily characterised by terrestrial land masses, or by oceanic areas including islands. Surfaces covered by Permafrost, ice and snow reduce the atmospheric 210Pb concentrations (El-Daoushy, 1988). Atmospheric fallout of 210Pb is normally assumed to be constant at any given site, measured on timescales of a year or more. The 210 Po ux may, however, vary spatially by an order of magnitude, depending on factors such as rainfall and geographical location. These basic concepts have been investigated by carrying out direct measurements of 210Po fallout on both short and long timescales, and by developing mathematical models of 210Po in the atmosphere (Piliposian and Appleby, 2003). Direct measurements of 210Po fallout on weekly or monthly timescales using bulk deposition collectors have been made at a number of sites in Europe and beyond. Indirect measurements of

In Directive 98/83/EC, the European Commission requires Member States to monitor the concentrations of natural radionuclides in drinking water. However, radon and its decay products are excluded from the scope of the Directive (Prammer, 1998). Nonetheless, according to a new recommendation, 210Po and 210Pb should not be disregarded in monitoring and in taking action to reduce exposures caused by natural radionuclides in drinking water. The new EC recommendation state reference maximum concentration of 210Pb and 210Po in drinking water to 200 mBq l1 and 100 mBq l1 respectively (Wallstrm, 2001). The activity concentration of 210Pb and 210Po has been investigated in Finnish drinking water from various sources (Vesterbacka, 2007). The highest activity concentrations, 40 mBq l1 of 210Pb and 48 mBq l1 of 210Po, were found in water from drilled wells. The activity concentration in water from dug-wells was much lower, 13 mBq l1 of 210Po and 7 mBq l1 of 210Pb. From water works, however, the activity concentration was as low as 3 mBq l1 for both 210Pb and 210Po. In ground water, 210Po is present in both soluble and particlebound forms. The amount of particle-bound Po-210 depends on the combined concentration of iron and manganese and humic substances (Lehto et al., 1999; Vaaramaa et al., 2003). Solideliquid distribution coefcients (Kd) for Ra, Pb and Th are generally about 10-fold higher than for Po and U, although the number of observations are limited (Pereira et al., 2005; Vandenhove et al., 2009a), It is important to consider the size and composition of deposits in water and sediments in the analysis procedure to achieve high accuracy in application of 210Pb dating procedures (El-Daoushy et al., 1991). The results of studying 210Pb and 210Po in the water column of the Black Sea indicate that biological rather than inorganic particles are the major carrier phases for polonium (Wei and Murray, 1994). Monitoring of radioactivity in mineral waters collected in Italy resulted in 210Po levels in the range 0.04e21 mBq l1, with 72.5% of samples presenting an activity concentration lower than 1.00 mBq l1. Polonium, in fact, has a very low solubility and it only occasionally appears at elevated concentrations in mineral water (Desideri et al., 2007). In Italian drinking water samples, the mean activity concentrations of 210Pb and 210Po were 4 4 mBq l1 and 3 3 mBq l1 respectively. The mean estimated dose to an adult from the intake of water was estimated to 2.8 3.3 mSv a1 due to 210Po, and 2.1 2.1 mSv a1 due to 210Pb while the contribution from 228Ra was 2.4 3.2 mSv a1, 226Ra was 1.8 3.1 mSv a1 and all Uranium isotopes together contributed about 0.8 1 mSv a1 (Jia et al., 2009). Although the concentrations of uranium and radium isotopes are higher, it is obvious that 210Pb and 210Po are among the most

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B.R.R. Persson, E. Holm / Journal of Environmental Radioactivity 102 (2011) 420e429

important dose contributors in drinking water intake. The dose contribution from intake of these radionuclides in drinking water to members of the public in Italy are 48% from radium isotopes (224,226 and 228Ra), 31% from 210Po, and 20% from uranium isotopes (234,235, and 238U) (Jia and Torri, 2007). Occurrence and distribution of 210Pb in selected California groundwater wells, ranged from 3.7 mBq l1 to 1481 mBq l1 and the 210Po activity ranged from 0.25 mBq l1 to 555 mBq l1. Almost 20% of the groundwater wells tested had activity concentrations above the proposed maximum concentration limits set at 37 mBq l1 for 210Pb and 26 mBq l1 for 210Po (Ruberu et al., 2007). In groundwater, samples from Guarani aquifer in Brazil, however, the activity concentrations were much lower resulted in averages of 7 mBq l1 for 210Pb and 2 mBq l1 for 210Po (Bonotto and Bueno, 2008). 1.4.
210

Po and

210

Pb in mosses and peat

Mosses such as Polytrichum and Sphagnum have no mineral uptake from ground, but are occasionally submerged below surface water. Beard mosses Alectroria, however, might be contaminated by re-suspension from soil. In various moss samples collected 1979e1980 around Lilljuhatten in Sweden, the min and max level of 210Po in Polytrichum was 300e960 Bq kg1 dry mass, in Sphagnum 185e700 Bq kg1 dry mass and in Alectoria 570e640 Bq kg1 dry mass (Holm et al., 1981). Moss samples Pterobryopsis tumida from the environment of Kaiga nuclear power plant site in the south western region of India shows a level of 210Po activity as high as 2724 13 Bq kg1 dry mass (Karunakara et al., 2000). In the Gokova Region, where Yatagan is located, there are three major coal-red power plants (CPPs) causing some pollution in the surroundings. The mosses Grimmia pulvinata, Hypnum cupressiforme were investigated for their potential use as bio-indicators for 210 Po and 210Pb deposition. The maximum 210Po and 210Pb activities were observed around the hill close to ash stacks. The efciency of capturing airborne 210Po and 210Pb was highest in the moss species, G. pulvinata with the activity concentration ranges of 600e1228 Bq kg1 for 210Po, and 446e650 Bq kg1 for 210Pb, respectively (Ugur et al., 2003). Levels of 210Po, 210Pb were studied in two of the most common mosses (Lycopodium cernuum and Funaria hygrometrica) in the eastern Mediterranean Sea region (Syrian coastal mountains series). In L. cernuum the activity concentration of 210Po was 1322 and of 210Pb 1140 Bq kg1 dry mass. The moss species F. hygrometrica was found to have even higher values of 210Po and 210Pb with activity concentrations of 2392 and 2119 Bq kg1 dry mass, respectively (Al-Masri et al., 2005). In the region of Katirli Mountain in north western Turkey, mosses have been collected as bio-indicators of environmental radioactive contamination of airborne 210Po and 210Pb activities (Kahraman et al., 2006). Peat mosses are characterized as being primitive plants that grow from the top while the dead bottom part develops to peat. Peat is a heterogeneous mixture of partially humied remains of several groups of plants together with inorganic material. The organic material decomposes to insoluble humic acid and lignin derivatives. The humic and fulvic fractions efciently absorb 210Pb (El-Daoushy and Garcia-Tenorio, 1988). Pb-210 was analyzed in lichen, moss, grass and soil samples, as well as in lake sediments, collected in 1988 from the South Shetland Islands in the Antarctic. The average excess inventory of 210Pb was 280 110 Bq m2 (n 15). From the maximum value of unsupported 210Pb, the annual deposition was estimated to be 18 5 Bq m2 (Roos et al., 1994).

Peat cores collected from three sites in the Jura Region of Switzerland were analysed for the fallout radionuclide 210Pb. Unsupported 210Pb inventories of the cores were all in the order of 4000 Bq m2 and are consistent with the atmospheric deposition of about 130 Bq m2 a1 (Appleby et al., 1996). Data on 210Pb levels in an ombrotrophic peat sequence from a mountain site on the east coast of Ireland were compared with data from a similar sequence at an Atlantic peat-land site on the west coast. The unsupported 210Pb inventory at the east coast site was about 6500 Bq m2 which is higher than at the west coast 5300 Bq m2 and was consistent with the difference in wet deposition at the two sites (Gallagher et al., 2000). In Fig. 1, the proles of unsupported 210Pb in peat cores sampled 1979 by Elis Holm in Sweden is presented. Peat cores of about 0.5 m in depth through bog hummocks with Sphagnum species were sampled at Stordalen in the North and Getamossen in the South of Sweden. The unsupported 210Pb inventory at Stordalen was 1300 350 Bq/m2 and at Getamossen 4000 650 Bq/m2. The corresponding average activity concentrations of 210Pb in the upper 12 cm of the peat prole were 192 37 Bq kg1 dry mass at Stordalen and 439 117 Bq kg1 dry mass at Getamossen. The 210Pb dating method is reliable only in the lower parts, i.e. layers that are more than 50 years old, due to the mobility of lead in the upper parts of the prole (Malmer and Holm, 1984). According to our previous investigations of the distribution of fallout radionuclides in lichen carpets the activity concentration (Bq kg1) varies with depth z according to the equation (Mattsson, 1972; Persson et al., 1974):

log Az a b$z0:75
The activity concentration at different depths in peat cores collected in the south of Sweden at the Toftahult peat-land site exhibit different depth proles of 210Po and 210Pb as shown in Figs. 2 and 3.These proles indicate that 210Pb is mobile in the upper part of the prole, while 210Po is xed to the top layer. 1.5.
210

Po and

210

Pb in communities of lichen (Cladonia alpestris)

In the studies of fallout from the atmospheric nuclear weapons tests during 1950ies and 60ies high activities of 137Cs were found in lichens (Svensson and Lidn, 1965). In the Nordic countries lichens of the Cladonia family are grazed by reindeer which are consumed by man to whom, by this way, the radioactive fallout was

Fig. 1. The proles of unsupported

210

Pb in peat cores at Stordalen and Getamossen.

B.R.R. Persson, E. Holm / Journal of Environmental Radioactivity 102 (2011) 420e429

423

Fig. 2. 210Po activity distribution according to the z3/4 depth distribution (Persson et al., 1974).

transferred (Svensson and Lidn, 1965; Witkamp, 1966). Evidently the same pathways apply for the naturally occurring fallout radioisotopes 210Po and 210Pb (Persson, 1970b). Lichens are slowly growing perennials that have high interception potentials for aerosols in precipitation, and therefore contain signicantly higher 210Po and 210Pb concentrations than vascular plants (Holtzman, 1966; Jaworowski, 1969; Kauranen and Miettinen, 1969; Kauranen et al., 1971) and fungi (Skwarzec and Jakusik, 2003). The 210Po/210Pb activity ratio in lichen is typically equal to one as 210Po approaches secular equilibrium with 210Pb (Kauranen and Miettinen, 1969; Kauranen et al., 1971; Mattsson and Persson, 1971; Persson, 1970a, 1972; Persson et al., 1974; Thomas et al., 1994). Measurements of 210Po in communities of lichen (C. alpestris) in central Sweden during the past 40 years seem to indicate a quite constant level of about 560 70 Bq m2 with an average activity concentration of about 250 Bq kg1 dry weight, and a 210Pb/210Po activity ratio of 1.0 0.1. The specic activity of 210Pb was about 23 2 Bq mg1 of stable lead (Persson, 1970a, 1970b, 1972, 1974; Persson et al., 1974).

Fig. 4. Results from measurement of 210Po in communities of lichen samples from different counties. By assuming radioactive equilibrium the levels are equivalent to 210 Pb. a)(Ramzaev et al., 1969); b)(Persson, 1972); c)(Blanchar and Moore, 1970); d)(Jaworowski, 1969); e)(Holtzman, 1966); f)(Kauranen and Miettinen, 1969); g)(Blanchar and Moore, 1969); h)(Hill, 1965); i)(Kauranen et al., 1971); j)(Holtzman, 1966); k)(Kauranen et al., 1971); l)(Holtzman and Ilcewicz, 1971); m)(Skuterud et al., 2005); n)(Ugur et al., 2004).

The measurement of 210Po in communities of lichen samples from different counties are displayed in Fig. 4. Assuming radioactive equilibrium, the levels are equivalent to 210Pb. There is a slight decrease during this period from 1894 to 2003 although this decrease is not signicantly different from zero (p 0.23). There is, however, a large variation in lichen species, sampling locality, and analytical method. Measurements of 210Po in communities of lichen (Cladonia alpestris) at a specic location 63.2 N in central Sweden (LakeRogen) during 1961e1970 are displayed in Fig. 5.The results indicate a more pronounced decrease 3.7% per year although again the decrease is not signicantly different from zero (p 0.08). During the same period the specic activity of 210Pb/Pbstable shown in Fig. 6 was quite constant at 23 2 Bq per mg of stable lead. Linear regression with respect to wet weights given to the error of each value, indicate a quite constant value at 22 Bq/mg during this period (Persson, 1972, 1974).

Fig. 3. 210Pb activity distribution according to the z3/4 depth distribution (Persson et al., 1974).

Fig. 5. Radioactivity concentration of annually in Sweden 63,2 N.

210

Pb in lichen (Cladonia alpestris) collected

424

B.R.R. Persson, E. Holm / Journal of Environmental Radioactivity 102 (2011) 420e429

Fig. 6. The ratio of 210Pb activity concentration to stable lead concentration in lichen (Cladonia alpestris) collected annually in Sweden 63,2 N.

The values recorded in Sweden in 1970 at Rogen 63,2 N agree very well with the values recorded in Norway in 2001 (Skuterud et al., 2005). Thus during the past 40 years there seems to have been a quite constant level of 210Po fallout. The question is, however, if the 210Po fallout will change with future progressed climate changes. More rigorous studies of seasonal variations of 210 Po/210Pb activity ratio as well as cosmogenic 7Be might be used to investigate the impact of climate change on terrestrial ecological systems particularly in the polar regions (Rosswall, 1989, 1994). Stable lead, 210Pb and 210Po levels has been determined in dated sequential growth of thalli of the foliose lichen Flavoparmelia baltimorensis from Great Falls and Plummers Island, Maryland. (Schwartzman et al., 1991). The average 210Po level derived from their experimental data was estimated to 109 11 Bq mL2 and the 210 Pb level 142 14 Bq mL2 corresponding to an activity concentration of 64 Bq kg1. The specic activity of lead, 210Pb/Pbstable, was estimated to 72 11 Bq per mg of stable lead. Those values are in the same order of magnitude as the other studies referred to above. They also conrm the decrease of the specic activity, 210Pb/Pbstable, which was due to the release of stable Pb into the atmosphere by using leaded gasoline for automobiles (Persson, 1972, 1974; Persson et al., 1974). 2. 2.1.
210

Po and Po and

210

Pb in the terrestrial food chains Pb in the food chain lichen-reindeer and man

210

210

The food chain: lichen-reindeer man has been used to model the terrestrial food chain for human uptake of 210Pb and 210Po and to study the specic activity ratio of 210Pb/Pbstable in a historical perspective (Persson, 1970b). However, observations had already been made in the 1960ies by several investigators that northern diets, based largely on reindeer or caribou, contained abnormally large amounts of fallout nuclides from nuclear weapons tests (Liden, 1961) as well as natural 210Po and 210Pb (Baskaran et al., 1991; Blanchar and Moore, 1970; Blanchar and Moore, 1970; Kauranen and Miettinen, 1969; Macdonald et al., 1996; Persson et al., 1974). Measurements of 210Po activity concentrations in reindeer meat samples from Finnish Lapland showed activity concentrations of about 3 Bq kg1 wet weight in Autumn, 5 Bq kg1 wet weight in Winter and 12 Bq kg1 wet weight in Spring. For 210Pb the annual average activity concentrations in reindeer meat were ten times

lower, i.e. 0.22 0.04 Bq kg1 wet weight, with less seasonal uctuation. This maintains a high 210Po concentration in soft tissues of reindeer breeding Lapps (about 12 times higher than in the southern Finish population) (Kauranen and Miettinen, 1969). This was shown to be true also for Alaskan residents consuming caribou or reindeer meat (Blanchar and Moore, 1970). Po-210 average activity concentrations in Swedish reindeer meat samples from animals slaughtered in March 1970 and 1971 was 10.6 0.6 Bq kg1 wet weight. These animals, two years old, had grazed within the same reindeer breeding district where the lichen sampling area was situated (Mattsson and Persson, 1971; Persson, 1972, 1970b, 1974). In the bone of reindeer from the island Novaya Zemlya in the Arctic Sea, the concentrations 210Po and 210Pb in bone of recent reindeer (570 190 Bq kg1) was similar to that which was in the teeth of reindeer that existed one hundred years ago (650e750 Bq kg1) but signicantly higher than in recent mainland reindeer from different regions (180e170 Bq kg1) (Klevezal et al., 2001). Po-210 was analyzed in tissues from caribou (Rangifer tarandus) in Canada between 1992 and 1994. The highest mean bone and liver Pb-210 activities were observed on south Bafn Island, which included one bone sample with 3800 Bq kg1 wet weight of Pb-210 and 3070 Bq kg1 wet weight of Po-210. These high values were attributed to high atmospheric deposition rates and lichen species composition. In samples collected during 1989e1994 from various caribou herds in the Canadian Arctic, the mean activity concentration of 210Pb in femur and jaw was around 610 (490e800) Bq kg1 (Macdonald et al., 1996). This compares well with the level of 170 190 Bq kg1 wet weight, found in Finnish reindeer during 1964e1967 (Kauranen and Miettinen, 1969). By allowing 14 volunteers to consume 2.0 kg of caribou meat containing 9e40 Bq kg1 wet weight, and collecting urine and fecal sample, the average GI absorption factor was estimated to be 56 4%. This value agreed well with the value of 50% recommended by the ICRP (ICRP, 1994; Thomas et al., 2001). A study of concentrations of 210Po and 210Pb in Norwegian reindeer during years 2000e2003 focused on potential differences in concentrations of these nuclides in reindeer of different ages (Skuterud et al., 2005). Concentrations of 210Po and 210Pb in muscle and liver tissues collected in central (stre Namdal) and southern Norway (Vg) showed no signicant difference in 210Po and 210Pb concentrations between adults and calves or between reindeer from the two different study areas. Mean 210Po activity concentrations in muscle tissue from December 2000, were 23.7 3.7 and 35.5 9.2 Bq kg1 dry mass in calves and females (7 years) respectively, which were not signicantly different from those in 2002. These values corresponds to 6 1 and 9.2 2.3 Bq kg1 wet weight respectively, which is in agreement with the values recorded in Sweden in 1970e71 (ICRP, 1994; Mattsson and Persson, 1971; Persson, 1970b, 1972, 1974). The 210Pb and 210Po activity concentrations determined in muscle and liver tissue of reindeer from Norway were similar to values reported from other Nordic areas (Gwynn et al., 2006; Kauranen and Miettinen, 1967, 1969; Persson, 1972, 1974; Skuterud et al., 2005; Tracy, 1993). The transfer of 210Pb, and 210Po through the lichen-caribouhuman food chain were analyzed in tissues from 18 barren-ground caribou (Rangifer tarandus groenlandicus) collected in mid-March 1995 approximately 60 miles north of the community of Wollaston Post in Canada. The activity average concentration (wet weight) of 210 Pb, and 210Po in bone was 670 40 Bq kg1 and 220 30 Bq kg1 and in muscle tissue 1.1 0.3 Bq kg1 and 14 0.6 Bq kg1. The effective annual dose in man due to 210Pb, and 210Po by consuming 100 g per day of that caribou meat was estimated to 28 and 610 mSv a1 respectively (Thomas and Gates, 1999).

B.R.R. Persson, E. Holm / Journal of Environmental Radioactivity 102 (2011) 420e429

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2.2.

210

Po and

210

Po in soil

Airborne particles, with attached 210Pb and 210Po, are carried back to the earths surface through fallout resulting in the deposition and accumulation of the nal long-lived 210Pb (22.3 a) which decays to 210Bi (5 d), 210Po (140d) and nally to stable 210Pb in plants or the top soil. Most of the natural radioactivity content in wild leafy plants is 210Po resulting from the direct deposition of 222Rn daughters from atmospheric precipitation (Hill, 1960). Soil consists of particles of different minerals as well as organic matter in various stages of degradation. It is one of the most important components in the evaluation of radionuclide migration behaviour and distribution of uranium series radionuclides and thus 210Po and 210Pb in a terrestrial ecosystem. The 210Po in soils may originate either as a product of the radioactive decay of radionuclides of 238U series present in the soil (supported) or the result of the precipitation of radon decay products from the atmosphere (unsupported). The 210Po content of soil varies with soil type. The levels of 210Pb and 210Po contained in the top layer of soil can be correlated with the amount of atmospheric precipitation. In soils, 210Po is in equilibrium with 210Pb, suggesting that the 210Pb in the soil is the main source of 210Po irreversibly adsorbed on clay and organic colloids in the soil (Parfenov, 1974). The average activity concentration levels of 210Po in various soils are in the range of 20e240 Bq kg1 (Al-Ari et al., 2006; Hasanen, 1977; Karunakara et al., 2000; Myrick et al., 1983). The vertical distribution of 226Ra and 210Po has been investigated in the cultivated soils of the Buyuk Menderes Basin in Turkey (Akyil et al., 2008). The activity concentrations of soil cores range from 80 to 1170 Bq kg1 for 226Ra and from 10 to 870 Bq kg1 for 210Po with depth. Analysis of the vertical soil proles indicate that the activity concentrations of 226Ra and 210Po for soil strata at all sites did not change to an extreme degree with depth. Although the activity concentrations of 210Po are slightly higher in the surface of all the soil cores while the activity concentrations of 226Ra are slightly lower. The distribution of 210Pb and 210Po concentrations in soil from two districts located in the southwest region of Syria have recently been studied (Al-Masri et al., 2008). The soil of Daras elds was originated by the erosion and degradation of basaltic volcanic primary rocks, which formed dark brown soils, while the soil of Daher Al-Jabal site is clay texture >30% and reddish brown or dark red colour. Due to soil cultivation, homogeneous distributions of the studied natural radionuclides with depth were observed. However, differences were found for 210Pb and 210Po concentrations, where high levels of these two radionuclides were observed in the top soil layers. The 210Po concentrations varied between 1.2 and 110 Bq kg1. The highest concentration (110 Bq kg1) was also found to be in the grape eld soil of Daher Al-Jabal, which also exhibited the highest concentration of 226Ra (36 Bq kg1 and 238U (33 Bq kg1) (Al-Masri et al., 2008). Phosphate fertilizers are derived from phosphate ores containing 210Pb and 210Po (Al-Masri et al., 2002; Othman et al., 1994). Most of the contaminants are left in the solid gypsum waste, and some of the 210Pb and 210Po are transferred to the fertilizers (Aoun et al., 2010; Rutherford et al., 1994). Disposing gypsum waste directly into the environment and the use of phosphate fertilizers may affect the levels of 210Pb and 210Po in water sediments and soil (Aoun et al., 2010; Barisic et al., 1992; Becker, 1985; Carvalho, 1995). The phosphate industry is claimed to be a major source of enhancement of 210Pb and 210Po in the surrounding environment (Jimenez et al., 2007). The environmental effects of Po-210, Pb-210 and Ra-226 input from waste of the phosphate industry and the use of phosphate as fertilizer has been extensively studied in the south west of Spain (Jimenez et al., 2007; Martinez-Aguirre et al., 1996, 1997; Tome

et al., 2003). These studies have generated extensive knowledge about mechanisms in the transfer of these radionuclides to plants as reviewed in the section below. 2.3. Transfer of
210

Po and

210

Po from soil to plants

Uptake of radionuclides from soil to plant is characterized using a transfer factor (TF) which is dened as the ratio of radionuclide activity concentration per unit mass concentrations (Bq kg1) of plant (Cplant) and soil (Csoil) respectively. TF Cplant/Csoil The TF for a given type of plant and for a given radionuclide can vary considerably from one site to another, with season and with time after contamination. These variations depend on several factors such as the physical and chemical properties of the soil, environmental conditions, and chemical form of the radionuclide in soil. Usually a linear relation implies a constant ratio of plant concentration to soil concentration (Al-Masri et al., 2008). However, variations in soil properties such as mineralogical composition, organic matter content, and pH as well as fertility components affect uptake resulting in a non-linear relation (Martinez-Aguirre and GarciaLeon, 1995; Martinez-Aguirre et al., 1996, 1997). Indeed, it has been shown, for radionuclides from the 238U decay chain, that the relationship between the TF and the specic activity in the substrate soil seems to be hyperbolic. From experimental measurements of the transfer factor of the plant Spartina densiora in the Odiel river estuarine system in Spain, the following relationship was found for 210Po (Perianez and MartinezAguirre, 1997). TF 2.456 [Csoil]0.663 Vegetation is also contaminated by 210Pb and 210Po by direct deposition (Ewers et al., 2003). Most of the natural radioactivity content in fresh outdoor living plants is 210Po as the result of the direct deposition of 222Rn daughters from atmospheric precipitation. Already in the 1960ies it was estimated that about 80% of the radioactive materials in plants was due to 210Po as a result of the direct deposition of 222Rn daughters from atmospheric precipitation (Hill, 1960; Mayneord et al., 1960). Plants, however, get radioactive nuclides both by absorption from the soil (supported Po) and by deposition of radioactive fallout on the plants directly (unsupported Po). Therefore, the 210Po in soil contributes to the uncertainty of using plants with root system as monitors for deposition of 210Po. Studies on transfer of natural radionuclides from soil to plant have been carried out in different regions in the world (Bunzl and Trautmannsheimer, 1999; Ewers et al., 2003; Paul and Pillai, 1986; Pulhani et al., 2005; Tome et al., 2003; Tracy et al., 1983). A systematic study has been carried out on 210Po in soil and vegetation samples in the south western Spain. The vertical prole of 210 Po in soil, variation of activity with particle size, activity concentration in vegetation, seasonal variation of activity and dry deposition rate were studied. Studies have also been made for those plants used for human use and consumption (Martinez-Aguirre and Garcia-Leon, 1994; Martinez-Aguirre and Perianez, 1998, 1999; Martinez-Aguirre and GarciaLeon, 1995; Martinez-Aguirre et al., 1996, 1997; Simon and Fraley, 1984; Simon and Ibrahim, 1987; Staven et al., 2003). Transfer factor estimates for major crop groups (Cereals, Leafy vegetables, Non-leafy vegetables, Root crops, Tubers, Fruits, Herbs, Pastures/grasses, Fodder), and also for some compartments within crop groups have recently been reviewed and compiled (Vandenhove et al., 2009b). 2.4.
210

Po and

210

Pb in tobacco

In 1964, it was pointed out that appreciable concentration of polonium-210 occur in tobacco which is inhaled by smoking

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(Radford and Hunt, 1964). The concentration of polonium-210 in tobacco is highly affected by the use of phosphate fertilizers (Nain et al., 2006; Santos et al., 1992; Tso et al., 1968). The activity concentrations in tobacco harvested at different years in various countries are displayed in Fig. 7. The overall average activity concentration of 210Po is 13 2 Bq kg1, and tends to be rather constant over time and with respect to geographical location. The average 210Po activity content of one cigarette is about 20 mBq. Some brands, however, have a 210Po activity content as low as 4 mBq per cigarette. By smoking, polonium is volatilized, which is evidenced by the low 210Po activity measured in cigarette ash as compared with the total content in an unburned cigarette. The fraction of 210Po contents of the ash varied between 4 and 65% of the content in fresh tobacco (average 26 24%) of different brands. Prior to smoking, the 210Po activity of lters was small, with values in the range of 0.02e0.76 mBq. The lters absorbed only about 0.1e16.5% (mean value 2.5) of the polonium contained in the tobacco (Skwarzec et al., 2001). This effect is due to the different tobacco-burning temperatures of smoking (between 500 and 700  C), which cause 210Po to sublime more or less into the smoke which is inhaled by the smoker (Martell, 1974). Therefore the activity of 210Po in smoke inhaled from a cigarette varied a lot, ranged from 2 to 23 mBq with an average of 10 6 mBq. The average (range) activity concentration of 210Po in cigarette tobacco of Greece was 16.6 (9.7e22.5) mBq/cigarette. The average percentages of 210Po content in fresh tobacco plus wrapping paper that were recovered by post-smoking lters, ash and smoke were 4.6, 20.7 and 74.7, respectively. It was estimated that cigarette smokers are inhaling on average 6 mBq per cigarette of 210Po and 210 Pb each which is in good agreement with the value given above (Khater, 2004). Assuming a light smoker (3 cigarettes per day) inhales about 10 Bq per year by smoking and that the dose-conversion factor is 1.1 mSv per Bq, the annual committed dose equivalent is 11 mSv a1 (UNSCEAR, 2000). For a heavy smoker (30 cigarettes per day) the annual committed dose equivalent is in the order of 100 mSv a1. 2.5.
210

Po and

210

Pb in general food

210 Po and 210Pb ingested with foodstuffs is considered to contribute signicantly to the internal radiation dose to man. The

data on 210Po and 210Pb concentrations in daily foods reported by various authors indicate that their concentrations depend on the geological, climatic and agricultural conditions. Various terrestrial general food chains contribute to various extents and range from 40 to 400 mBq of polonium-210 per day corresponding to an annual intake of about 10e100 Bq (UNSCEAR, 2000). Direct dry and wet deposition of 210Po and 210Pb on leafy plants enhance the concentration of unsupported 210Po in vegetables (Hill, 1960, 1965; Radford, 1974). Accumulation of 210Po in marine food chains contribute considerably more (about 80%) to the total 210Po ingestion than food of terrestrial origin (Carvalho, 1995; Heyraud and Cherry, 1979; Lee et al., 2009). To provide an overview of radiological implications of 210Po in general food, samples of cereal, fruit, root and green vegetables were collected from 11 sites, including regions of potential enhanced levels of 210Pb and 210Po (McDonald et al., 1999). Considerable variability was evident in levels of 210Pb and 210Po from all sites and in all food types investigated. Ordering the data expressed on a fresh mass basis in descending activity and by food type, the highest activity concentration of 210Pb was found in liver (0.2 1.3 Bq kg1) and cereals (0.1 0.7 Bq kg 1). The average in most other foodstuffs was 0.005 0.29 Bq kg1. Generally, the lowest concentrations were found in root vegetables 0.005 0.02 Bq kg1. Similarly, for 210Po, higher concentrations are present in liver (0.5 3.0 Bq kg kg1) and cereal (0.01 0.6 Bq kg1) than in other foodstuffs (typically 0.001 0.15 Bq kg1). High levels of 210Po (0.43 Bq kg1) were found in Blackberries, with levels similar to those found in wild berries in Finland (Vaaramaa et al., 2007). The maximum dose arising from consumption of 210Pb and 210Po in foods surveyed in this study is estimated to be around 120 mSv per year to adults. This compares with an estimated UK average consumption dose from all nuclides and foodstuffs of 300 mSv per year (broad range 100e1000 mSv a1) (McDonald et al., 1999). In the Korean population, the effective dose from 210Po for an adult was estimated to about 270 mSv per year with about 80% contributed from consumption of seafood (24 kg a1) due to its high activity concentration (19e33 Bq kg1 fresh). The consumption of terrestrial food was much higher (360 kg a1) but with an average activity concentration of 0.15 Bq kg1 fresh weight (Lee et al., 2009). The distribution and activity intake of 210Pb and 210Po in food, diet, and potable water have been studied in samples from Goa. The activity concentration of 210Pb in sh and prawn samples were signicantly higher than concentrations found in vegetable and rice samples. Activity concentrations of 210Pb and 210Po were higher in leafy vegetables than in non-leafy vegetables. The annual committed effective dose due to ingestion 210Pb from various diets was found to be 82 mSv a1 due to non-vegetarian meal and 60 mSv a1 due to vegetarian meal, and of 210Po 95 mSv a1 and 50 mSv a1, respectively (Avadhani et al., 2001). Consumption of seafood is the cause of the relatively high intake of 210Pb and 210Po ratio in the diet (UNSCEAR, 2000). The median daily dietary intakes of 210Pb and 210Po for each Japanese adult was estimated to 200 mBq and 610 mBq (Yamamoto et al., 2009), corresponding to annual effective doses 50.4 mSv and 267 mSv a1 (based on cofcients from ICRP, 1991), respectively. Portuguese are also known to consume relatively large quantities of seafood, and their individual daily intake levels of 210Pb and 210Po were estimated to be 470 mBq and 1200 mBq, respectively (Carvalho, 1995). 3. Summary and discussions

Fig. 7. Activity concentrations in tobacco harvested at different years in various countries. a (USA)(Tso et al., 1964); b (USA)(Tso et al., 1966); c (NZ,USA)(Gregory, 1965); d (Peres and Hiromoto, 2002); e (Greece)(Savidou et al., 2006); f (Pakistan) (Tahir and Alaamer, 2008).

The long-lived radionuclides 210Pb and 210Po in the terrestrial environment are the nal radionuclides in the decay chain 238U in the ground. The noble gas Radon-222 originates from the decay of

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427

uranium-238 in the earths crust and diffuses from soil to the atmosphere and decays to 210Pb and 210Po. The natural ground air levels of 210Po varies in the range of 0.03e0.3 Bq m3 and for 210Pb in the range of 0.2e1.5 Bq m3 The activity concentration of these long-lived radionuclides increase with height and reaches a maximum in the stratosphere estimated to 1.1 Bq m3 for 210Pb, and 1.9 Bq m3 for 210Po. Atmospheric fallout of 210Pb is normally assumed to be constant at any given site, measured on timescales of a year or more. The 210 Po uxes may, however, vary spatially by an order of magnitude, depending on factors such as rainfall and geographical location. There is a west to east increase in 210Pb fallout within the major continents at northern mid-latitudes and in the Northern Hemisphere it is about an order of magnitude higher than in the Southern Hemisphere. The activity concentration of 210Pb and 210Po in drinking water from private wells are in the order of 11e40 and 7e48 mBq l1 respectively. From water works, however, the activity concentration is only in the order of 3 mBq l1 for both 210Pb and 210Po. Although the concentrations of uranium and radium isotopes and radon in drinking water are much higher than 210Pb and 210Po, these are among the most important dose contributors in drinking water. The mean estimated annual dose to an adult from the water intake was estimated to be in the order of 3 mSv a1 due to 210Po and 2 mSv a1 due to 210Pb, while the contribution from 228Ra is 2 mSv a1 , 226Ra is 2 mSv a1 and all Uranium isotopes together was estimated to be about 1 mSv a1. Mosses and peat are highly efcient at capturing 210Pb and 210Po from atmospheric fallout and exhibit high inventory of 210Pb and 210 Po in the order of 0.5e5 kBq m2. The high efciency by mosses and peat of capturing airborne 210Po and 210Pb makes them useful as bio-indicators of environmental radioactive contamination. Unsupported 210Pb inventories of peat correlate with the seasonal variations in atmospheric deposition and long-term studies of the temporal variations might be used for studying the effect of climate change on the terrestrial biosphere. Lichens are slowly growing perennials that have high interception potentials for aerosols in precipitation, and therefore contain signicantly higher 210Po and 210Pb concentrations than vascular plants. The measurement of 210Po in communities of lichen (Cl. alpestris) samples from North Europe indicate a quite constant average activity concentration of about 250 Bq kg1 dry weight, and a 210Po/210Pb activity ratio close to one. The level of 210Po and 210Pb activity in lichen is quite high and, as a consequence of their extensive grazing of lichen, the activity concentration of these radionuclides in reindeer or caribou meat is about 1e15 Bq.kg1, which should be compared with 0.08 Bq.kg1 in ordinary esh and meat on the market. Due to the high intake of these radionuclides in the food chain lichen-reindeer or caribou, and Man, this system constitutes a unique model for studying the uptake and retention of 210Po and 210Pb in humans. The effective annual dose due to 210Po, and 210Pb in people with a high consumption of reindeer/caribou meat is estimated to be around 260 and 132 mSv a1 respectively. Although reindeer meat is regularly consumed by a minor part of the world population more efforts should be taken to support studying this unique food chain. The 210Po content of soil varies with the type of soil. The levels of 210 Po and 210Pb contained in the top layer of soil correlate with the amount of atmospheric precipitation. Deeper in the soil, 210Po is in equilibrium with 210Pb, suggesting that the 210Pb in the soil is the main source of 210Po and irreversibly adsorbed to clay and organic colloids in the soil. The average activity concentration levels of 210 Po in various soils are in the range of 20e240 Bq kg1. Phosphate

fertilizers are derived from phosphate ores containing 210Pb and 210 Po. Most of these radionuclides are left in the solid gypsum waste, and some of the 210Pb and 210Po are transferred to the fertilizers. Disposing gypsum waste directly into the environment and the use of phosphate fertilizers may affect the levels of 210Pb and 210Po in water sediments and soil. The phosphate industry is claimed to be a major anthropogenic source of 210Pb and 210Po in the environment. Uptake of radionuclides from soil to plant is characterized by using a transfer factor (TF) which is dened as the ratio of activity per unit mass (Bq kg1) of plant (Cplant) and soil (Csoil) respectively. The TF for a given type of plant and for a given radionuclide can vary considerably from one site to another, with season and with time after harvesting. These variations depend on several factors such as the physical and chemical properties of the soil, environmental conditions, and chemical form of the radionuclide in soil. Plants, however, receive radioactive nuclides both by absorption from the soil (supported Po) and by deposition of radioactive fallout on the plants directly (unsupported Po). In fresh leafy plants, 210Po is particularly high as the result of the direct deposition of 222Rn daughters from atmospheric deposition. Tobacco is a terrestrial product with high activity concentrations of 210Po and 210Pb. The overall average activity concentration of 210 Po is 13 2 Bq kg1, at levels that are rather constant over time and with respect to geographical location. Assuming that a light smoker (3 cigarettes per day) inhales about 10 Bq per year by smoking and that the dose-conversion factor is 1.1 mSv per Bq, the annual committed dose equivalent is 11 mSv a1 (UNSCEAR, 2000). For a heavy smoker (30 cigarettes per day) the committed annual dose equivalent is in the order of 100 mSv a1. Due to the impact of 210 Po and 210Pb activity levels in tobacco on human health, it has been suggested mandatory to specify the amount of inhaled 210Pb on the cigarette package of each brand (Tahir and Alaamer, 2008). This might conduce to minimize the activity concentrations of levels of 210Po and 210Pb in tobacco by studying the growing conditions and fallout levels in the tobacco elds (Muggli et al., 2008). The average median daily dietary intakes of 210Po and 210Pb for the adult world population was estimated to 160 mBq day1 and 110 mBq day1, corresponding to annual effective doses of 70 mSv a1 and 28 mSv a1, respectively. The dietary intakes of 210Po and 210Pb from vegetarian food was estimated to only 70 mBq day1 and 40 mBq day1 corresponding to annual effective doses of 30.6 mSv a1 and 10 mSv a1, respectively. Since the activity concentration of 210Pb and 210Po in seafood are signicantly higher than in vegetarian food, the effective dose to populations consuming a lot of seafood might be 5e15 fold higher. Acknowledgement This article is dedicated to our former tutor, Professor Kurt Lidn (1915e1987). The rst professor of Medical Radiation Physics at Lund University (1964e1980). Pioneer in studying Environmental Radioactivity. References
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