A record of atmospheric 210 Pb accumulation in the industrial city

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A record of atmospheric 210 Pb accumulation in the industrial city E.A. Buraeva, V.S. Malyshevsky 1, V.V. Stasov, L.V. Zorina Southern Federal University, 344090, Rostov-on-Don, Russia B.I. Shramenko National Science Center «Kharkov Physical-Technical Institute», 61108, Kharkov, Ukraine Abstract The deposition flux of total atmospheric 210 Pb in the industrial city Rostov-on-Don, Russia from 2002 to 2010 has been measured. The variations in annual 210 Pb deposition flux appear to be mainly correlated with the number of rains and significant amount of anthropogenic 210 Pb, polluted into the surface layer of air in the homeheating period. The average 210 Pb deposition is 1.75 mbq/m 3. Several meteorological parameters which are strongly associated with the fluctuations of concentrations of 210 Pb are identified. These results are useful to provide typical information on the atmosphere radioactivity in an industrial city. Keywords: Lead-210, radioactive lead, atmospheric deposition, precipitation. 1. Introduction Natural radionuclide of terrestrial origin 210 Pb is decay products of 238 U. The half-lives of this radionuclide is 22.3 years. The 210 Pb appears in the atmosphere from the decay of inert gas 222 Rn. The higher levels of radon in the air is characteristic of areas with radioactive anomalies in uranium deposits, as well as in areas of tectonic faults. Thus the 222 Rn (and as a result 210 Pb) may be either of natural and technogenic origin (for instance, due to various processes with the mineral raw materials). The purpose of this paper is to determine the characteristics of the climate effects, weather, and possibly man-made factors on the variation of 210 Pb in aerosols and precipitation in the surface air of industrial city Rostov-on-Don, Russia (moderate latitudes and temperate arid climate. Latitude: 47 14.1834' N, Longitude: 39 42.8334' E). The long-term monitoring of radioactivity in air provides useful information about the radiation in the environment due to natural and man-made sources and helps to evaluate their impact on man. Monitoring of the 210 Pb behavior in the atmosphere is carried out in different laboratories. Here are just some of the earlier studies. For instance, concentration 210 Pb in air was continuously monitored, using a high-volume air sampler and a high-resolution gamma-ray spectrometer, at the University of Málaga (Duenas C., et.al. 2009). Studies of radionuclide activities in aerosol particles have been carried out by Duenas C. et.al. (2011). The 210 Pb deposition over the North Sea was investigated by Beks J.P. et. al. (1998). Activity concentrations of the long-lived natural radionuclide 210 Pb in surface air were measured by Hotzl H. et.al. (1987) twice monthly at a semi-rural location 10 km north of Munich (FRG) for the time interval 1983-1985. The 7 Be to 210 Pb concentration ratios in ground level air on two monitoring stations in Belgrade area were determined from 1996 to 2001 by Todorovic D. et.al (2005). 1 Corresponding author. E-mail address: vsmalyshevsky@sfedu.ru

According to Todorovic D. the 7 Be to 210 Pb ratios were in the range of 1.7 12.7, with summer maxims and winter minimums. There is a strong correlation between the seasonal radionuclides concentrations and the seasonal average of temperature; it is quite likely this is one of the master variables that control the amount of radionuclides concentrations in air (Azahra M., et. al. 2004). The results presented in this paper are a part of research on atmospheric radioactivity in the south of Russia (Buraeva E.A. et. al. 2007). 2. Experimental Measurements of the 210 Pb content in aerosols (1 per week) and precipitation (1per month) are performed at the aspiration station of the Southern Federal University (Rostov-on-Don, Russia) in 2002 2010 as part of the monitoring of the radioactivity of the atmospheric layer at the ground in Rostov-on-Don (47 14 NL; 39 42 EL). The location of the station at temperate latitudes with a temperate continental climate and comparatively low precipitation imparts special significance to the systematic monitoring of 210 Pb in the atmosphere. A ventilation setup with a filter consisting of FPP-15-1.7 Petryanov fabric with total area 0.56 m 2 and a liquid Lambrecht micromanometer were used to obtain the samples. According to the measurements, the air flow rates were approximately 630 m 3 /h initially ( fresh filter) and 510 m 3 /h after 7 days of exposure. The exposed filter was air dried and pressed into 35 mm in diameter and 10 30 mm high pellets. Three or four days after the filter was removed, the γ-ray spectrum was measured in 12 24 h with a Ge(Li) or HPGe detector of the low-background setup. The dust content in air was found according to the mass difference between the exposed and clean filter. 3. Results and discussion The 210 Pb volume activity in the lower atmosphere of industrial city Rostov-on-Don (Russia) was measured during 2002-2010. In general, the activity of 210 Pb in the lower atmosphere varies within a wide range (0,12-9,05) mbq/m 3, with the average for the whole period of observation 1.75 mbq/m 3 (see Fig.1 and Table 1). Obviously, regardless of the origin of 210 Pb (natural or man-made) its content in atmospheric aerosols decreases with the increase in rainfall due to more intensive leaching. Additionally for the natural 210 Pb decreases due to reducing the rate of radon exhalation from the moist soil as well. The maximum values of the activity 2.2-3.3 mbq/m 3 achieved with a combination of relatively high temperatures 16-26 0 C and the relatively small amount of precipitation 29-43 mm/month (Table 2).

Seasonal dependence of the 210 Pb activity is shown in Fig. 2. To illustrate the overall picture of the relationship of the individual parameters that characterize the radioactivity of the atmosphere, we present their seasonal dependence, averaged over the whole observation period (Fig.3). It is seen that in the winter months with minimal amounts of precipitation and minimum temperatures the 210 Pb activity in aerosols reach the highest values. This can only be associated with a significant amount of anthropogenic 210 Pb, polluted into the surface layer of air in the home-heating period. High values of 210 Pb activity of anthropogenic aerosols are accompanied by stability of the atmosphere in the winter. A slight increase in activity in the winter after the 2006 is associated with colder winters in these years and as a consequence a great burning of fossil fuels. The low 210 Pb activity values in aerosols in this period (for instance in March) associated with the turbulent mixing in certain months. For the spring-summer period the behavior of the 210 Pb activity are explained by the restructuring of the spring atmosphere and the maximum amount of precipitation in June. This maximum rainfall separates spring and summer maximum of 210Pb activity for two (April and September) and deposition density of 210 Pb on the Earth's surface in June. Acknowledgement This work is supported by Federal Program of the Russian Ministry of Science and Education "Scientific and scientific-pedagogical personnel of innovative Russia" (grant number 14.A18.21.0633) and Russian Foundation for Basic Research and by National Academy of Sciences of Ukraine grant number 12-08-90401-Ukr_a. References Azahra M., Gonzalez-Gomez C., Lopez-Penalver J.J., El Bardouni T., Camacho Garcia A., Boukhal H., El Moussaoui F., Chakir E., Erradi L., Kamili A., Sekaki A., 2004. The seasonal variations of 7 Be and 210 Pb concentrations in air. Radiation Physics and Chemistry 71, 789 790. Beks J.P., Eisma D., Van der Plicht J., 1998. A record of atmospheric 210Pb deposition in The Netherlands. The Science of the Total Environment. 222, 35-44. Buraeva E.A., Davydov M.G., Zorina L.V., Malyshevsky V.S., Stasov V.V., 2007. Content of cosmogenic 7 Be in the air layer at the ground at temperate latitudes. Atomic. Energy. 102, 6, 463-468. Duenas, C., Fernández, M.C., Canete, S., Pérez, M., 2009. 7Be to 210Pb concentration ratio in ground level air in Málaga (36.7 N, 4.5 W). Atmos. Res. 92, 49 57.

Duenas C.,. Orza J.A.G, Cabello M., Fernández M.C., Canete S., Pérez M., Gordo E., 2011. Air mass origin and its influence on radionuclide activities (7Be and 210Pb) in aerosol particles at a coastal site in the western Mediterranean. Atmos. Res. 101, 205 214. Hotzl H. and Winkler R., 1987. Activity Concentrations of 226 Ra, 228 Ra, 210 Pb, 40 K and 7 Be and their Temporal Variations in Surface Air. Journal of Environmental Radioactivity. 5, 445-458. Todorovic D., Popovic D., Djuric G., Radenkovic M., 2005. 7 Be to 210 Pb concentration ratio in ground level air in Belgrade area. Journal of Environmental Radioactivity. 79, 297 307.

Tables Table 1. Volume activity of 210 Pb in surface air. Year Volume activity, mbq/m 3 Max Min Mean 2002 4,96 0,32 1,41 2003 7,40 0,12 1,55 2004 3,40 0,20 1,26 2005 3,28 0,48 1,40 2006 8,84 0,68 2,19 2007 9,05 0,15 1,85 2008 8,44 0,71 2,05 2009 7,90 1,00 2,27 2010 5,41 0,94 2,25 Table 2. Volume activity of 210 Pb and meteorological parameters averaged over the year Year Activity, mbq/m 3 Precipitation, mm Temperature, 0 С Wind speed, m/s Relative humidity, % Atmospheric pressure, mm Hg 2002 1,41 38,5 10,0 1,8 65,9 756,1 2003 1,55 50,7 8,3 2,0 71,5 756,7 2004 1,26 25,3 9,6 1,8 74,6 755,8 2005 1,40 32,7 10,3 1,9 72,3 756,2 2006 2,19 38,2 10,6 3,2 69,4 755,7 2007 1,85 37,6 10,9 4,3 65,1 755,6 2008 2,05 27,6 11,1 4,2 69,4 756,1 2009 2,27 27,3 11,0 4,2 71,6 755,2 2010 2,25 25,3 9,7 5,6 71,3 755,3

Captions Fig. 1. Volume activity of the 210 Pb. Fig. 2. Volume activity of 210 Pb in surface air from January 2002 since December 2010. Fig. 3. Mean monthly atmospheric volume activity of 210 Pb averaged over the period 2002-2010.

Figures Fig. 1. Fig. 2.

Fig. 3.