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7be Behaviour in The Atmosphere of The City of Granada - 2012 - Atmospheric Env PDF
7be Behaviour in The Atmosphere of The City of Granada - 2012 - Atmospheric Env PDF
Atmospheric Environment
journal homepage: www.elsevier.com/locate/atmosenv
7
Be behaviour in the atmosphere of the city of Granada January 2005
to December 2009
F. Piñero García a, M.A. Ferro García a, *, M. Azahra b
a
Radiochemistry and Environmental Radiology Laboratory, Inorganic Chemical Department, Faculty of Sciences, University of Granada, Av. Fuentenueva, 18077 Granada, Spain
b
Physics Department, Faculty of Sciences, Abdelmalek Essaadi University, 93002 Tétouan, Morocco
a r t i c l e i n f o a b s t r a c t
Article history: This paper focuses on 7Be concentration in the atmospheric surface aerosols of the Spanish city of
Received 29 August 2011 Granada, in the southern Iberian Peninsula. We analyze the effects of meteorological conditions in the
Received in revised form geographical zone over the period 2005e2009. A prediction model is suggested to describe the
24 October 2011
behaviour of atmospheric aerosols containing 7Be. The model was applied from January to May 2010 and
Accepted 14 November 2011
shows that temperature, relative humidity and precipitation are the meteorological factors responsible
for the behaviour of atmospheric aerosols. The statistical significance of the results was 99%. This study
Keywords:
7 helps understanding of the atmosphere of Granada as well as the climate variables responsible for
Be
Ground-level air
transportation and deposition of atmospheric aerosols. Moreover, in case of a massive release of
Seasonal variations radionuclides into the atmosphere, the results of this study will help predict behaviour in this city and
Meteorological factors other continental areas with a similar climate.
Atmospheric deposition Ó 2011 Elsevier Ltd. All rights reserved.
1. Introduction are distributed over the earth’s surface and inserted into different
ecosystems through dry and/or wet deposition (Papastefanou and
7
Be is a natural cosmogenic radionuclide, approximately 70% of Ioannidou, 1995; Wallbrink and Murray, 1994; Dibb, 1990). There-
which is produced in the stratosphere (Kathren, 1984), with the fore, 7Be has been proposed as a natural atmospheric tracer (Lal and
remaining w30% being produced in the high troposphere (Lal and Peters, 1962; Brost et al., 1991; Vecchi and Valli, 1997).
Peters, 1967). Concentration of 7Be reaches is highest at 15e20 km 7
Be is widely used as a natural radiotracer in many environ-
and decreases exponentially with altitude. 7Be concentration in the mental processes due to its characteristics: it has high specific
troposphere and the stratosphere depends on the flow of cosmic activity as a result of its short period of half-disintegration, it is
rays at altitude, whose density has an inverse relation with solar easily detected by gamma emission, it is a radionuclide with low
activity, undergoing cyclical changes every 11 years (Hötzl et al., chemical reactivity and its concentration has not been altered by
1991; Azahra et al., 2003; Papastefanou and Ioannidou, 2004; anthropogenic inputs. Moreover, 7Be and fission products (137Cs)
Cannizzaro et al., 2004). usually behave in the same way despite having a different origin
The cosmogenic radionuclide 7Be (half-life: 53.3 days) is and distribution throughout the atmosphere, (Ioannidou and
produced by spallation reactions between the protons of the Papastefanou, 2006).
primary components and the secondary neutrons of cosmic rays Furthermore, the connection between air mass transport and
7
with nuclei of light elements found in the atmosphere, such as Be activity at ground level has also been identified, such as
carbon, oxygen and nitrogen (Papastefanou and Ioannidou, 1995). seasonal variations caused by: 1) air mass exchange between
After production, 7Be reacts with air constituents and turns into stratosphere and troposphere; 2) vertical transfer of aerosols in the
atoms or 7BeO and/or 7Be(OH)2 molecules, which diffuse in the troposphere coming from the tropopause at cloud level or below;
atmosphere until becoming attached to available aerosol particles 3) northesouth mixing due to the important difference in
(0.07e2 mm diameter) drifting in the atmosphere (Papastefanou production rates between higher and lower latitudes; 4) eastewest
and Ioannidou, 1995). These small particles and with attached 7Be circulation, where the differences between geographical and
geomagnetic latitudes play a key role; 5) heavy shower frequency
(Feely et al., 1989). Variations in 7Be concentration are therefore
* Corresponding author. Tel.: þ34 958 243325; fax: þ34 958 248526. a complex function of all these factors, as each process has its own
E-mail address: ferro@ugr.es (M.A. Ferro García). seasonal cycle and they do not happen in a controlled time or place.
1352-2310/$ e see front matter Ó 2011 Elsevier Ltd. All rights reserved.
doi:10.1016/j.atmosenv.2011.11.034
Table 1
Atmospheric 7Be specific activity reported at different locations.
Location Period Range (med. s) (mBq m3) Experimental conditions of aerosol sampling References
Málaga (Spain) 36.73N; 4.47W 2000e2006 2.47e14.9 (4.8 1.6) Samples collected to 12 m a.g.l. Flow rate: 40 L min1. Dueñas et al., 2009
Cellulose nitrate filters (15.90 cm2, øpore ¼ 0.8 mm).
Samples collected weekly and measured monthly.
Granada (Spain) 670 m a.s.l 37.18N; 3.59W 2005e2009 0.37e9.33 (4.51 0.23) Samples collected to 1.5 m a.g.l. Flow rate: 75 L min1. This work
Sevilla (Spain) 37.36N; 5.97W 2004e2005 3.1 Samples collected to 30 m a.s.l. Flow rate: 950 m3 h1. Gonzalez et al. (2004,2005)
Polypropylene filters 44 44 cm2.
Samples collected and measured weekly.
Tracy (California) 392 m a.s.l 37.65N; 121.53W 1977e1981 3.29e6.70 (5.14 0.7) Flow rate: 58.34 m3 h1. Samples collected using Feely et al., 1989
Microsorban air filter medium 99/97- 4200, of 20 cm.
Palermo (Italy) 38.12N; 13.35E 1982e2002 2.16e10.57 (5.06) Samples collected to 20 m a.g.l. Flow rate: 900 m3 h1. Cannizzaro et al., 2004
Cellulose filters 45 45 cm2.
Samples collected and measured daily.
Cáceres (Spain). 405 m a.s.l 39.51N; 6.34W 1992e1994 11.3e0.88 (4.4 1.8) Samples collected to 1.5 m a.g.l. Flow rate: 60 L min1. Baeza et al., 1996
Cellulose nitrate filters (15.90 cm2, øpore ¼ 0.8 mm).
Samples collected weekly and measured monthly.
Barcelona (Spain) 41.38N; 2.12E 2001e2005 2.70e4.4 (3.5 0.4) Flow rate: 800 m3 h1. Polypropylene filters (44 44 cm2). Vallés et al., 2009
Samples collected and measured weekly.
Bilbao (Spain) 43.27N; 2.94W 2000e2009 (3.06 1.02) Samples collected to 15 m a.g.l. Flow rate: 500 m3 h1. Alegría et al., 2010
Polypropylene filter (44 44 cm2, øpore ¼ 0.8 mm).
Samples collected and measured weekly.
Dome (France) 1465 m a.s.l 45.77N; 2.97E 2006e2008 3.64e10.7 Samples collected to 2 m a.g.l. Flow rate: 700 m3 h1. Bourcier et al., 2011
Polypropylene fibres. Collection twice a
week from 10-2005 to 06-2007 and once a week since 07-2007.
Dome (France) 660 m. a.s.l. 45.72N; 3.09E 2004e2008 1.73e7.73 Samples collected to 2 m a.g.l. Flow rate 300 m3 h1. Bourcier et al., 2011
Popolypropylene fibres. Collection twice a week
from 10-2005 to 06-2007 and once a week since 07-2007.
85
86 F. Piñero García et al. / Atmospheric Environment 47 (2012) 84e91
The average specific activity was 4.56 0.22 mBq m3 what is where: Z is the resulting normalization value; X is the real value, X
comparable with the concentration of 7Be measured by different is the arithmetic average and s is the standard deviation.
authors in their respective papers studied (see Table 1). The activity
of 7Be in August, 9.334 mBq m3, is the highest found in Granada
3.4. Factors controlling the atmospheric activity of 7Be
(Spain) since 1993, whereas the lowest was in January 2007,
0.534 mBq m3. The mean annual activity of 7Be (mBq m3) during
3.4.1. Variables studied
this period was in 2005 (4.06), in 2006 (4.31), in 2007 (3.26), in
We examined the effects of sunspots, atmospheric pressure,
2008 (5.37), and in 2009 (5.81). During the year 2009 the mean
precipitation, temperature, relative humidity on 7Be activity in the
annual of 7Be was 29% higher than the typical mean value of
aerosol samples. 7Be specific activity was statistically correlated
4.5 mBq m3 of Granada during 17 years of sampling. It was due to
with the normalized monthly averages of the variables studied.
the particular minimum of solar activity of that year and was also
There is 99% statistically significant correlation with tempera-
observed in the measurements in Thessaloniki, Greek (Ioannidou
ture, precipitation and relative humidity, but 7Be behaviour is little
et al., 2011).
affected by atmospheric pressure and sunspots.
Regarding atmospheric pressure, the correlation found is not
3.2. Statistical study statistically significant, (r ¼ 0.193, p-value ¼ 0.139). On the one
hand, this is due to the low influence, 5%, of this parameter on the
The overall results of 7Be specific activity were examined earth’s cosmic radiation (Rankama, 1963), while, on the other,
statistically in order to determine fit as defined by average and several authors (Dueñas et al., 1999) consider that the influence of
typical deviation. The frequency histogram of 7Be specific activity this variable is still unknown.
(Fig. 2) shows asymmetry on the right-hand side (Asymmetry A statistically significant correlation between the solar activity
coefficient As ¼ 0.379 > 0) and is higher than normal distribution and 7Be specific activity in aerosols over the sampling period
(Curtosis coefficient G2 ¼ 0.395 > 0). (2005e2009) has not been found. The Pearson correlation coeffi-
The KolmogoroveSmirnov test was applied to decide which cients obtained are very weak (r ¼ 0.024, p-value ¼ 0.854).
theoretical distribution (Normal, Normal-log, Uniform and Expo- Throughout the investigation studied we cannot observe an
nential) fits best to our data. The test confirms that normal and evident relation between two variables as it is shown in Fig. 4.
normal-log distribution are statistically significant for a 95% Although during some periods when solar activity is high, cosmic
confidence interval. The PP plot, Fig. 3, was used in order to decide rays are deflected away from the solar system and 7Be production
which the best distribution was. The Fig. 3 shows that normal decreases. In this sense, many studies have found correlation
distribution is better than normal-log one, because points are between solar activity and 7Be concentration in near-surface air
closed to the diagonal line. Once fitted into a normal distribution, (Hötzl et al., 1991; Azahra et al., 2003; Cannizzaro et al., 2004;
the values defining distribution were calculated (average value Aldahan et al., 2008; Kikuchi et al., 2009; Alegría et al., 2010).
4.56 mBq m3 and typical deviation 1.72 mBq m3). This can be explained by the fact that the period described in
this paper is not a complete solar cycle (11 years). In addition,
3.3. Standardization of data a change in the solar cycle occurred between 23 and 24, with the
end of the 23rd solar cycle being more extended than usual. As
The variables shown in this paper were normalized in order to a result, there was no significant change in solar activity over the
compare the results obtained as they fluctuate constantly during last two years (Fig. 4).
the period of time studied. The standardization criteria were used For this reason, the flow density of cosmic rays reaching earth’s
to convert the data into their normal form N(0, 1): atmosphere was approximately the same during these two years.
Consequently, the amount of 7Be produced in the higher layers of
Z ¼ ðX XÞ=s (1) the atmosphere varied only slightly. The variations detected in the
Fig. 6. Comparison of monthly average values of 7Be specific activity and the variation
Fig. 5. Comparison of monthly average values of 7Be specific activity and air temper- of mean monthly maximum and minimum temperatures, DT ¼ Tmax Tmin, C, during
ature during the period 2005e2009. 7Be e Histograms and Temperature e Line. the period 2005e2009. 7Be e Histograms and DT e Line.
F. Piñero García et al. / Atmospheric Environment 47 (2012) 84e91 89
Fig. 7. Comparison of monthly average values of precipitation and 7Be specific activity Fig. 9. Comparison of the standardized activity of 7Be during the period January
during the period 2005e2009. 7Be e Histograms and Precipitation e Line. 2010eMay 2010: Model vs. Measurements.
90 F. Piñero García et al. / Atmospheric Environment 47 (2012) 84e91
indicate that relative humidity over 60% produces a sudden of this radiotracer is strongly affected by seasonal variation of local
decrease in the specific activity values. meteorological variables, given the special characteristics of this
city’s geographical location as indicated. These results suggest that
3.5. Prediction model the 7Be concentrations in surface air have unique behavior at each
individual site that must be determined, because the factors
Having determined the climate parameters affecting 7Be controlling 7Be variations in the surface atmosphere can be appli-
behaviour in the atmosphere of Granada and by using the statistics cable to the behavior that other radionuclides of anthropogenic
program STATGRAPHICS-PLUS, we can draw up the most appro- origin might present in the case of a nuclear accident.
priate model for the standardized experimental data obtained. In
view of the results, we can say that the best meteorological vari- Acknowledgements
ables by which to explain the behaviour of 7Be bearing aerosols in
the surface atmosphere of Granada city are air temperature (T), We wish to thank the Spanish Nuclear Safety Council (CSN) for
relative humidity (Hr) and precipitation (P). the kind support given to the Radiochemistry and Environmental
Radiology Laboratory of the University of Granada since 1993 as
A7Be ¼ 1:125$105 0:284$Hr 0:179$P þ 0:476$T (2) a member of the laboratories of the Spanish Sparse Network for
Environmental Surveillance. This study was also supported by the
The Pearson coefficient was 0.849. This means that our model Spanish Ministry of Education (CGL2010-19849).
explains 72.16% of the variation observed in 7Be results obtained in
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