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Atmospheric Environment 39 (2005) 4057–4066


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Gross alpha, gross beta activities and gamma emitting


radionuclides composition of airborne particulate samples
in an oceanic island
F. Hernández, J. Hernández-Armas, A. Catalán,
J.C. Fernández-Aldecoa, L. Karlsson
Laboratorio de Fı´sica Médica y Radioactividad Ambiental, Departamento de Medicina Fı´sica y Farmacologı́a,
Universidad de La Laguna, 38320 La Laguna, Tenerife, España
Received 29 October 2004; received in revised form 8 March 2005; accepted 25 March 2005

Abstract

The radiometric compositions of airborne particulate samples, collected weekly during a 4 years period (1 January
2000 till 31 December 2003) at a site located 310 m a.s.l. in Tenerife (Canary Islands), are analysed in this paper. To do
this, measurements of gross alpha, gross beta, 7Be, 210Pb, 228Ac, 226Ra, 212Pb, 214Pb, 208Tl, 214Bi, 235U, 40K, 131I and
137
Cs concentrations were carried out in 376 cellulose and polypropylene filters. The time variations of the different
radionuclides concentrations have been discussed in relation with various meteorological factors and the mean values
have been compared to those published in recent literature for other sites located at the same altitude but different
latitudes.
The weekly activities of 7Be correlated linearly with the 210Pb activities (R ¼ 0:59). In disagreement with other
published studies, the 7Be activities did not correlate (R ¼ 0:05) with the temperature and maximum values were not
found during summer season. The gross beta activities showed correlations with the gross alpha (R ¼ 0:72) and 210Pb
activities (R ¼ 0:52), but not with the 7Be (R ¼ 0:16). The anthropogenic radionuclide 131I, emitted from a nearby
hospital, was detected slightly above detection limits (1.73  106 Bq m3) in 88 of the 210 weeks of measurement
considered in this work. 137Cs was detected in 31 of those weeks. The 4-year average calculated for 7Be and 210Pb were 3
and 0.3 mBq m3, respectively. These values are lower than those expected for a site at comparable latitude and altitude.
In general, the radionuclides which appeared most frequently in the airborne particulate filters (7Be, 210Pb, 212Pb and
40
K), did not correlate significantly with any of the meteorological parameters considered: rainfall, temperature,
pressure, relative humidity, visibility, wind speed and direction. Therefore, no predictive model could be established
with the available data as it has been done for continental sites. The long-range transport of aerosols from the Saharan
desert showed to be an important source of 137Cs and 40K in the particulate filters after low-level atmospheric dust
intrusions that reached the island.
r 2005 Elsevier Ltd. All rights reserved.

Keywords: Aerosols; Atmospheric radionuclides; Surface air; Saharan dust; Tenerife

Corresponding author. Tel.: +34 922 319422; fax: +34 922 643165.
E-mail address: jharmas@ull.es (J. Hernández-Armas).

1352-2310/$ - see front matter r 2005 Elsevier Ltd. All rights reserved.
doi:10.1016/j.atmosenv.2005.03.035
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4058 F. Hernández et al. / Atmospheric Environment 39 (2005) 4057–4066

1. Introduction uniform temperatures all year round. The lower atmo-


sphere over the Canary Islands is strongly stratified. A
The increasing interest on the role of airborne stable temperature inversion is observed at least once
particulate matter in regional and global environmental every day of the year (Viana et al., 2002; Rodrı́guez and
changes makes radiotracers an important tool for the Guerra, 2001). This unique situation originates by the
spatio-temporal modelling of aerosols. Some authors presence of high-pressure zones in the vicinity of the
(Gründel and Porstendörfer, 2004; Gerasopoulos et al., Azores Archipelago. It is characterised by a lower layer
2003; Aldahan et al., 2001; Lujaniene et al., 1999; Dibb of oceanic humid air and an upper layer of warm and
and Jaffrezo, 1993; Balkanski et al., 1993) have dry air. The mean thickness of the inversion layer
demonstrated the utility that the accurate determination reaches a maximum (560 m) during the summers and
of very small concentrations of 7Be and 210Pb, as well as minimum (360) between October and January. The
other aerosol radiotracers has in explaining, e.g., long- average altitude of the inversion is lowest in summer
range air mass transport, the exchange rate of air (770–1380 m a.s.l.) and highest in winter (1360–1850 m
between the stratosphere and the troposphere, aerosol a.s.l.). The predominant winds in this region are in the
residence time, cloud formation processes, atmospheric northeast direction. These winds favour the dispersion
aerosol scavenging, etc. Although gross alpha and gross of local anthropogenic aerosol sources over the ocean.
beta measurements are generally made as a means of Two different aerosol sampling pumps placed 100 m
‘‘screening’’ for unusual levels of radioactivity, these apart, a Saic Radeco AV-28A and a P.T.I. Sampling
measurements are of interest since they allow establish- Station ASS-500, were utilised to collect total suspended
ing trends in radionuclide concentrations in the atmo- particulate (TSP) matter. The sampling stations were
sphere and the calculation of aerosol residence times located at 310 m a.s.l. The air flow rates of the two
(Dueñas et al., 1999, 2004; Sheets and Thompson, 1992). pumps were set to collect, at normal conditions, 30 and
Airborne particulate matter was and is currently being 10,000 l min1 respectively, although these values oscil-
collected continuously in cellulose and polypropylene lated from week to week depending on the real atmo-
filters in Tenerife as part of a national monitoring spheric situation. The smaller pump used circular
programme coordinated by the Consejo de Seguridad cellulose filters (47 mm diameter) and the larger pump
Nuclear. The different data collected from the radio- used polypropylene G3-type square filters (440 mm side).
metric measurement performed on these filters during a Dust content in the filters was calculated gravimetrically
4-year period (1 January 2000 till 31 December 2003), by weighting the filters before and after exposure under
has been used in this paper to calculate the radiotracer the same laboratory conditions. The local sources of
composition of airborne particulate matter at the anthropogenic aerosols at the sampling sites are limited
surface air. The influence of meteorological parameters to emissions from cars and the smoke from two large
such as rainfall, temperature, relative humidity, pres- hospitals, which are within a 1 km radius. These fluxes
sure, visibility, wind speed and wind direction, which plus natural sources constitute the environmental radio-
can influence the concentration of aerosol radiotracers active level at that place.
in the atmosphere, has also been evaluated. In general, it Gamma measurements were performed with two
has been shown (Hotzl and Winkler, 1987; Feely et al., coaxial-type germanium detectors (Canberra Industries
1989) that the increment of environmental temperature Inc., USA). These detectors were calibrated using
correlates with the increment of 7Be in the atmosphere in certified reference gamma-ray cocktails purchased from
continental sites. Various studies have, also, shown some Amersham Industries (Amersham plc. UK), and known
relation between wet and dry deposition with the concentrations of chemically pure potassium chloride
concentration of 210Pb (El-Daoushy, 1988; Rangarajan (MERCK. E., Germany). These detectors have iron
and Eapen, 1967). In previously published results (e.g., shields and are placed, together with their associated
Dueñas et al., 2001), it has been even possible to relate electronic units, in a specially conditioned laboratory
with mathematical expressions various meteorological with air filters to provide an optimum environment for
parameters and gross alpha, gross beta and 7Be low-level gamma measurements. Temperature is kept
concentrations in air. constant at all times and the overpressure maintained at
this laboratory minimises the inflow of radon from its
surroundings. Each large aerosol filter sample was
2. Sampling and method of analysis measured twice, the first time on the same day of sample
collection, during 4 h, and the second time 3 days later
Airborne particulate samples were collected weekly at and during 96 h. The time delay between the first and the
Tenerife. The island of Tenerife is situated west second measurement allowed for the decay of 222Rn
(approximately 210 km) from the northern coast of short-lived daughters. The detectors’ backgrounds were
Africa, between 281180 and 281350 N and between 161070 measured twice per year. The measuring time used was 4
and 161490 W. The mean climatic features are mild with days each time.
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F. Hernández et al. / Atmospheric Environment 39 (2005) 4057–4066 4059

Spectra analyses and background subtraction were 0, 7, 13 and 18 h, carried out over the whole 4-year
performed with the Genie2K spectrometry software, period. The total rainfall was calculated by summing the
versions 1.4 and 2.0 (Canberra Industries Inc., USA). A total daily rainfall for the considered periods. The
library of radionuclides, which contained the energy of weekly averages for the wind speed and direction were
the characteristic gamma peaks for each nuclide calculated using a type of vector analysis based on the
analysed and their corresponding emission probabilities, values collected daily every 6 h.
was built from the data supplied in the mentioned
software. The characteristic gamma peaks selected for
the determination of the different radionuclides were: 3. Results and discussion
46.5 keV for 210Pb, 477 keV for 7Be, 364 keV for 131I,
186 keV for 226Ra, 238 keV for 212Pb, 351 keV for 214Pb, 3.1. Measurement and data statistics
583 keV for 208Tl, 911 and 969 keV for 228Ac, 609 keV
for 214Bi, 144 keV for 235U, 661 keV for 137Cs and Table 1 summarises the main statistical variables
1460 keV for 40K. The 210Pb activities were corrected for calculated for the gross alpha and gross beta activities as
the self-absorption process that occurs in volumetric well as for the measured gamma emitting radionuclides
samples following the method indicated by Hernández over the whole sampling period: 1 January 2000 till 31
and El-Daoushy (2002). Various tests were performed to December 2003. Unless otherwise specified, all the
check the correct interpretation of the spectrometric values reported here correspond to the second of the
data in those cases where 131I was detected in the measurements performed in all the filters, once the
polypropylene filters. These tests included performing short-lived radon daughters had decayed. Notice also
various repetitive 6 h long measurements on the same that although gross alpha and gross beta measurements
samples to verify the 8-day half-life of this nuclide. exist for the whole period, the gamma measurements in
Additional measurements were, also, carried out a the large filters only started in the second semester of the
month later on the same samples and no activity was year 2000 and therefore there are fewer data points. The
ever detected (above detection limit) in any of them. measuring uncertainties were very variable depending on
Furthermore, another two gamma lines (284 and the nuclide studied. On the one hand, measured
634 keV), also from the 131I, were detected in the spectra concentrations of 7Be were associated with the lowest
with highest activity confirming our identification. uncertainty, in the order of 2%. On the other hand, the
235
Gross alpha and gross beta measurements were U concentrations were associated with the largest
carried out twice on each cellulose filter. The first uncertainties, in the order of 50%. The mean measure-
measurement was performed 15 min after collection in ment uncertainties for the Gross alpha and gross beta
order to determine the contributions produced by the activities were calculated to be (see Table 1) approxi-
short-lived radon daughters. The second measurement mately 10% and 5%, respectively. The lowest measured
was made 3 days after collection to allow these short- concentration of a gamma emitting nuclide was in the
lived nuclides to decay. All these measurements were order of 0.2 mBq m3, obtained for the 208Tl.
carried out with a low background proportional counter In accordance with other published studies (Dueñas et
(Berthold LB770). All the alpha and beta activity al., 1999, 2001, 2004), the plots of the frequency
calculations were corrected for the mass thickness of distribution of gross alpha and gross beta activities in
the aerosol deposit collected in the different filters. The airborne particulate samples showed skewed histograms
average detection limit for this apparatus was 9.5  (see Figs. 1(a) and (b)). A similar behaviour was
106 Bq m3 for alpha activity and 1.5  105 Bq m3 observed for the frequency histograms corresponding
for beta activity. Due to the low concentration of alpha to the other measured gamma emitting radionuclides (an
and beta emitters in the filters, long counting times of example is given in Fig. 1(d)), except for 7Be, which
10 h were used for each measurement. Background showed a normal frequency distribution as shown in
measurements were carried out each week using similar Fig. 1(c). Due to the mentioned shape of the frequency
counting times as normal sample measurement. A distribution functions obtained for the different radio-
background subtraction procedure was applied on each nuclides, the arithmetic mean was used in further
of the gross alpha and gross beta analyses. analysis and comparisons as the main characterisation
The standard meteorological data: rainfall, relative factor for the 7Be activity and the geometric mean for
humidity, visibility, pressure, temperature, wind speed the other nuclides, gross alpha and gross beta activities.
and wind direction, collected at a measuring station While the mean yearly value of meteorological
located 4 km from the sampling site, have been provided parameters such as temperature, visibility, relative
by the Spanish National Institute of Meteorology. The humidity and pressure remained fairly constant over
temporal averages (weekly, seasonal, etc.) of the relative the studied period, the total yearly rainfall showed
humidity, visibility, pressure and temperature were significant differences, increasing, e.g., by a factor of 3 in
calculated based on four daily measurements taken at 2002 in comparison with the other considered years, see
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Table 1
Statistical summary of the radiometric data collected from 1 January 2000 till 31 December 2003
7 228 214 137 131
Gross a Gross b Be Ac Bi Cs I
a
N of cases 205 206 171 12 41 31 88
Geo. mean 9.60  105 4.77  104 2.72  103 3.21  106 5.06  106 9.18  107 3.83  106
Arit. mean 1.41  104 1.00  103 3.00  103 3.33  106 8.10  106 1.15  106 4.85  106
Minimum 1.40  105 9.31  105 1.94  104 2.09  106 1.14  106 3.50  107 1.05  106
Maximum 1.00  103 3.00  103 7.00  103 5.69  106 3.80  105 3.38  106 2.11  105
Range 1.00  103 2.00  103 7.00  103 3.60  106 3.69  105 3.03  106 2.01  105
Std. error 1.03  105 2.08  105 6.90  105 2.87  107 1.29  106 1.53  107 4.30  107
C.V. 1.045 0.554 0.311 0.299 1.024 0.742 0.833
Skewness (G1) 2.461 2.456 0.744 1.116 1.897 1.314 2.336
40 210 212 214 226 208 235
K Pb Pb Pb Ra Tl U

N of casesa 147 166 159 32 26 147 7


Geo. mean 1.77  105 3.10  104 9.08  106 4.44  106 1.37  105 9.42  106 2.49  106
Arit. mean 2.50  105 3.74  104 4.52  105 6.48  106 2.26  105 4.56  105 4.30  106
Minimum 3.31  106 1.20  105 1.09  106 1.21  106 3.90  106 2.04  107 8.59  107
Maximum 1.45  104 3.00  103 2.00  103 2.56  105 2.49  104 2.00  103 1.59  105
Range 1.42  104 3.00  103 2.00  103 2.44  105 2.45  104 2.00  103 1.50  105
Std. error 2.18  106 2.27  105 1.62  105 1.05  106 9.13  106 1.63  105 2.07  106
C.V. 1.055 0.783 4.534 0.915 2.059 4.338 1.275
Skewness (G1) 2.63 3.788 6.654 1.426 4.969 6.378 2.06

All the activities are given in Bq m3.


a
Number of detected cases above the limit of detection. Geo. ¼ geometric; Arit. ¼ aritmetic and C.V. ¼ covariance.

Fig. 2. Wind speed and direction were, also, very than the value 0.1 reported by other authors (Dueñas
variable over time. A proper study of the effect of these et al., 2004; Garcı́a-Talavera et al., 2001; Chamberlain,
two meteorological parameters on the concentration of 1991), indicating the possible existence of secondary
different nuclides would probably require daily or even sources of alpha radioactivity from soil dust or
shorter radiometric measurements. anthropogenic origin. In 15 occasions, mostly during
Some of the nuclides, such as 214Pb, 228Ac, 235U, the autumn seasons, the ratio alpha/beta was higher
226
Ra, etc. were seldom measured above the detection than 0.5, especially in the year 2003. The overall
limits. This explains the fewer number of available data seasonal variations of gross alpha and gross beta
points in their statistic summary. A thorough analysis of activities were relatively small in comparison with the
the data showed that the occasional detection of these standard deviation of the data. A similar behaviour was
nuclides could not be correlated with any significant observed for the yearly variations. No linear correlation
decrease of the measuring detection limit, or increase in could be found between the gross alpha and gross beta
the sampled air volume and/or dust content in the filters. activities with any of the meteorological parameters
In fact, some of the highest activity concentrations were considered; see Table 2. A more detailed analysis of the
measured in periods when the sampled volume was correlations of the gross alpha and gross beta activities
rather low. No correlation was found between the with meteorological parameters using the Spearman
sample volume and sample weight, indicating that, with coefficient showed a very weak positive correlation of
weekly data, a relationship between these two variables the gross alpha activity with the temperature (R-
could not be established. spearman ¼ 0.27). Based on the available data and the
low dependencies found between the different variables,
3.2. Gross alpha and gross beta activities no predictive model could be built.

A strong linear correlation (R ¼ 0:72) was found 3.3. Natural and cosmogenic radionuclides
between the weekly measured gross alpha and gross beta
activities over the 4-year period. The ratio between the The mean values calculated here for the 7Be and 210Pb
geometric means calculated for the alpha and beta activities for the whole 4-year period are lower than those
activities was closed to 0.2. Although 210Po is most likely reported for other Spanish sites situated in the Iberian
the main source of alpha activity, this ratio is higher Peninsula, such as Málaga (Dueñas et al., 2004), Salamanca
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F. Hernández et al. / Atmospheric Environment 39 (2005) 4057–4066 4061

Fig. 1. Frequency histogram of: (a) gross alpha activity, (b) gross beta activity, (c) 7Be activity and (d) 210
Pb activity, for the data
collected from 1 January 2000 till 31 December 2003. All the activities are given in Bq m3.

Fig. 2. Year rainfall (solid line) and seasonal rainfall (box), measured in mm during the study period.

(Garcı́a-Talavera et al., 2001) and Granada (Azahra and 208Tl appeared lower than those measured at a
et al., 2004). These three mentioned studies were continental site located at similar latitude and altitude
performed using analogous sampling and measuring but very different longitude (Al-Azmi et al., 2001). As
techniques as those applied in this work. Similarly, the reported by several authors (Cannizzaro et al., 2004;
mean values calculated for 7Be, 210Pb, 235U, 214Bi, 212Pb Al-Azmi et al., 2001; Aldahan et al., 2001), 7Be
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Table 2
Linear correlation studies (Pearson coefficient), between the considered meteorological parameters and the measured activities
7 228 214 137 131
Gross a Gross b Be Ac Bi Cs I

Temperature 0.22 0.11 0.05 0.43 0.15 0.32 0.02


Pressure 0.09 0.06 0.10 0.17 0.15 0.10 0.003
Rainfall 0.10 0.14 0.03 0.32 0.06 0.19 0.04
R. humidity 0.04 0.001 0.20 0.09 0.02 0.08 0.32
Visibility 0.10 0.24 0.05 0.44 0.19 0.25 0.04
Wind speed 0.15 0.15 0.07 0.10 0.08 0.45 0.24
W. direction 0.02 0.03 0.11 0.19 0.07 0.08 0.02
40 210 212 214 226 208 235
K Pb Pb Pb Ra Tl U

Temperature 0.20 0.10 0.10 0.49 0.19 0.11 0.50


Pressure 0.04 0.03 0.007 0.34 0.28 0.003 0.75
Rainfall 0.06 0.06 0.04 0.37 0.09 0.04 0.93
R. humidity 0.14 0.02 0.01 0.03 0.09 0.002 0.04
Visibility 0.15 0.20 0.07 0.60 0.12 0.08 0.77
Wind speed 0.05 0.22 0.03 0.18 0.07 0.03 0.17
W. direction 0.04 0.008 0.12 0.03 0.15 0.13 0.21

Notice that although some of the coefficients are relatively high (40.5), the total number of data points available in all those cases is
very limited as pointed out in Table 1.

Fig. 3. Temporal variation of the calculated seasonal mean of the 7Be concentrations in the air and the mean temperature over the 4
years period (1 January 2000 till 31 December 2003). The temperatures are given in 1C and the activities in Bq m3. The error bars in
the figure denote the standard deviation of the activities.

concentrations in ground level air are expected to observed here do not differ from each other signifi-
decrease as we move north from middle latitudes. Thus, cantly, if one considers the standard deviation of the
higher average values would have been expected for this weekly measured activities shown in the figure. Further-
nuclide at the oceanic island of Tenerife and not lower as more, the maximum calculated values happen during the
it has been found in this work. winter–spring periods. The inversion layer over the
Fig. 3 displays the temporal variations of the island of Tenerife is thicker during summer months,
calculated seasonal mean of the 7Be concentrations in when air mass intrusions into the region occur at higher
the air and the mean temperature over the studied altitude. This could explain why the 7Be concentration
period. Maximum values were expected to occur over maxima are not observed in our results during those
the summer months as discussed by other authors seasons. The negative correlation coefficient calculated
(Garcı́a-Talavera et al., 2001; El-Hussein et al., 2001; for the 7Be activity and the average temperature was
Dueñas et al., 1999). However, the seasonal variations very low (R ¼ 0:05), indicating very poor correlation
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Table 3
Linear correlation studies (Pearson coefficient), between some of the measured radionuclides
7 210 40 137
Gross a Gross b Be Pb K Cs

Gross a 1.00
Gross b 0.70 1.00
7
Be 0.03 0.16 1.00
210
Pb 0.26 0.52 0.60 1.00
40
K 0.21 0.18 0.13 0.28 1.00
137
Cs 0.30 0.21 0.28 0.40 0.46 1.00

with this parameter (see Table 2). Other publications since it was detected many more times than the other
(Azahra et al., 2004; Dueñas et al., 1999) point out the nuclides, having a comparable limit of detection. Only in
temperature as one of the most significant parameters one single event both the 40K and 226Ra activities
influencing the variation of 7Be concentrations in surface showed a common and considerably large increase not
air and therefore their prediction models. However, this shown by any other nuclide. The lack of correlation
has not been observed in this work. Low correlation between the 40K activities and those activities from other
factors were, also, obtained between the 7Be activities nuclides such as 7Be and 210Pb could be explained by the
and the average rainfall, pressure, relative humidity and daily occurrence of the inversion layer, which limits the
visibility. exchange of air between the lower and the free tropo-
Some common features were observed in the temporal sphere.
variations of the 7Be and 210Pb activity concentrations.
The calculated linear correlation factor was R ¼ 0:59 3.4. Anthropogenic radionuclides
(see Table 3). Furthermore, 210Pb activities correlated
well (R ¼ 0:52) with the gross beta activities, in a similar Several tests, including the study of the decay period
way that other authors have established (Dueñas et al., and the detection of multiple gamma lines, were
2004). Comparisons between the first and second performed to confirm the detection of the gaseous
measurement carried out in all the filters showed a artificial radionuclide 131I in the polypropylene filters.
decreased of 212Pb and 208Tl (short-lived 220Rn daugh- This nuclide, which is often used in medical applications,
ters) activities from levels in the order of several was measured above detection limits 88 times during the
mBq m3 to mBq m3, i.e., by a factor of 1000. The sampling period, most likely trapped in the pores of the
temporal variations of 210Pb did not indicate any filters or attached to particulate material. The source of
favourable season when the concentrations were sig- this nuclide was found to be one of the nearby hospitals.
nificantly higher or any linear correlation with the Additional measurements were made with active carbon,
meteorological data. The calculated yearly averages for cellulose and polypropylene filters in various places in
the 210Pb activities were very constant, including that this hospital, including in the areas where 131I wastes are
corresponding to 2002 when the total rainfall was kept. These measurements confirmed the existence of
highest. this nuclide in the air of the 131I storage room and the
Radionuclides from the 238U primordial chain (226Ra, ventilation outputs of the hospital as well as the
214
Pb, 214Bi) appeared seldom in the particulate filters, capability of both cellulose and polypropylene filters to
considerably less than those from the 232Th chain (228Ac, trap 131I. Although this hospital was supposed to be
212
Pb and 208Tl). 235U, the only nuclide detected above fully equipped with charcoal filters in its air outputs,
detection limits from its primordial chain, was recorded these filters had not been replaced periodically thus
only in 7 different weeks of measurement, while 40K was permitting the escape of this nuclide to the environment.
detected in 147 weeks. 214Pb and 214Bi, daughters of The concentrations measured in our atmospheric aero-
222
Rn, were in secular equilibrium with each other in sol filters were, in general, higher in spring and summer
almost all of the occasions when they were detected. seasons as compared to winter and autumn. No linear
212
Pb and 208Tl, daughters of 220Rn, showed a similar correlation was observed between the measured activity
behaviour. Differing with this, the activities of these two concentrations and any of the considered meteorological
pairs of radionuclides were not in secular equilibrium parameters. A weak negative linear correlation
with the 226Ra and 228Ac activities, most certainly due to (R ¼ 0:32) was observed with the relative humidity.
the mobility of the radon gases. During the 4 years of study, 131I was never detected in
Soils commonly contain measurable amounts of 40K, active charcoal filters which were placed adjacent to the
226
Ra and 228Ac. However, the source of 40K in the circular cellulose filters in the smaller pump (Radeco
filters does not seem to be same as that of 226Ra or 228Ac AV-28A). Although this type of filter is more
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Fig. 4. 40K and 137Cs concentrations in the large polypropylene filters obtained during 100 weeks of measurement. The weeks when
‘‘Calima’’ occurred are indicated in the upper part of the figure, each square represents a week with ‘‘Calima’’. The activities are given
in Bq m3. The error bars in the figure denote one sigma measuring uncertainties.

appropriate for the detection of gaseous radionuclides, daughters of 220Rn, 7Be and 210Pb were the main
the small volume which was actually pumped by this radionuclides in airborne particulate matter at this site.
sampler prevented us from detecting the 131I there. 212
Pb and 208Tl presented the highest activities in the
From the 171 measurements carried out in the large filters that were measured soon after collection. The
filters, 140 of them did not show 137Cs activities above maximum activity value found in the second set of filter
the detection limits. In 31 occasions this artificial nuclide measurements corresponded to 7Be with a concentration
was detected. The highest detected activity was of 7.370.2 mBq m3.
3.38 mBq m3. Therefore, the possible impact that the Significant linear correlations were found between the
inhalation by man of this nuclide may have, is very low. gross alpha and gross beta, gross beta and 210Pb as well
Several of the occasions when this nuclide was detected as 7Be and 210Pb activities. However, no important
coincide with the arrival of dust to the island from the correlations were found between these activities and the
Sahara desert (see Fig. 4). This phenomenon is locally considered meteorological parameters: temperature,
known as ‘‘Calima’’ and occurs several times per year, pressure, relative humidity, visibility, rainfall, wind
especially during winter season. The amount of speed and wing direction. The mean values calculated
dust which reaches the region is variable. During for the 7Be and 210Pb activities were lower than expected
‘‘Calima’’ episodes, the daily concentration of spherical for a continental site at the same latitude and altitude.
particles (TSP) in the lower atmosphere can reach mean Moreover, the relationship between 7Be and tempera-
values of 400 mg m3 (Davenport et al., 2004; Viana ture as well as the seasonal behaviour of this nuclide,
et al., 2002; Pérez-Marrero et al., 2002). 40K concentra- reported in recent literature for other continental sites,
tions were also clearly affected by this phenomenon was not observed in our data. The data measured in this
as shown in Fig. 4. 137Cs activities showed a positive insular environment do not fit with predictive models
linear correlation with 40K activities (R ¼ 0:46), indicat- developed for continental regions as mentioned earlier.
ing that the Saharan dust is an important source of 40K This, we consider of the outmost importance since it
in the atmosphere at this site. 137Cs activities, also, reflects that all atmospheric models developed for a
showed a weak negative linear correlation with the specific site should be critically tested when they are used
temperature (R ¼ 0:32) and wind speed (R ¼ 0:45). in other places and under different meteorological
However, the data is scarce to consider these correla- conditions.
tions significant. Two anthropogenic nuclides, 131I and 137Cs, were
detected in the particulate filters. The source of the 131I
was found to be a nearby hospital where cancer
4. Conclusions treatments are administered. No strong correlations
were observed between these nuclides and the considered
The measurements carried out on the aerosol filters meteorological parameters. The 137Cs showed a weak
soon after collection indicated that the short-lived negative linear correlation with the average temperature
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F. Hernández et al. / Atmospheric Environment 39 (2005) 4057–4066 4065

and wind speed. The 131I showed a weak negative linear Dibb, J., Jaffrezo, J.L., 1993. 7Be and 210Pb in aerosol and snow
correlation with the relative humidity. Measurements in the DYE 3 gas, aerosol and snow sampling program.
performed near the source of 131I confirmed the capacity Atmospheric Environment 27, 12865–12872.
of cellulose and polypropylene filters to trap this gaseous Dueñas, C., Fernández, C., Liger, E., Carretero, J., 1999.
nuclide. Gross-alpha, gross-beta activities and 7Be concentrations in
surface air: analysis of their variations and prediction
The data collected and analysed in this paper indicates
model. Atmospheric Environment 33 (22), 3705–3715.
that there exists a possible influence on the radiometric
Dueñas, C., Fernández, M.C., Carretero, J., Liger, E., Cañete,
concentration of airborne particulate matter due to the S., 2001. Gross-a and gross-b activities in airborne
long-range transport of aerosols loaded with 137Cs and particulate samples. Analysis and prediction models.
40
K from the African Continent and the frequent Applied Radiation and Isotopes 54, 645–654.
formation of a stable atmospheric inversion layer in Dueñas, C., Fernández, M.C., Carretero, J., Liger, E., Cañete,
the island. However, these hypotheses remain yet to be S., 2004. Long-term variation of the concentrations of long-
fully tested. It will be, also, important in the future to lived Rn descendants and cosmogenic 7Be and determina-
use atmospheric back-trajectory models to investigate tion of the MRT of aerosols. Atmospheric Environment 38,
the influence of the origin of the air masses on the 1291–1301.
concentration of the different radionuclides since this El-Daoushy, F., 1988. A summary on the lead-210 cycle in
nature and related applications in Scandinavia. Environ-
study may provide further clues to the source/s of
ment International 14 (4), 305–319.
different detected nuclides.
El-Hussein, A., Mohamemed, A., Abd El-Hady, M., Ahmed,
A.A., Ali, A.E., Barakat, A., 2001. Diurnal and seasonal
variation of short-lived radon progeny concentration and
Acknowledgements atmospheric temporal variations of 210Pb and 7Be in Egypt.
Atmospheric Environment 35, 4305–4313.
We wish to express our gratitude to the Consejo de Feely, H.W., Larsen, R.J., Sanderson, C.G., 1989. Factors
Seguridad Nuclear, Spain for their support to our that cause seasonal variations in be concentrations in
surface air. Journal of Environmental Radioactivity 9,
laboratory and to the Instituto Nacional de Meteor-
223–249.
ologı́a for all the meteorological data. Garcı́a-Talavera, M., Quintana, B., Garcı́a-Dı́ez, E., Fernán-
dez, F., 2001. Studies on radioactivity in aerosols as a
function of meteorological variables in Salamanca (Spain).
References Atmospheric Environment 35, 221–229.
Gerasopoulos, E., Zerefos, C.S., Papastefanuo, C., Zanis, P.,
Al-Azmi, D., Sayed, A.M., Yatim, H.A., 2001. Variations in O’Brien, K., 2003. Low-frequency variability of beryllium-7
7
Be concentrations in the atmosphere of Kuwait during the surface concentrations over the Eastern Mediterranean.
period 1994–1998. Applied Radiation and Isotopes 55, Atmospheric Environment 37, 1745–1756.
413–417. Gründel, M., Porstendörfer, J., 2004. Differences between the
Aldahan, A., Possnert, G., Vintersved, I., 2001. Atmospheric activity size distributions of the different natural radio-
interactions at northern high latitudes from weekly Be- nuclide aerosols in outdoor air. Atmospheric Environment
isotopes in surface air. Applied Radiation and Isotopes 54, 38, 3723–3728.
345–353. Hernández, F.J., El-Daoushy, F., 2002. Semi-empirical method
Azahra, M., González-Gómez, C., López-Peñalver, J.J., El for self-absorption correction of photons with energies as
Bardouni, T., Camacho-Garcı́a, A., Boukhal, H., El- low as 10 keV in environmental samples. Nuclear Instru-
Moussaoui, F., Chakir, E., Erradi, L., Kamili, A., Sekaki, ments and Methods A 484, 625–641.
A., 2004. The seasonal variations of 7Be and 210Pb Hotzl, H., Winkler, R., 1987. Activity concentrations of 226Ra,
228
concentrations in air. Radiation Physics and Chemistry Ra, 210Pb, 40K and 7Be and their temporal variations in
71, 789–790. surface air. Journal of Environmental Radioactivity 5,
Balkanski, Y., Jacob, D., Gardner, G., 1993. Transport and 445–458.
residence times of tropospheric aerosols inferred from a Lujaniene, G., Spirkauskaite, N., Lujanas, V., 1999. Meteor-
global three-dimensional simulation of 210Pb. Journal of ological factors and speciation of 7Be in the atmosphere.
Geophysical Research 98, 20,573–20,586. Journal of Aerosol Science 30 (1), 263–264.
Cannizzaro, F., Greco, G., Raneli, M., Spitale, M.C., Pérez-Marrero, J., Llinás, O., Maroto, L., Rueda, M.J., Cianca,
Tomarchio, E., 2004. Concentration measurements of 7Be A., 2002. Saharan dust Storms over the Canary Islands
at ground level air at Palermo, Italy—comparison with solar during winter 1998 as depicted from the advance very high-
activity over a period of 21 years. Journal of Environmental resolution radiometer. Deep-Sea Research II 49, 3465–3479.
Radioactivity 72, 259–271. Rangarajan, C., Eapen, C.D., 1967. Fitting empirical equations
Chamberlain, A., 1991. Radioactive Aerosols. Cambridge to rain scavenging ratios of atmospheric radioactive
University Press, Cambridge. aerosols. Atmospheric Environment 18, 2503–2506.
Davenport, R., Neuer, S., Fischer, G., Torres-Padron, M., Rodrı́guez, S., Guerra, J.C., 2001. Monitoring of ozone in a
Gelado-Caballero, D., Wefer, G., 2004. Geophysical marine environment in Tenerife (Canary Islands). Atmo-
Research Abstracts 6, 07662. spheric Environment 135, 1829–1841.
ARTICLE IN PRESS
4066 F. Hernández et al. / Atmospheric Environment 39 (2005) 4057–4066

Sheets, R.W., Thompson, C.C., 1992. Effects of polonium-210 Viana, M., Querol, X., Alastuey, A., Cuevas, E., Rodrı́guez, S.,
on the determination of atmospheric gross alpha radio- 2002. Influence of African dust on the levels of atmospheric
activity. Journal of Radioanalytical and Nuclear Chemistry particulates in the Canary Islands air quality network.
161, 465–474. Atmospheric Environment 36, 5861–5875.

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