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Home > Books > Air Quality

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TRACE ELEMENTS AND RADIONUCLIDES IN URBAN AIR MONITORED BY MOSS AND TREE LEAVES

Written By

Dragana Popovic, Dragana Todorovic, Mira Anicic, Milica Tomasevic, Jelena
Nikolic and Jelena Ajtic

Published: August 18th, 2010

DOI: 10.5772/9755

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Air Quality Edited by Ashok Kumar

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AIR QUALITY

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AUTHOR INFORMATION

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 * DRAGANA POPOVIĆ
   
    * University of Belgrade, Faculty of Veterinary Medicine, Serbia

 * DRAGANA TODOROVIĆ
   
    * 

 * MIRA ANIČIĆ
   
    * 

 * MILICA TOMAŠEVIĆ
   
    * 

 * JELENA NIKOLIĆ
   
    * 

 * JELENA AJTIĆ
   
    * University of Belgrade, Faculty of Veterinary Medicine, Serbia

*Address all correspondence to:

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1. INTRODUCTION

In urban areas, air quality is strongly influenced by numerous anthropogenic
activities. High population density, heavy traffic and domestic heating in
winters in the centre, and various industrial activities at the outskirts,
influence atmospheric concentrations of trace elements and radionuclides.
Consequently, large population is exposed to possible adverse effects arising
from the altered urban air composition. Therefore, air quality monitoring has
become one of the standard quality control procedures in urban areas.


1.1. TRACE ELEMENTS AND RADIONUCLIDES IN AIR

Due to changed atmospheric concentrations of trace elements, their availability
and cycling has changed, too. Numerous studies showed that trace metals as
persistent, widely dispersed and interacting with different natural components,
cause threat to human health and environment (Seinfeld & Pandis, 1998). Trace
elements in urban areas (such as Cu, Zn, and Pb) are mainly emitted by traffic,
including exhaust emissions and vehicle wear products (Harrison et al., 2003).
Even though the use of leaded gasoline has been drastically reduced, our
understanding of the effects of whole lead emission to air is far from
sufficient (Van der Gon & Appelman, 2009). As reported recently, though
atmospheric Pb had declined by a factor of 7 from 1980 to 2007, atmospheric
deposition is still recognised as a major pathway of Pb to vegetation and
topsoil (Hovmand et al., 2009). Since it offers a practical approach for
monitoring deposition of atmospheric trace elements on the surface environment
(Azimi et al., 2003; Tasić et al., 2008), collection of atmospheric deposition
using bulk sampling devices has been extensively used. However, instrumental
studies on atmospheric contamination are often limited by high cost and
difficulties in carrying out extensive monitoring surveys in time and space, and
do not offer reliable information about an impact of atmospheric pollutants on
the living systems.

Among the naturally occurring radionuclides in air, beryllium-7, radon and its
short lived progenies are most significant, while caesium-137 is of major
interest among the fission products. Long-lived radionuclides, potassium-40,
uranium and thorium, found in significant quantities in soils, are usually not
detectable in air, thus, if found on leaves, they are mainly resuspended from
soils (Vandenhove et al., 2009). The soil-to-plant transfer factor above 1.0 is
reported for 40K, while values for uranium and thorium are much lower (10-4)
(Uchida et al., 2007). In higher plants, the distribution of the radionuclides
is uneven. In tropical forest plants, for example, the highest 40K
concentrations are found in stem, and the lowest in root, while 137Cs is mostly
accumulated in root (Somashekarappa et al., 1996).

Beryllium-7 (half-life 53.28 days) is produced by cosmic rays in spallation
processes with light elements (nitrogen, oxygen, carbon) in the upper
troposphere and lower stratosphere. Its production depends on the Earth’s
magnetic field, and the variations in its annual mean concentrations are a good
indicator of changes in the atmospheric production rate caused by cosmic ray
intensity. The 7Be seasonal patterns are correlated to the
stratosphere–to–tropo-sphere exchange processes. The 7Be concentration in ground
level air in the midlatitudes has the maximum during spring and summer (e.g.,
Ajtić et al., 2008), caused by a seasonal thinning of the tropopause which
allows the 7Be rich stratospheric masses to enter the troposphere (Gerasopoulos
et al., 2003).

Lead-210 (half-life 22.3 years) is an effective tracer of continental surface
air masses history and often used to identify soil aerosols sources. It mostly
originates from the decay of uranium-238 in the Earth’s crust, but anthropogenic
sources (uranium ores sintering, coal combustion, production or use of phosphate
fertilizers) also contribute to the total 210Pb in air (UNCEAR, 1988).
Deposition of 210Pb varies with season and geographical position. The 210Pb
concentration maxima in fall could be attributed to an enriched emanation of
radon. Radon emanation, and therefore concentration of 210Pb in air, is affected
by atmospheric pressure, temperature inversions, covering vegetation, snow and
ice ground coverage, etc. Furthermore, important factors influencing the 210Pb
concentrations in air are soil geology, continental and areas masses
distribution, conditions of surface air layers, etc. (Delfanti et al., 1999).

Due to its half-life of 30 years, 137Cs is a good indicator of nuclear weapon
atmospheric tests and nuclear power plant accidents on global scale. Since 1986,
137Cs in ground level air has mainly originated from the Chernobyl nuclear
accident, with concentrations of the order of µBq/m3, and with one or two maxima
in summer and winter. The 137Cs winter maxima are attributed to the inversion
weather conditions and to soil dust air resuspension from the Chernobyl fallout
(Todorovic et al., 1999).


1.2. MOSS AND TREE LEAVES AS BIOMONITORS

For several decades, air quality biomonitoring has been widely applied to detect
and monitor the effects of trace elements pollution (Bargagli, 1998; Markert et
al., 2003). Mosses and lichens are recognised as the most appropriate
biomonitors of atmospheric trace elements and radionuclides contamination. Many
studies have demonstrated the ability of moss to absorb and accumulate trace
elements in their tissue. Due to the absence of root and cuticle, mosses uptake
their nutritive elements from wet and dry atmospheric deposition (Rühling &
Tyler, 1968). Mosses have also been recognised as valuable biomonitors in the
assessment of temporal trends in trace metal accumulation (Harmens et al.,
2008), and in spatial variations across national boundaries (Schröder et al.,
2008).

Mosses are also highly efficient in accumulating radionuclides and have been
widely used as reliable bioindicators of radioactive contamination of the
environment since the late 1960’s (Sumering, 1984; Steinnes, 2008; Frontaseyeva
et al., 2009; Aničić et al., 2007; Barandovski et al., 2008; Guillén et al.,
2009). Due to their continuous accumulation of elements, mosses offer
information about the sources of pollution long after the pollution episode
itself took place (Golubev et al., 2005). Being globally spread, mosses are an
important tool in mapping global distribution of radionuclides following nuclear
weapon atmospheric tests and in radioactivity monitoring in the vicinity of
nuclear and coal power plants (Delfanti et al., 1999; Uğur et al., 2003). In
1986, mosses and lichens proved to be reliable indicators of environmental
contamination after the nuclear plant accident in Chernobyl (Papastefanou et
al., 1989; Hofmann et al., 1993). In the late 1990’s, mosses and lichen were
used to estimate the level of contamination caused by the military use of
depleted uranium (DU) in the Balkans (UNEP, 2002; Loppi et al., 2003;
Frontasyeva et al., 2004; Popovic et al., 2008a).

Since naturally growing mosses are often rare or absent in urban areas, the
“moss bags technique’’ (active biomonitoring) has been developed in order to
spatially and/or temporally assess deposition of trace elements in highly
polluted areas (Goodman & Roberts, 1971; Vasconcelos & Tavares, 1998; Fernandez
et al., 2004; Culicov & Yurukova, 2006). The technique offers several advantages
compared to naturally growing mosses: one can precisely limit the time of
exposure, acquire data on the concentrations of different elements in the sample
prior to the exposure, and choose a most suitable site for moss transplantation.
The Sphagnum moss species are especially recommended for active biomonitoring
for their large surface area and a number of protonated anionic functional
groups (ion exchange sites) in the form of uronic acids. However, moss bags tend
to dry out and thus their efficiency in retaining elements varies with the
environmental conditions, especially humidity (Al-Radady et al., 1993). Until
now, only a few quantitative comparisons of biomonitoring methods with the
standard measurements of atmospheric deposition have been published (Berg &
Steinnes, 1997; Thöni et al., 1996; Aničić et al., 2009a,b). Moreover, the exact
relationship between the element content in moss and the actual atmospheric
deposition is not yet well understood, though some studies have given evidence
of possible quantitative conversion with unsedimentable dry deposited particles
(<0.8 μm) (Vasconcelos & Tavares, 1998).

In urban and industrial areas, however, where lichens and mosses are often not
found, higher plants could replace them. In areas with high atmospheric
pollutant loads, plants may provide information, not only about quality/quantity
of air pollutants, but also about effects on ecosystems. Leaves of both
evergreen and deciduous tree species have been recognised as valuable
accumulative biomonitors of atmospheric elements and radionuclides in urban
areas. Tree leaves are also very efficient in trapping atmospheric particles
(Freer-Smith et al., 2005; Peachey et al., 2009; Qiu et al., 2009), and they
have a special role in reducing the level of “high risk” respirable particulates
possibly harmful to the environment and human health (Beckett et al., 2000).
There are numerous studies searching for sensitive tree species, and their
validity for urban air quality biomonitoring (Alfani et al., 1996; Monaci et
al., 2000; Piczak et al., 2004; Mingorance & Oliva, 2006; De Nicola et al.,
2008). Some species show a good response to atmospheric trace elements
pollution, e.g. Q. ilex may be appropriate for biomonitoring in urban areas
where it is naturally present and widely distributed (Gratani et al., 2008). A
significant correlation was reported between the Cu and Fe contents in inhalable
atmospheric particles (PM10) and in leaves of Nerium oleander (Espinosa & Oliva,
2006). According to Bargagli (1998), the species of Tilia genus could be used as
biomonitors of trace elements in urban and industrial environments, while Baycu
et al. (2006) reported that, compared to other urban tree species, A.
hippocastanum accumulated the highest Pb concentrations in leaves.

Plants are also an important link in the transport and distribution of
radionuclides from the source of pollution to man and can be used as biomonitors
of atmospheric pollution by radionuclides (Djuric and Popovic, 1994).
Radionuclides can be deposited on plants from air (foliar deposition) where they
appear from fallouts or by natural sources, or can be taken through soil root
system. Most of the air borne radionuclides are quickly attached to aerosols,
and their concentration in air is manly due to behaviour of aerosols in the
atmosphere. Thus, the rate of their removal from the atmosphere and deposition
on ground and vegetation depends on the size of particles they are attached on
(Djuric and Popovic, 1994). Foliar deposition and absorption of radionuclides
from air to leaves are closely associated not only with morphological
characteristics of leaves, but also with local climate (moisture, concentrations
of dust particles, wind velocity and direction, amount of precipitation, etc).
Thus, some authors found radionuclides concentrations in leaves to be of an
order of magnitude or two less than those in stem or roots (Somashekarappa et
al., 1996). Accumulation of radionuclides by plants, e.g. estimation of
soil-to-plant transfer factors, foliar deposition rate and root uptake, has been
in focus of investigations of many authors, but mainly for agricultural plants,
cereals and vegetables, in laboratory and/or in field conditions (Djuric et al.,
1996; Djuric & Popovic, 1994; Golmakani et al., 2008; Koranda & Robison, 1978).
The main problem in assessing the contribution of air pollution compared to root
uptake is the fact that soil-to-plant/leaves transfer factors are found in the
large range of values (10-3–10-1) due to numerous factors, mainly
characteristics of soils and leaves/plant morphology (IAEA, 1994). Solubility,
pH, acidity, organic matter content, etc., play a vital role to radionuclides
availability by plants (Golmakani et al., 2008). Still, some studies found
similar seasonal variation pattern of 7Be and 210Pb between leaves and aerosol
samples, high in spring and low in summer (Sugihara et al., 2008).

Trace elements in Belgrade air are mostly bound to the particulates of the mixed
road origin (Rajšić et al., 2008). As reported previously for the area, the
leaves of A. hippocastamum and Corulys colurna showed a distinguished seasonal
accumulation of some elements (Cu, Zn and Pb). Among the two, A. hippocastanum
seems a more suitable biomonitor, not only by the leaf content, but also because
it was found that a level of the Pb accumulation reflected marked changes in the
atmospheric Pb concentrations (Tomašević et al., 2008).

Active biomonitoring with the moss bag (MB, Sphagnum girgensohnii Russow,
Russia) and bulk deposition (BD) measurements were performed for trace elements
(Al, V, Cr, Mn, Fe, Ni, Cu, Zn, As, Cd, Pb) atmospheric deposition in the urban
area of Belgrade in 2005 – 2006. The aim of the research was to evaluate trace
element accumulation in the moss bags, and to examine its relationship to the
atmospheric bulk deposition measurements. In order to assess the actual
responses of moss to trace element concentrations in air, and to investigate the
role of water supply on the moss accumulation ability, experiments with dry and
irrigated (wet) moss bags were carried out. The content of natural and fallout
radionuclides (7Be, 210Pb, 40K and 137Cs) in moss bags was also determined, with
an aim to assess the validity of the method for radioactivity monitoring and
control in ground level air.

The trace elements (Cr, Fe, Ni, Zn, Pb V, As, and Cd) accumulation and the
temporal trends were also assessed in leaves of the trees common for the city of
Belgrade: Aesculus hippocastanum (horse chestnut) and Tilia spp. (linden), over
a period of five years (2002 – 2006). The relationship between the trace
elements concentration in the leaves and the instrumental measurements of
atmospheric bulk deposition was also examined. The contents of radionuclides in
leaves in comparison with their activities in ground level were determined, too.

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2. EXPERIMENTAL


2.1. STUDY AREA

The study was conducted in Belgrade (44˚ 49’ N, 20˚ 27’ E; 117 m a.s.l.), the
capital of Serbia, with about 2 million inhabitants, situated at the confluence
of the rivers Sava and Danube. The climate is moderate continental with fairly
cold winters and warm summers. In winter, severe air pollution as aerosol smog
occurs frequently in the central city area, particularly during meteorologically
calm and stable conditions. The number of vehicles is around 500,000, including
heavy-duty trucks and over 1,000 city buses run on diesel. The average age of
passenger cars is more than 15 years, and leaded gasoline is still widely used.
There are many old buses and trucks in the city traffic, which could be the
major source of ambient particulates. The city is heated with a number of
heating plants run on natural gas or crude oil, but there are still individual
houses heated with coal (Todorović et al., 2005; Todorovic et al., 2007).
Natural gas has only been introduced in the last few years.

The moss bags measurements were carried out at three representative sites in
heavy traffic areas: the Faculty of Veterinary Medicine (VF), the Rector’s
Office Building of the Belgrade University (RB), and the Public Health Institute
(HI). The tree leaves samples were collected in the parks adjacent to those
three locations. Trace elements and radionuclides accumulation was investigated
in dry and wet moss bags and tree leaves (in May and September), while bulk
deposition and aerosols were collected on a monthly basis at the same places and
time. The map of Belgrade central area, with the sampling sites, is presented in
Figure 1.



FIGURE 1.



Map of Belgrade central city area with the sampling sites: A) the Rector’s
Office building of the Belgrade University RB, B) the Public Health Institute
HI, and C) the Faculty of Veterinary Medicine VF.




2.2. MOSS SAMPLING, BAG PREPARATION AND ANALYSIS

2.2.1. TRACE ELEMENTS

Moss (Sphagnum girgensohnii Russow) was collected in June 2005 from a pristine
wetland area near Dubna, Russia (56˚ 44' N, 37˚ 09' E; 120 m a.s.l.), and
cleaned from soil particles and other matter. About 3 g of moss was packed in
(10 x 10) cm2 nylon net bags (1 mm mesh size). The bags, with and without
irrigation (WET and DRY MB) were exposed at the same time at the three sampling
sites (Figure 1). Wet moss bags were placed on the top of cellulose sponge with
the bottom immersed in distilled water, and the setup was put in a polyethylene
box. Distilled water was added every several days, depending on meteorological
conditions (precipitation and temperature) (Aničić et al., 2009a). Using
specially constructed holders (1.5 m high) on platforms 5–10 m above the street
level, two dry (hung freely in the air) and two wet moss bags were exposed for
five 3-month periods, between July 2005 and October 2006. After the exposure,
the moss was removed from the net, homogenised and dried to a constant weight at
40 ºC for 24 h.

The concentrations of Al, V, Cr, Mn, Fe, Ni, Zn, and As were determined by
instrumental neutron activation analysis (detection limit 0.01–10 µg/g).
Short-term irradiation (2 min) was applied for short-lived radionuclides (Al, V,
and Mn). The long irradiation (100 h) was applied to determine elements
associated with long-lived radionuclides (Na, Cr, Fe, Ni, Zn, and As). The
concentrations of Cu, Cd, and Pb in moss were analysed by flame atomic
absorption spectrometry. Quality control was performed using the standard
reference material: Lichen (IAEA–336), Tomato Leaves (SRM–1573a) and Coal Fly
Ash (SRM–1633b).

2.2.2. RADIONUCLIDES

Moss (S. girgensohnii) was packed in nylon net bag (total mass 255 g), and
exposed on the VF site (Figure 1) for one year (May 2006 – May 2007). The site
is in the vicinity of a highway, and is one of the pollution “black spots” in
the city. It is also the sampling site for air radioactivity monitoring by
filter paper method (Todorovic et al., 2007).

Prior to exposure, the moss was dried and cleared of soil and other material.
After the exposure, the sample was divided into eight subsamples of 25–36 grams
to examine the uniformity of radionuclides’ distribution within the sample
(Popović et al., 2009b).

The activities of 7Be, 210Pb, 40K and 137Cs were determined on an HPGe detector
(Canberra, relative efficiency 23%) by standard gamma spectrometry. Geometric
calibration was performed using the standard reference radioactive material
IAEA-373 (grass, with 134Cs, 137Cs, 40K and 90Sr, total activity of 15 kBq d.w.
on 31.12. 1991). Counting time was 58,000 s, with the total standard error of
16% for 40K, 20% for 210Pb, and 10% for 137Cs (Popović et al., 2009b).


2.3. TREE LEAVES SAMPLING AND ANALYSIS

Leaves were sampled from Aesculus hippocastanum L. (horse chestnut), and Tilia
spp. (linden: Tilia tomentosa L. and Tilia cordata Mill.), at the beginning
(May) and the end (September) of the vegetation seasons from 2002 to 2006. Five
subsamples (10 to 15 fully developed leaves) were taken randomly from several
crowns 2 m above the ground (Tomašević et al., 2008). Leaves were washed with
bidistilled deionised water, dried at 40 ºC for 24 h, and pulverised with agate
mortars prior to analyses. About 0.4 g of leaves were digested for 2 h in a
microwave digester with 3 ml of 65% HNO3 (Suprapure, Merck) and 2 ml of 30%
H2O2, and then diluted with distilled water to a total volume of 25 ml. The
content of Cr, Fe, Ni, Cu, Zn, and Pb was determined by inductively coupled
plasma optical emission spectrometry, and V, As, and Cd by inductively coupled
plasma mass spectrometry. Quality control was performed using the standard
reference material Lichen-336 (IAEA).

For radionuclide analysis, the samples of leaves were collected in the identical
fashion (Tomašević et al., 2008). In addition, samples of soils were also
collected in the three sites. Soils and leaves were measured in native state,
leaves were dried up to 105 ºC. Aerosols were also sampled and analysed for the
contents of radionuclides by standard procedures (Todorović et al., 2005;
Todorovic et al., 2007).


2.4. SAMPLING AND ANALYSIS OF BULK DEPOSITION

Bulk depositions were collected monthly, in open polyethylene cylinders (29 cm x
40 cm) fixed in baskets at the measuring sites, from the beginning of 2002 to
the end of 2006. The samples were evaporated to dryness and digested with 50 ml
of 0.1 N HNO3 on an ultrasonic bath. The content of Al, V, Cr, Mn, Fe, Ni, Cu,
Zn, As, Cd, and Pb was determined by flame atomic absorption spectrometry
(Perkin Elmer AA 200) and graphite furnace atomic absorption spectrometry (Tasić
et al., 2009). For calibration, standard solutions containing all metals of
interest were prepared using Merck certified atomic absorption stock standard
solutions.


2.5. TRACE ELEMENTS DATA ANALYSIS

Data analysis included the basic statistics (mean/average, correlation, and
t-test) for Al, V, Cr, Mn, Fe, Ni, Cu, Zn, As, Cd, and Pb concentrations
measured in DRY and WET MB, the tree leaves and the monthly BD samples. To
assess the element accumulation in moss, the relative accumulation factors (RAF)
were calculated as the ratio of the moss content of element after and before the
exposure (Cexposed - Cinitial), and before the exposure (Cinitial):

RAF = (Cexposed− Cinitial) / CinitialRAF = (Cexposed− Cinitial) / Cinitial
E1
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3. RESULTS AND DISCUSSION


3.1. TRACE ELEMENTS IN MOSS BAGS

The initial (background) content of elements plays a crucial role in obtaining
the relative accumulation level in biomonitoring studies. For most of the
examined elements, the initial values in S. girgensohnii, used for active
biomonitoring in Belgrade (Aničić et al., 2009a,b), were significantly lower
than those from other sites (Adamo et al., 2003; Djingova et al., 2004; Culicov
& Yurukova, 2006) or in other Sphagnum spp. (Djingova et al., 2004). The initial
element concentrations in S. girgensohnii were even lower than the values
proposed by Markert (1992) as “reference plant values” used to compare elements
accumulation among the different species. This points to the variation in
natural Sphagnum element content from different areas and, consequently, to a
necessity to determine the background (control) levels prior to each
biomonitoring study. The advantage of low background levels is the higher method
sensitivity in areas with low atmospheric deposition (Culicov et al., 2005).

Significant accumulation of the majority of examined elements in the S.
girgensohnii moss bags were observed over the 3-month exposure periods (Table 1)
indicating that this species is an efficient trace element accumulator (Aničić
et al., 2009a). Higher element content was measured in the WET MB (except for
Mn) which is in agreement with other studies (Al-Radady et al., 1993). One of
the differences between the WET and DRY MB is that deposited particles are
trapped in higher quantities on wet surfaces. Furthermore, WET MB could
incorporate the elements in its tissues, whereby being less susceptible to
rinsing and thus better reflecting the atmospheric conditions (Astel et al.,
2008). This is in agreement with findings of Berg & Steinnes (1997) that
atmospheric humidity and precipitation are important factors for moss
accumulation.

To compare the element accumulation in DRY and WET moss bags, relative
accumulation factors RAF (Equation 1) were calculated. The RAF values, which are
inherently insensitive to the influence of the initial element content, have
been used to compare accumulation between different monitoring species (Adamo et
al., 2003; Culicov & Yurukova, 2006). The most accumulated elements in DRY MB,
according to the RAF value were V (22), followed by Cr (11) > Cu (9) > Pb (8) >
As (5) > Al (4) > Fe (3) > Ni (3) ≈ Zn (2.5) > Mn (0.9) > Cd (0.5). In WET MB,
the order for the most accumulated elements was somewhat different: Cu (68) > V
(26) > Cr (21) > Pb (13) > Al (6.5) > As (6) > Fe (5) > Zn (4.5) > Ni (4) > Cd
(1) > Mn (0.2) (Aničić et al., 2009b). The accumulation of Cu in WET MB was
about eight times higher than for DRY MB. Likewise, the content of Cr was about
twice as high in WET MB. Other elements, such as Pb, Al, Fe, and Zn, were
slightly more accumulated in WET MB than in DRY MB. In some moss bags, both dry
and wet, a loss of Mn, compared to the initial material, was evident (10% and
80%, respectively). The loss of Mn caused by washing out and leaching from moss,
was described in Couto et al. (2004). The RAF values, obtained in this study,
are significantly higher than the literature data (Adamo et al., 2003; Culicov &
Yurukova, 2006). This is most likely related to higher atmospheric pollution in
Belgrade urban area, and to lower initial concentration of the elements in used
S. girgensohnii moss.

S. g. S. girgensohnii (DRY MB) S. girgensohnii (WET MB) Element Initial Min Max
Median Min Max Median Al 254 659 1960 1363 802 3523 1870 V 0.54 2.9 112 13 2.9
69 14 Cr 0.25 2.0 6.8 3.1 3.7 8.3 5.8 Mn 113 92 322 215 77 212 134 Fe 297 732
2496 1219 1026 4810 1682 Ni 2.4 1.9 41 8.7 4.5 30 12 Cu 2.1 10 49 20 42 476 144
Zn 20 44 105 71 85 264 113 As 0.11 0.38 2.2 0.67 0.53 5.4 0.80 Cd 0.18 0.19 0.36
0.27 0.25 0.50 0.36 Pb 2.2 7.0 38 20 14 63 31


TABLE 1.

Trace elements (μg g-1 of dry weight) in DRY and WET MB of S. girgensohnii
exposed in Belgrade urban area.



3.1.1. TRACE ELEMENTS ACCUMULATION IN MOSS BAGS VS. BULK DEPOSITION

To compare the element accumulation in moss bags with the bulk deposition data,
the moss element concentrations (μg g-1) were expressed as the deposition fluxes
(μg m-2 day-1) and the Spearman rank correlation coefficients (r) were
calculated to estimate a relationship between the element deposition flux in DRY
MB/WET MB and BD. The correlation between the element BD and the element
deposition flux in WET MB was high for V (r=0.87), As (r=0.74), Fe (r=0.73), Al
(r=0.71), and Ni (r=0.68). No correlation was found for Cd, Mn, and Zn. The DRY
MB vs. BD highest correlation was found for Cu (r=0.85). Lower, but still
significant correlation (r > 0.50), was obtained for Pb, Cr, and Zn (Aničić et
al., 2009a).

In general, trace elements may be deposited onto the moss surface either as dry
particulates or dissolved and/or suspended in precipitation. The elements may be
retained by particulate entrapment, physicochemical processes such as ion
exchange or by passive and active intracellular uptake (Tyler, 1990). Therefore,
moss is not a mere passive filter. Poor correlation for some element deposition
fluxes in moss samples and BD probably indicates more complex mechanisms of
element accumulation in moss. Furthermore, due to splash effect and irregular
surfaces, it is difficult to estimate the exact atmospheric deposition fluxes in
moss bags. Nevertheless, the concentrations of some elements (e.g., V, Fe, Co,
As, Mo, Cd, Sb, and Pb) were found to be significantly correlated in moss and
wet deposition (Couto et al., 1994; Berg & Steinnes, 1997). The rate of element
uptake by moss increased markedly, but not regularly, with atmospheric humidity
and precipitation, whereas their atmospheric level decreased (wet deposition),
preventing the possibility of establishing a conversion factor for wet weather
conditions (Vasconcelos & Tavares, 1998).

Studies on the capture of atmospheric particles by moss have demonstrated that
standardised active biomonitoring with moss bags provides a better capture
efficiency of particles over 20 μm in diameter (sedimentable particles) less
influenced by abiotic conditions like wind speed. Therefore, it was suggested
that particles trapped by bryophytes may be a major source of poorly
water-soluble elements, and that moss content can reflect recent environmental
conditions for dry and coarse depositions, especially for active biomonitoring
experiments in highly polluted areas (Amblard-Gross et al., 2002).

3.1.2. SEASONAL VARIATIONS OF TRACE ELEMENTS IN MOSS

Trace elements content in moss bags was also analysed for the summer (May –
October) and winter (November – April) seasons. Seasonal variations in both DRY
and WET MB samples were observed for all of the elements except Pb, Al, and Mn.
At all three sites, the highest variations were noticed for V and Ni, whose
content was two and three times higher in winter than in summer, respectively
(Figure 2).

The content of As and Fe in moss bags were 1.5 times higher in winter than in
summer. This was not unexpected as these elements are markers for oil and coal
combustion. However, concentrations of Cu were increased in summer, especially
in WET MB. Moreover, the concentrations of Zn and Cd in WET and DRY MB were
slightly higher in summer than in winter period. These elements are markers for
traffic sources, but our results point to some other local sources, more
expressed during the warm period (Aničić et al., 2009a).

Seasonal variations were also found for the elements in the bulk deposition,
being higher in winter season (except for Pb, which was increased during summer
time). In winter, much higher contents of V, Ni, As, and Fe were found in the
bulk deposits.


3.2. RADIONUCLIDES IN MOSS BAGS

Fission product 137Cs and naturally occurring 40K and 210Pb were detected in all
of the eight subsamples of moss bags, while 7Be was detected only in one, with
the activity of 60 Bq/kg.



FIGURE 2.



Seasonal variation of V and Ni daily fluxes (mg m-2 day-1) for DRY MB and WET
MB, and BD for 3-month periods in 2005/2006 at the study sites (VF, RB, and HI).



The absence of 7Be in the subsamples could be explained by its decay, since the
period between the sample arrival in the laboratory and the analysis was nearly
60 days. Taking into account the standard uncertainty of the method and the
volume of the composite sample, the distribution of the activities of the
detected radionuclides in the eight subsamples was rather uniform with the
differences not exceeding 30% (Popović et al., 2009b). The level of the annual
activities of the radionuclides implied that the exposure time could be reduced
to a month, and that would enable monitoring seasonal variations in the content
of radionuclides in air. The mean activities with standard deviations of 40K,
210Pb, and 137Cs in moss bags (S. girgensohnii), are given in Table 2. For
comparison, the content of these radionuclides in naturally growing mosses
(Hypnum cupressiforme) in Southern Serbia (Borovac) are also presented in the
table.

Location Activity (Bq/kg) 40 K 210 Pb 137 Cs 7 Be 245 ± 34 315 ± 25 28 ± 4 /
Borovac 298 ± 42 210 ± 52 226 ± 22 228 ± 34


TABLE 2.

Activities of the radionuclides in moss bags (S. girgensohnii) exposed in
Belgrade (Popović et al., 2009b) and in H. cupressiforme, Borovac (Popovic et
al., 2008b).



The activity ratio 210Pb/40K of 1.30 was calculated. The ratio could provide a
sound basis for the 210Pb activity estimation by solely measuring the activity
of 40K, which is more easily detected, and with a lesser uncertainty than 210Pb
(Popović et al., 2009b). The mean activities of the detected radionuclides in
moss bags were in the range of the values reported for the local moss (H.
cupressiforme) in the region (Krmar et al., 2007; Popovic et al., 2008b), with
differences arising from the species, the method, local climate and soil
characteristics. Krmar et al. (2007) found measurable, even significant
concentrations of 7Be in H. cupressiforme, with an increase in summer and autumn
(up to 920 Bq/kg), but the sampling in the study took place over a 14–month
period. Beryllium-7 was also found in naturally growing moss (H. cupressiforme)
in the rural area of Southern Serbia (Popovic et al., 2008b) (Table 2).

As can be seen from Table 2, there are no significant differences in the content
of 40K in naturally growing mosses in Southern Serbia and in the urban area of
Belgrade. On the other hand, higher concentrations of 210Pb in Belgrade indicate
a contribution of anthro-pogenic air pollution sources. Significantly higher
activities of 137Cs, as well as the detectable amount of 7Be, in mosses sampled
in Southern Serbia are due to a longer, undefined exposure period (in the
Belgrade study, the exposure period of one year was precisely defined). Hence,
the observed differences mirror the differences in the accumulation period.

Before the Chernobyl nuclear plant accident in 1986, the concentrations of 137Cs
in moss and lichen in Serbia were under 1 Bq/kg (Djuric & Popovic, 1994).
Immediately after the accident and later, the contents of 137Cs in mosses and
lichens, sampled in a mountainous region, was in the range of 8–18 kBq per kg of
dry weight (Djuric et al., 1992, 1996; Popović et al., 1996). In 1997, the
activities of 137Cs in the naturally growing mosses in a region in Serbia were
up to 3 kBq/kg, while the soil-to-moss transfer factors calculated for the same
region in 2000 were in the range of 3.0–10.0 (Popović et al., 2009a). High
transfer factors for 137Cs and 210Pb from soil to mosses were also found in
Southern Serbia, in the range of 1–10 and 4–10, respectively (Popovic et al.,
2008a).

Still, as already mentioned, naturally growing mosses are unlikely to be found
in urban areas, and the active moss monitoring is therefore a suitable
alternative technique for monitoring contents of radionuclides in urban air.
Furthermore, this method solves some of the problems in monitoring using
naturally growing mosses, such as intercalibration of different species of
mosses and transformation of concentrations in moss to absolute deposition rate
(Steinnes, 2008).

Frontasyeva et al. (2009) proposed a linear correlation between the
concentrations of 137Cs in mosses Amoss and in air Aair:

Aair(Bq/m3) = 3.3 x 10−8(kg/m3) x Amoss(Bq/kg)Aair(Bq/m3) = 3.3 x 10−8(kg/m3) x Amoss(Bq/kg)
E2

When applying this relationship to the activity of 137Cs in moss obtained in our
study, the calculated 137Cs activity in air is 0.924x10-6 Bq/m3, which is under
the lower limit of detection in our measurements (1x10-6 Bq/m3).

To conclude, since the Belgrade study showed that the exposure time for the moss
bags technique could be reduced to a month, the technique could be used to
monitor the level of radionuclides’ contents in air, as well as to follow their
seasonal variations.


3.3. TRACE ELEMENTS IN TREE LEAVES

Seasonal accumulation trends of elements’ concentration in leaves have been well
known and reported for many plant species (Kim & Fergusson, 1994; Bargagli,
1998; Piczak et al., 2003). In Belgrade urban area, the elements’ concentration
were determined in leaves of A. hippocastanum and Tilia spp. at the beginning
(May) and the end (September) of the vegetation seasons over a period of 2002 –
2006. An increase of the element concentrations (p<0.001) from May to September,
i.e. seasonal element accumulation, was evident in all of the A. hippocastanum
samples throughout the investigated years for V, Cr, Fe, As, Ni, Zn, and Pb
(Figure 3). However, in Tilia spp. leaves the elements’ increase was not regular
(Figure 4).

On the other hand, in A. hippocastanum leaves there was no regularity in the
seasonal accumulation of Cu (p<0.15) and in Tilia spp. leaves for Cu (p<0.2) and
Zn (p<0.09). For A. hippocastanum, such seasonal discrepancy in the Cu and Zn
concentrations was previously noted by Kim & Fergusson (1994), who pointed out
that these elements concentrations were the highest in new leaves, and decreased
over the vegetation season. Thus, variations in seasonal accumulation of Cu and
Zn in some samples of A. hippocastanum and Tillia spp. may be a result of the
fact that these elements are essential constituents of plant tissue. It is
considered that the Cu remobilisation to non-senescent parts occurs before the
senescence, and leaf fall takes place. In walnut trees, the concentration of Cu
in old leaves was just 8 % of the maximum Cu value in younger mature leaves
(Drossopoulos et al., 1996). Moreover, some recent data for the black spruce
needles supported the previous hypothesis and confirmed that an active
translocation of essential metals, particularly Cu, takes place from senescent
to non-senescent parts of a plant. However, the results for Pb, as a
nonessential metal, were in accordance with a hypothesis that the passive
sequestration of toxic metals was attained in the senescing foliage as a
detoxification process (Aznar et al., 2009).

3.3.1. SPATIAL AND TEMPORAL TRACE ELEMENTS’ VARIATION IN LEAVES VS. BULK
DEPOSITION

Evaluation of biomonitoring validity is a complex process and, apart from the
accumulation level, requires other data, such as temporal trend consistency in
accumulation capability. Moreover, the biomonitor should be in correspondence
with instrumental monitoring data. Following the previous assumptions, the
obtained elements concentration in leaves was compared to the bulk deposition
data. From 2002 to 2006, the Pb concentrations in leaves of A. hippocastanum at
the beginning and the end of vegetation seasons showed a decreasing trend at all
sites (Figure 3 and 4). Temporal decrease of the Pb concentrations in leaf
tissue of both species, observed in Belgrade urban area, might be a consequence
of a diminishing use of leaded gasoline over the period. This is in accordance
with the data reported for other European countries (Dmuchowski & Bytnerowicz,
2009). Furthermore, as shown by a long-term study of Hovmand et al. (2009),
though atmospheric Pb declined by a factor of 7 from 1980 to 2007, airborne Pb
is still considered a major pathway to vegetation and topsoil.



FIGURE 3.



Median concentrations (μg g-1) of Cd, As, V, Cr, Ni, Pb*, Cu*, Zn*, and Fe** in
the leaves of A. hipposactanum, sampled from the urban area of Belgrade in May
and September from 2002 to 2006.



Note: Concentrations of Pb*, Cu* and Zn* are divided by 10 and Fe** by 100 to
clearly present the results on the graph



FIGURE 4.



Median concentrations (μg g-1) of Cd, As, V, Cr, Ni, Pb*, Cu*, Zn*, and Fe** in
the leaves of Tilia spp., sampled from the urban area of Belgrade in May and
September from 2002 to 2006.



Note: Concentrations of Pb*, Cu* and Zn* are divided by 10 and Fe** by 100 to
clearly present the results on the graph

Uncertainty in element uptake pathways has generally been seen as a disadvantage
for the use of the vascular plant leaves as biomonitors of trace element
atmospheric pollution. However, Hovmand et al. (2009) investigated the origin of
Pb in leaves and showed that less than 2 % of the Pb content of needles and
twigs of Norway spruce comes from root uptake, i.e. approximately 98 % is of
atmospheric origin. Tomašević et al. (2008) showed that in the Belgrade urban
area there was a good correlation between the Pb leaf content of A.
hippocastanum with a significantly increased level of atmospheric Pb in
suspended particles during two successive years (1996 and 1997). Therefore, the
Pb concentration in the leaves of A. hippocastanum reflected changes in
atmospheric Pb pollution.

Among the sites, Cu concentrations were obtained at significantly higher level
at the RB site, which was also shown by some instrumental monitoring techniques:
BD, PMs (Rajšić et al., 2008) and active moss biomonitoring (Aničić et al.,
2009a,b) pointing to an additional local source. Through the investigated years,
the observed Cu concentration at this site showed a decreasing trend, a more
regular one for A. hippocastanum (Figure 5) than for Tilia spp. Presumably, a
local Cu emitter (metal arts and crafts manufacturing) contributed to a much
higher atmospheric Cu levels in 2002, 2003 and 2004 at the RB site, tending to
decrease throughout the years until it closed down. Namely, at this site the Cu
concentration was the highest in September 2002, and the accumulation level was
about nine times higher in A. hippocastanum leaves (88 μg g-1) than in the
“reference plant” (10 μg g-1, given by Markert, 1992). At the same time, Cu
concentrations in bulk deposition were 3–4 time higher in the first than in the
final year of the study (Figure 5). Thus, the temporal trend for Cu accumulation
in A. hippocastanum leaves follows the Cu contents in the BD for the RB site.
The Cu content in Tilia spp. leaves did not show a clear seasonal nor temporal
dependence.



FIGURE 5.



The Cu concentrations in A. hipposactanum leaves in May and September (2002 –
2006), and bulk deposition (BD) at the RB site.



The soil Cu concentration at the RB site also decreased from 98 μg g-1 in 2002
(Tomašević et al., 2004) to 50 μg g-1 in 2008 (Marjanović et al., 2009).
However, the presence of the elements in soil does not imply that they are
available to plants, as plant-to-soil concentration ratio is far from a linear
one (Bargagli, 1998). The results of Chojnacka et al. (2005) showed that there
is a low correlation between the transfer factors of metals from polluted soils
to plants. Moreover, the pH of the soil samples at the RB site was 8.8, and it
is not likely that the element availability for the root uptake would be
considerable. Consequently, it may be concluded that in our study the Cu content
in leaves was mainly of atmospheric origin.

Temporal trends of V and As in the investigated years were slightly decreasing
(Figure 3 and 4), but no correlation with the bulk deposition was observed.
However, there was no substantial variation in the accumulated content of Cr,
Fe, Ni, Zn, and Cd thought the years, and no agreement in temporal trends with
the bulk deposition measurements.


3.4. RADIONUCLIDES IN TREE LEAVES

The mean activities and standard deviations for the radionuclide contents in
soils in Belgrade urban area are given in Table 3. The measured activities are
within the range reported for the region and elsewhere (Djuric et al., 1992; RA
Report, 2002; Todorovic et al., 2005) with no significant differences among the
sites.

Site Activity (Bq/kg) 226 Ra 232 Th 40 K 137 Cs 238 U 235 U 210 Pb VF 39 ± 5 33
± 5 402 ± 40 21 ± 2 15 ± 5 2.9 ± 0.3 / HI 33 ± 3 34 ± 4 395 ± 35 31 ± 3 27 ± 9
1.6 ± 0.3 / RB 26 ± 3 27 ± 4 378 ± 30 35 ± 2 16 ± 10 / / Mean ± SD 32 ± 4 32 ± 4
392 ± 35 29 ± 2 16 ± 8 1.7 ± 0.3 51 ± 10


TABLE 3.

Radionuclides in soils in Belgrade urban area. Lead-210 in soils was estimated
using two measuring episodes (4 samples).



Soil-to-leaves transfer factors (TF) were calculated as a ratio of an element’s
activity in leaves and its activity in soil (IAEA, 1994). The results for 40K,
210Pb and 137Cs are presented in Table 4. The high TFs for 40K show that its
predominant route of accumulation in Tilia spp. and A. hippocastanum leaves is
by root uptake, which could also be concluded for Pb, although, considering the
scarcity of the Pb data in soils (Table 3), this result should be taken with
caution.

The activities of radionuclides in leaves of Tilia spp. and A. hippocastanum (in
Bq/kg) and aerosols (in Bq/m3) in Belgrade parks, over the period 2002 – 2008
are presented in Table 5. The presented results include the mean, standard
deviation and the coefficient of variation (in %) (Todorović et al., 2009).

Species Transfer factor 40 K 210 Pb 137 Cs Tilia spp . 1.2 9 0.90 0. 09
A.hippocastanum 1.2 6 0.90 0.0 3 Tilia spp. & A.hippocastanum 1.2 7 0.90 0. 06


TABLE 4.

Transfer factors soil–to–leaves for Tilia spp. and A. hippocastanum in Belgrade.



The coefficient of variation, calculated as a ratio of standard deviation and
the mean, shows dispersion of the mean activity for a detected radionuclide. The
dispersion is the lowest for 40K, the radionuclide generally uptaken from soil
through roots. The seasonal variations, therefore, are not expected to be
pronounced. The seasonal variations for 210Pb are higher than for 7Be, which can
be explained by an additional input, resulting from coal burning and traffic, in
winters. The variations in the 137Cs activity, on the other hand, are very high.
They are mainly influenced by low measurable quantities of this radionuclide, a
very limited data set, and a large standard error. The concentrations of 137Cs
in Belgrade air before the Chernobyl nuclear plant accident were of an order
10-5 Bq/m3, increased to 0.39 Bq/m3 immediately after the accident, and
decreased to 9.5x10-5 Bq/m3 in 1988 (Popović et al., 2009a).

Activity variations in leaves of Tilia spp. and A. hippocastanum show a very
similar behaviour (Table 5). In turn, these variations resemble those in air,
thus confirming that 7Be and 137Cs are mainly deposited in leaves by foliar
deposition. Since the 210Pb variations are higher in plants than in air, Pb
accumulation is influenced by root uptake and by foliar deposition.

Species Activity in leaves (Bq/kg) and in aerosols (Bq/m 3 ) 40 K 210 Pb 137 Cs
7 Be Tilia spp. 504 ± 196 (39) 46 ± 29 (63) 2.6 ± 2.2 (85) 131 ± 56 (43) A.
hippocastanum 494 ± 184 (37) 46 ± 34 (74) 1.0 ± 0. 8 ( 8 0) 121 ± 60 (49) Tilia
spp. & A. h ippoca st. 499 ±191 (38) 46 ± 31 (67) 1.7 ± 1.6 (94) 126 ± 57 (45)
Aerosols / (5.6 ± 2.7) x 10 -4 (48) (2.5 ± 1.8) x 10 - 6 (94) (2.9 ± 1.2) x 10
-3 (41)


TABLE 5.

Activity of radionuclides in leaves of Tilia spp. and A. hippocastanum and
aerosols in Belgrade, 2002 – 2008 (the mean and standard deviation, and the
coefficient of variation (in %) in the parenthesis).



To estimate the concentrations of radionuclides in air due to resuspension, we
applied the following equation (SRS, 2006):

Cair/res(Bq/m3) = RF(m−1) x Csoil(Bq/m2)Cair/res(Bq/m3) = RF(m−1) x Csoil(Bq/m2)
E3

where Cair/res is concentration of radionuclides in air due to resuspension
(Bq/m3), RF is the resuspension factor (estimated to 10-7 for urban and
non-agricultural soils, and to 10-5 for agricultural soils), and Csoil is the
surface concentrations. It was calculated using (SRS, 2006):

Csoil(Bq/m2) = Csx ρsx dsCsoil(Bq/m2) = Csx ρsx ds
E4

where ds is the mean depth (15 cm), ρs is the density of soils (global average
1.6 g/cm3), and Cs is the average annual concentration in soils (in Bq/kg).
Thus, the calculated global average for ρsxds is 240 kg/m2. The results for the
calculated concentrations of radionuclides in air caused by resuspension,
together with the annual mean concentrations measured in air (Cair), are
presented in Table 6.

The correlation coefficients for the content of radionuclides in aerosols and
leaves of Tilia spp. and A. hippocastanum were calculated (Table 7). The lack of
linear correlation between 7Be in air and leaves could be explained mainly by
leaching (rainfalls) effects and short half-life of 7Be. There is a low
correlation for 210Pb, for both Tilia spp. and A. hippocastanum, but the uptake
of lead by plants is due to many factors and is more complex than for 7Be.

Concentration (Bq/m 3 ) 40 K 210 Pb 137 Cs C air/res 94.08x10 -4 12.24x10 -4
6.96x10 -4 C air (0.9-1.5)x10 -4 5.6x10 -4 2.5x10 -5


TABLE 6.

Concentrations of radionuclides in air caused by resuspension from soil in
Belgrade, 2002 – 2008. The activity of 40K in air was estimated from the
measurements with a new pump, with higher air flow capacity (average flow 30–50
m3/h and volume up to 40,000 m3).



Species Correlation coefficient 7 Be 210 Pb Tilia spp. -0.266 0.302
A.hippocastanum -0.241 0.347 Tilia spp. and A. hippocastanum -0.139 0.311


TABLE 7.

Correlations coefficients for the 7Be and 210Pb activities in leaves and in
aerosols.



3.4.1. SEASONAL VARIATIONS OF RADIONUCLIDES IN TREE LEAVES

The seasonal variations of the radionuclides’ activities in leaves of Tilia spp.
and A. hippocastanum in Belgrade urban area, from 2002 – 2008, are presented in
Figure 6. The concentrations of 40K and 137Cs are the highest over the
spring–summer periods, probably caused by a higher accumulation in young leaves.
For 137Cs, this conclusion should be taken with caution since there were only a
few measurable episodes in the data set (up to 2005), and very low
concentrations of this radionuclide were detected both in leaves and air.
Concentrations of 210Pb were the highest in autumn, and concentrations of 7Be in
summer, and both follow the pattern of seasonal variations of those
radionuclides in air (Popovic et al., 2008b; Todorovic et al., 1999, 2000, 2005,
2007; Todorović et al., 2005; Sugihara et al., 2008). Thus, for these two
radionuclides, leaves of higher plants could be used to monitor their
concentrations and seasonal variations in air in urban areas.

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4. CONCLUSION

Moss biomonitoring study in the urban area of Belgrade showed that most of the
analysed trace elements (Al, V, Cr, Mn, Fe, Ni, Cu, Zn, As, Cd, Pb) were
significantly accumulated in Sphagnum girgensohnii bags exposed in five
consecutive 3-month periods. The highest relative accumulation factors were
obtained for V, Cr, Cu, and Pb in both wet and dry moss bags. However, in
general, higher element contents were noticed in the wet moss bags. Significant
correlations were found between the element bulk deposition fluxes and elements
concentration in dry (Cu, V, Zn, Fe, Pb, As, Cr) and wet (V, As, Fe, Al, Ni, Cu)
moss bags. It may be concluded that active moss biomonitoring with S.
girgensohnii could be used for screening monitoring of atmospheric trace element
pollution in urban areas.



FIGURE 6.



Seasonal variations of radionuclides’ activities in leaves of Tilia spp. and A.
hippocastanum in Belgrade, 2002 – 2008 (the mean value for Tilia spp. is given
in black, for A. hippocastanum in white, and the mean for Tilia spp. and A.
hippocastanum in grey).



The mean activities of the detected radionuclides in S. girgensohnii were in the
range of the values reported for other local naturally growing moss species in
the region, with differences arising from the species, the method, local climate
and soil characteristics. For the long lived 40K there were no significant
differences in its content in naturally growing mosses in a rural region of
Southern Serbia and in the urban area of Belgrade. On the other hand, higher
concentrations of 210Pb in Belgrade indicate a contribution of anthropogenic air
pollution sources. Significantly higher activities of 137Cs, as well as the
detectable amount of 7Be, in mosses sampled in Southern Serbia are a consequence
of a longer, unknown exposure period, while in the Belgrade study, the exposure
period was limited to exactly one year. Hence, the observed differences mirror
the differences in the accumulation period. Since naturally growing mosses are
unlikely to be found in urban areas, the active moss monitoring proved to be a
suitable alternative technique for monitoring contents of radionuclides in urban
air. Furthermore, the exposure period in the moss bags technique could be
reduced to one month, thus nominating the technique as an efficient means to
monitor the level of radionuclides’ contents in air, as well as to follow their
seasonal variations.

Seasonal accumulation of the examined trace elements in leaves of Aesculus
hippocastanum L. and Tilia spp. (Tilia tomentosa L. and Tilia cordata Mill.) was
evident for V, Cr, Fe, Ni, As, and Pb, and it was more regular for A.
hippocastanum. Considering the temporal trends of the trace elements content in
leaves, some elements displayed a variation throughout the investigated years.
The most obvious was the Pb variation, showing a decreasing trend from 2002 to
2006, in accordance with the lead trend in bulk atmospheric deposition
measurements. Likewise, the temporal concentration trend for Cu in A.
hippocastanum was decreasing, similarly to the Cu trends seen in the bulk
atmospheric deposition at the site with the high atmospheric Cu loading. No
agreement was observed between the accumulation trend of V and As in leaves and
bulk deposition, although they exhibited decreasing temporal trends, as well as
Cr, Fe, Ni, and Zn. The results implied that those elements’ content in leaves
could not reflect atmospheric deposition directly. Therefore, due to its higher
accumulation capability, temporal trend consistency, and better agreement with
the bulk deposition measurements, A. hippocastanum may be suggested as a more
appropriate biomonitor of the trace elements atmospheric deposition than Tilia
spp. The lead leaf content clearly reflected the atmospheric Pb contamination,
and it may as well be assumed for Cu in highly polluted areas.

As for the examined radionuclides, the study showed that the predominant route
of 40K accumulation in Tilia spp. and A. hippocastanum leaves is by root uptake.
The accumulation pathways for lead seem more complex, although, according to
Hovmand et al. (2009), less than 2 % of Pb content comes from root uptake and 98
% is of atmospheric origin. The dispersions of the mean activities of the
radionuclides in leaves were the lowest for 40K, which is generally uptaken from
soil by roots. Its seasonal variations, therefore, were not expected to be
pronounced. The seasonal variations for 210Pb were higher than for 7Be. This
could be explained by an additional 210Pb input, e.g., coal burning and more
traffic, in winter. The 137Cs variations, on the other hand, were very high.
They were influenced by low measurable quantities of 137Cs, a limited data set,
and a large standard error. Variations of 7Be and 137Cs in air and in leaves of
Tilia spp. and A. hippocastanum showed similar behaviour, confirming that these
radionuclides are mainly deposited on leaves by foliar deposition. Since the
210Pb variations are higher in plants than in air, lead accumulation is
influenced both by root uptake and by foliar deposition. The comparison of the
radionuclides’ content in aerosols and leaves of Tilia spp. and A. hippocastanum
showed no linear correlation for 7Be, which could be explained mainly by
leaching effects and short half-life of 7Be. There was a low correlation for
210Pb, for both Tilia spp. and A. hippocastanum, but the uptake of lead by
plants is influenced by many factors and is more complex than for beryllium-7.

The seasonal variations of the radionuclides’ activities in leaves of Tilia spp.
and A. hippocastanum in Belgrade urban area, from 2002 – 2008, showed that the
concentrations of 40K and 137Cs were the highest over the spring–summer periods,
probably caused by a higher accumulation of young leaves. For 137Cs, this
conclusion should be taken with caution as there were only a few measurable
episodes in the data set (up to 2005), and the content of 137Cs was generally
very low in leaves and air. The concentrations of 210Pb were the highest in
autumn, those of 7Be in summer. Both 210Pb and 7Be in leaves follow the pattern
of their seasonal variations in air. Thus, leaves of Tilia spp. and A.
hippocastanum could be used to monitor concentrations and seasonal variations of
these radionuclides in air in urban areas.

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ACKNOWLEDGMENTS

This work was carried out within the framework of the project No. 141012 funded
by the Ministry of Science and Technological Development of the Republic of
Serbia.


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SECTIONS

Author information
 * 1.Introduction
 * 2.Experimental
 * 3.Results and Discussion
 * 4.Conclusion
 * Acknowledgments

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