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An analysis of naturally occurring radionuclides and 137Cs in the soils of urban

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An analysis of naturally occurring
radionuclides and 137Cs in the soils of
urban areas using gamma-ray spectrometry

I. Vukašinović, D. Todorović, Lj. Životić,

L. Kaluđerović & A. Đorđević

International Journal of
Environmental Science and
Technology

ISSN 1735-1472
Volume 15
Number 5

Int. J. Environ. Sci. Technol. (2018)

15:1049-1060
DOI 10.1007/s13762-017-1467-z

1 23
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 Author's personal copy
Int. J. Environ. Sci. Technol. (2018) 15:1049–1060
https://doi.org/10.1007/s13762-017-1467-z
ORIGINAL PAPER
An analysis of naturally occurring radionuclides and 137Cs
in the soils of urban areas using gamma-ray spectrometry
I. Vukašinović1 • D. Todorović2 • Lj. Životić1 • L. Kalud̄erović1 • A. Ðord̄ević1
Received: 20 September 2016 / Revised: 6 March 2017 / Accepted: 16 July 2017 / Published online: 25 July 2017
Ó Islamic Azad University (IAU) 2017
Abstract This study of environmental radioactivity was
carried out in the soils of an urban area. Naturally occur-
ring gamma-emitting radionuclides and man-made 137Cs
were found in the soil profiles collected from four parks in
the central Belgrade city area and the soil layer was
examined every 10 cm and to a depth of 50 cm.
Radioisotope activity concentrations (Bq kg-1) in the
samples of urban soil using the gamma-ray spectrometry
method were in the range of 14–46 for 238U, 33–50 for
226
Ra, 29–63 for 210Pb, 1.2–3.4 for 235U, 28–50 for 232Th,
424–576 for 40K and 0.7–35.8 for 137Cs. Some of the basic
physicochemical soil properties (pH, organic matter con-
tent, calcium-carbonate content, particle size distribution)
were determined to investigate the impact on the vertical
distribution of radionuclides. The results of this investi-
gation showed that variations of activity concentration
ratios of radionuclides that belong to the same (238U/226Ra)
or different radioactive series (232Th/226Ra; 235U/238U),
including 210Pb/137Cs ratios could well be explained by the
properties of the soil. Alkaline pH reaction, the accumu-
lation of organic matter in the uppermost and of carbonates
in the deepest layers of urban soil had an effect on
238
U/226Ra, and 210Pb/137Cs activity concentration ratio
values, while 232Th/226Ra and partially 235U/238U ratios
Editorial responsibility: Zhenyao Shen.
& I. Vukašinović
ivanavu@agrif.bg.ac.rs
1
Faculty of Agriculture, University of Belgrade, Nemanjina 6,
11080 Belgrade, Serbia
2
Department of Radiation and Environmental Protection,
‘‘Vinča’’ Institute of Nuclear Sciences, University of
Belgrade, Mike Petrovica Alasa 12-16, Belgrade 11001,
Serbia
were associated with the particle sizes vertical distribution.
A study of radionuclides in the samples of leaves of two
deciduous tree species common for these parks was also
conducted and 210Pb and 40K were found concentrated in
leaves rather than other investigated radionuclides.
Keywords Radioactivity  Activity ratio  Vertical
distribution
Introduction
The soils of urban areas develop from the impact of cli-
mate, living organisms and landscape on parent material
over time, whereas the anthropogenic impact often prevails
in further soil genesis and becomes dominant. Urban soil is
regularly contaminated by one or more trace elements in
comparison to their natural surroundings, which may rep-
resent the main concern due to its impact on human health
and the environment (Biasioli et al. 2006). The soil from an
urban area can be understood as a type of non-paved land
within the city limits that acts as a source and as a sink of
those pollutants (Charlesworth et al. 2011). About 85% of
the annual human exposures to ionizing radiation originate
from natural sources and the remaining 15% from man-
made sources, including the use of fuels or materials
containing naturally occurring radionuclides (UNSCEAR
2010). Natural terrestrial radioactivity arises mainly from
the nuclides of the three natural radioactive series 238U,
235
U and 232Th and from the primordial potassium isotope
40
K. The activity levels of these radionuclides in soil,
which are primarily related to the geological origin of the
site, are used for the gamma dose rates assessment of the
terrestrial origin (UNSCEAR 2010). Human activity in
residential areas in the form of industrial discharges,
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1050
vehicular emissions, combustion of fossil fuel, waste dis-
posal and use of phosphate fertilizers generate soil distur-
bances and initiate naturally occurring radioactivity
redistribution (IAEA 2011). Due to the proximity of soil to
humans, the most important exposure pathways that should
be considered are the direct exposure from contaminated
soil, inhalation of airborne radionuclides and incidental
ingestion of soil.
Natural radionuclides discharged into the atmosphere
from coal-fired power plants in a gaseous and particulate
form and subsequently deposited in soil may have an effect
on activity levels of nearby residential areas (Flues et al.
2002). Deposition of coal fly ash particles poses a partic-
ular environmental hazard due to enrichment of naturally
occurring radionuclides in fly-ash after coal combustion
(Charro et al. 2013). Soil mixing, including the addition or
removal of layers of soil, agricultural and construction
activities, contributes to a greater extent to the changes of
soil radioactivity compared to the atmospheric deposition.
The maintenance of soils from fourteen public parks in São
Paulo city with phosphate fertilizers are believed to be the
cause of the higher uranium concentrations recorded (Ca-
margo et al. 2009). An important anthropogenic contribu-
tion to the terrestrial gamma dose rate in urban areas is the
incorporation of construction materials into the soil due to
its own natural activity that may exceed background
activity levels (Todorović et al. 2015). On the other hand,
particles from soil surface layers do not remain undisturbed
and can become part of urban street dust reported to con-
tain relatively high activity levels of natural 40K and 210Pb
and, to a lesser extent, of fallout 137Cs (Charlesworth et al.
2011).
Migration and downward transport of potential con-
tamination due to anthropogenic activities may influence
the depth distribution of natural radionuclides in soil, their
further concentration in plants or possible transfer to the
groundwater. Studies of a coal-fired power plant’s impact
on soil radioactivity levels demonstrated natural radionu-
clides enhancement in the surface soil in regard to deeper
soil layers (Flues et al. 2002) or no enhancement due to
homogeneous depth distribution (Charro et al. 2013).
Natural radionuclides dispersion along the soil depth
occurs spontaneously as it is related to the characteristic
features of soil. It was observed that the activity concen-
trations of radionuclides 238U (Navas et al. 2011) and 40K
(Fujiyoshi and Sawamura 2004), which were leached down
and accumulated into the deeper sections of soil, were
associated with particle-size or organic matter distributions
and/or changes of soil pH values. The depth distribution of
man-made radionuclide 137Cs (t1/2 = 30.2 years) is often
simultaneously determined in soil as valuable information
to indicate the degree of soil modification in residential
areas. If the soil profile is undisturbed (or uncultivated), it
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Int. J. Environ. Sci. Technol. (2018) 15:1049–1060
is characterized by radiocesium inventories concentrated
mostly in the 0–20 cm soil depth and rapidly decrease
below that depth, while in disturbed (or cultivated) soil the
radiocesium profile is generally longer due to mechanical
soil mixing (Belivermis 2012; Soto and Navas 2008).
The main sources of pollution in the Belgrade urban
area, apart from industrial and coal fired plant emissions
and traffic, are heating with plants run on natural gas and
crude oil, while many individual houses are still heated
with coal. Previous studies of air, plant and soil compart-
ments of the Belgrade urban area have all shown lead
contamination (Tomašević et al. 2013; Todorovic et al.
2013). Changes of activities of the radioactive lead isotope
210
Pb in the ground level air of the same area was attributed
to sources such as coal combustion and heavy city traffic
via emission of fuel combustion products that contain
natural Pb and its isotopes. In the urban area where natu-
rally growing mosses and lichens are rare or absent, the
leaves of two deciduous tree species Aesculus hippocas-
tanum (horse chestnut) and Tilia spp. (linden) common in
the city of Belgrade, were alternatively used as accumu-
lative biomonitors of isotope 210Pb in the central city area
(Todorovic et al. 2013).
The objective of the present study is to investigate envi-
ronmental radioactivity levels of soil from the urban areas of
the city of Belgrade, Serbia. Naturally occurring 238U, 226Ra,
210
Pb, 235U, 232Th, 40K including the man-made 137Cs
activity concentrations in soil were determined using the
gamma spectrometry method and these values are used to
examine if background activity levels of the terrestrial origin
are modified. Urban soils environmental radioactivity
modifications might occur from multiple sources and con-
tribution from each source could not be exactly quantified
since all the various inputs are integrated in the soil over time
(Charlesworth et al. 2011). The vertical distribution of
radionuclides in soils was used to conduct the study of
potential radioactive pollution by analyzing the mutual
relationships between them and the basic physical and
chemical soil properties. Activity concentration ratios
between members of the same or different decay series were
used as indicators of the radionuclides’ vertical transport in
soil. Additionally, the leaves of two deciduous tree species
(Aesculus hippocastanum and Tilia spp.) were used to
investigate their potential to reflect activity concentration of
radionuclides recorded in the soil of the urban environment.
Samples of soil and leaves were collected during 2011.
Materials and methods
This study was conducted in Belgrade, the capital of Serbia
(44° 490 1400 N, 20° 270 4400 E; 117 m a.s.l; population
around 2 million). The climate in Belgrade is moderate
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Int. J. Environ. Sci. Technol. (2018) 15:1049–1060
continental with fairly cold winters and warm summers
with average temperatures of 2.4 and 22.2 °C, respectively.
The geology of the Belgrade city area is heterogenous. It
consists of alluvial plains around the Danube and Sava
rivers, a loess plateau on the west part of the city area and a
tertiary sediment basin on the south and east area of a city.
The study was conducted in the four city parks belonging
to the central zones of the city (Fig. 1). The Botanical
Garden (BG) and Student’s Park (SP) are located on
limestones, clays and sands, while Karadjordjev park (KP)
is located between limestones, clays, sandy clays and
sands. Zemunski park (ZP) is located at the far west of the
sandy part of the alluvial plain, covering about 100 m in
the direction of the west Loess plateau initiate.
In May 2011, soil samples were collected at depths of
0–10 cm, 10–20 cm, 20–30 cm, 30–40 cm and 40–50 cm
at BG, SP and ZP sites while at KP the sampling was
conducted at a depth of up to 30 cm due to significant
consolidation of material below. Composite soil samples
(n = 22) were obtained by mixing the three subsamples
collected at every depth of soil in the vicinity of the trees,
below the tree crowns. Adjacent to these sampling sites, an
additional four samples were collected at depths of
0–10 cm in the area of the park soil not sheltered by tree
crowns. The collected soil samples were air-dried and
Fig. 1 A section of the
geological map of the Belgrade
city area (1:100 000 scale)
including the investigated sites
(BG—Botanical Garden, SP—
Student’s Park, ZP—Zemunski
Park, KP—Karadjordjev Park)
1051
ground to pass through a 2-mm sieve to analyze the
physical and chemical characteristics. The particle-size
distribution was analyzed by the sieve and pipette method.
Soil reaction in water (1:2.5) and in 1 M KCl (1:2.5) sus-
pension was determined potentiometrically. Organic matter
content was determined by Tjurin method modified by
Simakov. Calcium-carbonate content was measured volu-
metrically according to the Scheibler calcimeter method.
The determined soil fractions are sand (particle sizes 0.2–2
and 0.05–0.2 mm), silt (0.01–0.05 and 0.002–0.01 mm)
and clay (\0.002 mm). At each park, soil samples richest
in clay size fraction (below the 0–10 cm) were used for
mineral composition analysis. Mineral composition was
determined by semi-quantitative powder X-ray diffraction
(XRD) method by diffractometer Philips (PW-1010) to
evaluate the interlamellar distance in the modified clays.
The X-ray diffraction patterns were recorded using Cu-Ka
´
radiation (k = 1,54184 Å) in the 2h range from 2° to 30°.
A step size width 0.02° (2h) was used with a time of 1 s per
step. Minerals have been characterized by recording ori-
ented samples that were air-dried, saturated with ethylene
glycol and heated to 550 °C.
Measurements of radionuclide activity concentration in
soil samples were conducted by the standard gamma spec-
trometry method using HPGe detectors (Canberra Industries,
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 Author's personal copy
1052
Inc., USA) with 20 and 18% relative efficiency and energy
resolution of 1.80 and 1.69 keV at the 1332 keV gamma ray
energy of 60Co, respectively. Prior to measurement, the soil
samples were packed in 500 ml Marinelli beakers and kept
sealed for one month to attain radioactive equilibrium
between 238U and 232Th and their progenies. The detector
was calibrated in the same 500 ml Marinelli beaker geom-
etry using standard reference material (silicone resin matrix
with homogeneously dispersed radionuclides 241Am, 109Cd,
139
Ce, 57Co, 60Co, 137Cs, 113Sn, 85Sr, 88Y, and 203Hg; total
activity 40.624 kBq at April 15, 2008; Czech Metrological
Institute Praha, 9031-OL-208/08).
Leaves were sampled from horse chestnut and linden in
spring and in autumn at the BG, SP and KP sites. Five
subsamples (10–15 fully developed leaves) were taken
randomly from tree crowns 2 m above the ground, and a
composite sample was made (Tomašević et al. 2013). The
leaves were dried at room temperature or at 105 °C and
then mineralized at 450 °C. To determine annual activity
concentration in the leaves, a joint sample was made by
mixing individual samples of leaves taken from the spring
and autumn collections. The samples were packed in
100 cm3 plastic cylinders and sealed with a film of bees-
wax. Geometric calibration for leaves was performed with
a secondary reference material obtained from the primary
reference material (mineralized grass with homogeneously
dispersed radionuclides 241Am, 109Cd, 139Ce, 57Co, 60Co,
88
Y, 113Sn, 85Sr, 137Cs, and 210Pb total activity 72.40 kBq
at 31.08.2012.; Czech Metrological Institute, Praha
9031-Ol-116/8, type ERX).
The activity of 238U was determined by its daughter product
234
Th at 63 keV. The activity of 226Ra was determined by its
decay products: 214Bi (609, 1120, and 1764 keV) and 214Pb
(295 and 352 keV) and of 232Th by its decay product 228Ac
(338 and 911 keV). 235U was determined through 185.7 keV
corrected for 226Ra (186 keV). The 210Pb activity was deter-
mined using its 46.5 keV gamma photons. The activities of 40K
and man-made 137Cs were obtained from their single gamma
ray lines of 1460 and 661.66 keV energy, respectively. The
spectra were recorded and analyzed using Canberra Genie
2000 software. Counting time was 60,000 s. The measure-
ment uncertainty of the method is expressed as an expanded
measurement uncertainty for the factor k = 2 that corresponds
to a normal distribution with a confidence level of 95%.
Statistical analysis of data was conducted by one-way
analysis of variance (ANOVA) to specify the main differ-
ences in radionuclides activity concentrations and measured
soil properties between investigated sites and with the depth.
Significant differences were considered at the 95% confi-
dence level. To find relationships between radionuclide
activity ratios and the soils’ physical and chemical proper-
ties, Pearson’s linear correlation analysis was performed.
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Int. J. Environ. Sci. Technol. (2018) 15:1049–1060
Results and discussion
Soil properties
It was observed that soil from the Botanical garden (BG) is
natural, so-called virgin soil, which has kept its original
profile differentiation and was not anthropogenically
modified. According to the national classification system, it
belongs to the Rendzina soil type with very shallow topsoil
(0–10 cm) and a mollic horizon of very dark grey brown
silty clay loam with less than a 10% sand fraction. The
topsoil, rich with soil organic matter (SOM) content
(*5%), presents a hummus-accumulative A-horizon and
underneath that there is a small transitional horizon
(10–20 cm) with about *2% of SOM and higher sand
content compared to the topsoil. The samples from lower
depths (20–50 cm) with very homogenous texture have
much lower SOM content and they clearly indicate that the
upper part is of unconsolidated parent material, rich in
CaCO3 which allows plants to root but which was not
changed in pedogenesis. The soil from Zemunski Park
(ZP), on the other hand, is formed of loamy alluvial sedi-
ments rich in calcium carbonate which has undergone
considerable alteration in the past, since the broader area of
the alluvial plain has been reclaimed and the drainage
systems have diminished the ground water level. Since the
soil texture is silt loam and loam, the parent material cor-
responds more to loess than to alluvial sands. The dis-
tinction between these two geological formations is
somewhere in the area of Zemunski Park. Student’s Park
(SP) and Karadjordjev Park (KP) are situated in very urban
zones of the Belgrade city center. Compared to BG and ZP,
the soil from SP is of similar texture, but with the SOM
content much higher ([3%) at the lowest depth (40–50 cm)
and with the topsoil layer rich in sand fraction (*33%)
irregularly distributed by depth. Unlike other parks, the soil
from KP had lower CaCO3 and sand content (\10%) and
different, silty clay loam texture. In this park, soil was not
dry or very dry during the sampling, but it was difficult to
reach its lower depths due to significant consolidation of
material below 30 cm. Based on these observations, the
natural characteristics of the soil of SP and KP changed at
some point, which is why it should be recognized as
anthropogenic soil.
The results of the determination of the physical and
chemical properties of soils in the Belgrade urban area are
presented in Table 1. The soil from parks is rich in calcium
carbonate which is in the range of 3.7–26.0% and with a
pH in the range 7.4–8.1. All examined soil profiles are
alkaline and calcareous with the lowest CaCO3 content in
the topsoil increasing with depth, indicating soil genesis in
the direction of calcium-carbonate leaching. At each site,
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Int. J. Environ. Sci. Technol. (2018) 15:1049–1060 1053

Table 1 Soil chemical and physical characteristics at the four investigated parks
Location Depth pH pH SOM CaCO3 Sand (2–0.05 mm) Silt (0.05–0.002 mm) Clay (\0.002 mm)
(cm) H2O KCl (%) (%) (%) (%) (%)

BG 0–101 7.78 7.46 4.96 9.8 19.0 53.4 27.6

0–10 7.43 7.12 5.13 16.6 7.2 66.2 26.6
10–20 7.90 7.35 2.10 20.2 18.8 54.1 27.2
20–30 8.05 7.52 1.33 22.2 17.8 57.6 24.6
30–40 7.96 7.50 1.53 21.0 18.4 60.3 21.3
40–50 7.93 7.60 1.40 21.8 24.8 53.5 21.7
Mean 7.84 7.42 2.74 18.6 17.7 57.5 24.8
SD 0.2 0.2 1.8 4.8 5.7 5.1 2.8
CV 3 2 66 26 32 9 11
ZP 0–101 7.61 7.29 5.44 12.4 24.8 52.8 22.4
0–10 7.72 7.07 4.90 14.0 19.9 59.4 20.7
10–20 7.90 7.17 3.29 14.3 29.4 47.8 22.8
20–30 7.92 7.31 2.92 16.1 25.1 49.8 25.0
30–40 8.02 7.42 2.43 15.1 24.1 51.7 24.1
40–50 8.02 7.50 1.68 20.8 29.3 49.1 21.6
Mean 7.86 7.29 3.44 15.4 25.4 51.8 22.8
SD 0.2 0.2 1.5 2.9 3.6 4.2 1.6
CV 2 2 42 19 14 8 7
SP 0–101 7.44 7.20 4.21 11.9 16.0 53.8 30.2
0–10 7.75 6.94 4.38 18.3 33.0 46.1 20.8
10–20 7.81 7.09 4.16 22.8 23.4 52.3 24.3
20–30 7.90 7.22 3.39 23.9 26.2 49.2 24.6
30–40 7.91 7.31 3.37 26.0 25.3 50.7 24.0
40–50 7.93 7.39 3.23 24.4 24.2 55.4 20.4
Mean 7.79 7.20 3.95 21.2 24.7 52.5 24.1
SD 0.2 0.2 0.5 5.3 5.5 2.3 3.5
CV 2 2 11 25 22 4 15
KP 0–101 7.86 7.21 2.60 3.7 9.3 62.2 28.6
0–10 7.73 7.15 2.61 3.8 8.6 59.0 32.4
10–20 7.86 7.31 2.69 8.8 7.2 60.5 32.3
20–30 7.94 7.31 2.77 8.2 6.6 60.2 33.2
Mean 7.85 7.25 2.67 6.1 7.9 60.5 31.6
SD 0.1 0.1 0.1 2.8 1.2 1.3 2.1
CV 1 1 3 45 16 2 7
Summary
Minimum 7.4 6.9 1.3 3.7 6.6 47.8 20.4
Maximum 8.1 7.6 5.4 26.0 33 66.2 33.2
Mean 7.8 7.3 3.2 16.2 19.9 55.1 25.3
SD 0.2 0.2 1.3 6.6 7.9 4.9 4.0
CV 2 2 39 41 40 9 16
1
Soil samples collected from soil not covered by the tree crowns of 0-10 cm depth

soil alkalinity increases along the profiles depth and,
indicated by a one-way Anova test, the means of pH
(p \ 0.001) are significantly different at a depth of
0-10 cm, compared to any deeper soil layer. It has been
recognized already that urban soils have a tendency for
modified, alkaline reactions, with elevated pH levels
relative to their natural surroundings (Biasioli et al. 2006).
The SOM content of 4–5% is highest at the topsoil and
gradually decreases with depth at BG and ZP. The preva-
lence of SOM in the topmost layer of soil is connected to
its addition by annual litterfall. Some investigations of
temporal changes of urban SOM showed that younger

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1054
urban soils are dominated by free litter compounds while
the older have more SOM incorporated into the humic
matrix (Scharenbroch et al. 2005). At KP and SP, the
content of SOM did not vary considerably with a depth (of
only 3 and 11%, respectively) indicating soil profiles are
comprised of the same pedogenic horizons. Statistically,
between the soil layers along the 0–50 cm depth with a step
of 10 cm, the means of SOM were distinguishable
(p \ 0.05) between the upper layer of 0–10 cm depth and
any deeper layer. Soil samples from all sites have a silt
content higher than 45% with soil texture that varies from
loam to silty clay loam. The means of silt (p \ 0.01) and
sand (p \ 0.001) were different from one park to another,
but silt fractions had a small coefficient of variation of 9%
in contrast to sand which varied 40%, and was similarly
distributed as the carbonates. A slightly higher clay content
(p \ 0.001) is found only at KP (*32%) compared to
other sites (*22%).
The results of the soil mineral composition analysis
from the four parks showed very similar XRD patterns of
clay size mechanical fractions. The samples from the SP,
ZP and KP sites indicated a mineral composition with the
presence of illite as the dominant mineral with smaller
amounts of smectite, kaolinite and chlorite minerals. In
contrast, at the BG site, illite was present in much smaller
amounts in comparison to the smectite and kaolinite con-
tents. All the examined soils could be grouped together
according to their similar mineralogical composition and
higher pH as the main soil characteristic that reflects the
underlying geology of the sites of carbonaceous origin.
Activity concentrations
Radioisotope activity concentrations (Bq kg-1) in the soil
samples collected from the four parks are in the range of
14–46 for 238U, 33–50 for 226Ra, 29–63 for 210Pb, 1.2–3.4
for 235U, 28–50 for 232Th and 424–576 for 40K while each
data set indicated normal frequency distribution. The 210Pb
was less than the MDC (minimum detectable activity
concentration) value in one soil sample of 0–10 cm depth.
The results reported in this study were all comparable with
natural background gamma radiation activity concentration
(Bq kg-1) ranges for soils accepted in the UNSCEAR
(2010) report: 16–110 for 238U, 17–60 for 226Ra, 11–64 for
232
Th, 140–850 for 40K. In the investigated soil, the lower
activity concentration variation was found for 40K (8%)
and 226Ra (11%), slightly higher for 232Th (16%) and 210Pb
(19%), while uranium isotopes 238U and 235U varied 26%.
As indicated by the one-way Anova test results, the highest
activity concentration for 226Ra was at SP (p \ 0.01) and
for 232Th at BG (p \ 0.001) while 40K was statistically
different at all parks mutually (p \ 0.01). At the KP site
238
U (p \ 0.05) and 235U (p \ 0.01) activity concentration
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Int. J. Environ. Sci. Technol. (2018) 15:1049–1060
means differed from the rest of the parks and there 238U
had its minimum (25 Bq kg-1) while 235U had its maxi-
mum (2.6 Bq kg-1) mean value. The vertical distribution
of activity concentration of natural radionuclides 238U,
226
Ra, 232Th, 210Pb, 40K and fallout 137Cs are presented in
Fig. 2. It should be noted, that at each park activity con-
centration vertical variations of naturally occurring
radionuclides were comparable with measurement uncer-
tainty of their activity concentrations. Based on the low
variation in the soil, naturally occurring radionuclides are
uniformly distributed along the soil depth which is to be
expected if their activity concentrations reflect the under-
lying geology of the sites (Milenković et al. 2015; Beliv-
ermis et al. 2012).
137
Cs derived from nuclear fission products from the
Chernobyl accident and the radioactive fallout from the
previous atmospheric nuclear weapon tests is in homoge-
neously distributed in the soils of Serbia (Milenković et al.
2015). The observed range of radiocesium activity con-
centration (Bq kg-1) was 0.7–35.8 except for one value
that was less than MDC. Similar activity concentration
ranges and profiles are found in the studies of 137Cs vertical
distribution in soil (Krstić et al. 2004; Fujiyoshy et al.
2011). In the parks’ soil anthropogenically introduced
cesium had higher mean activity concentration (p \ 0.01)
in the upper 0–20 cm part of the soil of 17 Bq kg-1
compared to the lower 20–50 cm depth of 7 Bq kg-1. It is
known that in undisturbed soils physico-chemical pro-
cesses and bioturbation are responsible for fallout 137Cs
migration in the soil profile, while in disturbed soils its
redistribution is primarily associated with mechanical
mixing (Soto and Navas 2008; Ayub et al. 2007). The
specific and different radiocesium depth distributions found
in the city parks were used to distinguish undisturbed from
disturbed soil profiles. The soil profile from the BG site is
one in which 137Cs, detected in soil near the trees, is
rapidly decreasing, disappears at a 20–30 cm depth (137-
Cs \ 0.14 Bq kg-1) and again appears in the next layer
(30–40 cm) of soil. The Botanical Garden’s ‘‘virgin’’ soil,
densely covered with treetops was identified as undisturbed
and may be compared to undisturbed temperate forest soil
where similar radiocesium profiles were registered and
explained by the action of percolating water and biological
activity (bioturbation, root distribution) (Fujiyoshi and
Sawamura 2004). The soil of the ZP site could also be
identified as undisturbed according to the typical radio-
caesium behavior which vertical migration is well descri-
bed by the diffusion–convection model (Krstić et al. 2004).
At the two other parks, 137Cs is transported deeper in the
soil (below 20 cm) with a weak peak at a depth of
30–40 cm at SP and with an almost uniform distribution
with depth at KP (Fig. 2). It cannot be assumed that those
distributions under the topsoil are due to 137Cs higher
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Int. J. Environ. Sci. Technol. (2018) 15:1049–1060
Fig. 2 The activity concentration variation of 238U, 226Ra, 210Pb, 232Th, 40K and 137Cs radionuclides along a 0–50 cm soil depth in the parks:
Botanical Garden (BG), Studentski Park (SP), Zemunski Park (ZP) and Karadjordjev Park (KP)
convective migration with depth since convective transport
is found to be enhanced in sandy soils (Ayub et al. 2007).
At SP and KP, 137Cs is more likely mechanically trans-
ferred below the surface during the perturbation of soil as a
result of previous mechanical mixing. These more uniform
radiocesium profiles are used to confirm earlier assumption
of soil disturbances at the SP and KP sites.
Activity concentration ratios
If natural radionuclides have a common source in soil
(parent material), they are expected to be mutually highly
correlated (Navas et al. 2011). Pearson’s linear correlation
analysis showed significant (p \ 0.05) but weak correla-
tions of natural radionuclides among each other while only
238
U correlated according to depth (p \ 0.05). Since the
investigated urban soils were similar according to their
properties and mineralogical composition, the lack of
higher correlations could be owed to the differential
mobility of natural radionuclides within the same or
between two different decay chains. In temperate climates,
in the absence of processes responsible for natural
radionuclides mobility in soils such as leaching, dissolution
1055
and precipitation the members of the decay chains will be
in approximate secular equilibrium with the parent
radionuclide (IAEA 2014). On the contrary, in the presence
of these processes the removal of some radionuclides from
the point of origin may occur as well as the introduction of
disequilibrium within or between the decay chains.
If parents of the 238U and 232Th decay series are in
secular equilibrium with their progenies in soil due to their
very long half-lives, the activity concentration ratios within
the same series such as 238U/226Ra and 210Pb/226Ra would
be equal to 1. The ratio of activity between members of the
238
U and 232Th decay chain like 232Th/226Ra is typically
equivalent to 1.1 in most environmental samples (Navas
et al. 2011 and references therein). 235U/238U activity
concentration ratio approximately equal to 0.046 is often
evaluated to show uranium’s natural origin in the envi-
ronment (IAEA 2014). Therefore, the natural radionuclides
activity concentration ratios are calculated and used as
indicator of the radioactive disequilibrium that may occur
if one or more decay products in a decay series are
removed or added to the system. The vertical distribution
of activity ratios along 0–50 cm soil depth are presented in
Table 2.
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1056 Int. J. Environ. Sci. Technol. (2018) 15:1049–1060

Table 2 Activity concentration Location Depth (cm) 238

U/226Ra 232
Th/226Ra 235
U/238U 210
Pb/226Ra 210
Pb/137Cs
ratio values of 238U/226Ra,
232
Th/226Ra, 235U/238U, BG 0–101 0.93 1.07 0.054 0.98 2.4
210
Pb/226Ra and 210Pb/137Cs for
0–10 0.83 1.25 0.063 1.17 6.0
investigated soil samples
according to 0-50 cm depth 10–20 1.03 1.21 0.055 1.18 27.1
20–30 1.07 1.22 0.052 0.83 –
30–40 1.24 1.24 0.043 0.97 45.0
40–50 0.90 1.18 0.051 0.74 41.4
Mean 1.00 1.19 0.053 0.98 24.4
SD 0.15 0.07 0.006 0.18 19.6
CV 15 5 12 18 81
ZP 0–101 0.65 0.97 0.067 0.92 1.1
0–10 0.45 0.85 0.080 1.36 1.2
10–20 1.03 0.92 0.048 1.08 1.2
20–30 0.92 0.90 0.044 1.21 3.9
30–40 1.17 1.06 0.049 0.94 10.0
40–50 0.92 0.89 0.034 0.92 26.9
Mean 0.86 0.93 0.054 1.07 7.4
SD 0.26 0.07 0.020 0.18 10.2
CV 30 8 31 17 138
SP 0–101 0.82 0.94 0.063 0.82 2.4
0–10 0.95 0.77 0.051 0.88 2.0
10–20 0.79 0.84 0.057 1.03 3.0
20–30 0.71 0.76 0.052 1.32 4.9
30–40 0.84 0.70 0.031 1.26 4.5
40–50 0.98 0.82 0.037 1.18 13.3
Mean 0.85 0.80 0.049 1.08 5.0
SD 0.10 0.08 0.012 0.20 4.2
CV 12 10 25 19 84
KP 0–101 0.76 1.00 0.074 – –
0–10 0.42 1.24 0.1792 1.15 5.4
10–20 0.56 0.91 0.088 0.95 3.4
20–30 0.74 1.05 0.1172 1.13 3.4
Mean 0.62 1.10 0.114 1.10 4.1
SD 0.16 0.10 0.050 0.05 1.2
CV 26 14 41 10 29
Summary
Minimum 0.42 0.70 0.031 0.74 1.1
Maximum 1.24 1.25 0.088 1.36 45.0
Mean 0.85 0.99 0.055 1.05 10.4
SD 0.20 0.19 0.015 0.17 13.5
CV 25 19 27 16 129
Frequency distribution Normal Normal Normal Normal Log-Normal
1
Soil not covered by the tree crowns of 0-10 cm depth
2
Values excluded from summary analysis

In the park soils, the values of 238U/226Ra activity con-
centration ratios were in the range 0.42–1.24. Activity ratio
means were found to be significantly different (p \ 0.05)
between the soil layers at depths of 0–20 cm (0.77) and
20–50 cm (0.95). The changes of 238U/226Ra activity ratio
previously reported in surface soils in Serbia (0.71–1.60)
are attributed to the soil weathering and the influence of
water on the soil (Anagnostakis et al. 2001). In most soil
samples in the parks, 238U/226Ra ratios were \1 (Table 2)
indicating disturbance from radioactive equilibrium in the

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238
U chain. The two lowest values (0.42 and 0.45), estab-
lished as most extreme, were accompanied with high
measurement uncertainty of 238U activity concentration.
After their exclusion, 238U/226Ra activity ratios showed
significant correlations with the soil properties resulted
from Pearson’s correlation analysis (Table 3). It appeared
that activity ratio changes could be explained (p \ 0.05) by
soil pH, carbonate and SOM contents and by 238U activity
concentration variations (p \ 0.001). A well-known cause
of 238U/226Ra radioactive disequilibrium in soil is larger
uranium mobility compared to the relative immobility of
radium. Small changes of properties such as pH and
organic matter content together with leaching of carbonates
across the soil would favor the leaching of uranyl com-
plexes (Koch-Steindl and Pröhl 2001). In the alkaline soils,
in particular, this is accompanied with uranium accumu-
lation into the deeper soil layers that contribute to
238
U/226Ra disequilibrium along the soil profile (Navas
et al. 2011). The high and positive correlation of
238
U/226Ra ratio with 238U implies that activity ratio
changes are connected with variations of labile 238U
activity concentration in the soil as the latter increases with
total 238U activity concentration (Blanco Rodrı́guez et al.
2008). Besides, the smallest 238U/226Ra disequilibrium
values, which suggest 226Ra enrichment over 238U, are
found in the topsoil where SOM content is most abundant.
This is in accordance with strong radium retention by the
organic material in soils (Vandenhove et al. 2009) that is
expressed here by the negative correlation between
238
U/226Ra ratio and SOM content.
The uranium and thorium series are commonly associ-
ated in initial parent rock, and thus in the soil derived from
it (IAEA 2014). The 232Th/226Ra ratio is often found to be
strictly higher than 1.1 in soils of different geological
origin (e.g. Navas et al. 2011; Belivermis 2012) which is
explained by naturally higher thorium activity concentra-
tion over radium due to specific mineral composition of the
parent bedrock of the study area. In this study, the ratios of
232
Th/226Ra activity values were in the range of 0.70-1.25
and most were lower than 1.1. 232Th as well as 226Ra are
preferentially found in the most resistant phases of soil
(sand and silt particles), but concurrently 226Ra is found
also in the most labile fractions of soil (Blanco Rodrı́guez
et al. 2008). Accordingly, disturbances from 232Th/226Ra
natural equilibrium depended on soil texture (Table 3), i.e.
fractions of silt (p \ 0.05, positively) and sand (p \ 0.05,
negatively) which may reflect two nuclides fractionation
between different soil fractions during the weathering
process. Additionally, a strong and positive correlation of
232
Th/226Ra ratio is found with an activity concentration of
232
Th (p \ 0.001) and weaker and a negative one with
226
Ra (p \ 0.05). Most likely, 232Th remained part of the
resistant soil’s phases while 226Ra become partially cycled
by the trees which diminished its influence on activity ratio
changes in soil. High soil sorption is reported for 232Th in
our pH range (7.4–8.1) while 226Ra sorption showed to be

Table 3 Results of Pearson’s 238

U/226Ra 232
Th/226Ra 235
U/238U Ln (210Pb/137Cs)
correlation analysis between
activity concentration ratios and 238
U/226Ra 1 0.50a -0.68c 0.50a
soil properties 232 226
Th/ Ra 1 0.46a
235 238
U/ U 1
210 137
Ln ( Pb/ Cs) 1
238
U 0.92c -0.72c
235
U 0.47a
226
Ra -0.48a
210
Pb -0.56b -0.48a
232
Th 0.54a 0.81c
40
K
137
Cs -0.60b -0.43a 0.54a -0.89c
a c
CaCO3 0.49 -0.71 0.46a
a a
pH 0.45 -0.48 0.63b
Sand -0.52a -0.66b
a
Silt 0.52 0.51a
Clay 0.53a
a
SOM -0.48 -0.75a
a c
Depth 0.49 -0.70 0.72c
Significance level: ap \ 0.05; bp \ 0.01; cp \ 0.001; not significant correlations at the 95% level of
confidence are not presented

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1058
less responsive to soil pH and radium is found mostly
present in an available form in the soil (IAEA 2014;
Vandenhove et al. 2009). The disproportionality within the
232
Th and 238U decay chains might be described better by
232
Th distributions, probably due to thorium’s greater
spread of activity concentration values (16%) in compar-
ison to that of radium (11%).
The 210Pb (t1/2 = 22.3 yr.) radionuclide from the 238U
decay series is produced in the soil pores and partially
released into the atmosphere as a product of radon gas
222
Rn, a daughter product of the 226Ra nuclide decay. The
total concentration of 210Pb in soil consists of the in situ
produced, supported fraction which is in equilibrium with
its parent 226Ra and the unsupported fraction that is con-
tinuously retained from the atmosphere by wet or dry
deposition. Subsequently, 210Pb/226Ra activity ratio values
are expected to be higher than 1 in the uppermost soil layer
and to decrease with depth due to radioactive decay during
penetration into the deeper layers of soil (Charro et al.
2013; Flues et al. 2002). The range of 0.70–1.36 of
210
Pb/226Ra activity ratio is consistent with the range
0.74–2.0 previously reported (Anagnostakis et al. 2001),
but the disequilibrium or equilibrium between the isotopes
without a clear trend according to depth is found.
It is well known that after deposition from atmosphere
fallout radionuclides 210Pb and 137Cs have affinities with
similar particles of soil. 137Cs and 210Pb binding to soil
organic matter particularly have a significant effect on their
distribution by depth (Belivermis 2012; Fujiyoshi et al.
2011). It was already observed that SOM of 4–5% content
was accumulated in the top 0–10 cm soil depth (except at
KP). At each investigated park the maximum concentration
of 210Pb was not found in the uppermost soil layer, but
downward, below the first 0–10 cm depth and two vertical
137
Cs profiles were extended deeper in the soil, below a
depth of 20 cm (Fig. 2). Activity concentration ratio values
210
Pb/137Cs were evaluated to, at least roughly, analyze
210
Pb and 137Cs redistribution in the soil. The values
obtained were of the same order of magnitude and in the
range of 1.1–6.0 in the 0–40 cm soil depth. One order of
magnitude higher ratio values is found at the 40–50 cm soil
depth and immediately below the 10 cm at the BG site, in
the range of 13.3–45.0. 210Pb/137Cs data set was log-nor-
mally distributed which is why a correlation analysis was
conducted after taking logarithms of the data. An appar-
ently strong and negative correlation was found between
Ln (210Pb/137Cs) and radiocesium inventories in the soil
(p \ 0.001) and SOM content (p \ 0.01), due to their
gradual decrease with depth. Dörr and Münnich (1989)
have suggested that 137Cs and 210Pb are vertically trans-
ported together associated to soil organic matter, only
210
Pb to its insoluble fraction, which downward migration
was enhanced in neutral to weakly alkaline forest soils. In
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Int. J. Environ. Sci. Technol. (2018) 15:1049–1060
weakly alkaline park’s soil, moderate and positive corre-
lation (p \ 0.05) was obtained between Ln (210Pb/137Cs)
values and pH values and CaCO3 content. The tendency of
210
Pb to accumulate deeper in soil is most likely related to
its strong sorption by soil which increases under alkaline
conditions (pH [ 7) and furthermore with a significant
amount of CaCO3 content ([10%) (Sipos et al. 2005). A
similar 210Pb profile with the maximum value at a deeper
portion of soil characterized as carbonaceous, with higher
pH (6–7) was found in the vicinity of the city of Ljubljana
(Fujijoshy et al. 2011). Mutual correlation between
238
U/226Ra ratio values and of the logarithms of
210
Pb/137Cs and their increasing trend with depth related to
the same soil properties, indicated a greater influence of
physicochemical processes in the soil on the radionuclides
vertical distribution than the impact of human activities.
The activity ratio of 235U/238U was in the range of
0.031–0.179 in these parks. The two highest values (0.179
and 0.117) due to high measurement uncertainty of 238U
activity concentration, were excluded from further analysis
after which 235U/238U data showed normal frequency dis-
tribution in the range 0.031–0.088. 235U/238U ratio values
decreased and depended on depth negatively (p \ 0.001),
demonstrating again 238U migration and accumulation into
the deeper layers of soil. 235U/238U ratio changes are
attributed to variations of all investigated soil features,
except SOM content (Table 3). Studies investigating nat-
ural variability in 238U/235U isotopic ratio has revealed that
mechanisms controlling 238U and 235U isotopes fractiona-
tion in the environment are associated with oxidation–re-
duction reactions during transformations of U6? (soluble)
to U4? (insoluble), two uranium primary oxidation states
with different solubilities in the soil (Stirling et al. 2015).
The strong correlation of 235U/238U ratio values with
CaCO3 contents (p \ 0.001) could be explained by the
particularly high solubility of uranium U6? in the presence
of carbonates due to the formation of uranium-carbonate-
complexes, the main form of uranium transport in alkaline
soils (Koch-Steindl and Pröhl 2001).
Activity concentration in the samples of leaves
An additional examination is conducted when activity
concentrations of radionuclides in the soil, which were at
background activity levels, could be detected in leaves of
two deciduous tree species Aesculus hippocastanum (horse
chestnut) and Tilia spp. (linden) commonly found in the
parks. Measurements showed only a few results (Table 4):
that leaves concentrate 210Pb and 40K rather than other
radionuclides found in the soil; that chestnut leaves con-
centrate 226Ra (with one order of magnitude lower activi-
ties than in soil) and that all investigated radionuclides are
detected in only one sample of horse chestnut leaves.
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Int. J. Environ. Sci. Technol. (2018) 15:1049–1060 1059

Table 4 Activity concentration (Bq kg-1 dry weight) of naturally occurring radionuclides and 137
Cs in the samples of tree leaves
40 210 226 238 235 232 137 210
Activity ratio K Pb Ra U U Th Cs Pb/40K
Bq kg-1 (dry weight)

Horse chestnut SP 530 ± 32 37 ± 7 4.0 ± 0.4 7.4 ± 2.0 0.42 ± 0.03 1.7 ± 0.6 0.42 ± 0.11 0.070
KP 216 ± 15 28 ± 6 1.5 ± 0.2 \3.2 \0.18 \0.27 \0.09 0.130
BG 463 ± 32 37 ± 7 3.9 ± 0.5 \4.2 \0.25 \0.74 \0.32 0.080
Linden SP 433 ± 28 25 ± 6 \1 \0.3 \0.2 \0.3 \0.08 0.058
KP 376 ± 25 20 ± 5 \0.9 \3 \0.2 \0.35 0.26 ± 0.09 0.053
BG 427 ± 32 22 ± 6 \0.7 \3.5 \0.2 \0.5 \0.25 0.052

According to Manigandan and Shekar (2015), reduced
availability of radionuclides for uptake from soil to leaves
of woody plants is affected by the sorption properties of the
soil. Soil sorption is pH dependent and if the soil is alkaline
and the pH increases, as in the park’s soil, the transport and
availability of radionuclides in soil decreases (Vandehove
et al. 2009). 40K activity concentration in leaves in this
study was found to increase with a decrease of clay per-
centages in soil (p \ 0.05) and with an increase of soil pH
and CaCO3 content (p \ 0.05). Activity concentration
values of 210Pb and 40K in the leaves were of the same
order of magnitude as in the soil and 210Pb/40K ratio range
in the leaves (0.052–0.130) could not be statistically dis-
tinguished with that in soil (0.058–0.127) which indicated
their common source of origin in the environment. As an
essential element for plant growth, potassium was taken up
from the soil along with its radioactive isotope 40K and was
accumulated in the leaves through the main pathway of
uptake, the root system of the trees, while the lead isotope
210
Pb was incorporated in the leaves by both, foliar depo-
sition and root uptake. It was also noted that values of
210
Pb/40K ratio for the linden were in the different and
narrower range (0.052–0.058) than for the chestnut leaves
(0.070–0.130), suggesting 210Pb and 40K accumulation in
leaves differs due to their morphological characteristics
(Tomašević et al. 2013).
Finally, soils from the four city parks investigated were
grouped together according to their similar physicochemi-
cal properties and mineralogical composition. In the soil
samples, the values of 238U/226Ra, 232Th/226Ra, 235U/238U
and 210Pb/137Cs activity concentration ratio were found to
be in the range 0.42–1.24, 0.77–1.05, 0.031–0.179 and
0.8–45.0, respectively. The analysis of variations of those
ratio values according to depth were shown to be related to
distributions of the main properties determined to charac-
terize the soil. Activity concentration ratio values of
238
U/226Ra and of logarithms of 210Pb/137Cs were mutually
correlated and their increasing trend with depth were
connected with the same characteristics of urban soil, such
as the weakly alkaline pH reaction and the content of
organic matter and calcium-carbonates, which were accu-
mulated in the uppermost and deepest soil layers, respec-
tively. As uranium and thorium series are commonly
associated in the initial parent rock, and thus in the soil
derived from it, the preservation or departure from
232
Th/226Ra natural equilibrium depended here on soil
texture that probably reflected the two nuclides fractiona-
tion during the weathering process. The decreasing trend
by depth of two uranium isotopes ratio 235U/238U demon-
strated higher 238U downward migration known to be
enhanced in the presence of calcium-carbonates in the
alkaline soils.

Acknowledgements This paper was realized as a part of the project

Conclusion
A study of the vertical distribution of natural radionuclides
238
U, 226Ra, 210Pb, 232Th, 235U, 40K and man-made 137Cs in
the soils of the urban city area was conducted. According
to the measured activity concentrations of natural
radionuclides and their vertical distributions, human
activities conducted in the study area have not modified the
natural background activity levels. According to pedolog-
ical analyses, the soil from two parks was recognized as
natural (BG and ZP) and from the other two (SP and KP) as
anthropogenic soil, which was confirmed by a vertical
distribution analysis of 137Cs activity concentrations.
‘‘Studying climate change and its influence on the environment:
impacts, adaptation and mitigation’’ (43007) financed by the Ministry
of Education and Science of the Republic of Serbia within the
framework of integrated and interdisciplinary research for the period
2011–2014.
Compliance with ethical standards
Conflict of interest The authors declare that they have no conflict of
interest.
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