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Natural radioactivity around former uranium mine, Gabrovnica in Eastern

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Article  in  Journal of Radioanalytical and Nuclear Chemistry · October 2014

DOI: 10.1007/s10967-014-3203-1

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J Radioanal Nucl Chem
DOI 10.1007/s10967-014-3203-1
Natural radioactivity around former uranium mine, Gabrovnica
in Eastern Serbia
Jovana Nikolov • Sofija Forkapić • Jan Hansman •
Ištvan Bikit • Miroslav Vesković • Nataša Todorović
Dušan Mrd̄a • Kristina Bikit
Received: 10 March 2014
Ó Akadémiai Kiadó, Budapest, Hungary 2014
Abstract Gabrovnica near Kalna village was the first
uranium mine established in Yugoslavia. In 1963, the
Nuclear Energy Commission began operating the mine and
mill. Between 1964 and 1966, the staff at Kalna extracted
and produced an estimated 900 kg of UO2 and 400 kg of
uranium metal. The Kalna ore was of poor quality, con-
taining very low uranium content, which required higher-
cost mining and refining methods. That was the main
reason for closing this mine. This paper presents results
obtained by measuring the activity concentration of soil
samples measured by gamma spectrometry and also indoor
222
Rn activity concentrations in houses in the nearby vil-
lage Kalna. There is a presence of elevated radioactivity
levels in the most of the measured samples. The mine was
never officially decommissioned. The results obtained
might be useful for the future decommissioning procedure.
Keywords Uranium mine  Elevated radioactivity 
Hazard index
Introduction
Uranium mining and milling activities usually generate an
enhancement of radionuclide concentrations in the envi-
ronment that may cause increased radiological exposure to
mankind [1]. Uranium is an element that is naturally
radioactive, which makes it an energy-significant material,
and the subject of geological exploration and investigation
J. Nikolov (&)  S. Forkapić  J. Hansman  I. Bikit 
M. Vesković  N. Todorović  D. Mrd̄a  K. Bikit
Department of Physics, Faculty of Sciences, University of Novi
Sad, Novi Sad, Serbia
e-mail: jovana.nikolov@df.uns.ac.rs
•
into its geochemical behavior. The use of uranium as fuel
for energy production was very common in previous years.
Current Nuclear Power plants require the use of the rare
uranium isotope 235U and consequently only use one fifti-
eth of the total energy content. It is assumed that 235U can
produce 3.7 million times as much energy as the same
amount of coal. There are a lot of different opinions about
justification of the use of uranium as fuel for energy pro-
duction. Uranium mining legacy sites are of current con-
cern in many European countries and elsewhere due to the
eventual occurrence of waste materials with high radio-
nuclide concentrations and their potential environmental
health impact [2]. Geological prospecting in the Stara
Planina in Eastern Serbia has revealed several locations of
uranium minerals identified as being the fissure-filling type
of deposit [3].
The territory of Eastern Serbia is well-known by a
number of natural occurrences and deposits of nuclear
mineral ores with higher uranium content. There are sev-
eral uranium deposits in Serbia. The occurrences of ura-
nium mineralization are present at several localities in
Central and Eastern Serbia. The exploration of those
localities has been carried out since the middle of the last
century, with some interruptions. The uranium ore was
exploited only in Stara Planina Mountain in Eastern Serbia
in the vicinity of the Bulgarian border (Fig. 1). Stara
Planina Mountain represents a significant area, with variety
of mineral paragenesis formed, both of endogenetic or
atmospheric/surface origin. Particular points of interests
are hercinyan orogeny ore deposits, such as uranium, gold,
silver and bismuth deposits [4]. Detailed geology of this
area is given in the Ref. [3]. Exploitation of the uranium in
this region started in the late fifties of the twentieth century,
but after the year 1996, all of the mines were closed. Two
mines, ‘‘Mezdreja’’ and ‘‘Gabrovnica’’ exist within the
123
 J Radioanal Nucl Chem

Fig. 1 Geological map of Stara

Planina in the Serbian territory
[4]. Legend: 1 Marlstone and
claystone (Miocene); 2
Conglomerate, sandstone,
limestone, and dolomite
(Jurassic and Cretaceous); 3
Limestone and dolomite
(Triassic); 4 Clastics (Permo-
Triassic); 5 Red sandstone
(Permian); 6 Granodiorite
porphyry (Permian); 7
Volcanogenic-sedimentary
rocks (Carboniferous); 8
Terrigene rocks
(Carboniferous–Permian); 9
Granitic rocks (Carboniferous);
10 Gabbroid rocks
(Carboniferous); 11 Diabase
(Riphean–Cambrian); 12
Greenstone, greenschist and
metasedimentary rocks
(Riphean–Cambrian); 13 Fault;
and 14 River

study area together with number of exploratory galleries on
the ‘‘Srneći Do’’ and ‘‘Aldina reka’’ locations [4].
In the Ref. [4] the area surrounding the village Kalna on
Stara Planina Mountain in Eastern Serbia, is defined as a
location characterized by the increased content of natural
radioactive elements.
The investigations of radioactivity content of the
samples collected around abandoned mine ‘‘Gabrovnica’’
were carried out in order to determine the present state of
the environment in this area. This paper presents results
obtained by measuring the activity concentration of
environmental samples (soil, moss and stone) by gamma
spectrometry and also indoor 222Rn activity concentra-
tions in houses in the nearby village Kalna. In Slovenia
near former uranium mine radon (222Rn) was recognized
as most significant contributing to the radiation dose to
the population in the nearby village [5]. The present
situation ‘‘on site’’ is that this abandoned mine ‘‘Gab-
rovnica’’ is closed for public entrance but not secured
properly. The main mine shaft is closed. It is in institu-
tional surveillance by one public corporation in Serbia,
but never officially decommissioned. The results obtained
might be useful for the future decommissioning
procedure.
Materials and methods
Soil samples (9) were collected together with three samples
of stones and two samples of moss on seven different
locations in the vincinity of former Uranium Mine (Fig. 1).
All sampling locations are in the area marked as Aldina
Reka on the Fig. 1.
The activity of radionuclides in all collected samples
was determined using HPGe detector, by gamma spec-
troscopy methodology [6].
The homogenized samples were dried at 105 °C to con-
stant mass. After that, all mechanical contaminants, mainly
small rocks and pieces of plant material were removed.
Dried soil samples were mechanically fragmented and
homogenized to a fine powder. Prepared soil samples were
packed in cylindrical measurement vessels—sample hold-
ers, 62 mm in height and 67 mm in diameter. Typical
sample mass was between 200 and 300 g. Due to the
urgency of carrying out radioactivity measurements, there
was not enough time for the radon to reach equilibrium in the
samples. To achieve this equilibrium, a time period of at
least 30 days is needed. Therefore the measured concen-
trations of 226Ra were lower than the equilibrium values by
about 20 % [6]. The duration of measurement was 70,000 s.

123
J Radioanal Nucl Chem
Gamma spectrometry measurements were performed
with high resolution HPGe gamma spectrometer produced
from CANBERRA. This detector has a nominal relative
efficiency of 36 % and a resolution of 1.79 keV. The
detector was operated inside the 12 cm thick lead shield
with a 3 mm Cu inner layer [7].
Through CANBERRA type pre-amplifiers and amplifi-
ers the signals were connected to a multichannel analyzer
MCA with two 8192 channel analog to digital converters.
The MCA was directly connected to a PC where measured
spectra were stored and analyzed. The gamma spectra were
acquired and analyzed using the Canberra Genie 2000
software. The program calculates the activity concentration
of an isotope from all prominent gamma lines after peaked
background subtraction. All measurement uncertainties are
presented at a 95 % confidence level, which is determined
as the statistics of the counting. This means that the
probability for obtaining a result lying outside the pre-
sented limits in a repeated measurement of the same
sample is less than 5 % [6]. The detection energy and
efficiency calibration for HPGe detector were performed
using a certified calibration source 152Eu of exactly the
same geometry as the measured samples, produced by
AREVA. This source was placed in contact geometry in
front of the detector and a spectrum was recorded on both
detectors. It was necessary to adjust these results to the
corresponding sample matrix (soil) using the computer
program Angle [8].
For determination of radon concentrations in air in
dwellings in the nearby village Kalna, we used method of
charcoal canisters. Charcoal canisters represent the sim-
plest device for measuring radon concentration, but the
most applicable for monitoring purposes. Accuracy is fair
(\20 %) and is greatly affected by humidity and air
movement. The accuracy of the charcoal canister decreases
the longer the test evaluation is delayed. Radon is adsorbed
onto the charcoal grains and decays to several particulate
decay products: 218Po, 214Pb, 214Bi, 214Po and 210Pb. Radon
concentration was determined by counting the gamma-ray
emissions of both 214Pb (295 and 352 keV) and 214Bi
(609 keV). This method is possible due to the relatively
short half-life of these progenies. Within 3 h, the progenies
are in equilibrium with 222Rn. The efficiency of the
detectors was determined using the Environmental Pro-
tection Agency (EPA) 226Ra reference source [9]. The
passive nature of activated charcoal allows both adsorption
and desorption; in addition, the adsorbed radon undergoes
radioactive decay during the exposure period. However,
the canister can be calibrated to yield precise result for
radon concentrations in structures during the deployment
period of 48 h used by EPA [10].
The charcoal canisters were exposed to air in eight
houses and working objects in the nearby village Kalna for
around 48 h and after that they were closed and the activity
concentration of radon in them was determined using two
HPGe detectors by standard gamma spectroscopy method.
We made a decay correction when calculating the absorbed
radon activity concentrations on charcoal. The calculation
of activity concentrations measured by charcoal canisters is
made according to the EPA standard operating procedures
[9]. Every canister is weighted before and after it was
exposed and the weight difference is taken into account in
the activity calculation.
Results and discussion
In Table 1 the results of gamma-spectroscopy measure-
ments of collected samples from the vicinity of former
uranium mine Gabrovnica are presented.
The external hazard index is given in the seventh col-
umn in Table 1. calculated according to the Eq. (1) from
the Ref. [11]:
ARa ATh AK
Hex ¼ þ þ 1 ð1Þ
370 259 4;810
where ARa , ATh and AK are the activity concentrations of
226
Ra, 232Th and 40K [Bq kg-1]. The value of external
hazard index should be less than one in order to have
insignificant radiation hazard on the examined area.
Radium equivalent activity (last column in the Table 1)
is a widely used hazard index and it is calculated according
to the following equation [11, 12]:
Raeq ½Bq kg1  ¼ ARa þ 1:43ATh þ 0:077AK ð2Þ
In the Eq. (2) it has been assumed that 370 Bq kg-1 of
226
Ra or 259 Bq kg-1 of 232Th or 4,810 Bq kg-1 of 40K
produce the same gamma dose rate. Recommended maxi-
mum value for radium equivalent activity is 370 Bq kg-1
[11]. From obtained results in Table 1, it can be concluded
that more than half of the analyzed samples exceed this
limit.
The contribution of natural radionuclides to the absor-
bed dose rate in air [D(nGy h-1)], given in the Table 1, at
a height of about 1 meter above the ground are calculated
by using the conversion factor of 0.0417 nGy h-1 Bq-1 kg
for 40K, 0.462 nGy h-1 Bq-1 kg for 226Ra and
0.604 nGy h-1 Bq-1 kg for 232Th, Eq. (3) [13] and
assuming that 137Cs and 235U decay series can be neglected
as they contribute very little to the total dose from envi-
ronmental background [11, 14]:
 
D nGy  h1 ¼ 0:462ARa þ 0:604ATh þ 0:041AK ð3Þ
Those obtained values for absorbed dose rate can be
used for estimation of Annual Effective Doses
(AEDE½lSv  y1 ). The factors which have to be included
123
 Table 1 Activity concentrations of radionuclides in samples from surrounding area of former uranium mine ‘‘Gabrovnica’’
Sample ID (GPS coordinates) Activity concentration (Bq kg-1) Hex D (nGy h-1) AEDE Raeq
238 226 232 40 137 (lSv year-1) (Bq kg-1)

123
U Ra Th K Cs

1. Stone—entrance to the mine shaft (N43°260 23.50 ’ E22°250 37.90 ’) 134 ± 8 2,290 ± 270 111 ± 9 1,080 ± 40 \4 6.8 1,169 1,434 2,532
2. Soil—entrance to the mine shaft (N43°260 23.50 ’ E22°250 37.90 ’) 131 ± 6 51.6 ± 1.4 136.2 ± 2.3 1,110 ± 30 1.0 ± 0.3 0.9 152 186 332
3. Soil—in front of the entrance (N43°260 23.300 E22°250 37.100 ) 249 ± 11 1,308 ± 100 69 ± 4 960 ± 30 15.3 ± 0.8 4.0 685 840 1,481
4. Soil—in front further (N43°260 23.500 E22°250 36.800 ) 279 ± 16 3,030 ± 160 78 ± 3 1,260 ± 80 42.1 ± 2.3 8.8 1,499 1,838 3,239
5. Soil—in front of the nearby house (N43°260 25.500 E22°250 37.500 ) 120 ± 7 46 ± 4 118 ± 8 1,030 ± 40 53.4 ± 2.1 0.8 135 165 294
6. Stone (N43°260 22.600 E22°250 37.200 ) 112 ± 6 40.1 ± 1.3 114 ± 4 1,220 ± 30 \1.7 0.8 137 169 297
7. Moss—entrance (N43°260 23.500 E22°250 37.900 ) 92 ± 8 51 ± 19 144 ± 15 520 ± 40 13.7 ± 2.2 0.8 132 162 297
8. Road to the mine shaft (N43°260 24.900 E22°250 36.200 ) 123 ± 8 114 ± 5 66.3 ± 1.9 790 ± 30 60.1 ± 2.6 0.7 125 153 270
9. Rubbish mining 1 (N43°260 18.500 E22°250 2700 ) 262 ± 11 390 ± 9 137 ± 7 1,300 ± 40 6.5 ± 0.6 1.9 316 388 686
10. Rubbish mining 2 (N43°260 17.700 E22°250 26.800 ) 273 ± 11 495 ± 13 109.2 ± 2.5 1,070 ± 30 7.0 ± 0.6 2.0 339 415 734
11. Stone—rubbish mining (N43°260 18.500 E22°250 2700 ) 231 ± 10 230 ± 5 132 ± 5 1,510 ± 40 \2.5 1.4 248 304 535
12. Moss—rubbish mining (N43°260 18.500 E22°250 2700 ) 442 ± 18 880 ± 50 170 ± 4 1,290 ± 50 74.0 ± 2.2 3.3 562 689 1,222
13. Rubbish mining—river (N43°260 15.600 E22°250 29.600 ) 44.6 ± 2.9 28.6 ± 2.0 32.9 ± 2.1 616 ± 20 2.5 ± 0.6 0.3 58 72 123
14. Soil—around well (N43°260 30.600 E22°250 33.600 ) 207 ± 9 63 ± 5 160 ± 8 1,280 ± 40 29.2 ± 1.5 1.1 178 219 390


environment
 

equivalent factor, Raeq = 370 Bq kg-1


lated according to Ref. [11] via Eq. (4):


 0:7½Sv Gy1   103


AEDE lSv year1 ¼ D nGy h1  8;760 h year1  0:2
an outdoor occupancy of 20 % [13]. The AEDE is calcu-
the absorbed rate into human effective dose equivalent with
conversion factor of 0.7 Sv Gy-1, which is used to convert

Fig. 3 Radium equivalent factor calculated for all collected samples.

Straight line represents recommended limit Hex B1 for safe radiation
Fig. 2 External hazard index calculated for all collected samples.
absorbed dose in air to effective dose and (b) the outdoor
in this calculation are: (a) the conversion coefficient from

Straight line represents recommended maximum level for radium

From the results presented in the Table 1, it can be
dose equivalent received by a member is calculated using a

ð4Þ
J Radioanal Nucl Chem

from outdoor terrestrial gamma radiation is 70 lSv year-1.

The world average annual effective dose equivalent
occupancy factor. The annual estimated average effective
J Radioanal Nucl Chem

results also show higher activity concentration of 137Cs in

Fig. 4 Annual effective dose equivalent calculated for all collected
samples. Straight line represents the world average annual effective
dose equivalent from outdoor terrestrial gamma radiation,
AEDE = 70lSv year-1
222
Table 2 Activity concentrations of
charcoal canisters
Location ID
House 1—ground floor
House 2—basement
House 3—ground floor (old building)
House 4—ground floor (new building)
House 5—ground floor
Building 6 –working area—ground floor
Building 6—working area—basement
House 7—basement
House 8—ground floor
House 8—basement
some samples.
In the nearby village Kalna, there is no need for concern,
the highest activity concentration of 222Rn is found in the
building 6—which is working area. According to recom-
mendations from the International Commission on Radio-
logical Protection Statement on Radon, from November
2009, the upper level for radon gas in dwellings is
300 Bq m-3. Taking account of differences in the lengths
of time spent in homes and workplaces of about a factor of
three, a level of radon gas of around 1,000 Bq m-3 defines
the entry point for applying occupational protection for
existing exposure situations [15]. All houses are very well
ventilated which greatly affect 222Rn activity concentra-
tions in air, so there is no need for any intervention.
From all obtained values and calculated indexes we
confirmed that this area of former uranium mine ‘‘Gab-
rovnica’’ has elevated levels of natural radioactivity. This
is abounded area and most of the houses nearby are empty,
there are few houses which are used occasionally during
Rn in houses measured by year. This investigation provided information about
necessity of decommissioning of this area and better secure
Activity concentration of the entrance in the former uranium mine area. Inside this
of 222Rn, A (Bq m-3)
area there is also one small house and garden around with
107 ± 6 some fruits which should not be used for food.
50 ± 4 Future investigations should include other mentioned
49 ± 5 locations in East Serbia. Stara Planina is well known as
33 ± 3 mountain with high content of naturally occurring radio-
93 ± 6 active uranium. Part of this mountain is in Bulgaria (our
903 ± 14 neighboring country) and there were also couple of ura-
231 ± 9 nium mines in the past which are closed and decommis-
120 ± 6 sioned or in the phase of decommissioning.
114 ± 7
Acknowledgments This study was supported by Ministry of Edu-
137 ± 6 cation, Science and Technological Development of Republic of Ser-
bia within the projects No. 43002 and 171002.

concluded that all analyzed samples exceed this average

annual effective dose equivalent.
All calculated indexes are presented on Figs. 2, 3 and 4.
Table 2 presents obtained results of 222Rn activity
concentration in the air in houses in the nearby village
Kalna.
Conclusion
Most of the examined samples from the vicinity of the
former uranium mine ‘‘Gabrovnica’’ near small village
Kalna in East Serbia show elevated radioactivity. Only six
samples (from 14 measured by gamma-spectroscopy) have
external hazard index less than one. There are two soil
samples taken from the entrance to the main shaft which
have really high external hazard index. The obtained
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