Assessment of Inhalation Exposure Potential of Broken Uranium Ore Piles in Low-Grade Uranium Mine

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Assessment of inhalation exposure potential of


broken uranium ore piles in low-grade uranium
mine

Article in Journal of Radioanalytical and Nuclear Chemistry · October 2014


Impact Factor: 1.03 · DOI: 10.1007/s10967-014-3288-6

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J Radioanal Nucl Chem
DOI 10.1007/s10967-014-3288-6

Assessment of inhalation exposure potential of broken uranium


ore piles in low-grade uranium mine
Durga Charan Panigrahi • Patitapaban Sahu •

Devi Prasad Mishra • Vivekanand Jha •


R. Lokeswara Patnaik

Received: 3 March 2014


Ó Akadémiai Kiadó, Budapest, Hungary 2014

Abstract This paper presents the assessment of inhala- primarily done by underground mining methods. Among
tion exposure potential of broken uranium ore piles in the oxides of uranium, uraninite and pitchblende are the
different stopes of Jaduguda uranium mines of India. 222Rn most common mineral forms of uranium. Uranium in the
emanation coefficient of broken uranium ore was measured ore is always associated with the members of its decay
in laboratory by collecting air sample from airtight glass jar series. Radioactive equilibrium in the ore among the
containing ore sample. An attempt was also made to cor- members of the series may or may not exist depending on
relate the emanation coefficient with 226Ra content of the the nature of the deposit, which in turn depends on the
ore. The 222Rn progeny doses estimated based on radon factors like age, weathering conditions and ecological
activity concentration of broken ore, occupancy period and factors. In the absence of suitable control measures, the
equilibrium ratio in different stopes were well below the radioactive nature of the uraniferous minerals may cause
prescribed limit of International Commission on Radio- occupational hazards to the mine workers. The contribution
logical Protection. The maximum 222Rn progeny dose to the radiological hazards from 238U (half-life of
contribution from broken ore piles was worked out to be 4.47 9 109 years) and its decay products is of primary
0.22 mSv year-1. This suggests that the broken ore piles concern in uranium mines due to the large abundance of
238
are not the significant contributor of inhalation exposure U (99.2739 %) in the natural uranium [1]. Radium
under the existing ventilation condition of Jaduguda ura- (226Ra), which is formed in the disintegration series of
238
nium mine. U, is the natural source of high radiation level in ura-
nium mines [2, 3]. Since 226Ra has a long half-life of
Keywords Underground uranium mine  Broken uranium 1,600 ± 7 years [4], it acts as an effective source of 222Rn
ore  222Rn emanation coefficient  226Ra content  222Rn gas with a relatively short half-life of 3.82 days in mine air.
222
progeny exposure  Mine ventilation Rn and its decay products constitute the main occu-
pational radiation exposure and their residence in under-
ground uranium mine environment depends on the
Introduction ventilation conditions of the mine. The freshly formed decay
products of radon readily attach themselves to the surface of
Uranium-bearing minerals mostly occur at greater depths airborne ultrafine dust particles. When the dust laden mine
below ground and hence extraction of uranium ore is air is inhaled, radon decay products deposit preferentially in
the respiratory tract and emit alpha particles. Extensive
epidemiological studies have revealed a significant correla-
D. C. Panigrahi  P. Sahu  D. P. Mishra (&)
Department of Mining Engineering, Indian School of Mines, tion between exposure to radon decay products and induction
Dhanbad 826 004, India of lung anomaly in underground uranium mines [5–12]. It
e-mail: [email protected] has been reported that the dose to the lung from inhalation of
radon is insignificant in comparison to the dose delivered by
V. Jha  R. L. Patnaik
Environmental Assessment Division, Bhabha Atomic Research its decay products [13]. The wide coverage in inhalation dose
Centre, Trombay, Mumbai 400 085, India evaluation methodology of radon progeny is based on the

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J Radioanal Nucl Chem

estimation of radon activity concentration, equilibrium ratio Jharkhand, India (Fig. 1). The shear zone is of about
and occupancy period [14]. If radon which emanates into the 160 km length and 1–10 km width. The uranium ore
mine atmosphere can be removed through rapid air change, lenses of Proterozoic age are hosted in the highly folded
then the radon gas entering the mine air will have insufficient and sheared metamorphic rocks. Uranium-bearing miner-
time to build-up appreciable quantities of its decay products. als occur in a very finely disseminated form. The host
An average 20 min residence time of radon in mine air will rocks are brecciated quartzite and quartz-chlorite-biotite-
develop 30 % of the equilibrium decay product working magnetite schist. The primary ore mineral is uraninite
levels in the mines [15, 16]. Thus, radon in mine air can be occurring as discrete grains along with autunite and tor-
considered as an indicative of the inhalation hazards and bernite [23]. The strike of the main ore body at Jaduguda
monitoring of radon activity concentration level in uranium dipping towards north is in the east–west direction. The
mines is essential to ensure the regulatory compliance for maximum vertical extent and thickness of the ore body
protecting the occupational workers. are about 905 and 10 m, respectively. Horizontal cut-and-
Broken ore piles constitute one of the important sources of fill method is the principal stoping method adopted in
radon emanation in underground uranium mines and mea- Jaduguda mine, in which the stoped out area is filled with
surement of emanation coefficient of the uranium ore forms an the aqueous slurry of de-slimed coarser fraction mill
important basis for assessing the potential hazards to the tailings.
miners. The radon concentration contributed by broken ura-
nium ore in mines can be evaluated by measuring the radon
emanation coefficient, i.e. the fraction of radon which escapes Materials and methods
from the ore matrix [17]. The measurement of emanation
coefficient of broken uranium ores has been conducted by Materials
several researchers [18–20]. Raghavayya [21] used an accu-
mulation jar for determination of emanation coefficient of the Thirty-two broken uranium ore samples were randomly
uranium ore samples based on measurement of surface area of collected from nine stopes of Jaduguda uranium mine for
the samples. This method may not be suitable for determina- determination of radon emanation coefficient and radium
tion of emanation coefficient from the irregular ore samples activity concentration. The collected ore samples were kept
because of the inaccuracy in the measurement of surface area in plastic bags and the location and date of sample col-
of irregular ore samples. Although, periphery tracing method lection were noted on the plastic bags. The samples were
is used to measure the surface area of irregular samples, this broken into small pieces of less than 5 cm thickness using a
may not give accurate result since it does not take into con- hammer for determination of emanation coefficient. After
sideration the curvature of the ore samples. Bossew [22] determination of emanation coefficient, the samples were
measured the radon emanation coefficient of rock samples dried in a temperature controlled oven at 105 °C for 24 h to
using active charcoal enclosed with the investigated sample in completely remove the moisture for determination of
a sealed container for more than 1 week. This technique may radium activity concentration. The samples were then kept
give high uncertainties in the results due to leakage of air in the in the desiccators for cooling to room temperature and
longer period of experiment. preventing ambient moisture absorption.
Keeping this in view, we measured the radon emanation
coefficient of the uranium ore samples enclosed in an air- Measurement of radon emanation coefficient
tight glass jar of 1 L capacity in the laboratory based on of uranium ore samples
measurement of mass of the ore sample. This mass-related
approach is comparatively simpler and quicker than the The emanation coefficient of the broken ore samples was
aforementioned techniques. Furthermore, it would not add measured in the laboratory by enclosing the ore samples in
large uncertainties which are associated with the mea- a 1 L capacity airtight jar into which radon gas emanating
surement of surface area of the samples. The aim of this from the ore sample was allowed to accumulate. After a
study is to estimate 222Rn progeny doses based on radon build-up period of 5–6 h, air sample from the jar was
activity concentration of broken ore, occupancy period and drawn into an evacuated scintillation cell. For determina-
equilibrium ratio in the stopes. tion of the radon activity concentration, the scintillation
cell was connected to the photomultiplier assembly and
alpha counting set up after a delay period of about 200 min
Description of the study area to ensure equilibrium between the radon and its short-lived
progeny in the cell. The detailed experimental method for
The present investigation was carried out at Jaduguda determination of the radon activity concentration has been
uranium mine located in the Singhbhum shear zone of described elsewhere [24].

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J Radioanal Nucl Chem

Fig. 1 The location and lithological units of Jaduguda uranium mine

The radon activity concentration in the accumulation jar of 226Ra activity concentration of the ore samples is
increases till it attains equilibrium activity concentration available elsewhere [27, 28]. The radium activity ‘226Ra’
(Ceq) after 30 days. This equilibrium concentration in the (Bq) in the ore samples was estimated at 95 % confidence
accumulation chamber is presumed to be equal to the radon interval using the relation
concentration in the pore spaces among solid grains. The ck
226
radon build-up curve can be expressed as [25] Ra ¼ ð3Þ
3Eekt ð1  ekh Þð1  ekT Þ
Ct ¼ Ceq ð1  ekt Þ ð1Þ
where c is the number of alpha counts during time T, k is
where Ct is the radon concentration measured at time ‘t’ the decay constant of 222Rn (s-1), E is the efficiency of the
(Bq m-3), k is the radon decay constant (2.09 9 10-6 s-1) counting set up (%), t is the delay time after end of the
and t is the accumulation time of radon in the jar (s). sampling (s), T is the counting duration (s), h is the build-
The emanation coefficient ‘f’ was calculated using the up time in bubbler (s). The radium activity concentration
relation [26] ‘CRa’ (Bq kg-1) in the ore sample was worked out using
Ceq Ve C t Ve the above equation and other sampling parameters such as
f ¼ ¼ ð2Þ weight of the sample, volume of the solution loaded in the
CRa M CRa M ð1  ekt Þ
bubbler (50 ml) and the total volume of solution prepared
where Ve is the effective volume of jar (m3), M is the mass from the sample (100 ml).
of ore sample (kg) and CRa is the radium activity concen-
tration (Bq kg-1). Assessment of inhalation exposure due to 222
Rn
For measurement of 226Ra activity concentration (CRa), progeny
the oven-dried ore samples were crushed, sieved though
standard sieve of 200 mesh size and homogenized. 2 g of Assessment of exposure due to radon progeny by the
the powdered sample was subjected to repeated leaching in miners can be theoretically worked out if the information
8 N HNO3 after initial evaporation in concentrated nitric about attributable factors such as radon emanation from the
acid. The mixture was filtered using 0.45 lm filter paper ore, equilibrium ratio and radon elimination by ventilation,
and the residue was subjected for silica removal using radioactive decay are available. Radon production rate
hydrofluoric acid. The residue was dissolved in dilute nitric from ore was calculated using the relation [29]
acid and mixed with the original aliquot. Thereafter, the
q ¼ m  CRa  k  f  1;000 ð4Þ
mixture was made up to 100 ml maintaining the resultant
-1
acid normality at 4 N [27]. 50 ml of the leach aliquot was where q is the radon production rate (Bq s ), m is the
transferred to a radon bubbler. The radon sample from the quantity of broken ore (ton) and 1,000 is the factor for
solution was drawn from the bubbler into an evacuated conversion of tonnage to kilogram. The concentration of
scintillation cell after a delay period ([20 days) allowing radon ‘CRn’ (Bq m-3) emanated from the ore samples was
sufficient build-up of radon. The method of measurement calculated using the relation [25, 30]

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J Radioanal Nucl Chem

q Table 1 Statistical parameters of 226


Ra content and emanation
CRn ¼ ð5Þ
V  ð k þ kv Þ coefficient of uranium ore samples
226
where V is the air volume of the stope (m3) and kv is the Parameters Ra content Emanation
(Bq kg-1) coefficient
ventilation rate in the stope (s-1). The ventilation rate in
the stope was calculated using the following relation Minimum 259 0.008
Maximum 19,950 0.072
Q
kv ¼ ð6Þ Arithmetic mean 4,729 0.025
V
Median 3,569 0.022
where Q is the airflow rate in the stope (m3 s-1). Standard deviation 4,436 0.016
The annual effective dose ‘HE’ (mSv year-1) contrib- Skewness 1.54 1.66
uted by broken ore was calculated using the relation Kurtosis 3.31 3.04
Tex  F  CRn  Dcf Geometric mean 2,705 0.022
HE ¼ ð7Þ
170  3;700 Geometric standard deviation 3.42 1.75

where Tex is the time of exposure within a year (in hours), F is


the equilibrium factor, Dcf is the dose conversion factor
(mSv WLM-1), 170 is the number of hours per working month samples analysed in this study. 226Ra content of the ore
and 3,700 is the 222Rn concentration (Bq m-3) which is in samples varied in the range of 259–19,950 Bq kg-1 with
equilibrium with its progeny corresponding to a potential alpha geometric mean of 2,705 Bq kg-1 and geometric standard
energy concentration of 1 working level ‘WL’. The Interna- deviation of 3.42. This variation in 226Ra content may be
tional Commission on Radiological Protection has recom- due to the heterogeneous distribution of uranium-bearing
mended an equilibrium factor value of 0.4 for the purpose of minerals in the ore. The emanation coefficient of the ore
radiation protection in uranium mines where the equilibrium samples varied in the range of 0.008–0.072 with the geo-
factor is unknown or difficult to determine experimentally [9]. metric mean of 0.022 and geometric standard deviation of
However, an equilibrium factor value of 0.5 determined by 1.75. Austin and Droullard [18] reported the emanation
Eappen et al. [31] for Jaduguda uranium mine has been used for coefficient of uranium ores ranging from 0.01 to 0.91.
calculation of annual effective dose. The total occupational Thompkins [3] reported the emanation coefficient of Elliot
exposure period, which is normally taken as 2,000 h per year, Lake ore, Italy ore and Australia ore as 0.0197, 0.0097 and
includes the time spent by the miners at different places starting 0.0877 respectively with their respective ore grades of
from the surface facilities to mine entrance, underground travel 0.075, 0.029 and 0.025 %. The emanation coefficients of
ways and finally at actual work sites such as stopes, develop- different types of uranium ore such as autunite, carnotite
ment drivages, etc. Relaxation period in change room and time and uraninite were reported in the ranges of 0.02–0.04,
spent at surface job are also included in this overall occupancy 0.12–0.19 and 0.12–0.15 respectively [34]. Mudd [19]
period. Further, occupancy is highly dependent on the nature of reported the emanation coefficient in the range of 0.1–0.3
job such as mining, blasting, mucking, drilling and mainte- for Australian uranium rock. This shows that the emanation
nance. A realistic dosimetric reference equation, which incor- coefficient obtained in the present study are falling within
porates all these features, has been provided elsewhere [32, 33]. the earlier reported values. However, the variation in the
Keeping this in mind, the maximum time spent by a miner in emanation coefficients reported by different authors may
stopes or the actual ore winning areas can be worked out to be be due to variation in mineralogy, porosity, moisture con-
4 h day-1. Therefore, the maximum annual occupational tent, grain size, uranium distribution, weathering and rock
exposure period in operations associated with handling of type.
broken ore piles can be presumed to be about 1,000 h year-1. In The 226Ra content and emanation coefficient of the ore
the present study, the conversion factor of 5 mSv WLM-1 samples determined in the present study are highly skewed
reported by ICRP-65 was used for the calculation of internal depicting asymmetrical nature of the distributions. The
dose received by a miner. positive kurtosis of these data indicates higher and nar-
rower distribution than the normal distribution. The normal
probability plot of emanation coefficient of uranium ore
Results and discussion samples has been presented in Fig. 2. In this figure, the data
distribution shows that the data are deviated much from the
222
Rn emanation coefficient of the ore samples straight line and hence the distribution of data set is
probably not normal. Moreover, the median and geometric
Table 1 presents the statistical parameters of 226Ra content mean values of emanation coefficient were found to be
and emanation coefficient of 32 broken uranium ore same. So the assumption of log-normal distribution of data

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J Radioanal Nucl Chem

2.5 ore piles in different stopes. The 222Rn concentration from


2.0 broken ore piles in the stopes was worked out using Eqs.
1.5 (4) and (5). In order to derive the radon activity concen-
Expected normal value

1.0
tration levels in the stopes, the geometric mean values of
226
Ra activity concentration and emanation coefficient
0.5
were used, since their data sets followed log-normal dis-
0.0
tribution as discussed earlier. The 222Rn concentration from
-0.5 broken ore piles in the stopes varied in the range of
-1.0 12–56 Bq m-3 with arithmetic mean of 23 ± 15 Bq m-3,
-1.5 which is far below the upper value for workplace reference
-2.0 level of 1,500 Bq m-3 recommended by ICRP [35]. This
-2.5
reveals the fact that under the existing ventilation condition
-0.03 -0.02 -0.01 0.00 0.01 0.02 0.03 0.04 0.05 of the mine, broken ore piles are not prominent source of
Residuals radon progeny exposure. Although, the present radon level
in the mine is well below the prescribed limit, increase in
Fig. 2 Normal probability plot of emanation coefficient of uranium
ore samples radon activity concentration can be anticipated due to other
attributes such as backfill tailings, mine water and exposed
0.08
ore surface. This may warrant regular update of the
designing and planning of ventilation system of the mine.
0.07
The annual effective dose due to radon emanation from
Emanation coefficient

0.06 r = - 0.32, p = 0.07


broken ore varied in the range of 0.05–0.22 mSv year-1
0.05
with mean value of 0.09 ± 0.06 mSv year-1. This is far
0.04 below the prescribed limit of 20 mSv year-1 recom-
0.03 mended by ICRP [35]. It may be mentioned here that the
0.02 annual effective inhalation dose received by the miners
0.01 depends upon the overall radon concentration in work-
0
places, which arises due to radon emanation from broken
0 5000 10000 15000 20000 25000 ore piles, waste rock, backfill tailings, ore body and mine
226 Ra content (Bq kg-1 ) water. It is further affected by ventilation planning of the
226
workplaces. Over the years, it was observed that the mean
Fig. 3 Relationship of emanation coefficient with Ra content of 222
uranium ore samples
Rn concentration in the same mine varied in the range of
190–410 Bq m-3 with corresponding overall internal doses
varying from 1.90 to 2.79 mSv year-1 [33], which is also
well below the ICRP prescribed limit of 20 mSv year-1.
set can be approximated both for 226Ra activity concen- Quick removal of broken ore piles, waste rock and proper
tration and emanation coefficient. ventilation planning of the stopes may further reduce the
The variation of emanation coefficient with 226Ra con- radon dose received by the miners.
tent of uranium ore samples is shown in Fig. 3, which Figure 4 shows the variation of radon concentration with
indicates an insignificant correlation (r = -0.32, p = 0.07) ventilation rate in different stopes of Jaduguda uranium
between 226Ra content and emanation coefficient. The error mine. The error bars in the figure represent 5 % error. From
bars in the figure represent 5 % error. A similar finding has this figure, it may be observed that the radon concentration in
also been reported by Austin and Droullard [18]. The stopes decreases with ventilation rate indicating a negative
independence between the activity concentration of 226Ra correlation (r = -0.66) between them. From Table 2, it is
and emanation coefficient of 222Rn reveals the fact that the evident that the radon concentration and the annual effective
ore characteristics have an important bearing on the ema- dose in Stope 2 and Stope 7 are comparatively higher than the
nation. Further, spatial distribution of radium and presence other stopes. This is attributed to lower ventilation rates in
of porous network in the ore samples can also contribute to these two stopes. Although the ventilation rate in Stope 8
radon emanation. (1.19 9 10-4 s-1) was even lower than the ventilation rate
in Stope 2 (1.81 9 10-4 s-1), the radon concentration in
222
Inhalation exposure due to Rn progeny Stope 2 was higher than that in Stope 8 by a factor of two
despite both the stopes were containing almost identical
Table 2 presents the radon concentration and correspond- quantity of broken ore piles. This may be due to the larger
ing annual effective internal dose contributed by broken volume of Stope 8 as compared to Stope 2 resulting in drastic

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J Radioanal Nucl Chem

Table 2 Summarised results of Location Volume Amount Ventilation Radon Annual effective
radon concentration and of stope of broken rate concentration dose (mSv year-1)
corresponding annual effective (m3) ore (t) (910-4 s-1) (Bq m-3)
internal dose received by miners
in different stopes exclusively Stope 1 4,615 250 4.55 15 0.06
contributed by broken ore piles
Stope 2 2,592 150 1.81 40 0.16
Stope 3 5,573 223.6 2.94 17 0.07
Stope 4 2,359 127.4 5.69 12 0.05
Stope 5 2,608 163.8 5.39 14 0.06
Stope 6 2,871 188.5 3.56 23 0.09
Stope 7 9,067 358.8 0.88 56 0.22
Stope 8 6,975 143 1.19 21 0.09
Stope 9 6,480 133 2.11 12 0.05
Arithmetic mean 23 0.09
Standard deviation 15 0.06

decrease in radon concentration in stopes with ventilation


70
rate indicating a negative correlation between them was
m-3 )

60 222 Rn = 5.5057λ
- v + 40.562 observed. The 222Rn concentration and internal dose levels
r = - 0.66
222 Rn concentration (Bq

50
in the stopes were found to be well below the prescribed
limits recommended by ICRP. Therefore, it may be con-
40
cluded that the broken ore piles do not significantly con-
30 tribute to the inhalation exposure of the miners in a well
ventilated low-grade uranium mine.
20

10 Acknowledgments The authors wish to express their sincere thanks


to Mr. D. Acharya, Chairman and Managing Director, Uranium Cor-
0 poration of Indian Ltd for granting necessary permission to carry out the
0 1 2 3 4 5 6
research work in Jaduguda uranium mine. Authors are also thankful to
Ventilation rate 'λ v ' (× 10-4 s-1 ) all the staff members of Health Physics Unit, BARC, Jaduguda for
extending all kinds of supports for carrying out the experiments.
Fig. 4 Variation of radon concentration with ventilation rate in
stopes
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