Journal of Environmental Radioactivity 75 (2004) 4757 www.elsevier.

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Occupational exposure of phosphate mine workers: airborne radioactivity measurements and dose assessment
Ashraf E. Khater , M.A. Hussein, Mohamed I. Hussein
National Center for Nuclear Safety and Radiation Control, Atomic Energy Authority, P.O. Box 7551, Nasr City, Cairo 11762, Egypt Received 1 June 2003; received in revised form 1 September 2003; accepted 1 October 2003

Abstract Under the Egyptian program for radiation safety and control, airborne radioactivity measurements and radiological dose assessment were conducted in some phosphate and uranium mines. Abu-Tartor mine is one of the biggest underground phosphate mines in Egypt. Airborne radioactivity, radon (222Rn) and its short-lived decay products (progenies) and thoron (220Rn), were measured in selected locations along the mine. The environmental gamma and workers dose equivalent rate (mSv/y) were measured inside and outside the mine using thermo-luminescence dosimeters (TLD). The results were presented and discussed. The calculated annual eective dose due to airborne radioactivity is the main source of occupational exposure and exceeding the maximum recommended level by ICRP-60 inside the mine tunnels. A number of recommendations are suggested to control the occupational exposures. # 2004 Published by Elsevier Ltd.
Keywords: Occupational exposure; Phosphate; Airborne Radioactivity; Dose calculation

1. Introduction Among the decay products of uranium, special attention has been directed towards radon (222Rn), a noble gas, that disseminates into the atmosphere and reaches radioactive equilibrium with its relatively short-lived daughters in about 2 h. Its highenergy alpha particles are known to contribute substantially to the induction of lung neo-plasias and skin cancer (Santo et al., 1995). Phosphate rock is the starting raw

Corresponding author. Tel./fax: +20-2-274-0238. E-mail address: khater_ashraf@yahoo.com (A.E. Khater).

0265-931X/$ - see front matter # 2004 Published by Elsevier Ltd. doi:10.1016/j.jenvrad.2003.11.001

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material for all phosphate products. The concentration of 238U and its decay products tend to be elevated in phosphate deposits of sedimentary origin. A comparison of the radiological impacts associated with the phosphate industry with those of uranium mining and milling indicates that most impacts are within one order of magnitude of each other per unit uranium production (Othman et al., 1992). A typical concentration of 238U in sedimentary phosphate deposits is 121 mg kg1 (1500 Bq/ kg) with a range of 30260 mg kg1 (3723224 Bq/kg) (UNSCEAR, 1993; Altschuler, 1980). The uranium contents of some Egyptian phosphate rocks in the Red Sea coast and several Nile valley sites are in the ranges of 19142 mg kg1 (2351761 Bq/ kg) and 48185 mg kg1 (5952294 Bq/kg), respectively (Bigu et al., 2000). The average 238U content in Abu-Tartor phosphate rock is about 32.9 mg kg1 (408 Bq/kg) (Khater et al., 2001). The primary potential environmental radiation problem is associated with phosphate rock mining and processing concerns, mining spoils and processing waste products. Occupational exposures mainly occur during mining process and transportation of phosphate rock, as well as during transportation and utilization of phosphate fertilizers. It has been indicated that 222Rn gas (a decay product of 238 U226Ra series) and its progeny constitute the largest single contributors to human radiation exposure from natural and man-made radioactive sources (UNSCEAR, 1988, 1977). Inhalation of radon and its short-lived decay products constitutes the most important occupational exposure of workers in mines (Amer et al., 2002). It is obvious that extraction of phosphate ore presents potential health hazards in addition to its chemical toxicity, particularly when the ore requires building subterranean facilities, i.e. underground mines, for its extraction. The problem is a consequence of poor or inadequate air ventilation which has a close relationship to 222 Rn concentration in the underground mine tunnels (Altschuler, 1980; Bigu et al., 2000). The increased incidence of lung cancer in uranium miners and uorspars miners due to radon daughters concentrations in an underground miner has been documented (Boothe, 1977). Radiation monitoring of workers engaged in phosphate mining and processing activities is essential. In spite of the fact that monitoring itself does not improve working conditions, but demonstrates if operational radiation protection measures function as intended, or whether further protection measures should be considered (Othman et al., 1992). A number of studies have been made to evaluate the occupational exposure in uranium, phosphate, and coal mines (Bigu et al., 2000; Kenawy et al., 1999, Hussein et al., 1997; Amer et al., 2002). Our work aims at the evaluation of the occupational radiation exposure in Abu-Tartor phosphate mine through airborne radioactivity measurements and, assessment of environmental and personal radiation dose rate. Since the mine is still in the experimental operation stage, the results of this work are preliminary. The present work has been conducted under the national program for radiation safety and control of the Egyptian Atomic Energy Authority. 2. Experimental work This study reports the occupational radiation doses received by the workers in Abu-Tartor phosphate mine. Occupational exposures arise from conventional

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mining activities. Abu-Tartor mine is a close cast underground mine. The current reserve estimate in the exhaustively investigated area is in the order of a billion tons of phosphate ore (Said, 1990). The planned annual production is 4 million tons of ore rock and 2.2 million tons of wet rock. The ore rock are crushed, sieved, and transported to beneciation plant to produce the wet rock. The wet rocks are stocked in large open piles for sale or transport to a phosphate chemical plant (Khater et al., 2001). The chart plan of the mine site and ore processing activities are shown in Fig. 1. There are two mechanical ventilation stations, one for the east side and another one for the west side. Auxiliary air pumps are used for ventilation of the side tunnels during build up of the side tunnels and long wall retreats (ore rock cutting). During sampling, the west side ventilation station was not in operation. As a safety procedure, temperature, humidity and air ow rate in the working places inside the mine tunnels are measured and recorded on a routine basis. v Average ranges from 18 to 46 (36.6) C temperatures, from 18 to 56 (39.5)% 3 humidity, and 721 (15) m /s air ow rates were recorded during sampling (personal communication). Two types of measurements were carried out in this work: airborne radioactivity measurements (222Rn, 222Rn daughters, and 220Rn), and area and personal gamma dose rate (mSv/y) measurements. Airborne radioactivity measurements were carried out in 20 locations along the mine tunnels, Fig. 2. Radon gas concentration measurements were conducted by the scintillation cell method (Lucas method) (Lucas, 1957). The air sample was sucked into an alpha scintillation chamber. The scintillation chamber, of 160-ml capacity, has inside walls coated with silver activated zinc sulphide, which emit light ashes when struck by alpha particles. The scintillations emitted are measured by placing the transparent surface of the chamber in contact with a photo-cathode detector in a light tight enclosure. Alpha particle count (radioactive gas and decay products) was done using an alpha particle

Fig. 1. Chart plan of the mine site and ore processing.

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Fig. 2. Sampling locations for airborne radioactivity measurement in the mine tunnels.

counter/scalar; model RDR-511, manufactured by EDA Instruments (Toronto, Canada). A sensitivity of 0.190.37 Bq/l (510 pCi/l) is attainable with a short counting period. The radon concentration is evaluated by dividing the counts due to alpha particles over the cell factor, which is determined using standard radon gas source. The standard radon gas source is composed mainly of a standard solid radium slat source model Pylon-150 developed by Pylon Electronic Development (Ottawa, Canada), traceable to the National Institute of Standards and Technology (NIST, USA). The estimated cell factor usually ranges from 1.6 to 1.8. Radon (222Rn) progeny concentrations were measured using the Rolle method (Rolle, 1972). Air samples were collected for 5 min at a ow rate about 6 l min1 on high eciency lter paper (Millipore, diameter 2.5 cm), followed by alpha counting after a delay time of about 5 min. The period of delay was selected to minimize the error resulting from variations in radon daughter ratios. The lter papers were counted using an EDA (RDA-200 Radon Daughter detector, EDA Instrument Inc.) type counting system by placing the lter paper on a scintillation tray coated with silver-activated zinc sulphide. A Pylon RN-190 radon progeny standard source was used for calibration to determine the counting eciency calibration of the scintillation tray. It houses a dry 226Ra source, which emanates radon gas into a sealed chamber. Radon decays into its daughters, which deposit on the inner surface of the chamber and on an enclosed lter paper. The RN-190 is designed so that the radon progeny are deposited uniformly over the lter and the chamber surface with an activity deposition of 73:16 Bq cm2 4%. For 4 min

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counting time measurement, a radon progeny of 0.03 WL (working level) can be measured with a reproducibility of 15%. The radon progeny concentration, expressed as WL, was calculated using the following equation: WL R=EvtF 1 where R is the alpha count rate in count min1 , E is the counting eciency, v is the volumetric sampling rate in l min1 , t is the sampling time in min, and F is a conversion factor, which may be approximated by 212 for sampling periods of 120 min. One working level represents any combination of short-lived radon daughters concentration in 1 l of air that results in the ultimate emission of 1:3 105 MeV of alpha energy, taking no account of the radon (Amer et al., 2002). Thoron (220Rn) progeny concentrations were measured using Rock method (Rock, 1975). Thoron progeny was collected on a high eciency membrane lter paper for 5 min at a ow rate of about 6 l min1 , followed by alpha counting of the lter after a delay of 5 h or more after the end of sampling. The 212Pb (ThB), a beta emitter, is in transient equilibrium with its alpha-emitting daughters, enabling its air concentration at the time of sampling to be calculated readily from the alpha count. A minimum detectable activity of 0.02 Bq/l is obtained using such technique. Thoron was calculated using the following equation: CThB 0:411Re0:001086T =Evt 2

where CThB is the ThB concentration, R is the count rate at T min from the end of sampling (count min1 ), T is the interval from the end of sampling until counting (>300 min) in min, E is the counting eciency, v is the volumetric sampling rate in l min1 and t is the sampling time in minutes. Forty locations and 45 workers were chosen to carry out area and personal eective dose measurements using TLD, respectively. The TLD Dosimeters for area monitoring of the mine tunnels were hung in the middle of the tunnels. The 45 workers were provided with TLD Dosimeters. They wore the dosimeter on the part of the body between their neck and waist that was most likely to be exposed to the greatest amount of radiation. The dosimeter assemblies consist of two parts, a TLD card and a holder. The TLD card consists of four hot-pressed LiF-100 (LiF:Mg,Ti) TL chips of 3 3 0:38 mm3 encapsulated between two sheets of Teon 10 mg/cm2 thick and mounted on an aluminium substrate. The holder is made of durable, tissue-equivalent, ABS plastic, and is sealed to retain the card in a light and moisture excluding environment. It also protects the card from environmental damage and retains the ltration media. A Harshaw 6600 reader was used. 3. Results and discussion 3.1. Airborne radioactivity measurements The results of airborne radioactivity measurements in Abu-Tartor phosphate mine are shown in Table 1. The average standard deviation (range) values of 222 Rn (Bq/m3), 222Rn daughters (WL, mSv/y) and 220Rn (Bq/m3) in Abu-Tartor,

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Table 1 Activity concentrations of radon gas (222Rn) and thoron gas (220Rn) in Bq/m3, and radon daughter products (222Rn daughters) estimated in level unit (WL) and annual eective dose (mSv/y) in Abu-Tartor phosphate mine Serial no. Sample code 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 1 17 18 19 20 10 11 12 13 14 15 16 17 18 19 20 6 3 7 2 1 5 4 9 8 Distance (m)a 451 385 193 0 250 500 800 1000 1200 1400 1600 2148 2532 2632 2672 2723 2865 2905 3206 3232 Distance (m)b 93 66 40 190 51 436 463 776 790
222

Rn (Bq/m3)

222

Rn daughters mSv/y 30.46 80.99 63.00 16.34 11.65 10.10 7.86 7.20 7.93 7.28 4.63 20.99 3.12 27.80 11.61 0.69 50.22 53.52 51.53 71.56
c

220

Rn (Bq/m3)

WL 4903:0 242 5153:0 248 1801.3 147 3543:0 208 5535.0 258 0.25 0.67 0.52 0.14 0.10 0.08 0.07 0.06 0.07 0.06 0.04 0.17 0.03 0.23 0.10 0.01 0.42 0.45 0.43 0.60

3.40 16.37 9.05 5.17d 1.98 1.00 5.74d 1.66d 5.15d 13.15 8.81d

Minimum and maximum values are italicized. a Distance from mechanical ventilation station. b Distance from the side tunnel entrance. c C:F: 62:5 lSv h1 =WL. d Natural ventilation.

Red Sea phosphate mines, El-Missikat uranium mine, and Erediya uranium mine are given in Table 2. The 222Rn concentrations in Bq/m3 were measured in ve locations in the side tunnels. All measurements are exceeding the limits for occupational exposure to radon (1000 Bq/m3) (IAEA, 1996). The mean 222Rn concentration standard error (SE) is 4187 685 Bq=m3 with a range of 18015535 Bq/m3. The mean 222Rn concentration in other Egyptian phosphate mines is 5772 Bq/m3 where some of these mines depend on the natural ventilation as in the west side of AbuTartor mine during our eld measurements (Bigu et al., 2000). The mean conce ntration SE (range) of 222Rn decay products in working level unit and its eective annual dose rate in mSv/y are 0:22 0:05 (0.010.67) and 26:90 5:67 (0.6980.99), respectively. The annual eective dose rate due to 222Rn decay products is exceeding the recommended limit, 20 mSv/y (ICRP-60), especially in the side tunnels locations by a factor of up to 4-fold because of the inadequate and bad ventilation (Bigu et al., 2000; ICRP, 1991). The relationship between the concentration of 222Rn decay products in units of working level and distance

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Table 2 The average standard deviation (range) values of 222Rn (Bq/m3), 222Rn daughters (mSv/y and WL) and 220Rn (Bq/m3) in Abu-Tartor phosphate mine and other Egyptian phosphate and uranium mine Abu-Tartor phosphate mine
222

Red Sea phosphate mines (131112448)

El Missikat uranium mine

Erediya uranium mine

Rn (Bq/m3)

4187 685 (18015535)

222

Rn daughters mSv/y

WL

26:90 5:70 (0.6981.99) 0:22 0:05 (0.010.67) 6:50 1:48 (1.0016.40)

(1.405.60)

(2.266.22)

220

Rn (Bq/m3)

from the main mechanical ventilation station in the main tunnel, RG3, (sample codes: 1320) is shown in Fig. 3. This relationship shows clearly the eect of ventilation eciency on the concentration of 222Rn daughters and subsequently

Fig. 3. The concentration of 222Rn daughters (WL) in Abu-Tartor phosphate mine tunnels and the distance from the main ventilation station (A).

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on the other airborne radioactivity and worker radiation exposure. This relation does not t to the other locations especially in the side tunnels because of the complex layout of the mine and the dierent ventilation mechanisms. The mean 220 Rn concentration SE was 6:50 1:48 Bq/m3 with a range of 1.0016.40 Bq/m3. The inhalation hazard of 220Rn daughters is almost entirely dependent on the air concentration of only one radionuclide, 212Pb. The concentrations of 222 Rn (Bq/m3), 222Rn daughters (Bq/m3), and 220Rn in units of Bq/m3 inside the mine tunnels are given in Fig. 4. There is an inverse relationship between the concentration of airborne radioactivity in the mine tunnels and the air ventilation. In the side tunnels, only auxiliary fans were used for air ventilation, which are not enough to control the airborne radioactivity within the recommended limit. For this reason, mechanical ventilation is conventionally used as

Fig. 4. Activity concentration of 222Rn (Bq/m3), tance (m) from the ventilation station (A).

222

Rn daughters (WL) and

222

Rn (Bq/m3), and the dis-

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an eective way to control airborne radioactivity and other airborne pollutants in the underground mines (Bigu et al., 2000). The correlations between 222Rn and 222Rn daughters, and 220Rn and 222Rn daughter concentrations are given in Fig. 5, with correlation coecient values of 0.87 and 0.86, respectively.

Fig. 5. The correlations between the concentrations of 222Rn (Bq/m3) and 222 Rn daughters and 220Rn (Bq/m3) in Abu-Tartor mine tunnels.

222

Rn daughters (WL), and

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3.2. Dose assessment The environmental and personal eective dose rate (mSv/y) measured using TLD are shown in Table 3. Forty locations in three sites in the mine were selected for environmental gamma dose rate measurements. The mean environmental eective dose rate was 8.97 mSv/y. Forty-ve workers in ve sites in dierent mining activity areas were selected. The mean value of the workers eective dose rate was 11.66 mSv/y. The maximum values were measured for the mine tunnel workers. The average total eective dose rate (due to 222Rn, 222Rn progeny, and 220Rn progeny) in other Egyptian phosphate mines was 70.2 mSv/y with a range of 12.2136.9 mSv/y. The workers response should be considered, which may be aecting the precision of any survey results in radiation safety and control application (Hussein, 1998). 3.3. Conclusion and recommendations The occupational radiation exposure in the underground conventional mines is one of the major aspects in the Egyptian national program of radiation safety and control. This study, in addition to pervious studies in uranium and phosphate underground mines, implies the urgent need to impose the radiation regulations and standards through improving the working conditions to reduce the occupational radiation exposure to the accepted levels recommended by ICRP-60 and IAEA-Safety series 115. In such working condition, it is a necessity to impose a periodical radiation-monitoring program in order to continuously dene and assess possible radiological problems and to carry out the proper countermeasures. So, we can summarize our conclusion in the following prevention and remedialmeasures and recommendations: ecient ventilation is a must. Job rotation of
Table 3 Environmental and personal eective dose rate (mSv/y) measured in Abu-Tartor phosphate mine tunnels using TLD Mean Worker eective dose rate (mSv/y) Mine worker Mine maintenance worker Ore crushing and transport workers Beneciation factory workers Ore drying and storage workers Average 15.55 10.25 11.34 10.95 10.21 11.66 SE 2.73 0.97 1.03 0.35 0.15 SD 12.20 3.64 1.78 0.79 0.26 Minimum 6.78 5.90 9.83 10.09 9.97 6.78 Maximum 53.52 18.23 13.31 12.11 10.49 53.52 No.a 20 14 3 5 3

Environmental gamma eective dose rate (mSv/y) Mine 8.51 Ore crushing 10.06 Beneciation factory 8.35 Average 8.97 SE, Standard error (1 r); SD, standard deviation. a Number of measurements.

0.60 0.31 0.52

3.36 0.70 1.08

2.19 8.94 6.82 2.19

17.09 10.81 9.07 17.07

31 5 4

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workers is very important to decrease occupational radiation dose. Radiological safety should be considered in conventional mines. Regulations should be issued and applied by the administration of these sites. Radiological follow up should be a routine. Medical follow up system should be applied. Acknowledgements Authors wish to express their deep gratitude to Abu-Tartor phosphate mine project authority and Mr. Walid El-Moafy for their assessment and support during eld measurement activities. References
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