Pergamon

Atmospheric Environment Vol. 29, No. 23, pp. 3433-3439, 1995 Copyright 1995 ElsevierScience Ltd Printed in Great Britain. All rights reserved 1352-2310/95 $9.50 + 0.00

1352-2310 (95)00204-9

RADON AND RADON PROGENY OUTDOORS IN A VALLEY OF ENHANCED NATURAL RADIOACTIVITY DOBROMIR S. PRESSYANOV
Departmem of Atomic Physics, Faculty of Physics, Sofia University, 5 James Bourchier Blvd., Sofia BG-1126, Bulgaria

METHODY G. GUELEV
Institute of Nuclear Research and Nuclear Energy, Bulgarian Academy of Sciences, Sofia BG-1784, Bulgaria

and BORISLAV G. SHARKOV

Eleshnitsa BG-2782, Bulgaria (First received 8 April 1994 and in final form 2 April 1995) Abstract--Results of a pilot study of 222Rn and 222Rn progeny outdoors and indoors in a valley of enhanced radioactivity, affected by uranium mining and millinghave been summarized.Diurnal and spatial variations have been followed, and 222Rnconcentrations in soil-gas have been determined. High outdoor concentrations of radon progeny during nights and at early mornings have been observed under the conditions of high air stagnation. The indoor concentrations were greater than the outdoor ones, however in most of the studied houses, the contribution of outdoor radon to the total exposure was found to be dominating. The cumulative exposure (for over 90% of the inhabitants) due to outdoor radon was estimated to be about 0.9 WLM per annum. These results reveal that lung-cancer risk excess by about 80% could be attributed to outdoor radon, provided that one assumes the risk coefficients(the cancer risk per unit of exposure) determined for occupational exposures. The study of different radon sources suggests that except for the uranium mining and milling,the generallyenhanced natural radioactivity and meteorological conditions in this valley are of substantial importance. Valleys, such as the questioned one, may give an opportunity to check up the hypothesis about the existenceof health effects at low doses of 222Rnprogeny exposure. Key word index: Radon, risk assessment, outdoor air, uranium mining.

1. INTRODUCTION Since the inhalation of' 2 2 2 R n progeny has been recognized as being the major radiation hazard, the emphasis has always been put on radon indoors which is believed to contribute', to most of the exposure. The weighted average concentration of indoor radon, for the population, was tound to be about 40 Bqm -3, versus about 10 Bqra -3 outdoors, in continental areas (UNSCEAR, 1993). However, high outdoor 222Rn concentrations at sites of enhanced natural radioactivity and/or frequent air stagnation have been observed recently (Kobal et al., 1988; Krizman and Stegnar, 1992; Robe et al., 1992). In addition, recent reports suggest that higher outdoor 222Rn concentrations could be detected over large areas in dry seasons (Grasty, 1994), or at sites of raised levels of 222Rn in soil-gas (Price et al., 1!994).

In Bulgaria, high concentrations of 222Rn outdoors were observed in the village of Eleshnitsa (Dimitrov et al., 1990; Uzunov et al., 1992). This village (population about 2600) is located in a valley surrounded by sandstone hills (Fig. 1) where the natural ventilation is poor and thermal inversions occur frequently. The valley has been a center of uranium mining and milling industries since 1956, but most of the activities have now ceased. Large areas are contaminated with wastes from uranium mining (the milling tailing is outside the valley and about 2.5 km away from the village). The region, as a whole, exhibits enhanced radioactivity associated with natural uranium (Nikolov et al., 1993; Redmet Ltd., 1959). There are no sources of other industrial air pollutants in this valley. In this report we summarized the results from a pilot study of 222Rn and 222Rn progeny (i.e. 21gpo, 21*pb and 214Bi + 214po) outdoors and indoors. The

3433

3434

D.S. PRESSYANOV et al+

ELESHNITSA

PART B

"%.'..1" QUA,,,

Fig. 1. The valley of Eleshnitsa.The areas are marked as follows: i~--uraniummining wastes; 8--areas of natural radioactive anomalies; - - a point of outdoor measurement.

concentrations of 222Rn in soil-gas were determined, as well, in order to rank the sources of 222Rn exhalation (with the emphasis put on the uranium mining wastes and natural radioactive anomalies existing in this area). The exposure due only to outdoor sources of 222Rn was found to be 0.9 WLM per annum. For a considerable number of the inhabitants, the contribution of outdoor radon to the total exposure seems to be of primary importance. This was indicated as by indoor measurements, so indirectly due to the low concentrations of Z2ZRnin the soil-gas of the soil lying under the village. The results suggest that in areas of higher natural radioactivity and frequent air stagnation, raised levels of outdoor radon could be expected. This circumstance should be taken into consideration when planning the mining and milling of radioactive ores or waste disposing. Such sites may give also an additional possibility to check the non-threshold hypothesis of radiation-induced carcinogenesis.

2. PROCEDURES

2.1. Grab sampling of ZZ2Rn progeny The basic method used for z22Rn progeny measurements was that of Kritidis et al. 0977). A proportion of the measurements were made through the express method of Markov et al. (1962). Both of the methods employ air sampling with the aerosol filter and consequent gross ~-counting of the filter at three (Kritidis) or two (Markov) time intervals. The methods provide a set of equations for determining the activity concentrations of 222Rn progeny and the potential alpha energy concentration (PAEC). The equilibrium factors (F) were determined by radon progeny concentrations, while assuming an equilibrium between Z22Rnand zlSPo. About 400 grab samplings were taken in 1992-1994 in different seasons, and at random moments of the day and night. Such measurements,too, were made indoors, in randomly selected dwellings. 2.2. lnteorated measurements of 222Rn The 2ZZRnconcentrations in soil-gas were determined by means of integrated measurements. Filter-covered plastic boxes ( ~ 8 x 10 cm) were used, with passive detectors placed

Radon and radon progeny outdoors inside. Two types of detectors were used: solid state nuclear track detectors (LR-115 type II, film Kodak-Pathe*), and thermoluminescent detectors (TLDs)-- O 5 x 0.8 nun dishes containing CaSO4:Dy + 5% B4C.I" The B4C additive reduces the detectors' fl and ), sensitivity significantly and makes them useful for registration of u-particles.Two sets of TLDs were used--the detectors of the first one were open, and those of the second one were covered with a 20 mg cm- 2 plastic absorber. The difference between the two signals was ascribed to ~t-particles. The plastic boxes were buried at a depth of 60 cm and left there for a controlled time. Integrated measurements of 222Rnin the ambient air were performed by filter-covered plastic cups ( ~ 6 x 5 cm), with the LR-115 type II detector attached to the inside bottom of the cup. These cups were placed at heights 1.5-2 m above the ground, for about a month. The calibration was performed on a 2 m3 radon box at the National Center of Metrology, where a steady Z22Rnconcentration (2.4 104 Bq m-3) was maintained.
160-oa '~--- 1 2 0 +

3435

+~.'~

18

20

22

Time (h) Fig. 2. Typical trend of activity concentrations of 222Rndaughters in late afternoons and nights. (o) 21Spo, ( q - ) 214pb; ( A ) 2t4Bi.

3. RESULTS AND DISCUSSION

5oo0r 400~
30~

3.1. Diurnal variation The values of PAEC showed a deviation from the background levels ( < 200 M e V f - 1 ) reaching about 14,000 MeV E- 1. An increase of the 222Rn progeny concentrations was observed in late evenings and nights. It usually started after the slow local winds subsided. This occurs frequently in the evenings in this area. This process is presented in Fig. 2. As seen, two stages can be distinguished. In the beginning, the radon progeny concentrations increase rapidly (in 2-3 h). At the second stage, a relative stabilization takes place, usually until 8 - 1 0 h a.m. Under stabilization, the radon progeny equilibrium is full (F = 1.0), while for the rest of the day and night the average equilibrium factor is about F = 0.8, in agreement with other estimations of F outdoors (UNSCEAR, 1993). The averaged diurnal distribution (based on about 400 measurements made in 1992-1994) is presented in Fig. 3. The time interval of higher concentrations is 22-10 h, which is typical of daily variations of radon and radon progeny (Gesell, 1983). In the present case, however, the average PAEC varies for the day and night by a factor of 13. The arithmetically averaged PAEC was found to be about 2300 MeV E-~ (or 17.7 mWL, where the working level {WL) is the traditional PAEC unit; l W L - - 1 . 3 x l 0 sMeV~'-1, exposure to 1WL for 170 h is defined as a WLM). The PAEC values averaged for 3 months were strongly related to the seasonal humidity--the highest PAEC (3200 M e V f - 1 ) found in the dry autumn of 1993 and the lowest one [1600 M e V f - 1) in the wet winter of 1994. The resultant annual exposure, due to the outdoor radon progeny, was found to be about 0.9 WLM.

L)
2~

I000
0 2 4 6 8 10 12 14 16 18 20 22 24

Time (h) Fig. 3. Daily variation of the potential alpha energy concentration (PAEC) of radon decay products outdoors in the village.

3.2. Spatial distribution of 222Rn and 222Rn progeny The horizontal variations of 222Rn and 222Rn progeny were investigated by integrated measurements at 14 randomly selected points over the village area (Fig. 1), and by instantaneous measurements made quickly through the express method of Markov et al. (1962). The living area was subdivided into two parts (Fig. 1). Part A consists of the actual village areas, where over 90% of the population live. Part B has been recently populated. Results from the integrated measurements in part A showed a uniform distribution of 222Rn concentrations (all the results differing from the average value by _+ 30% and without visible systematic prevalence in some parts of this area). Fast radon progeny measurements confirmed this, too, as the PAEC values differed by the factor of 2, but no systematic prevalence in a given region of part A was observed. The results found for this part have not showed visible differences in periods of active mining (ventilation works), and when the mining and mine ventilation are stopped for a long time. The results found for part B do not differ from those for part A when the mining is stopped. However,

*Kodak-Pathe LR-115, type-II film, 8-6 Rue Viilot, 75594 Paris, France. ~"Protecta Partnership, 105-125 Maria-Louisa Blvd.,Sofia 1202, Bulgaria.

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D.S. PRESSYANOV et al. indicate a much higher radon supply potential of these sites. The highest concentrations were observed with the natural surface radioactive anomalies, which were found in a considerable area near the village (Fig. 1), and at places at longer distances. For the industrial wastes, the radon potential of uranium mill tailing (area: 0.42 km 2) was the highest. However, it is relatively far (2.5 km) from the village, and, under a normal operation, most of its surface is covered with a water layer, which considerably reduces the release of radon. The mining wastes (total area 0.2 km 2) have higher 222Rn concentrations in the soil-gas, as compared with those found in not contaminated and anomaly free areas, but as an average, they are considerably lower than those which are found with natural anomalies. For the wastes near by the village, the highest concentrations were found at the quarry (up to 300kBqm-3). The radon concentrations in the sandstone hills which surround the valley, were also considerably higher than those in the village soil or in the lands outside the valley. 3.5. Sources of 222Rn outdoors The possible sources of 222Rn in the valley are: (1) Radon exhalation from contaminated and not contaminated areas. (2) Exhaust air from mine ventilation. (3) Natural exchange of air between open mine adits and pits. The lack of information on 222Rn in the ambient air in the valley, before the development of uranium mining (i.e. before 1956), is the main problem of assessing the real contribution of uranium industry to the high outdoor levels of radon in the village. The main, recognized single source of radon in the valley was the central ventilation of the mines. It releases ( 0 . 3 - 1 ) x l 0 7 B q s -1 222Rn in the atmosphere (radon-supply rate = radon concentration x air flow rate). About half of this amount is emitted near the village (the pentacle on Fig. 1). Therefore, in preliminary investigations (Dimitrov et al., 1990), the mines' ventilation was considered to be the most important cause for the higher concentrations of 222Rn outdoors. However, about 100 measurements were made in 1992, in periods when the central ventilation

when mine ventilation works, the time integrated concentrations are up to 3 times higher at the points closer to the ventilation exhaust, and by about 50-70% in the center of this part (Fig. 1). 3.3. Indoor pro#eny concentrations of 222Rn and 222Rn

Indoor measurements were performed only in order to indicate if there is a major problem with indoor radon in this village. Integrated measurements of 222Rn indoors were made in 12 dwellings randomly selected over the whole village area. The results for 11 of the houses revealed radon concentrations which were less than 50% over the outdoor ones. In one house, the indoor 222Rn concentration was by 80% higher than the outdoor one. Instantaneous grab sampling measurements were made under normal and under specially arranged conditions (doors and windows kept closed for a long time). They, too, had not revealed extremely high indoor concentrations in most of the cases. However, some exceptions were observed. The first was the kitchen in one of the houses, where mining wastes had been added to the building materials. The integrated indoor radon concentration in this kitchen, in the heating season, was twice higher than the outdoor one. In other rooms of this same house (where the family usually spend the time 22-8 h), the values of this concentration were by 20-30% higher than the outdoor concentration value. In three dwellings (one now inhabited), when the doors and windows were kept closed for more than 3 h, the indoor concentrations were higher than those outdoors by 200-500 Bq m - 3 when measured at one and the same time. Two of these dwellings showed signs of use of radioactive wastes as building materials and the third was in contact with a sandstone material of enhanced radioactivity. 3.4. 222Rn in soil-gas The concentrations of 222Rn in soil-gas are summarized in Table 1. The background concentrations (outside the valley) were 3-5.5 kBq m - 3. The underlying soil in the village is also of a relatively low 222Rn concentration in the soil-gas. The values found for natural radioactive anomalies, mining and milling wastes, and sandstone hills surrounding the valley,

Table 1. Concentrations of 222Rn in soil gas 222Rn concentration (kBq m- 3) Place Background - - away from the valley Soil in the village Surrounding hills Natural radioactive anomalies Mine wastes (incl. quarries) Mill tailing Range 3-5.5 3-9 25-90 45-1400 16-460 150-650 Average 4 7 50 400 160 300

Radon and radon progeny outdoors system of the active mines had been stopped for a long time, but no visible differences in the results for part A of the village were observed (the average registered PAEC was also about 2300 MeV d- t). This was confirmed also by a number of measurements made in weekends, when the central ventilation was usually stopped. Hence, the impact of the ventilation exhaust could be excluded as dominating for the village as a whole. It is significant for a little proportion of the population living in the "new" part B. The old, mine adits near the village were not recognized to supply large amounts of 222Rn by natural air exchange ( < 104 Bq s-1). Greater is the supply by large adits in the technological area (near the ventilation exhaust), mainJ[y by two of them, where a radon supply as high as 1.5 x 10s Bq s- 1 has been measured (under the conditions of maximum air exchange). In the vicinity of these adits, the radon and radon progeny concentrations are above the natural ones (far away, but in the, same valley), usually at distances of 50-100 m. However, for one of them, which enters a narrow furrow, so that the fast horizontal dispersion is embarrassed, under the conditions of air stagnation, an influence has been observed at a distance of 400-500 m. In either case, while these adits are disposed at similar or longer distances than the ventilation exhaust, and while even under maximum air exchange they supply 5-10% of radon delivered by ventilation, their impact is unlikely to be dominant at long distances. Among the sources of 222Rn exhalation, the natural radioactive anomal:ies are probably of primary importance. The mining and milling wastes are serious sources, but based on the measured 222Rn concentrations in the soil-gas and in the area of contaminated sites (0.2 km 2 mining and 0.42 km 2 milling wastes), they are unlikely to release more radon in the atmosphere than the anomalies, and the sandstone hills which surround the valley (Fig. 1). The soil underlying the village is of much lower concentrations of 222Rn in soil-gas and its contribution to the outdoor concentrations is assumed as negligible. The norraal (in comparison with the surrounding hills) radioactivity of the soil at the bottom of the valley, was cc)nfirmed also by gamma spectrometry of soil samples (Nikolov et al., 1993) and by a relatively constant gamma background in the village (19.3 + 2.3 #R h-1), as found in long-term measurements (Nikolov et al., 1993) by TLDs (Guelev et al., 1994). As a result of this, the radon-entry rate from soil to houses is expected to be low, which could explain the minimum excess of indoor concentrations above those outdoors, for part of the studied houses. In general, it is difficult to attribute the high outdoor 222Rn concentrations to a single source, It seems that uranium industry and its wastes are an important, though not the only factor that makes the radon problem in this village. The enhanced radioactivity of the region, and the, meteorological conditions, are of substantial importance. Therefore, searching for

3437

222Rn sources and clarifying the air-transport mechanisms become a complex task necessitating further experimental investigations and mathematical modelling. In either case, one could conclude that when planning radioactive-ore mining, milling or waste disposing in sites of frequent thermal inversions/air stagnation, a considerably stronger impact of the radon released in the air, on people's health, should be expected and taken into consideration. At present, isolating all the mine adits and pits, and removal/restoration of the contaminated areas is recommended by experts (Nikolov et al., 1993; Tzenov et al., 1994) and should be carried out by governmental authorities. They comprise the main proportion of the plan for liquidation of the uranium industry in this valley, which is expected to be performed within about ten years. Thus, by "turning off" the different sources, it could be possible to assess "a posteriori" the real impact of uranium industry on radon outdoors. We do, however, anticipate, that even after completing this program, the levels of 222Rn outdoors will remain relatively higher than those which are normally reported for outdoor air. 3.6. Risk due to 222Rn progeny exposure The annual exposure to 222Rn from outdoor sources was found to be about 0.9 WLM, for more than 90% of the inhabitants (part A). For a proportion of persons living in part B it was higher, depending on mining activities. Assuming, in accordance with ICRP (1993), that the risk coefficient is 3 x 10-4 WLM -1, the risk of lung cancer in part A, which is due to 222Rn outdoors was found to be 2.7 x l0 -4 per annum. The lung-cancer risk for the whole population of Bulgaria is 3.5 x 10 -4 per annum (NOC, 1994). Thus, the basic risk for the population living in part A of the village, is expected to be higher by about 80% due to 222Rn outdoors. This is the minimum level of the risk, i.e. if taking the indoor exposure into consideration, the real risk will be higher. A long-term survey of radon indoors in a large number of houses is necessary in order to reveal the detailed distribution of the exposures. At present, this program is limited by administrative and financial factors. The preliminary results, however, suggest, that the number of inhabitants, for which the main fraction of the exposure is due to outdoor radon, could be significant. The risk excess assessment made after BEIR IV (1988) is similar--for adults above 50 yr of age, the relative risk excess reaches 70-80% (only about 8% of the lung-cancer cases in Bulgaria are diagnosticated before the age of 50 yr (NOC, 1994)). If we assume a multiplicative effect of radon exposure and smoking (suggested in recent studies (Pershagen et al., 1994)), the above relative risk (which is related to not exposed persons of the same smoking habits) could be applied to smokers and non-smokers. However, the number of affected smokers will be much bigger, due to the higher absolute risk for them (Maillie et al., 1994).

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D.S. PRESSYANOV et al. Sites of high outdoor radon concentrations could possibly be found in many countries. Just like the present one, they may become important sources of information regarding the health impact of low doses of inhaled radon progeny.
Acknowledgements--This work was supported in part under

The above risk coefficients were obtained for the case of much higher occupational exposures. However, they are commonly used, due to the lack of conclusive information regarding low radon exposures. At present, many epidemiological studies of populations exposed to environmental radon have been carried out, or are in progress (Neuberger, 1992). Some of them report on positive trends (Pershagen, 1994). Others are inconclusive or even report on a negative correlation (Neuberger et al., 1992; Cohen and Colditz, 1994). The current strategy of the radiation protection is based on the linear non-threshold hypothesis of radiation carcinogenesis. In the recent ICRP Publication 65 (1993), an action level which corresponds to 0.88 WLM of the annual exposure to radon progeny, is proposed. As this limit is going to be adopted in the legislations of a number of countries, the test of the risk hypothesis, for the corresponding values, could be of substantial importance. It is our opinion that populations in valleys like the one considered here, are very suitable for such investigations. The main reasons are: (1) Large populations are exposed to outdoor radon and radon progeny near and above the currently recommended levels of intervention. The persons for which the main part of exposure is due to the outdoor sources can be considered as a group, exposed in approximately equal conditions for a long time. (2) Due to the radon and radon progeny equilibrium, the results of the long-time integrated measurements of radon could be directly converted into radon progeny exposure. The situation for indoor studies is much more complicated, and this results in great biases in the estimations. (3) The risk is within limits where it could be estimated quantitatively in epidemiological studies. In fact, the relative risk, expected in the present case (even if account only the outdoor radon) is comparable with the risks observed in the Swedish study (Pershagen et al., 1994).

Contracts 1560/1993 of the Institute of Nuclear Research and Nuclear Energy, and 19/1993 of "Georedmet" Ltd. We are grateful to P. Nikolov, Tz. Tzenov, M. Zlatkova, A. Kuzmanov and G. Varadinov for the help in the field work, to M. Dimitrov and P. Kritidis for valuable comments and suggestions, to L. Minev and P. Uzunov for helpful discussions.

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Cohen B. L. and Colditz G. A. (1994) Tests of the hnear-no threshold theory for lung cancer induced by exposure to radon. Envir. Res. 64, 65-89. Committee on the Biological Effects of Ionizing Radiation (1988) Health Risks of Radon and Other Internally Deposited Alpha Emitters, BEIR IV. National Academy Press, Washington D.C. Dimitrov M., Tosev I. and Pressyanov D. (1990) An estimation of air-contamination with radon and radon progeny in some regions of the country. In Proc. 12th Colloquium Physics in the Human and Environmental Safety, pp. 135-138 (in Bulgarian). Gesell T. F. (1983) Background atmospheric 222Rnconcentrations outdoors and indoors: a review. Health Phys. 45, 289-302. Grasty R. L. (1994) Summer outdoor radon variations in Canada and their relation to soil moisture. Health Phys. 66, 185-193. Guelev M. G., Mischev I. T., Burgkhardt B. and Piesch E. (1994) A two-element CaSO4:Dy dosemeter for environmental monitoring. Radiat. Prot. Dosim. 51, 35-40. International Commission of Radiological Protection (1993)
Protection Against Radon-222 at Home and at Work. ICRP Publication, Pergamon Press, Oxford, No. 65; Ann. ICRP 23.

4. CONCLUSION High concentrations of 222Rn and 222Rn progeny outdoors were measured in a valley affected by uranium mining and milling. However, the results suggest that except for the uranium industry and its wastes, the generally enhanced radioactivity and poor air circulation are of substantial importance. The intervals of extremely high values correspond to times of air stagnation. Therefore, the radon sources placed in areas of poor natural ventilation could be expected to have a greater health impact on the population in such sites. Probably, the populated valleys (or hollows) of frequent air stagnation should be avoided, or taken a special care of, when planning radioactive-ore mining and milling or waste disposing.

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Radon and radon progeny outdoors E., Radicheva M. and Penev I. (1993) Research on a biological restoration of technologically contaminated areas: MDP "Drouzba'-Eleshnitsa. Institute of Nuclear Research and Nuclear Energy, Contract No. 1560/1993, Final Report to the Bulgarian Ministry of Environment (in Bulgarian). Pershagen G., Akerblom G., Axelson O., Clavensjo B., Damber L., Desai G., Enflo A., Lagarde F., MeUander H., Svartengren M. and Swedjemark G. A. (1994) Residential radon exposure and lung cancer in Sweden. New Engl. J. Med 330, 159-164. Price J. G., Rigby J. G., Christensen L., Hess R., La Pointe D. D., Ramelli A. R., Desilets M., Hopper R. D., Kluesner T. and Marshall S. (1994) Radon in outdoor air in Nevada. Health Phys. 66, 431;-438. Redmet Ltd. (1959) Results of geological and geophysical survey in the west Rhodops, in regions "Eleshnitsa", "Selishte" and "Dospat" conducted in 1959. Final Report

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deposited in the archives of Redmet Ltd. (in Bulgarian). Robe M. C., Rannou A, and Le Bronec J. (1992) Radon measurement in the environment in France. Radiat. Prot. Dosim. 45, 455-457. Tzenov T., Pressyanov D., Zlatkova M. and Kuzmanov A. (1994) Radioecological investigation and prognosis of MDP "Drouzba'. Georedmet Ltd., Contract No. 19/23.09.1993, Final Report to the Bulgarian Ministry of Energy (in Bulgarian). UNSCEAR (1993) Sources, effects and risks of ionizing radiation. United Nations Scientific Committee on the Effects of Atomic Radiation, 1993 Report to the General Assembly, with annexes. United Nations Publications, New York. Uzunov I., Dimitrov M. and Steinhausler F. (1992) Environmental radiation levels and occupational exposure due to uranium mining and milling operations in Bulgaria. Radiat. Prot. Dosim. 45, 141-143.