Indian Journal of Pure & Applied Physics Vol. 44, April 2006, pp. 287-291 Assessment of radon-222 concentrations and exhalation rates of rocks and building materials A M El-Arabi, A Abbady, N K Ahmed, R Michel*, A H El-Kamel** & A G E Abbady Physics Department, Faculty of Science Qena, South Valley University, Egypt *Institute of the Radiation Protection and Radioecology, Hanover University, Germany **Physics Department, Faculty of Science, Assiut University, Egypt Received 14 March 2005; revised 22 November 2005; accepted 31 January 2006 One hundred samples were collected from two regions (Bir El-Sid and Wady El-Gemal ) in the Nile Valley. It contain various types of igneous and metamorphic rock samples (acidic dykes, intermediate dykes, basic dykes, serpentinite, metagabbro, menalge). Another set of samples were collected from different regions of Germany. Samples were analyzed and the concentrations in Bq/kg dry weight of radium were determined by gamma-ray spectrometry using hyper-pure germanium (HPGe) detector. A direct method is used to measure 222Rn emanated from the samples, which was analyzed in laboratory using the portable radon monitor Prassi. 222Rn activity concentrations (Bq/m3) were in the range from 36.1± 2 to 96.4 ± 6, 17.8 ± 3 to 73.6 ± 4 and 18.0 ± 2 to 188.1± 15 Bq/m3 for samples collected from Bir Elsid, Wadi El-Gemal and samples from Germany respectively. The corresponding values of exhalation rates were from 0.0012 to 0.004, 0.005 to 0.015 and 0.007 to 0.0069 Bq/gs for these areas respectively. Keywords: Radon, Building materials, Exhalation rates IPC Code: H01J65/08 1 Introduction In the last ten years, there have been many studies aimed at detecting a correlation between the incidence of lung cancer and exposure to radon in dwelling. Some of these have shown positive correlation, but many have not1,2 . The radon exhalation properties of porous materials both naturally occurring like soil and rocks and man-made, like mining wastes and many building materials have been investigated8,9. Most of these studies have been geographical correlation studies. These involve selecting two or more areas, some of high and others of low, and average concentration of radon in dwellings. Although the basic theory of radon exhalation-or release of radon from materials-is the same whether the radon comes from the soil or from a slab of building material some features of the exhalation process are usually very different in the two cases. In the case of exhalation from the soil, one is naturally limited to measure the exhalation from a very small part of the exhaling surface although the sample can be considered to extend indefinitely in the exhalation direction. If the measurements do not change the exhalation process scaling up results obtained for one small area to larger areas is only a question of homogeneity of the soil as far as radioactivity, porosity, permeability etc is concerned. Similar methods have also been applied in the case of building materials10. The greatest fraction of the natural radiation exposure in humans results from inhalation of the short-lived decay products of radon, which occur in the free atmosphere and higher concentrations in the room air of buildings. Radon and its decay products in air are known carcinogens, and a proportion of indoor radon comes from building materials. 2 Experimental Details In the present work, a simple method is used for the measurement of radon-222 in laboratory. The rock and building materials samples were analyzed in the laboratory with the portable radon monitor PRASSI. This monitor is suitable for radon gas continuous or grabs sampling measurements with scintillation cell technique. It consists basically of 1.83 1 cell coated with zinc sulphide activated with silver [ZnS(Ag)] coupled to a low-gain-drift photomultiplier. The sample air is pre-filtered before reaching the measurement chamber and the sampling flow rate is electrically regulated to compensate for filter clog-up. The measurement is performed in a closed loop circuit as shown in Fig. 1. INDIAN J PURE & APPL PHYS, VOL 44, APRIL 2006 288 .... (3) located in the Pan-African basement of Egypt. The area covers about 96 km2 of crystalline basement rocks of Egypt. The second area is Wady El-Gemal located at the Red Sea some 220 km east of Kom Ombo in the Nile Valley. It contains various types of rocks, acidic dykes, intermediate dykes, basic dykes, serpentinite, metagabbro, menalge. Another set of igneous and metamorphic rock samples was collected from different regions of Germany. The PRASSI Mod.5S has a built-in detector suitable for measurements of radon concentrations based on a broadly-accepted technique. It consists of a 1.83-liter cell coated with zinc-sulphide activated with silver ZnS(Ag) coupled with a low-gain-drift photomultiplier. The cell characteristics provide the detection of very low radon concentration levels in the sampled air. The instrument has two operating modes: continuous and grab sampling. In the continuous mode, air is allowed to circulate in the measuring cell at a constant rate, electronically regulated to 3 L/min. PRASSI measures the counts in a preset time and at preset intervals, from which the radon concentration in Bq/m3 or pCi/l is then determined. A key feature of the PRASSI is the ability to compensate for the count rate due to radon daughters adherent to the cell walls. The resulting count rate is, therefore, strictly proportional to the concentration of radon gas only. In the grab sampling mode, air is flushed into the measuring cell for some minutes, which is then closed by two electric valves. After a preset time (normally 2.5 h), repeated counting periods had been performed with the sampled air. This method confers very high sensitivity to the system, which turns out to be extremely useful in particular applications, such as measurements of radon in solids or rocks performed with suitable probes or measurements of radon in water with the aid of suitable de-gassing devices. where R is the activity concentration in (Bq/m3), c is the exhalation rate in (Bq /gs), λ is the decay constant in (= 2.1 × 10-6 s-1) and Vd is the dead-space volume (= 0.00075 m3) It follows, however from the theory and it has been documented experimentally9 that c will decrease as N increases because of back diffusion. The decrease in c depends upon the properties of the material and upon the ratio of the sample volume to the dead space volume. One hundred samples were collected from two regions. The first is the Bir El-Sid area, which is 3 Results and Discussion Fifty-four samples from different rock types were collected from Wadi El-Gemal area as follows: 16 dyke, 22 ophiolit (Serpintinite, Metagabbro, Menalge), 10 granite and 6 amphibolites rocks. From radon concentration, results measured by PRASSI, the exhalation rates (Bq.g-1s-1) can be calculated for acid, intermediate and basic dyke rocks from Wadi ElGemal. The minimum value 22±8.1 found in basic dykes where the maximum value 141.2±2.7 was found in the acid dykes. The average values of radon222 activity concentration in acid, intermediate and Fig. 1— Samples measurement set-up The exhalations of radon from the samples were determined by studying the growth of radon activity in the bottle containing the samples of materials. Let us consider a sample with the volume Vb enclosed in a container with a deadspace volume Vd . If the total exhalation rate (number of atoms per unit time) of the sample is c, the radon concentration (number of atoms per unit volume) N will grow with the time t according to the equation dN / dt = ( c / Vd) - λ N ... (1) In Eq. (1), it is assumed that radon atoms are removed from the container only by radioactive decay. If furthermore, c is assumed to be constant and independent of N (free exhalation rate). Equation (1) has the solution: N = (c / λ Vd) (1 - e -λt ) ... (2) or, expressed as activity (concentration). R = (c / Vd) ( 1 - e -λt ) ARABI et al.: ASSESSMENT OF RADON-222 CONCENTRATIONS basic dykes (Bq.m-3) are 75.5 ± 5.4, 349.2± 3.8 and 28.1 ± 5.7, respectively. In ophiolit rocks it was found that the minimum value 10.8 ± 3.6 in serpintinite where the maximum value 59.4 ± 5.4 in the menalge. The average values of radon-222 activity concentration (Bq.m-3) in serpintinite, metagabbro and menalge are 21.2±3, 28.2±2.6 and 45.6± 6.2, respectively. The values of radon concentration level (Bq.m-3) for granite rocks vary from 39.7±2.8 to 89±5.5 with average 73.6±4.2. The corresponding values of amphipolite were 10.8±3.6 to 32.3±3.7 with average value 17.8±3.1. The highest values of radon concentration were found in acid and granite rocks, while the lowest value was found in amphipolite rocks. The variation of concentration value of radon and exhalation rates from 17.8±3.1 to 75.5±5.4 (Bq.m-3) and 0.0005 to 0.0027 Bq.g-1s-1 in all samples rocks in Wadi El-Gemal as presented in Table 1. The measured concentration and exhalation rate of radon in rocks collected from Bir El-Sid area are shown in Table 2. In dyke rocks, the minimum values 24.8±1.4 Bq.m-3, 0.0008 Bq.g-1s-1 found in dolerite, while the maximum values 87.1±2.1 Bq.m-3, .0032 Bq.g-1s-1are found in felsite with mean values 28.9±2.9, 36.1±2, 63.7±4.3 and 57.3±3.7 (Bq.m-3) for dolerite, diorite, lamprophyre and felsite respectively. As a Table 1—Mean activity concentration and exhalation rates of Rn222 in different rocks from Wadi El-Gemal area Rn-222 Exhalation rate Type of rock Bq m Bq.g-1s-1 granite serpentinite meragabbro menalge acid dyke interm. dyke basic dyke amphibolite 73.6 ±4.2 21.2 ±3 28.2 ±2.6 45.6 ±6.2 75.5±5.4 49.2±3.8 28.1±5.7 17.8 ±3.1 0.0025 0.0007 0.0009 0.0016 0.0027 0.0018 0.0010 0.0005 -3 Table 2—Mean activity concentration and exhalation rate of Rn222 in different rocks from Bir El-Sid area 289 general trend, the low values are found in dolerite and the highest values are found in felsite, which are due to the variation of these radium content. For Fawakher granitioide, the minimum values 32.8±4.5 Bq.m-3, 0.0015 Bq/gs found in quartz diorite, while the maximum values 113±18.4 Bq.m-3, 0.0052 Bq.g-1s-1 are found in granite. The average values of radon-222 activity concentration (Bq.m-3) in quartz diorite, granodiorite and granite are 33.5±3.7, 72.8±2 and, 96.4±6.6 respectively. In serpentinite the minimum and maximum values of radon are 25.6±2.2, 50.4±5.8 (Bq.m-3) with mean value of 40.7±3.2. The average values of radon concentration varied from 28.9±2.9 to 96.4±6.6 and exhalation rates from 0.0012 to 0.0040. As a general trend, the low values are found in dolerite and the highest values are found in granite, which are due to the variation of their radium content. The last series of experiments have been carried out to measure the concentration of radon and exhalation rates of some type rock and building materials in Germany, the mean calculated values are given in Table 3. Minimum concentrations of radon were 18±1.9 (Bq.m-3) for amphibolites and maximum value were 188.4±15 (Bq.m-3) for granite group. Also the minimum exhalation rates of radon were 0.0007 for amphibolites and the maximum values were 00.0069 for granite rocks. The classifications and coding legends of the building material samples in Table 4 denote to: G1 (granite type Rosa point from Spain), G2 (Silver Cloud from North-America), G3 ( Rojo Sevilla from Venezuela), G4 (Bianco Cistal from Spain), G5 (Indian Stars Galaxy), G6 (Giallo California. from Brazil ), G7 (Kashmir White from India), RB (Red Brick from Hannover), Ce (Portland Cement from Hanover) and GV (Gravel from Hanover). These samples are used as building materials in Germany. Table 3—Radon activity concentration and exhalation rate in rocks from different areas. Germany using PRASSI Type of rock Rn-222 Bq m-3 Exhalation rate Bq.g-1s-1 Type of rock Rn-222 concentration Bq m-3 Exhalation Bq.g-1s-1 felsite lamprophyer diorite dolerite granite q-diorite granodiorite serpintinite 57.3±3.7 63.7±4.3 36.1±2 28.9±2.9 96.4±6.6 33.5±3.7 72.8±2 40.7±3.2 0.0024 0.0030 0.0024 0.0012 0.0040 0.0012 0.0031 0.0017 granite serpentinite metagabbro acid dyke lamprophyer diorite dolerite amphibolite 188.1±15 25.1±6.2 54.4±2.9 84±8.2 102 ± 8.6 39.8±3.1 40.5±3.2 18±1.9 0.0069 0.0010 0.0018 0.0032 0.0045 0.0014 0.0013 0.0007 INDIAN J PURE & APPL PHYS, VOL 44, APRIL 2006 290 Table 4—Radon-222 activity concentration and exhalation rate for selected building materials used in Hanover City, Germany using PRASSI Sample Type Rn-222 Bq m-3 Exhalation rate Bq.g-1s-1 G1 G2 G3 G4 G5 G6 G7 RB Ce GV 203.7±33.1 175.2±14.2 250±16 238.5±7.9 92.1±8.1 234.8±59.5 212.7±8.3 82.8±4.2 65.4±11.6 56 ±7 0.0007 0.0008 0.0011 0.0006 0.0002 0.0006 0.0006 0.0003 0.0002 0.0002 The values of radon concentration level (Bq.m-3) in building materials were from minimum value 24±5.2 measured in sand to maximum value 250±16 measured in granite. Except granite rocks, it is evident that sand as building material has the lowest value of concentration and exhalation compared with red bricks, which has the highest values. Building materials have internal properties that affect the recoil, transport and exhalation of radon in a complex manner12. These intrinsic properties of materials include radium content and its distribution within the material size of the mineral grains that compose the material size distribution, configuration of the pore Fig.2⎯Mean activity concentration (Bq/m3) and exhalation rates (Bq/gs) in the areas under consideration ARABI et al.: ASSESSMENT OF RADON-222 CONCENTRATIONS 291 Table 5—Average values of radon activity concentration (Bq.m-3) and radon exhalation rates (Bq/gs) for different rock types in the areas under investigation Type of rock granite serpentinite metagabbro acid dyke lamprophyer diorite dolerite amphibolite Bir El-Sid Exh. (Bq.g-1s-1) Con. (Bq.m-3) 96.4±6.6 0.0040 40.7±3.2 0.0017 …….. ……. 57.3±3.7 0.0024 63.7±4.3 0.0030 36.1±2 0.0024 28.9±2.9 0.0012 ……. ……. Wadi El-Gemal Con. (Bq.m-3) Exh. (Bq.g-1s-1) 73.6 ±4.2 0.0025 21.2 ±3 0.0007 28.2 ±2.6 0.0009 75.5±5.4 0.0027 49.2±3.8 0.0018 ……. ……. 28.1±5.7 0.0010 17.8 ±3.1 0.0005 system and the composition of the fluid within the pores. The complex interaction of these properties is that a building material may have a high radium content and a high porosity but may have a low exhalation of radon due to a predominance of small pores and a low probability of radon entrainment because of the absence of water in the pores. A summary of the average values of radon concentration (Bq.m-3) and exhalation (Bq.g-1s-1) from the rocks of different regions are presented in Table 5. These values are shown in Fig. 2. Considering the values of maximum and minimum, it can be noticed that these are corresponding to maximum and minimum values of radium content. Comparing between the results of different regions, it is evident that the samples of granite and acid dyke rocks show the maximum values of concentration and exhalation rate, while the values of basic dykes and amphibolites are the minimum. A result, which can be accepted owing to the correlation between Rn-222 and Ra-226. Information on the rock types and distribution of lithologic units and other geological features are of primary importance in radon assessment. Lithological and mineralogical descriptions not only indicate the possible uranium content but also aid in the predication of general radon emanation. For instance rock types with natural high uranium are most likely to cause indoor radon problems. 4 Conclusions The samples of granite and acid dyke rock show the maximum values of concentration and exhalation rates of radon. While the minimum values are due to basic dykes and amphibolites. The radon level (Bq.m-3) in building materials was from minimum 24±5.2 for sand to maximum value 250±16 for granite. Except for granite rocks, it is evident that sand has the lowest values of content compared with Germany Con. (Bq.m-3) Exh. (Bq.g-1s-1) 188.1±15 0.0069 25.1±6.2 0.0010 54.4±2.9 0.0018 84±8.2 0.0032 102 ± 8.6 0.0045 39.8±3.1 0.0014 40.5±3.2 0.0013 18±1.9 0.0007 red bricks. Other factors which could influence significantly radon indoors are certain natural building materials, as has been gamma absorbed dose rates in air and radon concentration13. In future, the number of measurements in high radon areas will be increased and detailed studies on radon sources, entry pathways, etc., will be performed. In this context, the involvement of laboratories at district level is particularly important. References 1 2 3 4 5 6 7 8 9 10 11 12 13 Samet J M, J Nat Cancer Inst, 81 (1989) 745. Stidlely C A & Samet J M, Health Phys, 65 (3) (1993) 234. 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