The Science of the Total Environment 272 2001.

85 89

Radon permeability and radon exhalation of building materials

G. Keller U , B. Hoffmann, T. Feigenspan
Institute of Biophysics, Uni ersitaetskliniken, Uni ersity of Saarland, Building 76, Homburg 66421, Germany

Abstract High radon concentrations indoors usually depend on the possibilities of radon penetration from the surrounding soil into the buildings. Radon concentrations in dwellings up to 100 kBqrm3 were found in some special regions i.e. SchneebergrSaxony, UmhausenrTyrol., where the soil shows a high uranium content and additionally, a fast radon transport in the soil is possible. To reduce the radon exposure of the inhabitants in these radon prone areas it is necessary to look for building and insulating materials with low radon permeability. We examined several building materials, like cements, concretes and bricks of different constitutions for their diffusion coefcients and their exhalation rates. The insulating materials, like foils and bitumen were tested also on their radon tightness. The measurements were performed with an online radon measuring device, using electrostatic deposition of 218 Po ions onto a surface barrier detector and subsequent alpha spectroscopy. The mean diffusion lengths for the investigated building materials range from lower than 0.7 mm i.e. for plastic foil., up to 1.1 m for gypsum. The diffusion length R was calculated from the diffusion coefcient D with R s Dr . If the thickness of the material is more than 3 times the diffusion length, then it is called radon-tight. The mean 222 Rn exhalation rates for the building materials varied between 0.05 and 0.4 mBqrm2 s. The samples were investigated as stones, plates, blocks, foils, coatings, powders etc., no statement can be made about working at the construction site of a building. Also the fabrication and processing of the materials has to be considered, because the material characteristics may have changed. 2001 Elsevier Science B.V. All rights reserved.

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Keywords: Radon-diffusion; Radon-exhalation; Diffusion length; Radon-tight; Insulating materials; Building materials

Corresponding author. Tel.: q49-6841-166211; fax: q49-6841-166227. E-mail address: gert.keller@med-rz.uni-sb.de G. Keller.. 0048-9697r01r$ - see front matter 2001 Elsevier Science B.V. All rights reserved. PII: S 0 0 4 8 - 9 6 9 7 0 1 . 0 0 6 6 9 - 6

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1. Introduction In several studies Lubin et al., 1994., it has been conrmed that the inhalation of radon and its progeny is a well-known risk factor for lung cancer at uranium underground miners. A German case control study on indoor radon Wichmann et al., 1998. and the corresponding extrapolations of data from miners suggest that exposure to residential radon contributes in a relevant manner to the lung cancer risk in the general population. Higher radon concentrations indoors usually depend on the possibilities of radon penetration from the surrounding soil into the buildings. The contribution of building materials to the radon values indoors can be neglected in high radon areas. For mitigation measures in high radon houses, it is important to know the radon permeability of different insulation and building materials. The decision whether a material is radon-tight or not depends on the density and the hindrance of radon penetration in the material.

2. Materials and methods For the determination of the radon diffusion

coefcient and the exhalation rate, we used an online radon-measuring device Fig. 1., in which the positive charged 218 Po-ions were electrostatically deposited on surface barrier detectors and analysed simultaneously by alpha spectroscopy. In the case of diffusion measurements, the sample was held tightly between two chambers and 222 Rn from a dry 226 Ra source was circulated through the reservoir chamber until a constant and high concentration was reached typical range 10 5 10 6 Bqrm3 .. The concentrations in both chambers, the reservoir chamber with a constant concentration and the measuring chamber with increasing values, were determined periodically. During the time of a constant diffusion ux through the sample, the diffusion coefcient can be determined, with the solution of the time independent diffusion reaction equation combined with Ficks rst law Folkerts et al., 1984.. For the measurement of the exhalation rate, only the upper hemisphere of the measuring device was used. The measuring chamber was pressed on one side of the sample, whereas, the other side was placed on a plastic foil to avoid radon penetration from the soil. To determine the exhalation rate of powder or granular material, the sample was lled into a glass bowl, which

Fig. 1. Measuring device for the determination of radon diffusion coefcient.

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ts exactly around the opening of the measuring device. The exhalation rate was calculated from the linear increase of the radon concentration in the measuring chamber. To avoid back diffusion, the concentration inside the chamber had to be low compared with the radon concentration inside the sample. Each measurement was made under laboratory conditions. The samples were stored for 2 weeks under normal conditions. In the case of expected or observed leakages, especially during measurements of small or permeable materials, the outer surfaces of the building materials were sealed with radon tight foil or silicone. Whether there is a leakage or not could be seen in the measurement diagram.

3. Results The results of the investigations for the 222 Rn and 220 Rn exhalation rate of various building materials are shown in Table 1. Represented are rounded mean values of the exhalation rate minimum number of examined samples: ve; maximum more than 100 samples. and for the purpose of comparison the thickness of the material was normalised arithmetically on 10 cm, according to the diffusion theory and applicable

boundary conditions. For every sample the necessary diffusion coefcient was determined separately. For each group of building materials, the mean and rounded activity concentration of 226 Ra and 232 Th was also declared. The mean values of the 222 Rn exhalation rates for building materials varied between 0.05 and 0.4 mBqrm2 s excluding the rate for the test product phosphorite gypsum., for 220 Rn, the range amounted to 10 55 mBqrm2 s. The contribution of 220 Rn to the whole inhalation dose amounts to approximately 30% Keller et al., 1987.. Therefore, the determination of 220 Rn exhalation rates is relevant. The intensive use of industrial waste materials and by-products in the production of building materials is an issue of some controversy. Table 2 shows some results of our investigations on 222 Rn exhalation rates and activity concentrations for the admixture secondary raw materials, by-products, etc.. and the nal building materials. The results of our investigations for the diffusion coefcients of some building and insulation materials as rounded mean values are shown in Table 3. The diffusion coefcients for the investigated building materials were between 10y9 and 10y6 m2rs, which corresponds to a diffusion length of approximately 6 and 1 cm, respectively see Table 3.. In the case of the insulating materials, the diffusion coefcients ranged from values below the detection limit 10y1 2 and 10y 14 m2rs,

Table 1 Mean radium and thorium concentrations and mean 222 Rn- and various building materials, normalized on 10-cm thickness Building material Number of samples 12 9 24 14 30 6 18 104 14 20 5
226

220

Rn-exhalation rates with the variation minimum maximum. of

222 220

Ra Bq kgy1 55 10 10 50 60 75 80 50 20 5 260

232

Th Bq kgy 1 75 10 15 15 50 20 60 10 15 15 15

Rn-exhal. rate mBq my 2 sy 1

Rn-exhal. rate mBq my 2 sy 1

Granite Sandstone Limestone Brick Pumice Slagstone Stone with y ash Concrete Aerated concrete Natural gypsum Ind. gyps. Phosph.

0.25 0.08 0.62. 0.30 0.14 0.48. 0.25 0.15 3.00. 0.05 0.01 0.21. 0.40 0.17 1.75. 0.20 0.13 0.62. 0.35 0.04 0.78. 0.30 0.05 0.75. 0.30 0.12 0.68. 0.05 0.02 0.08. 6.70 5.1 8.3.

30 17 68. 45 16 94. 25 14 120. 10 5 40. 50 27 565. 30 19 66. 55 28 112. 20 10 107. 15 8 44. 10 5 25. 20 5 35.

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Table 2 Special experimental results of the nuclide concentrations and the radon exhalation rate of building materials with additives made from industrial waste materials and by-products thickness approx. 10 cm. Material Activity concentration Bq kgy 1 .
226 222 40

Ra

232

Th

Rn-exhal. rate mBq my2 sy 1 . 0.10 0.43 0.19 0.27 0.31 0.33 0.21 0.40 0.14 0.04 0.17 0.19 0.21 0.35 0.50

Copper slag Mansfeld. Concrete with copper slag Lignite y ash Coal y ash Germany. Coal y ash Poland. Stone with coal y ash Concrete with coal y ash Boiler slag Stone, boiler slag and y ash Brick with y ash Israel. Foundry slag Slag stone Aerated clay Aerated schist Aerated concrete with shale

230 65 55 110 125 85 50 85 35 105 75 45 20 50 30

40 35 25 90 95 65 10 65 30 135 60 60 30 60 25

730 970 310 1130 610 910 450 990 405 140 120 90 570 860 1180

respectively., to values of approximately 10y1 1 m2rs. The diffusion coefcient is independent of the material thickness, therefore, the calculated diffusion length was compared with the thickness of the investigated sample. According to our experiences, a material can be considered as radon-tight

when less than 3% of the available radon concentration can penetrate the sample. From diffusion theory, this condition is fullled if the thickness of the sample is 3 times its relaxation length. If the thickness of the material is smaller than 3 times the diffusion length, the investigated material is called radon-permeable.

Table 3 Experimental mean values and the variation minimum maximum. of the diffusion coefcient D and the diffusion length R of 222 Rn in some materials Material Numbers of samples 12 8 5 8 3 5 8 2 2 6 18 6 1 4 19 5 Thickness 10y3 m. 100 150 150 150 100 100 100 40 3 3 1 3 1.5 5 3 3 Diff. coeff. 10y 6 m2 sy 1 . 2.35 1.3 3.4. 1.50 0.9 2.3. 0.34 0.2 0.5. 0.35 0.1 0.5. 2.20 1.8 2.6. 1.30 1.0 2.0. 0.007 10y3 10y 2 . - 10y6 10y6 - 10y6 - 10y6 - 10y6 10y5 - 10y6 - 10y6 - 10y6 Diff. length 10y 3 m. 1100 850 400 400 1000 800 60 7 0.7 - 0.7 - 0.7 - 0.7 2 - 0.7 - 0.7 - 0.7 Valuation

Gypsum Pumice Limestone Brick Sandstone Aerated concrete Heavy concrete Polymer concrete PCC Asphalt-asbestos Bitumen PEHD foil Silicone rubber Butyl rubber Polyurethane coating Plastic foil Epoxy resin

Permeable Permeable Permeable Permeable Permeable Permeable Permeable Tight Tight Tight Tight Tight Permeable Tight Tight Tight

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4. Conclusion Our investigations on radon exhalation of building materials show that the application of conventional building materials contributes unessentially to the whole radiation exposure of the population. The judgement of a resulting radiation inuence of building materials only by their content of natural radioactive nuclides may lead to an incorrect valuation. For instance, building materials like stones mixed with y ashes and pumice or slag stones exhale less radon because of their closed surface structure glass bead conguration. than other very porous materials with a lower content of natural radionuclides Keller et al., 1997.. Customary building materials except for polymer concrete are normally not radon-tight. Thin paints, plasters and wallpapers are generally radon-permeable, whereas, plastic coatings with a thickness of more than 2 mm, show good sealing results against radon gas. Plastic foils with few exceptions are radon-tight, but our measurements show, that the critical points with regard to radon-tightness are their welding seams or their adhesive sealings. It was surprising that the butyl rubber foil, in contrary to all similar materials, was not radon-tight. The reason for this result was the high content of soot or graphite to colour this material. A similar sample of white butyl rubber was radon-tight. The samples were investigated as stones, plates, blocks, foils, coatings, powders etc., no statement can be made about working up at the construction of a building. At this time only few practical values about the applicability, the durability and the reaction of the investigated material on stress, i.e. pressure or temperature effects in the building construction are available. Our investigations using experimentally mitigated houses using plastic foils, polymer bitumen, polyurethane coating, silicon rubber etc.. showed that the radon concentration indoors, did not signicantly increase during a 10 year follow-up period Hamel et al., 1996.. The processing of the materials is

also a very important fact. In the case of cement or concrete for example, it is important to consolidate the material carefully, because the permeability of these materials depend strongly on the pore system. Also the materials ageing process may be interesting Rogers et al., 1995..

Acknowledgements Investigations for this report were carried out within a research project nancially supported by the Bundesminister fur Umwelt, Naturschutz und Reaktorsicherheit and the Bundesamt fur Strahlenschutz of the Federal Republic of Germany. The authors accept full responsibility for the content of this publication. References
Folkerts KH, Keller G, Muth H. An experimental study on diffusion and exhalation of 222 Rn and 220 Rn from building materials. Rad Prot Dosim 1984;9:27 34. Hamel P, Lehmann R, Kube G, Couball B, Leiring B. Modellhafte Sanierung radonbelasteter Wohnungen in Schneeberg. Bundesamt fuer Strahlenschutz, BfS-ST-10r96, 1996. Keller G, Folkerts KH, Muth H. Discussing possible standards of natural radioactivity in building materials. Radiat Environ Biophys 1987;26:143 150. Keller G, Puch K-H, Nickels RM. Radioactivity of coal ash in building materials. Proceedings of the Second Regional Mediterranean Congress on Radiation Protection, Tel-Aviv, Israel, 1997; 161 163. Lubin JH, Boice JD, Edling CH, Hornung R, Howe G, Kunz E, Kusiak A, Morrison HI, Radford EP, Samet JM, Tirmarche M, Woodward A, Xiang YS, Pierce DA. Radon and Lung Cancer Risk: A Joint Analysis of 11 Underground Miners Studies. US National Institutes of Health, 1994. NIH publication No. 94-3644. Rogers VC, Nielson KK, Holt RB. Radon diffusion coefcients for aged residential concretes. Health Phys 1995;68:832 834. Wichmann HE, Kreienbrock L, Kreuzer M, Gerken M, Dingerkus G, Wellmann J, Keller G. Lungenkrebsrisiko durch Radon in der Bundesrepublik Deutschland West.. Fortschritte in der Umweltmedizin. Landsberg: Ecomed verlagsgesellschaft, 1998.