Proceedings of the 11th International Conference on Environmental Science and Technology Chania, Crete, Greece, 3 – 5 September 2009 INDOOR EXPOSURE TO ASBESTOS-LIKE FIBERS RELEASED FROM CONTAMINATED GROUNDWATER P. ROCCARO and F. G. A. VAGLIASINDI* Department of Civil and Environmental Engineering, University of Catania, Italy *e-mail: fvaglias@dica.unict.it EXTENDED ABSTRACT Fluoro-edenite (NaCa2Mg5(Si7Al)O22F2), a new asbestos-like fiber, was found in the rock of the Etna Volcano at Biancavilla (Catania, Italy). Fluoro-edenite fibers are under investigation to evaluate their toxicity and carcinogenicity due to its similarity with asbestos. Overall, epidemiological studies have shown that asbestos fibers cause bronchial carcinoma and pleural mesothelioma by inhalation, while more studies are needed to asses their effect by ingestion. Even thought the ingestion is the main route of exposure associated to asbestos-like fibers in water in terms of potential risk for human health, other scenarios can occur such as the release of fibers in the air by evaporation or humidification, and the deposition on textiles during washing and rinsing processes and subsequent release of fibers during wearing/use of cloth. Thus, the objective of this study is to explore the indoor occurrence of asbestos-like fibers associated with the use of fluoro-edenite contaminated tap water. Experiments were conducted in the bathroom of a residential house in Biancavilla, where the airborne asbestos-like fibers released by the use of the shower were collected using a digital constant sampler (mod. ZB1, Zambelli, Italy) equipped with an esters mixed cellulose membrane (25 mm diameter and 0.8 μm porosity) at the end of each tests. Experiments were carried out at varying the time of shower and the exposure time. Temperature and relative humidity in the bathroom were periodically monitored. The collected filters were first treated by acetone-triacetyne method and then analyzed for asbestos-like fibers by using a phase contrast microscopy. Obtained results have shown that the release of asbestos-like fibers during the shower occurs if contaminated waters are supplied. The concentration of the airborne asbestoslike fibers in the bathroom during and following the shower is much higher than the limit values set by the European and National regulations. Strong correlations were found between the concentration of the airborne asbestos-like fibers and, on the other hand, the relative humidity or the water consumed obtained at fixed exposure time. These correlations can be used to control and monitor the asbestos-like fibers exposure during the shower. These results highlight that the risk for the human health related to the exposure to asbestos-like fibers present in tap water may be relevant and therefore the removal of these fibers may be pursued at water treatment plant. Further investigations concerning the exposure scenarios and the removal of asbestos-like fibers from contaminated water will be conducted in future work. KEYWORDS: Air, Airborne asbestos-like fibers, Fluoroedenite, Shower, Water. 1. INTRODUCTION Subsequent to an epidemiological survey (carried out from 1988 to 1992) on the mortality due to malignant pleural neoplasm in Italy, a cluster of cases was found in Biancavilla, a town located in the Etnean Volcanic Complex (Catania, Italy) of eastern Sicily. Several A-1194 epidemiological studies and environmental monitoring were carried out and a new asbestiform fibre, named fluoro-edenite (NaCa2Mg5(Si7Al)O22F2), was discovered in a stone quarry (Gianfagna et al., 2001; Bruno et al., 2006). The residents of Biancavilla, for whom a diagnosis of pleural mesothelioma had been made, never had any relevant exposure to asbestos during their professional life. The possible cause of such unusual distribution of the pathology was proposed to be the exposure of the population to stone quarries located in ‘‘Monte Calvario’’ that contains the fluoro-edenite fibres and was largely used in the local building industry (Paoletti et al., 2000; Bruno et al., 2006; Bruni et al., 2006). As a consequence, the Biancavilla site was defined “site of national interest” for environmental reclamation and on site characterization and remedial investigation were conducted as well as monitoring programs, still ongoing. Despite epidemiological studies have shown that asbestos-like fibres cause bronchial carcinoma and pleural mesothelioma by inhalation, there is no unequivocal evidence of the carcinogenicity of these fibres by ingestion (Kjærheim et al., 2005; Bruni et al., 2006). Recently, it was observed that, in lung epithelial cells, fibrous fluoro-edenite behaved similarly to the unrelated asbestos type crocidolite, whose connection with severe inflammation and cancer of the lung is well known (Travaglione et al., 2006). The human exposure to fluoro-edenite fibres may be related to the presence of those fibres in different natural matrices. Indeed, even thought the ingestion is the main route of exposure associated to asbestos-like fibres in water, other scenarios can occur such as the release of fibres in the air by evaporation or humidification, and the deposition on textiles during washing and rinsing processes and subsequent release of fibres during wearing/use of cloth (Webber et al., 1988; Hardy et al., 1992; Highsmith et al., 1992). Therefore, more research is needed to asses the toxicity and carcinogenicity of fluoroedenite fibres by different rote of exposure (inhalation and ingestion). This study, which is part of an ongoing research aiming at evaluating the occurrence, fate and control of asbestos-like fibres at Biancavilla site, is devoted to investigate the indoor human exposure to asbestos-like fibres associated with the use of fluoro-edenite contaminated tap water. In particular, the objective of this paper is to explore the release of asbestos-like fibres in the air during the shower. 2. MATERIALS AND METHODS 2.1. Experimental methods Experiments were conducted in the bathroom of a residential house located at Biancavilla town (Catania, Italy), where the airborne asbestos-like fibres released from the shower were collected by a digital constant air sampler (mod. ZB1, Zambelli, Italy) equipped with an esters mixed cellulose membrane (25 mm diameter and 0.8 μm porosity). The air sampler was used at a flow rate of 1 L/min during the experiments and the flow rate of the shower was 9 litre per minute. In order to have similar initial ambient conditions inside the bathroom, prior to start each test, the room was ventilated opening the window for some minutes. Experiments were carried out at varying operating conditions (Table 1) to asses the effect of the time of shower and exposure time on the presence of airborne asbestos-like fibres. In particular, the time of shower varied from 4 to 15 minutes, while the exposure time ranged from 6 to 20 minutes. Temperature and relative humidity in the bathroom were monitored every minute by using an electronic thermo-hygrometer (Delta OHM HD 8901). 2.2. Analytical methods The collected filters were dried for 12 hours in a desiccator containing blue silica gel as desiccant and then treated by acetone-triacetyne method and analysed by using a phasecontrast optical microscopy (Axioskop 40 Pol, Zeiss) with a x40 objective and a x500 A-1195 magnification. The fibres were counted in accord to (WHO, 1997) employing 200 counting fields per filter. The concentration of the fibres were calculated with the following relationship (WHO, 1997): C(ff/L) = (106 N D2)/(V n d2) with: N = total number of fibres counted; n = number of counting fields; D = filter diameter (mm); d = diameter of the Walton Beckett graticule (100 μm); V = volume of air or water passed through the filter (litres). All the analyses were carried out at the Laboratory of Environmental and Sanitary Engineering of the University of Catania. 3. RESULTS AND DISCUSSION 3.1. Occurrence of airborne asbestos-like fibers released during the shower under different conditions Asbestos-like fibres were found in aquifers at Biancavilla site at relatively high concentration compared to the average Sicilian water quality. The concentration of fibres found in the tap water of the house investigated was 8229 ff/L. Picardo 1 and Picardo 2 that are the major water sources (wells) used for water supply in Biancavilla had a concentration of fibres of 8073 ff/L and 8958 ff/L, respectively. The groundwater contamination may be related to the percolation of rainwater throughout the volcanic rocks containing the fluoro-edenite. The concentration of these fibres may vary during the season and may cause heath effects by ingestion or inhalation. As shown in Table 1 the release of asbestos-like fibres in the bathroom ambient occurs due to the shower if contaminated water is supplied. Indeed, in this study airborne asbestos-like fibres were detected at concentration ranging from 350 to 850 fibres per litre (Table 1). The observed concentrations of airborne asbestos-like fibres are much higher than the limit values set by the European Directive 2003/18/EC and the Italian regulation (D.Lgs. 257/2006) concerning the protection of workers from the risks related to exposure to asbestos at work (100 ff/L) and by the Italian regulation (DM 6/9/94) on the extraction, manufacture, processing and removal of asbestos from contaminated buildings (20 ff/L as threshold indicator of the presence of pollution by asbestos and 2 ff/L for the restitution of buildings after the remediation). It is noteworthy that the limit value of 2 ff/L was suggested by the local authorities as warning threshold during outdoor environmental monitoring at Biancavilla site. Obtained results highlight that a relevant risk for human health may be related to the supply of contaminated water by asbestos-like fibres. As reported in Table 1, the concentration of airborne asbestos-like fibres released from the shower is strongly affected by the water consumed (i.e. the time of shower) and the exposure time that can vary because of the behaviour of the users. As expected, at fixed exposure time, higher shower time results in higher airborne fibres concentration. On the other hand, at fixed shower time, higher exposure time results in lower concentration of airborne fibres. This observation highlights that the transfer of the asbestos-like fibres from the shower in the air inside the bathroom is a complex mechanism that is related to the simultaneous release of a significant amount of fibres in the air during the shower and to the dispersion of these fibres inside the bathroom. It can be concluded that the fibres concentration reported in Table 1 can not be intended as concentration value homogeneously distributed inside the chamber, but are point values that change during the release and dispersion mechanism. These values A-1196 Table 1. Concentration of airborne asbestos-like fibres detected inside the bathroom during or following the shower and related operating parameters. Time of shower (min) Test 1 2 3 4 5 6 7 8 9 10 11 12 13 Water consumed (L) 6 8 4 8 15 2 6 10 12 9 4 10 15 Final relative humidity inside the bathroom (%) Exposure time (shower + after shower) (min) 54 72 36 72 135 18 54 90 108 81 36 90 135 6 8 15 15 15 15 15 15 15 10 20 20 20 Concentration of airborne fibres (ff/L) 65 86 76 90 100 78 93 99 100 100 92 93 100 794 775 385 552 688 354 453 625 682 859 379 449 574 correspond to the concentrations that can be inhaled by a user that is in the same position of the air sampler (i.e. close to the shower box). Therefore, obtained results demonstrated that the portable air sampler working at a flow rate of 1 L/min can be used to simulate the real human exposure to fibres released during specific activities that involve multiple parameters. The release mechanism can also vary with the initial temperature and relative humidity inside the bathroom. Figure 1 shows the variation of ambient temperature inside the bathroom during the experiment for selected tests, while in Figure 2 is reported the changes of the relative humidity in the bathroom for the same experimental tests. 22 21 Temperature (°C) 20 19 18 17 16 15 Test 3 Test 4 Test 5 Test 6 Test 7 Test 9 Test 10 Test 11 Test 12 Test 13 Test 8 14 0 2 4 6 8 10 12 14 16 18 20 Time (minutes) Figure 1. Temperature variation inside the bathroom in different experimental tests A-1197 22 105 Relative Humidity (%) 95 85 75 65 55 45 35 Test 3 Test 4 Test 5 Test 6 Test 7 25 Test 9 Test 10 Test 11 Test 12 Test 13 10 12 Test 8 15 0 2 4 6 8 14 16 18 20 22 Time (minutes) Figure 2. Relative humidity variation inside the bathroom in different experimental tests As shown in Figure 1 and 2, both the temperature and relative humidity increased during the experiment reaching asymptotically the maximum value. However, the increasing rate is much prominent for the relative humidity, whose values first increase linearly until 7-8 minutes of exposure time and then reach their maxima asymptotically. Furthermore, the data of relative humidity have the same behaviour regardless of the different operating conditions (dissimilar experimental tests), with the exception of data carried out at the shorter shower times (tests 3 and 6) that have shown a different pattern. Indeed, for these two dataset the maxima values are lower than those obtained from the other tests and these maxima values are reached at shorter time. Overall, it can be concluded that when water consumed is about 54 litres or higher, corresponding to a shower time at least of 6 minutes, and the exposure time is higher than 8 minutes the relative humidity will reach its maximum value. In these conditions the risk of exposure to asbestos-like fibres may be higher. However due to the complexity of the mechanism of fibres release, the use of alternative parameters to predict the human exposure to airborne fibres released during the shower may be useful. This aspect is addressed in the following section. 3.2. Relationships between the concentration of airborne fibres and alternative parameters Strong correlations were found between the concentrations of airborne asbestos-like fibres released by the shower and alternative surrogate parameters at fixed exposure time. For instance, Figure 3 and 4 show the correlations between the concentration of asbestos-like fibres and, on the other hand, the relative humidity or the water consumed obtained at 15 minutes of exposure time. These surrogate parameters can be used to control or monitor the exposure to the airborne asbestos-like fibres during the shower and therefore to predict the relative risk of mesothelioma or lung cancer. A-1198 Concentration of fibres (ff/L) 800 700 R2 = 0.85 600 500 400 300 200 100 0 60 70 80 90 100 110 Relative humidity (%) Figure 3. Relationship between the concentration of asbestos-like fibres and the relative humidity at fixed exposure time of 15 minutes Concentration of fibres (ff/L) 800 R2 = 0.94 700 600 500 400 300 200 100 0 0 20 40 60 80 100 120 140 Water consumed (L) Figure 4. Relationship between the concentration of asbestos-like fibres and the water consumption at fixed exposure time of 15 minutes 4. CONCLUSIONS In this study it was observed that the shower is a relevant source of airborne asbestoslike fibres even when the supplied water contains trivial concentrations (at least compared with the current limit values for drinking water) of these fibres. The concentration of airborne asbestos-like fibres released by the shower at realistic time of A-1199 shower and exposure (after shower) was very high compared to the limit values set by the National and European regulations. The concentration of these airborne asbestos-like fibres can be predicted by the use of the relative humidity or the water consumed obtained at given exposure time. Although the risk for human health related to the ingestion of asbestos-like fibres is not well known, a relevant risk may result from the inhalation of these fibres released from the shower when contaminated water is supplied. The surrogate parameters found in this study may be also used to predict the risk for human health. Based on the results obtained in this study, the addition of specific limit values for asbestos in drinking water regulations is strongly recommended. In particular, a limit value more stringent than of that set by the EPA (7 million of fibres per litre) should be fixed. Furthermore the removal of the asbestos-like fibres must be pursued by treating drinking water sources used in Biancavilla. Further investigations concerning the exposure scenarios and the removal of asbestoslike fibres from contaminated water will be conducted in future work. ACKNOWLEDGEMENT This study was partially supported by the Italian Ministry of Instruction, University, and Research (MIUR), through the program Research Projects of National Interest “Criteria and tools for environmental remediation and functional regeneration of contaminated sites”. Authors are very thankful to Drs. 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