Polynuclear Aromatic Compounds and Genotoxicity in Particulate and

Phases of Ambient Air: Effect of Traffic, Season, and Meteorological. Conditions ... nuclear aromatic hydrocarbons (PAH), although increasing. *Author...
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Environ. Sci. Technol. 1988, 22,1228-1234

Barrick, R. C. Environ. Sci. Technol. 1982, 16, 682-692. Ostman, C. E.; Colmsjo, A. L.; Zebuhr, Y. U. Proceedings of the 9th International Symposium on PAH Battelle Press: Columbus, OH, 1986; pp 729-745. Ostman, C. E.; Colmsjo, A. L. Proceedings of the 10th International Symposium on PAH, Battelle Press: Columbus, OH, 1988; pp 673-685. Spitzer, T.; Dannecker, W. J. HRC & CC, J . High Resolut. Chromatogr. Chromatogr. Commun. 1982,5, 98-99. Butler, J. D.; Crossley, P. Atmos. Environ. 1981,15,91-94. Behymer, T. D.; Hites, R. A. Polynuclear Aromatic Hydrocarbons: Chemistry, Characterization and Carcinogenesis; Cooke, M., Dennis, A. J., Eds.; Battelle Press:

Columbus, OH, 1986; p 1052. Pierce, R. C.; Katz, M. Environ. Sci. Technol. 1975, 9, 347-353.

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New York, 1985; pp 1-198.

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12(3),192-199.

(74) Colmsjo, A. L.; Soderstrom, H.; Wadding, 8.;Zebuhr, Y. U.; Ostman, C. E. Chemosphere 1986, 15, 169-182. (75) Grandjean, P.; Nielsen, T. Residue Rev. 1979, 72, 97-148. (76) Habibi, K. Environ. Sci. Technol. 1970, 4 , 239-248.

Received for review October 6,1986. Accepted April 7,1988. The study was financially supported by the Stockholm Water and Wastewater Works, the Environmental Control Fund of Stockholm County Council, the National Swedish Environment Protection Board, and the Bank of Sweden Tercentenary Foundation.

Polynuclear Aromatic Compounds and Genotoxicity in Particulate and Vapor Phases of Ambient Air: Effect of Traffic, Season, and Meteorological Conditions Jari Tuominen,t Sisko Salomaa,' Heikki Pyysalo,t Eija Skytta, Leena Tlkkanen,t Tuomo Nurmela,* Marla Sorsa,t VelJo PohJola,IiMarketta Sauri,t and Kimmo Himberg+ *st

Food Research Laboratory, Technical Research Centre of Finland, Biologinkuja 1, SF-02 150 Espoo, Finland, Department of Industrial Hygiene and Toxicology, Institute of Occupational Health, Topeliuksenkatu 41 a A, SF-00250 Helsinki, Finland, Chemical Laboratory, Technical Research Centre of Finland, Biologinkuja 7, SF-02 150 Espoo, Finland, and Air Quality Department, Finnish Meteorological Institute, Sahaajankatu 22 E, SF-00810 Helsinki, Finland

Introduction To date, about 2800 compounds have been detected in the ambient atmosphere. Slightly more than 300 of them have been bioassayed (1). From the view of their health effects, most concern has been directed toward the polynuclear aromatic hydrocarbons (PAH), although increasing

evidence suggests that compounds other than the conventional, nonsubstituted PAH are responsible for the genotoxic effects of polluted air (2-9). For practical purposes, organic air pollutants can be divided into three phases according to the different sampling techniques: (1)the particulate phase, (2) the vapor phase consisting of compounds with boiling points higher than 100 "C (semivolatile compounds), and (3) the gas phase consisting of smaller and more volatile compounds. Each of these phases is known to include mutagenic/ carcinogenic compounds. The concentrations of PAH in the particulate phase of ambient air have been studied extensively (1U-13). Mutagenicity of airborne particulates has as well been tested in a number of studies by the Ames Salmonella/microsome assay (14-17) and several mammalian test systems (18-21). However, even though it is known that several airborne PAH exist partly, or exclusively, in the vapor phase, only a few studies have been made on their concentrations or genotoxicity (22-27). In this study, we have determined the levels of 30, mainly polynuclear compounds in particulate and vapor phases of ambient air at three different locations in Finland. The genotoxicity of the same samples was studied by using two short-term bioassays. Previously, in a similar study carried out in a small industrial town in Finland, we found relatively high concentrations of PAH in the vapor phase of ambient air (28). In the present study, the major interest was focused on the origin and seasonal variation of PAH in urban air, and special attention was given to the role of traffic exhausts.

to whom correspondence should be addressed. 'Food Research Laboratory, Technical Research Centre of Finland. $Instituteof Occupational Health. Chemical Laboratory, Technical Research Centre of Finland. 11 Finnish Meteorological Institute.

Experimental Section Sampling and Sample Preparation. Samples were collected during nine sampling periods in the cities of Helsinki (the capital, population -800 000) and ,,Lahti (population -100000) and in the rural commune of Ahtkri.

High-volume samples of ambient air were collected by glass-fiber filter (particulate) and XAD-2 resin (vapor) from three locations in Finland: two cities and a rural area. Samples were analyzed for polynuclear aromatic hydrocarbons (PAH) and selected other polynuclear compounds. Genotoxicity of the samples was assayed in the Ames Salmonellalmicrosome test and sister chromatid exchange assay before and after fractionation into four fractions of increasing polarity. The ratio of PAH in the vapor and particulate phases of the samples varied considerably with the season, and the scavenging effect of snow and rain was as well clearly demonstrated. The rural samples showed minimal or no genotoxic activity, whereas at the urban sites not only the particulate-phase but also the vapor-phase samples were mutagenic. The genotoxicity was mainly associated with the most polar fractions of both phases. Studies with the nitroreductase-deficient Salmonella strain TA98NR indicated that, in the urban air samples collected in winter, a considerable part of the mutagenicity detected in the Ames test was due to NO2-substituted compounds. Traffic is suggested to be the major determinant for the genotoxic activity in the ambient air.

*Author

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Environ. Sci. Technoi., Vol. 22, No. 10, 1988

0013-936X/88/0922-1228$0 1.50/0

0 1988 American Chemical Society

Table I. Meteorological Parameters sampling site

sampling period"

sample no.

mean wind speed, m/s (range)

Helsinki

1 (8) June-July 2 (w) Feb-Mar 3 (s) June 4 ( f ) Oct 5 (w) Mar 6 (s) July 7 (f) Sept 8 (w)Feb 9 (s) June

7 3 1 2 2 2 3 4 8

3.2 (2.5-4.5) 4.3 (3.8-5.3) 2.7 (2.3-3.0) 2.7 (1.8-3.5) 3.5 (2.4-5.0) 1.5 (1.0-2.0) 1.1 (0.5-3.3) 1.1(0.4-2.1) 2.1 (1.5-2.6)

Lahti Ahtari

mean temp, " C (range) +14.8 -7.1 +20.3 +4.6 -1.9 +15.9 +8.9 -19.1 +15.7

mean re1 humid., % (range)

(+11.2 to f20.9) 77 (61-89) 77 (50-85) (-14.6 to -1.4) (+18.5 to +22.0) 49 (47-50) 87 (80-92) (+3.5 to +6.5) 79 (71-95) (-2.9 to -0.8) (+14.7 to +17.5) 78 (72-85) (+7.1 to +13.7) 85 (74-92) 77 (72-82) (-16.3 to -27.6) (+9.3 to +21.2) 63 (59-78)

s, summer; f, fall; w, winter. *R, rain; S, snow. 'Rainfall

total mean traffic cloudiness, density , mean value rainfall,b rainy daysC vehicles/day mm 0-8 (range) 5.5 (2-8) 5.7 (1-7) 1.5 (1-2) 2.7 (2-5) 7.0 (6-8) 5.6 (4-8) 5.3 (3-6) 3.7 (0-8) 2.6 (0-6)

25.4 R 3.0 S 0.0 0.0 6.4 S 1.3 R 0.3 R 0.1 s 2.8 R

7 3 0 0 2 1 1 1 2

mean SOp concn, a/m3

24000-42000 38000 26000 21000 21000 21000