Ann. occup. Hyg., Vol. 41, Supplement 1, pp. 700-706, 1997 © 1997 British Occupational Hygiene Society Published by Elsevier Science Ltd. All rights reserved Printed in Great Britain 0003-4878/97 $17.00 + 0.00 Inhaled Particles V11I PII: S0003-4878(96)00175-5 PERSONAL EXPOSURE MEASUREMENTS OF THE GENERAL PUBLIC TO ATMOSPHERIC PARTICLES D. Mark,* S. L. Upton,t C. P. Lyons,! R. Appleby,* E.J. Dyment,t W.D. Griffith! and A.A. Foxt * Institute of Occupational Health, University of Birmingham, Birmingham, U.K.; tAerosol Science Centre AEA Technology, Harwell, Didcot, U.K.; and ^Environmental Pollution Unit, Birmingham City Council, Birmingham, U.K. INTRODUCTION Airborne particles in ambient atmospheres in the U.K. are continuously monitored using tapered element oscillator microbalances (TEOM) (Patashnick and Rupprecht, 1991), equipped with inlets that select the thoracic aerosol fraction according to the PM10 definition. These are part of the Automatic Urban Network (AUN) of the U.K. Department of the Environment, which is a network of sites located in cities throughout the U.K. In order to use this information to estimate the exposure and potential dose of particles to the general public, it is necessary to understand the relationship between these measurements and actual exposure as measured with personal samplers. These personal samplers are worn on the upper part of the chest close to the nose and mouth of the wearer and are specially designed to mimic the aerodynamic behaviour of the human respiratory system. The aim of this project is to obtain a reliable assessment of the particle exposures of a representative group of the general public and to use this information to determine how effectively data from the fixed site TEOM monitors can estimate that exposure. PREVIOUS PERSONAL EXPOSURE DATA TO PM10 PARTICLES So far, most of the published data on the personal exposure of the general public to ambient airborne particles has been carried out in the U.S.A. Since the early 1980s, a small number of long-term studies have been initiated to estimate the exposure of the general public to airborne pollutants, including particles. One of the major studies carried out in the U.S.A. during this period was the Six City study (Spengler, 1985), carried out by investigators mainly from the Harvard School of Public Health. In this study, estimates of respirable particle exposures in six cities in the U.S.A. were obtained using both personal samplers and microenvironmental and/or outdoor fixed-site monitors. In the total human environmental exposure study (THEES) (Lioy, et al., 1990) personal, indoor and outdoor concentrations of thoracic (PM10) particles were measured for the first time. The total exposure assessment methodology (TEAM) study (Wallace et al., 1993) involves the measurement of PM10 particles in a large number of residents in Riverside, California. 700 Exposure measurements of the public to atmospheric particles 701 However, despite the existence of these three large exposure studies, the number of measurements of particle exposure made with actual personal samplers is relatively small (250 respirable and 530 PM10). Instead, most of the exposure estimates were based on the use of exposure models in which particle levels in a number of micro-environments (normally five), measured using static monitors, are used in combination with information from activity diaries to build up exposure profiles for each subject. However, whilst these models may effectively estimate individual exposures to gases such as CO, NO2 and SO2 there is very little evidence concerning their validity for estimating particulate exposures. Consequently, many authors expressed a preference for personal sampling, but argued against largescale personal monitoring studies on the grounds of excessive cost. THE PERSONAL SAMPLER USED FOR THE STUDY The choice of sampler used in this study was severely limited by the lack of suitable samplers. Consequently, a modified version of the prototype personal sampler, reported by Mark et al. (1988), was used. The sampling head has an internal cassette with an inhalable aerosol entry followed by a cylindrical plug of porous polyester foam to select the thoracic fraction of the inhaled particles, which are collected on a 37 mm diameter filter. A specially-built (small, light and quiet) sampling pump was used, capable of sucking air at 2 1 min"1 for at least 16 h each day with a fast battery charging system that enabled the sampler to be used the next day. Particular attention was paid to making the sampler as quiet as possible. An unobtrusive, easily removable carrier harness, based around a small camera case, was used to carry both the pump and the sampler. The sampler itself was fixed to the carrying strap and was maintained in the lapel position by a combination of removable loops and clips. THE SAMPLING CAMPAIGN The sampling campaign was based around the two AUN sites within the City of Birmingham. One is situated in the centre of the city in the corner of a car park close to the Centenary Square, whilst the other is in the playground of a school within a suburban area of the city. Sampled population The sampled population comprised 15 members of the general public at each site, although some volunteers dropped out after the first exercise and were replaced with substitutes. The main criterion for the choice of subjects was that of reliability, to ensure that the samples obtained did represent actual personal exposure measurements for the periods specified. At each site we were able to identify three main sub-groups, who have similar living and working arrangements (called lifestyle in the analysis of the results), and therefore may have similar exposures. They were: (1) retired people who live very close to the AUN stations; (2) people who also live close to the AUN stations, but who work at least 3 miles away; and (3) people who work close to the AUN stations (Centre—office workers, 702 D. Mark et al. East—teachers), but who live at least 3 miles from the site. The gender of the volunteers was: Centre, 15 male, 3 female; East, 12 female, 3 male. Sampling programme For each group of subjects, three sampling surveys were carried out: Survey 1 in August/September 1995, Survey 2 in October/November/December 1995 and Survey 3 in February/March 1996. For each survey, a target of five replicate exposure periods for each subject was set. These were of variable duration from 16 to 33 hours, with the samplers being switched off during sleep time, and at some workplaces. Subjects completed an initial questionnaire about their housing, heating, method of cooking, occupation, hobbies and kept a diary of their major activities during the exposure measurements. Experimental analysis Glass fibre filters were used to collect the sampled particles. The mass of particles collected on each filter was determined by weighing the filter before and after sampling twice on a six-place electronic balance. A rigid system of filter conditioning and controls was employed to enable the maximum accuracy to be achieved with the expected small particulate masses (expected to be around 50-1000 u.g). The mean outdoor PM10 mass concentration levels were calculated from the 15 min averages of continuous measurements given by the TEOM instruments at the two AUN sampling stations. The raw data have been modified following the agreed acceptance criteria for the AUN network, but must still be considered as provisional at this stage. These were calculated for each personal exposure sample for the periods during which the personal samplers were in operation. Statistical analysis Two main statistical analyses were carried out. Firstly, descriptive statistics were calculated for the personal exposure measurements, subdivided according to survey, smoking status and lifestyle. In order to stabilise the variances, the natural logarithms of the personal exposure measurements have been used for all models tested. Regression analyses were carried out to investigate the relationship between the personal exposure measurements and the AUN measurements. Factors such as exposure to tobacco smoke or lifestyle were treated as confounders in some analyses and their effects on the relationship between personal exposure measurements and AUN measurements were explored using analyses of covariance. RESULTS The results of the descriptive statistics for the personal exposure measurements for both sites are shown in the box plots of Fig. 1 (a)-(c). In Fig. l(a), significant differences between surveys was found both between sites and between seasons (survey 1 being in the summer and 2 and 3 being in the winter). The effects of smoking on exposures can be seen in Fig. l(b), where for both sites, the differences were highly statistically significant, with smokers exposed to almost twice as much mass of thoracic particles as the non-smokers. Levels for the passive smokers at Exposure measurements of the public to atmospheric particles BIRMINGHAM CENTRE 703 BIRMINGHAM EAST Extreme data < 3 interquartile range 450 250 Data < 1.5 Interquartile range 200 75th Perccntile Sample mean* 50th perccntile (median) 400 350 300 150 BOX PLOT KEY 250 200 100 150 E 50 100 00 A Q u 50 a) ALL DATA 0 1 2 3 SURVEY NO 04 o x w 450 400 250 Z UJ 350 UJ 300 200 So -50 !-Ll b) SMOKING STATUS 200 100 150 OJ 100 O cu X T 50 o 1 2 3 SMOKING STATUS SMOKING STATUS < z o 1 - Active smoker 2 - Passive smoker 3 - Non - smoker 450 250 400 350 200 300 250 150 c) LIFESTYLE 200 100 150 100 50 50 1 - Live and work in vicinity 2 - Live in area and work away 3 - Work in area and live away 0 1 2 3 LIFF STYLE Fig. 1. Box plots of personal exposure measurements. 704 D. Mark et al. • SubjectCOl • Subject C06 A Subject C07 X Subject C08 XSubjectCIO • Subject Cll + Subject Cl 2 -Subject Cl 3 -Subject C14 O Subject Cl 5 D Subject C16 A Subject Cl 7 Co Subject Cl 8 a) Birmingham Centre - All Data 450 5b «? 400 350 tnora o 300 1 u 250 a 3 200 « 150 ;ure e 100 a u 50 X a c s - x ° •, X O x -r •° A • x - *• •;? Subject C19 O Subject C20 :: Subject C21 • Subject C22 0 10 20 30 40 50 60 80 70 AUN PM10 Concentration Levels (ng/m3) b) Birmingham East: - All Data • Subject E01 250 • Subject E02 A Subject E03 2 200 X Subject E04 X Subject E05 5 • Subject E06 150 + Subject E07 -Subject E08 — Subject E09 i O Subject E10 I DSubjectEll A Subject E!2 i • Subject E13 ; • >SubjectE14 j Z 0 ;; Subject EI5 20 40 60 100 80 3 AUN PM10 Concentration Levels (|ig/m ) Regression equation: In (personal exposure) = intercept + AUNx No of Samples CENTRE All subjects Non smokers EAST All subjects Non smokers 128 76 173 143 slope Intercept ln(ug/m3) Slope P R~ 4.262 4.077 0.009 0.009 0.0035 0.0086 0.066 0.09 3.576 3.438 0.02 0.022 0.0001 0.0001 0.144 0.145 Fig. 2. Relationship between personal exposure and AUN measurements. East were only slightly higher than those for the non-smokers. In Fig. l(c), the effects of where people live and work in relation to the AUN sites, can be seen. For Centre, those subjects living and working in the area and those living in the area, but working away are exposed to approximately twice as much mass of thoracic particles as those working in the area and living away. For East, the picture was slightly different, with those subjects living and working in the area experiencing Exposure measurements of the public to atmospheric particles 705 the lowest exposures and those living in the area but working away appeared to have the highest. These effects were statistically significant with P values < 0.001. The results of all the measurements of personal exposure and corresponding PM10 levels from AUN monitors for Centre and East are given in Fig. 2(a) and (b), respectively. Regression analyses carried out to investigate the relationships between the data are given on the figures. For centre, the overall positive association between personal exposure measurements and AUN PM10 values, just fell short of statistical significance both for the model with all subjects and for that with smokers excluded. For East, the overall positive association between personal exposure measurements and AUN values was statistically significant (P = 0.0001), both for the model with all subjects and that with smokers excluded. However, there is a wide spread of results with the regression relationship explaining only 14% of the variability (R2 = 0.14). DISCUSSION This is the first systematic study carried out in the U.K., to determine the personal exposure of members of the general public to airborne particles. It represents a 50% increase in the number of actual personal samples reported irrespective of size fraction measured and a 60% increase in measurements of the thoracic fraction. The main conclusion from this short study is that there is no simple relationship between PM10 levels obtained from the AUN particle monitors at Birmingham and the thoracic particle exposures of a small group of the general public living and/or working in the area. However, there is increasingly strong evidence of a correlation between PM10 levels in the ambient atmosphere and certain ill-health in the general public (Schwartz, 1991; Dockery et al., 1993). As people spend on average over 90% of their time indoors (confirmed in this study), the question that immediately springs to mind is: "Is there high penetration of outdoor aerosols into indoor environments?" If the answer to this question is "yes", then it is conceivable to suggest that it is the fine outdoor particles that are mainly responsible for the ill-health reported. This suggestion would lend some support to the proposition by Seaton et al. (1995) that ultra-fine particles (< 100 nm) are the main causative agents for the reported circulatory health effects. However, there are also many potentially harmful particles that are derived solely from indoor sources such as: particles from gas cookers and heaters, environmental tobacco smoke, mould spores, house dust mite faeces, dander, skin, cat, bird and insect allergens. These are variously reported to have potential allergenic, pathological and carcinogenic properties. Therefore, if the main aim of particle monitoring is to provide information for the minimisation of all particle-related ill-health, then it may not be sufficient just to monitor the ambient atmosphere via the AUN system. Further work is required. Acknowledgements—The authors would like to acknowledge the support both financially and technically of the U.K. Department of the Environment for this work. Our special thanks go to those people in Birmingham, who willingly and responsibly participated in the exposure measurements. 706 D. Mark et al. REFERENCES Dockery, D.W., Schwartz, J. and Spengler, J. D. (1992) Air pollution and daily mortality: associations with particulates and acid aerosols. Environ. Res. 59, 362-373. Lioy, P. J., Waldman, J. M., Buckley, T., Butler, J. and Pietarinen, C. (1990) The personal, indoor and outdoor concentrations of PM10 measured in an industrial community during winter. Atmos. Environ. 24B (1), 57-66. Mark, D., Borzucki, G., Lynch, G., Vincent J. H. (1988) The development of a personal sampler for inspirable, thoracic and respirable aerosol. In Aerosols: Their Generation, Behaviour and Applications, 2nd Conference of the Aerosol Society, Bournemouth, March 1988, pp. 183-187. Patashnick, H. and Rupprecht, E. G. (1991) Continuous PM10 monitoring using the tapered element oscillating microbalance. /. Air Waste Management Assoc. 41, 1079-1083. 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