Characterisation of urban inhalation exposures to benzene, formaldehyde and acetaldehyde in the European Union: comparison of measured and modelled exposure data.

BACKGROUND, AIM AND SCOPE: All across Europe, people live and work in indoor environments. On average, people spend around 90% of their time indoors (homes, workplaces, cars and public transport means, etc.) and are exposed to a complex mixture of pollutants at concentration levels that are often several times higher than outdoors. These pollutants are emitted by different sources indoors and outdoors and include volatile organic compounds (VOCs), carbonyls (aldehydes and ketones) and other chemical substances often adsorbed on particles. Moreover, legal obligations opposed by legislations, such as the European Union's General Product Safety Directive (GPSD) and Registration, Evaluation, Authorisation and Restriction of Chemicals (REACH), increasingly require detailed understanding of where and how chemical substances are used throughout their life-cycle and require better characterisation of their emissions and exposure. This information is essential to be able to control emissions from sources aiming at a reduction of adverse health effects. Scientifically sound human risk assessment procedures based on qualitative and quantitative human exposure information allows a better characterisation of population exposures to chemical substances. In this context, the current paper compares inhalation exposures to three health-based EU priority substances, i.e. benzene, formaldehyde and acetaldehyde. MATERIALS AND METHODS: Distributions of urban population inhalation exposures, indoor and outdoor concentrations were created on the basis of measured AIRMEX data in 12 European cities and compared to results from existing European population exposure studies published within the scientific literature. By pooling all EU city personal exposure, indoor and outdoor concentration means, representative EU city cumulative frequency distributions were created. Population exposures were modelled with a microenvironment model using the time spent and concentrations in four microenvironments, i.e. indoors at home and at work, outdoors at work and in transit, as input parameters. Pooled EU city inhalation exposures were compared to modelled population exposures. The contributions of these microenvironments to the total daily inhalation exposure of formaldehyde, benzene and acetaldehyde were estimated. Inhalation exposures were compared to the EU annual ambient benzene air quality guideline (5 microg/m3-to be met by 2010) and the recommended (based on the INDEX project) 30-min average formaldehyde limit value (30 microg/m3). RESULTS: Indoor inhalation exposure contributions are much higher compared to the outdoor or in-transit microenvironment contributions, accounting for almost 99% in the case of formaldehyde. The highest in-transit exposure contribution was found for benzene; 29.4% of the total inhalation exposure contribution. Comparing the pooled AIRMEX EU city inhalation exposures with the modelled exposures, benzene, formaldehyde and acetaldehyde exposures are 5.1, 17.3 and 11.8 microg/m3 vs. 5.1, 20.1 and 10.2 microg/m3, respectively. Together with the fact that a dominating fraction of time is spent indoors (>90%), the total inhalation exposure is mostly driven by the time spent indoors. DISCUSSION: The approach used in this paper faced three challenges concerning exposure and time-activity data, comparability and scarce or missing in-transit data inducing careful interpretation of the results. The results obtained by AIRMEX underline that many European urban populations are still exposed to elevated levels of benzene and formaldehyde in the inhaled air. It is still likely that the annual ambient benzene air quality guideline of 5 microg/m3 in the EU and recommended formaldehyde 30-min average limit value of 30 microg/m3 are exceeded by a substantial part of populations living in urban areas. Considering multimedia and multi-pathway exposure to acetaldehyde, the biggest exposure contribution was found to be related to dietary behaviour rather than to inhalation. CONCLUSIONS: In the present study, inhalation exposures of urban populations were assessed on the basis of novel and existing exposure data. The indoor residential microenvironment contributed most to the total daily urban population inhalation exposure. The results presented in this paper suggest that a significant part of the populations living in European cities exceed the annual ambient benzene air quality guideline of 5 microg/m3 in the EU and recommended (INDEX project) formaldehyde 30-min average limit value of 30 microg/m3. RECOMMENDATIONS AND PERSPECTIVES: To reduce exposures and consequent health effects, adequate measures must be taken to diminish emissions from sources such as materials and products that especially emit benzene and formaldehyde in indoor air. In parallel, measures can be taken aiming at reducing the outdoor pollution contribution indoors. Besides emission reduction, mechanisms to effectively monitor and manage the indoor air quality should be established. These mechanisms could be developed by setting up appropriate EU indoor air guidelines.

Sources of fine particulate matter in personal exposures and residential indoor, residential outdoor and workplace microenvironments in the Helsinki phase of the EXPOLIS study.

OBJECTIVES: This study assessed the source contributions to the mass concentrations of fine particles (PM2.5) in personal exposures and in residential indoor, residential outdoor, and workplace indoor microenvironments of the nonsmoking adult population unexposed to environmental tobacco smoke in Helsinki, Finland. METHODS: The elemental composition of 48-hour personal exposure and residential indoor, residential outdoor, and workplace indoor PM2.5 was analyzed by energy-dispersive X-ray fluorescence spectrometry for 76 participants not exposed to environmental tobacco smoke and 102 participating residences with no smoking in Helsinki as a part of the EXPOLIS study. Subsequently, a principal component analysis was used to identify the emission sources of PM2.5-bound elements and black smoke in each microenvironment, and this information was used to identify the corresponding sources in personal exposures. Finally, source reconstruction was done to determine the relative contributions of each source type to the total PM2.5 mass concentrations. RESULTS: Inorganic secondary particles, primary combustion, and soil were the dominant source types for the PM2.5 mass concentration in all the microenvironments and personal exposures. The ratio of the residential indoor-to-outdoor PM2.5 concentration was close to unity, but the corresponding elemental ratios and source contributions varied. Resuspension of soil dust tracked indoors was a much larger contributor to residential and workplace indoor PM2.5 than soil dust to residential outdoor PM2.5. Source contributions to personal PM2.5 exposures were best approximated by data from residential and workplace indoor microenvironments. CONCLUSIONS: Population exposure assessment of PM2.5, based on outdoor fixed-site monitoring, overestimates exposures to outdoor sources like traffic and long-range transport and does not account for the contribution of significant indoor sources.

Quantitative analysis of environmental factors in differential weighing of blank Teflon filters.

Mass differences less than 100 microg must be correctly measured in gravimetric analysis of particles collected on filters. Even small variations in mass measurement may contribute significant errors to calculated concentrations. In addition to the collected particles, a number of other factors affect the observed mass difference between the measurements before and after sampling. The most often controlled of these factors are static charge, temperature, and humidity. Using 951 laboratory blank filter weights, we have statistically analyzed these and other factors that affect the observed filter weight. Some of these are controllable or correctable; others are not and enter into the final results as errors. The standard deviation of differential blank filter weighing after applying all corrections was 2.7 microg. The most important correctable factors are air buoyancy variation and filter storage time. When weighing blank Teflon filters at relative humidity < 50%, these are an order of magnitude more important than weighing-room humidity. Using field blank filters in each weighing batch could control these three factors but also doubles the errors caused by balance random variation and filter handling contamination, because four weighing measurements and the handling of two filters are needed to obtain one corrected differential mass result.

Population exposure to fine particles and estimated excess mortality in Finland from an East European wildfire episode.

Long-range transported particulate matter (PM) air pollution episodes associated with wildfires in the Eastern Europe are relatively common in Southern and Southeastern Finland. In severe cases such as in August-September 2002, the reduced visibility and smell of the smoke, and symptoms such as irritation of eyes and airways experienced by the population raise the issue into the headlines. Because PM air pollution, in general, has been identified as a major health risk, and the exposures are of repeating nature, the issue warrants a risk assessment to estimate the magnitude of the problem. The current work uses the available air quality data in Finland to estimate population exposures caused by one of the worst episodes experienced in this decade. This episode originated from wildfires in Russia, Belarus, Ukraine, and the Baltic countries. The populations of 11 Southern Finnish provinces were exposed between 26 August and 8 September 2002, for 2 weeks to an additional population-weighted average PM(2.5) level of 15.7 microg/m(3). Assuming similar effect on mortality for these particles as observed in epidemiological time series studies on urban particles (0.5%-2% increase in mortality per 10 microg/m(3), central estimate 1%), this exposure level would be associated with 9-34 cases (17 cases central estimate) of additional mortality. Epidemiological evidence specific to particles from biomass combustion is scarce, affecting also the reliability of the current risk assessment. Do the wildfire aerosols exhibit the same level of toxicity as the urban particles? To shed light on this question, it is interesting to look at the exposure data in relationship to the observed daily mortality in Finland, even though the limited duration of the episode allows only for a weak statistical power. The percentage increases observed (0.8%-2.1% per 10 microg/m(3) of fine PM) are in line with the more general estimates for urban PM and those used in the current risk assessment.

Health effects caused by primary fine particulate matter (PM2.5) emitted from buses in the Helsinki metropolitan area, Finland.

Fine particle (PM(2.5)) emissions from traffic have been associated with premature mortality. The current work compares PM(2.5)-induced mortality in alternative public bus transportation strategies as being considered by the Helsinki Metropolitan Area Council, Finland. The current bus fleet and transportation volume is compared to four alternative hypothetical bus fleet strategies for the year 2020: (1) the current bus fleet for 2020 traffic volume, (2) modern diesel buses without particle traps, (3) diesel buses with particle traps, and (4) buses using natural gas engines. The average population PM(2.5) exposure level attributable to the bus emissions was determined for the 1996-1997 situation using PM(2.5) exposure measurements including elemental composition from the EXPOLIS-Helsinki study and similar element-based source apportionment of ambient PM(2.5) concentrations observed in the ULTRA study. Average population exposure to particles originating from the bus traffic in the year 2020 is assumed to be proportional to the bus emissions in each strategy. Associated mortality was calculated using dose-response relationships from two large cohort studies on PM(2.5) mortality from the United States. Estimated number of deaths per year (90% confidence intervals in parenthesis) associated with primary PM(2.5) emissions from buses in Helsinki Metropolitan Area in 2020 were 18 (0-55), 9 (0-27), 4 (0-14), and 3 (0-8) for the strategies 1-4, respectively. The relative differences in the associated mortalities for the alternative strategies are substantial, but the number of deaths in the lowest alternative, the gas buses, is only marginally lower than what would be achieved by diesel engines equipped with particle trap technology. The dose-response relationship and the emission factors were identified as the main sources of uncertainty in the model.

Comparison of black smoke and PM2.5 levels in indoor and outdoor environments of four European cities.

Recent studies on separated particle-size fractions highlight the health significance of particulate matter smaller than 2.5 microm (PM2.5), but gravimetric methods do not identify specific particle sources. Diesel exhaust particles (DEP) contain elemental carbon (EC), the dominant light-absorbing substance in the atmosphere. Black smoke (BS) is a measure for light absorption of PM and, thus, an alternative way to estimating EC concentrations, which may serve as a proxy for diesel exhaust emissions. We analyzed PM2.5 and BS data collected within the EXPOLIS study (Air Pollution Exposure Distribution within Adult Urban Populations in Europe) in Athens, Basel, Helsinki, and Prague. 186 indoor/outdoor filter pairs were sampled and analyzed. PM2.5 and BS levels were lowest in Helsinki, moderate in Basel, and remarkably higher in Athens and Prague. In each city, Spearman correlation coefficients of indoor versus outdoor were higher for BS (range rspearman: 0.57-0.86) than for PM2.5 (0.05-0.69). In a BS linear regression model (all data), outdoor levels explained clearly more of indoor variation (86%) than in the corresponding PM2.5 model (59%). In conclusion, ambient BS seizes a health-relevant fraction of fine particles to which people are exposed indoors and outdoors and exposure to which can be assessed by monitoring outdoor concentrations. BS measured on PM2.5 filters can be recommended as a valid and cheap additional indicator in studies on combustion-related air pollution and health.