Estimating separately personal exposure to ambient and nonambient particulate matter for epidemiology and risk assessment: why and how

This paper discusses the legal and scientific reasons for separating personal exposure to PM into ambient and nonambient components. It then demonstrates by several examples how well-established models and data typically obtained in exposure field studies can be used to estimate both individual and community average exposure to ambient-generated PM (ambient PM outdoors plus ambient PM that has infiltrated indoors), indoor-generated PM, and personal activity PM. Ambient concentrations are not highly correlated with personal exposure to nonambient PM or total PM but are highly correlated with personal exposure to ambient-generated PM. Therefore, ambient concentrations may be used in epidemiology as an appropriate surrogate for personal exposure to ambient-generated PM. Suggestions are offered as to how exposure to ambient-generated PM may be obtained and used in epidemiology and risk assessment.     

Estimating Separately Personal Exposure to Ambient and Nonambient Particulate Matter for Epidemiology and Risk Assessment: Why and How

ABSTRACT

This paper discusses the legal and scientific reasons for separating personal exposure to PM into ambient and nonambient components. It then demonstrates by several examples how well-established models and data typically obtained in exposure field studies can be used to estimate both individual and community average exposure to ambient-generated PM (ambient PM outdoors plus ambient PM that has infiltrated indoors), indoor-generated PM, and personal activity PM. Ambient concentrations are not highly correlated with personal exposure to nonambient PM or total PM but are highly correlated with personal exposure to ambient-generated PM. Therefore, ambient concentrations may be used in epidemiology as an appropriate surrogate for personal exposure to ambient-generated PM. Suggestions are offered as to how exposure to ambient-generated PM may be obtained and used in epidemiology and risk assessment.     

Inorganic and carbonaceous components in indoor/outdoor particulate matter in two residential houses in Oslo, Norway

A detailed analysis of indoor/outdoor physicochemical aerosol properties has been performed. Aerosol measurements were taken at two dwellings, one in the city center and the other in the suburbs of the Oslo metropolitan area, during summer/fall and winter/spring periods of 2002-2003. In this paper, emphasis is placed on the chemical characteristics (water-soluble ions and carbonaceous components) of fine (PM2.5) and coarse (PM2.5-10) particles and their indoor/outdoor relationship. Results demonstrate that the carbonaceous species were dominant in all fractions of the PM10 particles (cut off size: 0.09-11.31 microm) during all measurement periods, except winter 2003, when increased concentrations of water-soluble inorganic ions were predominant because of sea salt transport. The concentration of organic carbon was higher in the fine and coarse PM10 fractions indoors, whereas elemental carbon was higher indoors only in the coarse fraction. In regards to the carbonaceous species, local traffic and secondary organic aerosol formation were, probably, the main sources outdoors, whereas indoors combustion activities such as preparation of food, burning of candles, and cigarette smoking were the main sources. In contrast, the concentrations of water-soluble inorganic ions were higher outdoors than indoors. The variability of water-soluble inorganic ion concentrations outdoors was related to changes in emissions from local anthropogenic sources, long-range transport of particles, sea salt emissions, and resuspension of roadside and soil dusts. In the indoor environment the infiltration of the outdoor air indoors was the major source of inorganic ions.     

Modeling exposure to particulate matter

Exposure assessment, a component of risk assessment, links sources of pollution with health effects. Exposure models are scientific tools used to gain insights into the processes affecting exposure assessment. The purpose of this paper is to review the process and methodology of estimating inhalation exposure to particulate matter (PM) using various types of models. Three types of models are discussed in the paper. Indirect type of models are physical models that employ inventories of outdoor and indoor sources and their emission rates to identify major sources contributing to exposure to PM, and use fate and transport and indoor air quality models to estimate PM concentrations at receptor sites. PM concentrations and time spent by a subject at each receptor site are input variables to the conventional exposure model that estimates the desired exposure levels. Direct type models use measured exposure or exposure concentrations in conjunction with information obtained from questionnaires to formulate exposure regression models. Stochastic models use exposure measurements, estimates can also be used, to formulate exposure population distributions and investigate associated uncertainty and variability. Since models developed using databases from western countries are not necessarily applicable in developing countries, the difference in requirements among western and developing countries is highlighted in the paper. Employment of exposure modeling methods in developing countries requires development of local information. Such information includes local outdoor and indoor source inventories, local or regional meteorological conditions, adjustment of indoor models to reflect local building construction conditions, and use of questionnaires to obtain local time budget and activity patterns of the subject population.     

Sources of personal exposure to fine particles in Toronto, Ontario, Canada

Individuals are exposed to particulate matter from both indoor and outdoor sources. The aim of this study was to compare the relative contributions of three sources of personal exposure to fine particles (PM2.5) by using chemical tracers. The study design incorporated repeated 24-hr personal exposure measurements of air pollution from 28 cardiac-compromised residents of Toronto, Ontario, Canada. Each study participant wore the Rupprecht & Patashnick ChemPass Personal Sampling System 1 day a week for a maximum of 10 weeks. During their individual exposure measurement days the subjects reported to have spent an average of 89% of their time indoors. Particle phase elemental carbon, sulfate, and calcium personal exposure data were used in a mixed-effects model as tracers for outdoor PM2.5 from traffic-related combustion, regional, and local crustal materials, respectively. These three sources were found to contribute 13% +/- 10%, 17% +/- 16%, and 7% +/- 6% of PM2.5 exposures. The remaining fraction of the personal PM2.5 is hypothesized to be predominantly related to indoor sources. For comparison, central site outdoor PM2.5 measurements for the same dates as personal measurements were used to construct a receptor model using the same three tracers. In this case, traffic-related combustion, regional, and local crustal materials were found to contribute 19% +/- 17%, 52% +/- 22%, and 10% +/- 7%, respectively. Our results indicate that the three outdoor PM2.5 sources considered are statistically significant contributors to personal exposure to PM2.5. Our results also suggest that among the Toronto subjects, who spent a considerable amount of time indoors, exposure to outdoor PM2.5 includes a greater relative contribution from combustion sources compared with outdoor PM2.5 measurements where regional sources are the dominant contributor.     

Estimating the concentration of indoor particles of outdoor origin: A review

Recent toxicological results highlight the importance of separating exposure to indoor- and outdoor-generated particles, due to their different physicochemical and toxicological properties. In this framework, a number of studies have attempted to estimate the relative contribution of particles of indoor and outdoor origins to indoor concentrations, using either statistical analysis of indoor and outdoor concentration time-series or mass balance equations. The aim of this work is to review and compare the methodologies developed in order to determine the ambient particle infiltration factor (F _INF) (i.e., the fraction of ambient particles that enter indoors and remains suspended). The different approaches are grouped into four categories according to their methodological principles: (1) steady-state assumption using the steady-state form of the mass balance equation; (2) dynamic solution of the mass balance equation using complex statistical techniques; (3) experimental studies using conditions that simplify model calculations (e.g., decreasing the number of unknowns); and (4) infiltration surrogates using a particulate matter (PM) constituent with no indoor sources to act as surrogate of indoor PM of outdoor origin. Examination of the various methodologies and results reveals that estimating infiltration parameters is still challenging. The main difficulty lies in the separate calculation of penetration efficiency (P) and deposition rate (k). The values for these two parameters that are reported in the literature vary significantly. Deposition rate presents the widest range of values, both between studies and size fractions. Penetration efficiency seems to be more accurately calculated through the application of dynamic models. Overall, estimates of the infiltration factor generated using dynamic models and infiltration surrogates show good agreement. This is a strong argument in favor of the latter methodology, which is simple and easy to apply when chemical speciation data are available.

Implications: ?Taking into account that increased health risks may be related with ambient particles, a reliable estimation of the main parameters governing ambient particle infiltration indoors may assist towards the development of appropriate regulation and control measures, targeted to specific sources/factors contributing to increased exposures. The overall study of the methodological approaches estimating particle infiltration indoors suggests that dynamic models provide a more complete and realistic picture of ambient particle infiltration indoors, whereas the use of specific PM constituents to act as surrogates of indoor particles of outdoor origin seems also a promising new methodology.     

Future year ozone source attribution modeling study using CMAQ-ISAM

ABSTRACT

To achieve the current United States National Ambient Air Quality Standards (NAAQS) attainment level for ozone or particulate matter, current photochemical air quality models include tools to determine source apportionment and/or source sensitivity. Previous studies by the authors have used the Ozone and Particulate Matter Source Apportionment Technology and Higher-order Decoupled Direct Method probing tools in CAMx to investigate these source-receptor relationships for ozone. The recently available source apportionment for CMAQ, referred to as the Integrated Source Apportionment Method (ISAM), was used in this study to conduct future year (2030) source attribution modeling. The CMAQ-ISAM ozone source attribution results for selected cities across the U.S. showed boundary conditions were the dominant contributor to the future year highest July maximum daily 8-hour average (MDA8) ozone concentrations. Point sources were generally larger contributors in the eastern U.S. than in the western U.S. The contributions of on-road mobile emissions were around 5 ppb at most of the cities selected for analysis. Off-road mobile source contributions were around 20 ppb or nearly 30%. Since boundary conditions play an important role in future year ozone levels, it is important to characterize future year boundary conditions accurately. The current implementation of ISAM in CMAQ 5.0.2 requires significant computing resources for ozone source attribution, making it difficult to conduct long-term simulations for large domains. The computing requirements for PM source attribution are even more onerous. CMAQ 5.2 was released after this study was completed, and does not include ISAM. If an efficient version of ISAM becomes available, it could be used in long-term ozone and PM2.5 studies. Implications: Ozone source attribution results provide useful information on important emission source contribution categories and provide some initial guidance on future emission reduction strategies. This study explains a new source apportionment technique, CMAQ-ISAM, and compares it to CAMx OSAT. The techniques have similar results: ozone’s highest source contributor is boundary conditions, followed by point sources, then off-road mobile sources. The current version of ISAM in CMAQ 5.0.2 requires significant computing resources for ozone source attribution, while the computing requirements for PM source attribution are even more onerous. CMAQ 5.2 was released after this study was completed, and does not include ISAM.     

DEARS particulate matter relationships for personal,indoor, outdoor,and central site settings for a general population

This analysis provides the initial summary of PM_2.5 mass concentrations relationships for all seasons and participants for a general population in the Detroit Exposure and Aerosol Research Study (DEARS). The summary presented highlights the utility of the new methodologies applied, in addition to summarizing the particulate matter (PM) data.Results include the requirement to adjust the exposure data for monitor wearing compliance and measured environmental tobacco smoke (ETS) levels, even though the study design specified a non-smoking household. A 40% wearing compliance acceptance level was suggested as necessary to balance minimizing exposure misclassification (from poor compliance) and having sufficient data to conduct robust statistical analyses. An ETS threshold level equivalent to adding more than 1.5 μg m^?3 to the collected sample was found to be necessary to detect changes in the personal exposure factor (F_pex). It is not completely clear why such a large threshold level was necessary.Statistically significant spatial PM_2.5 gradients were identified in three of the six DEARS neighborhoods in Wayne County. These were expected, given the number of strong, localized PM sources in the Detroit (Michigan) metro area. Some residential outdoor bias levels compared with the central site at Allen Park exceeded 15%. After adjusting for ETS biases, the outdoor contributions to the personal exposure were typically larger by factors from 1.75 to 2.2 compared with those of the non-outdoor sources. The outdoor contribution was larger in the summer than in the winter, which is consistent with the fractions of time spent outdoors in the summer vs. the winter (6.7% vs. 1.1% of the time).Mean personal PM_2.5 cloud levels for the general population DEARS cohort ranged from 1.5 to 3.8 (after ETS adjustment) and were comparable to those reported previously. The personal exposure collections indoors were typically at least 13 times greater than those contributed outdoors.     

Inorganic and Carbonaceous Components in Indoor/Outdoor Particulate Matter in Two Residential Houses in Oslo,Norway

Abstract

A detailed analysis of indoor/outdoor physicochemical aerosol properties has been performed. Aerosol measurements were taken at two dwellings, one in the city center and the other in the suburbs of the Oslo metropolitan area, during summer/fall and winter/spring periods of 2002–2003. In this paper, emphasis is placed on the chemical characteristics (water-soluble ions and carbonaceous components) of fine (PM_2.5) and coarse (PM_2.5–10) particles and their indoor/outdoor relationship. Results demonstrate that the carbonaceous species were dominant in all fractions of the PM₁₀ particles (cut off size: 0.09–11.31 μm) during all measurement periods, except winter 2003, when increased concentrations of water-soluble inorganic ions were predominant because of sea salt transport. The concentration of organic carbon was higher in the fine and coarse PM₁₀ fractions indoors, whereas elemental carbon was higher indoors only in the coarse fraction. In regards to the carbonaceous species, local traffic and secondary organic aerosol formation were, probably, the main sources outdoors, whereas indoors combustion activities such as preparation of food, burning of candles, and cigarette smoking were the main sources. In contrast, the concentrations of water-soluble inorganic ions were higher outdoors than indoors. The variability of water-soluble inorganic ion concentrations outdoors was related to changes in emissions from local anthropogenic sources, long-range transport of particles, sea salt emissions, and resuspension of roadside and soil dusts. In the indoor environment the infiltration of the outdoor air indoors was the major source of inorganic ions.     

Comparative health impact assessment of local and regional particulate air pollutants in Scandinavia

The ongoing program Clean Air for Europe (CAFE) is an initiative from the EU Commission to establish a coordinated effort to reach better air quality in the EU. The focus is on particulate matter as it has been shown to have large impact on human health. CAFE requested that WHO make a review of the latest findings on air pollutants and health to facilitate assessments of the different air pollutants and their health effects. The WHO review project on health aspects of air pollution in Europe confirmed that exposure to particulate matter (PM), despite the lower levels we face today, still poses a significant risk to human health. Using the recommended uniform risk coefficients for health impact assessment of PM, regardless of sources, premature mortality related to long-range transported anthropogenic particles has been estimated to be about 3500 deaths per year for the Swedish population, corresponding to a reduction in life expectancy of up to about seven months. The influence of local sources is more difficult to estimate due to large uncertainties when linking available risk coefficients to exposure data, but the estimates indicate about 1800 deaths brought forward each year with a life expectancy reduction of about 2-3 months. However, some sectors of the population are exposed to quite high locally induced concentrations and are likely to suffer excessive reductions in life expectancy. Since the literature increasingly supports assumptions that combustion related particles are associated with higher relative risks, further studies may shift the focus for abatement strategies. CAFE sets out to establish a general cost effective abatement strategy for atmospheric particles. Our results, based on studies of background exposure, show that long-range transported sulfate rich particles dominate the health effects of PM in Sweden. The same results would be found for the whole of Scandinavia and many countries influenced by transboundary air pollution. However, several health studies, including epidemiological studies with a finer spatial resolution, indicate that engine exhaust particles are more damaging to health than other particles. These contradictory findings must be understood and source specific risk estimates have to be established by expert bodies, otherwise it will not be possible to find the most cost effective abatement strategy for Europe. We are not happy with today's situation where every strategy to reduce PM concentrations is estimated to have the same impact per unit change in the mass concentration. Obviously there is a striking need to introduce more specific exposure variables and a higher geographical resolution in epidemiology as well as in health impact assessments.     

Improving bioaerosol exposure assessments of composting facilities — Comparative modelling of emissions from different compost ages and processing activities

We present bioaerosol source term concentrations from passive and active composting sources and compare emissions from green waste compost aged 1, 2, 4, 6, 8, 12 and 16 weeks. Results reveal that the age of compost has little effect on the bioaerosol concentrations emitted for passive windrow sources. However emissions from turning compost during the early stages may be higher than during the later stages of the composting process. The bioaerosol emissions from passive sources were in the range of 10³–10⁴ cfu m⁻³, with releases from active sources typically 1-log higher. We propose improvements to current risk assessment methodologies by examining emission rates and the differences between two air dispersion models for the prediction of downwind bioaerosol concentrations at off-site points of exposure. The SCREEN3 model provides a more precautionary estimate of the source depletion curves of bioaerosol emissions in comparison to ADMS 3.3. The results from both models predict that bioaerosol concentrations decrease to below typical background concentrations before 250 m, the distance at which the regulator in England and Wales may require a risk assessment to be completed.     

The influences of ambient particle composition and size on particle infiltration in Los Angeles, CA, residences

Particle infiltration is a key determinant of the indoor concentrations of ambient particles. Few studies have examined the influence of particle composition on infiltration, particularly in areas with high concentrations of volatile particles, such as ammonium nitrate (NH4NO3). A comprehensive indoor monitoring study was conducted in 17 Los Angeles-area homes. As part of this study, indoor/outdoor concentration ratios during overnight (nonindoor source) periods were used to estimate the fraction of ambient particles remaining airborne indoors, or the particle infiltration factor (FINF), for fine particles (PM2.5), its nonvolatile (i.e., black carbon [BC]) and volatile (i.e., nitrate [NO3-]) components, and particle sizes ranging between 0.02 and 10 microm. FINF was highest for BC (median = 0.84) and lowest for NO3- (median = 0.18). The low FINF for NO3- was likely because of volatilization of NO3- particles once indoors, in addition to depositional losses upon building entry. The FINF for PM2.5 (median = 0.48) fell between those for BC and NO3-, reflecting the contributions of both particle components to PM25. FINF varied with particle size, air-exchange rate, and outdoor NO3- concentrations. The FINF for particles between 0.7 and 2 microm in size was considerably lower during periods of high as compared with low outdoor NO3- concentrations, suggesting that outdoor NO3- particles were of this size. This study demonstrates that infiltration of PM2.5 varies by particle component and is lowest for volatile species, such as NH4NO3. Our results suggest that volatile particle components may influence the ability for outdoor PM concentrations to represent indoor and, thus, personal exposures to particles of ambient origin, because volatilization of these particles causes the composition of PM2.5 to differ indoors and outdoors. Consequently, particle composition likely influences observed epidemiologic relationships based on outdoor PM concentrations, especially in areas with high concentrations of NH4NO3 and other volatile particles.     

Characterisation of urban inhalation exposures to benzene,formaldehyde and acetaldehyde in the European Union

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.     

Toxic Trace Elements Associated with Airborne Particulate Matter: A Review

This article provides a concise review of published literature pertaining to sampling and analytical methodologies, aerometric studies, source identification techniques and modeling activities for the elements arsenic, cadmium, nickel, lead, vanadium, zinc, cobalt, chromium, copper, iron, mercury, manganese, selenium and antimony, and their compounds, associated with airborne particulate matter. Sampling techniques discussed include filtration and inertial separation. Analytical methodologies such as atomic absorption and atomic emission spectrometry, neutron activation analysis, and X-ray fluorescence spectrometry are summarized. Data on atmospheric levels of 14 trace elements are presented in summary form from numerous studies in remote, rural and urban areas, and generally indicate that concentrations measured at rural locations are several orders of magnitude lower than those measured for urban areas. Source identification methodologies are discussed in terms of advantages and disadvantages, and various applications are cited for the following categories: size differentiation, enrichment factors, chemical mass balance, and multivariate models. Provided that reliable trace element data are available for both the source and the receptor, chemical mass balance and multivariate methods can account for up to 80 percent of all sources contributing to the observed ambient air concentration. Wet and dry deposition processes are reviewed and environmental measurement data are provided for each element for remote, rural and urban locations. Both wet and dry deposition fluxes need to be considered for trace elements when estimating the total annual amounts of various trace elements deposited at a particular locale. Global cycles and trace element budgets are introduced in the context of the types of models currently in use. Limitations include inadequate global scale surveys of heavy metal concentrations and the lack of knowledge of sources and/or sinks.     

Estimating the Effect of Being Indoors on Total Personal Exposure to Outdoor Air Pollution

A personal air quality model (PAQM) has been developed to estimate the effect of being indoors on total personal exposure to outdoor-generated air pollution. Designed to improve air toxics risk assessment, PAQM accounts for individual hourly activity patterns, indoor-outdoor differences, physical exercise level, and geographic location for up to 56 different population groups. Unique hourly activity profiles are specified for each population group; group members are assigned each hour to one of up to 10 different indoor and outdoor microenvironments. To illustrate PAQM use, we apply it to two example cases: a long-term example representative of situations where pollutant health impact is related to integrated exposure (as in the case of potentially carcinogenic air toxics) and a short-term example representative of situations where health impact is related to acute exposure to peak concentrations (as with ozone).

Case study results illustrate that personal exposure, and thus health risk, attributable to outdoor-generated air pollution is sensitive to indoor-outdoor differences and population mobility. Where health impact is related to long-term integrated exposure (e.g., air toxics), exposure and subsequent risk are likely to be lower than that estimated by previous modeling techniques which do not account for such effects.     

Personal monitoring of exposure to particulate matter with a high temporal resolution

Background

Continuous monitoring of air quality is implemented by government institutions at fixed ambient sites. However, the correlation between fixed site measurements and exposure of individual persons to air contaminants is likely to be weak.

Materials and methods

We measured particulate matter both outdoors and indoors by following the spatial movement of individuals. Sixteen test persons took part and carried a measurement backpack for a 24-h period. The backpack was comprised of a Grimm Aerosol Spectrometer model 1.109, a GPS device, and a video camera for tracking of human behavior. The spectrometer provided information about particle numbers and mass in 32-size classes with a high temporal resolution of 6 s.

Results

The personal exposure of individuals during 24 h could significantly exceed the outdoor particulate matter (PM)₁₀ concentrations measured at the fixed sites. The average 24-h exposure of all test persons for PM₁₀ varied from 27 to 322 ??g m^?3. Environmental tobacco smoke and cooking emissions were among the main indoor sources for PM. The amount of particulate matter a test person was exposed to was highly dependent on the spatial behavior and the surrounding microenvironment conditions.

Discussion

Large-scale experiments including personal measurements might help to improve modeling approaches to approximate the actual exposure on a statistically sound basis.     

Bayesian hierarchical modeling of personal exposure to particulate matter

In the US EPA's 1998 Baltimore Epidemiology-Exposure Panel Study, a group of 16 residents of a single building retirement community wore personal monitors recording personal fine particulate air pollution concentrations (PM_2.5) for 27 days, while other monitors recorded concurrent apartment, central indoor, outdoor and ambient site PM_2.5 concentrations. Using the Baltimore panel study data, we develop a Bayesian hierarchical model to characterize the relationship between personal exposure and concentrations of PM_2.5 indoors and outdoors. Personal exposure is expressed as a linear combination of time spent in microenvironments and associated microenvironmental concentrations. The model incorporates all available monitoring data and accounts for missing data and sources of uncertainty such as measurement error and individual differences in exposure. We discuss the implications of using personal versus ambient PM_2.5 measurements in characterization of personal exposure to PM_2.5.     

Source contributions to fine particulate matter in an urban atmosphere

This paper proposes a practical method for estimating source attribution by using a three-step methodology. The main objective of this study is to explore the use of the three-step methodology for quantifying the source impacts of 24-h PM2.5 particles at an urban site in Seoul, Korea. 12-h PM2.5 samples were collected and analyzed for their elemental composition by ICP-AES/ICP-MS/AAS to generate the source composition profiles. In order to assess the daily average PM2.5 source impacts, 24-h PM2.5 and polycyclic aromatic hydrocarbons (PAH) ambient samples were simultaneously collected at the same site. The PM2.5 particle samples were then analyzed for trace elements. Ionic and carbonaceous species concentrations were measured by ICP-AES/ICP-MS/AAS, IC, and a selective thermal MnO2 oxidation method. The 12-h PM2.5 chemical data was used to estimate possible source signatures using the principal component analysis (PCA) and the absolute principal component scores method followed by the multiple linear regression analysis. The 24-h PM2.5 source categories were extracted with a combination of PM2.5 and some PAH chemical data using the PCA, and their quantitative source contributions were estimated by chemical mass balance (CMB) receptor model using the estimated source profiles and those in the literature. The results of PM2.5 source apportionment using the 12-h derived source composition profiles show that the CMB performance indices; chi2, R2, and percent of mass accounted for are 2.3%, 0.97%, and 100.7%, which are within the target range specified. According to the average PM2.5 source contribution estimate results, motor vehicle exhaust was the major contributor at the sampling site, contributing 26% on average of measured PM2.5 mass (41.8 microg m-3), followed by secondary sulfate (23%) and nitrate (16%), refuse incineration (15%), soil dust (13%), field burning (4%), oil combustion (2.7%), and marine aerosol (1.3%). It can be concluded that quantitative source attribution to PM2.5 in an urban area where source profiles have not been developed can be estimated using the proposed three-step methodology approach.     

Use of a continuous nephelometer to measure personal exposure to particles during the U.S. Environmental Protection Agency Baltimore and Fresno Panel studies

In population exposure studies, personal exposure to PM is typically measured as a 12- to 24-hr integrated mass concentration. To better understand short-term variation in personal PM exposure, continuous (1-min averaging time) nephelometers were worn by 15 participants as part of two U.S. Environmental Protection Agency (EPA) longitudinal PM exposure studies conducted in Baltimore County, MD, and Fresno, CA. Participants also wore inertial impactor samplers (24-hr integrated filter samples) and recorded their daily activities in 15-min intervals. In Baltimore, the nephelometers correlated well (R2 = 0.66) with the PM2.5 impactors. Time-series plots of personal nephelometer data showed each participant's PM exposure to consist of a series of peaks of relatively short duration. Activities corresponding to a significant instrument response included cooking, outdoor activities, transportation, laundry, cleaning, shopping, gardening, moving between microenvironments, and removing/putting on the instrument. On average, 63-66% of the daily PM exposure occurred indoors at home (about 2/3 of which occurred during waking hours), primarily due to the large amount of time spent in that location (an average of 72-77%). Although not a reference method for measuring mass concentration, the nephelometer did help identify PM sources and the relative contribution of those sources to an individual's personal exposure.     

Source investigation of personal particulates in relation to identify major routes of exposure among urban residentials

Multiple 24-h average outdoor, indoor and personal respirable particulate matter (RPM) measurements were made in different urban residential colonies to determine major routes of personal exposure. The study area was Bhilai-Durg, District Durg, Chhattisgarh, India. About 100 residentials from each of two selected colonies have been surveyed for consent to participate in the study and for preparation of time–activity diary. On the basis of their time–activity diary, residentials have been categorized into three types: type-A, purely residential; type-B, residents who go out, and type-C, residence who go into work, specially in industrial area. A total of 28 adult participants (14 males and 14 females; mean age 40±15, range 21–61 years) were selected and monitored longitudinally during the summer (15 March–15 June) of 2004. Participants’ residential indoor RPM level and also local ambient outdoor RPM levels were measured,and these are done simultaneous with personal monitoring. Residential indoor and ambient outdoors RPM monitoring sessions were throughout the year to obtain infiltration factor more precisely. To compare RPM levels with Indian National Ambient Air Quality Standards (NAAQS) of PM₁₀, simultaneous measurements of PM₁₀ were also done with the course of ambient outdoor RPM monitoring. RPM levels in indoors were higher compared to ambient outdoors. The annual average ratio RPM/PM₁₀ was found to vary significantly among residential sites due to variation in surroundings. Source contribution estimates (SCE) of personal exposure to RPM in selected 12 residences (six from each colony) have been investigated using chemical mass balance model CMB8. Ambient outdoors, residential indoors, soils and road-traffic borne RPM were identified as main routes and principal sources of personal RPM. Results of model output have shown that residential indoors and soil-borne RPM are the major routes of personal exposure.