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.     

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.     

Characteristics of indoor aerosols in residential homes in urban locations: a case study in Singapore

As part of a major study to investigate the indoor air quality in residential houses in Singapore, intensive aerosol measurements were made in an apartment in a multistory building for several consecutive days in 2004. The purpose of this work was to identify the major indoor sources of fine airborne particles and to assess their impact on indoor air quality for a typical residential home in an urban area in a densely populated country. Particle number and mass concentrations were measured in three rooms of the home using a real-time particle counter and a low-volume particulate sampler, respectively. Particle number concentrations were found to be elevated on several occasions during the measurements. All of the events of elevated particle concentrations were linked to indoor activities based on house occupant log entries. This enabled identification of the indoor sources that contributed to indoor particle concentrations. Activities such as cooking elevated particle number concentrations < or =2.05 x 10(5) particles/cm3. The fine particles collected on Teflon filter substrates were analyzed for selected ions, trace elements, and metals, as well as elemental and organic carbon (OC) contents. To compare the quality of air between the indoors of the home and the outdoors, measurements were also made outside the home to obtain outdoor samples. The chemical composition of both outdoor and indoor particles was determined. Indoor/outdoor (I/O) ratios suggest that certain chemical constituents of indoor particles, such as chloride, sodium, aluminum, cobalt, copper, iron, manganese, titanium, vanadium, zinc, and elemental carbon, were derived through migration of outdoor particles (I/O <1 or - 1), whereas the levels of others, such as nitrite, nitrate, sulfate, ammonium, cadmium, chromium, nickel, lead, and OC, were largely influenced by the presence of indoor sources (I/O >1).     

The transformation of outdoor ammonium nitrate aerosols in the indoor environment

Recent studies associate particulate air pollution with adverse health effects; however, the exposure to indoor particles of outdoor origin is not well characterized, particularly for individual chemical species. We conducted a field study in an unoccupied, single-story residence in Clovis, California to provide data and analyses to address issues important for assessing exposure. We used real-time particle monitors both outdoors and indoors to quantify nitrate, sulfate, and carbon particulate matter of particle size 2.5 μm or less in diameter (PM-2.5). The results show that measured indoor ammonium nitrate concentrations were significantly lower than would be expected based solely on penetration and deposition losses. The additional reduction can be attributed to the transformation indoors of ammonium nitrate into ammonia and nitric acid gases, which are subsequently lost by deposition and sorption to indoor surfaces. A mass balance model that accounts for the kinetics of ammonium nitrate evaporation was able to reproduce measured indoor ammonium nitrate and nitric acid concentrations, resulting in a fitted value of the deposition velocity for nitric acid of 0.56 cm s⁻¹. The results indicate that indoor exposure to outdoor ammonium nitrate in Central Valley of California are small, and suggest that exposure assessments based on total particle mass measured outdoors may obscure the actual causal relationships for indoor exposure to particles of outdoor origin.     

Characteristics of Indoor Aerosols in Residential Homes in Urban Locations: A Case Study in Singapore

Abstract

As part of a major study to investigate the indoor air quality in residential houses in Singapore, intensive aerosol measurements were made in an apartment in a multistory building for several consecutive days in 2004. The purpose of this work was to identify the major indoor sources of fine airborne particles and to assess their impact on indoor air quality for a typical residential home in an urban area in a densely populated country. Particle number and mass concentrations were measured in three rooms of the home using a real-time particle counter and a low-volume particulate sampler, respectively. Particle number concentrations were found to be elevated on several occasions during the measurements. All of the events of elevated particle concentrations were linked to indoor activities based on house occupant log entries. This enabled identification of the indoor sources that contributed to indoor particle concentrations. Activities such as cooking elevated particle number concentrations ≤2.05 × 10⁵ particles/cm³. The fine particles collected on Teflon filter substrates were analyzed for selected ions, trace elements, and metals, as well as elemental and organic carbon (OC) contents. To compare the quality of air between the indoors of the home and the outdoors, measurements were also made outside the home to obtain outdoor samples. The chemical composition of both outdoor and indoor particles was determined. Indoor/outdoor (I/O) ratios suggest that certain chemical constituents of indoor particles, such as chloride, sodium, aluminum, cobalt, copper, iron, manganese, titanium, vanadium, zinc, and elemental carbon, were derived through migration of outdoor particles (I/O<1 or ≈1), whereas the levels of others, such as nitrite, nitrate, sul-fate, ammonium, cadmium, chromium, nickel, lead, and OC, were largely influenced by the presence of indoor sources (I/O >1).     

Indoor/outdoor relationships for ambient PM2.5 and associated pollutants: epidemiological implications in Lindon, Utah

Outdoor and indoor fine particulate species were measured at the Lindon Elementary School in Lindon, Utah, to determine which components of ambient fine particles have strong indoor and outdoor concentration correlations. PM2.5 mass concentrations were measured using tapered element oscillating microbalance (TEOM) monitors and by gravimetric analysis of Teflon filter samples. Gas-phase HNO3, sulfur dioxide, particulate nitrate, strong acid, and particulate sulfate were measured using annular denuder samplers. Soot was measured using quartz filters in filter packs. Total particulate number was measured with a condensation nucleus counter (CNC). Total particulate number and fine particulate sulfate and soot were correlated for ambient and indoor measurements. Indoor PM2.5 mass showed a low correlation with outdoor PM2.5 mass because of the influence of coarse material from student activities on indoor PM2.5. Fine particle acidity and the potentiation of biological oxidative mechanisms by iron were not correlated indoors and outdoors.     

Modeling particle loss in ventilation ducts

Empirical equations were developed and applied to predict losses of 0.01–100 μm airborne particles making a single pass through 120 different ventilation duct runs typical of those found in mid-sized office buildings. For all duct runs, losses were negligible for submicron particles and nearly complete for particles larger than 50 μm. The 50th percentile cut-point diameters were 15 μm in supply runs and 25 μm in return runs. Losses in supply duct runs were higher than in return duct runs, mostly because internal insulation was present in portions of supply duct runs, but absent from return duct runs. Single-pass equations for particle loss in duct runs were combined with models for predicting ventilation system filtration efficiency and particle deposition to indoor surfaces to evaluate the fates of particles of indoor and outdoor origin in an archetypal mechanically ventilated building. Results suggest that duct losses are a minor influence for determining indoor concentrations for most particle sizes. Losses in ducts were of a comparable magnitude to indoor surface losses for most particle sizes. For outdoor air drawn into an unfiltered ventilation system, most particles smaller than 1 μm are exhausted from the building. Large particles deposit within the building, mostly in supply ducts or on indoor surfaces. When filters are present, most particles are either filtered or exhausted. The fates of particles generated indoors follow similar trends as outdoor particles drawn into the building.     

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.     

Effects of soil moisture and physical-chemical properties of organic pollutants on vapor-phase transport in the vadose zone

Vapor-phase transport of organic pollutants is one of the important pathways in the distribution and attenuation of volatile organic compounds in the vadose zone. In this study, the impact of vapor-phase partitioning and of the physical-chemical properties of organic pollutants on vapor-phase transport was assessed. An experimentally derived relationship to predict vapor sorption for a variety of soil types under varying soil moisture conditions was incorporated into the two-dimensional finite-element model, Vocwaste. The revised model was then used to simulate the transport of volatile organics. Vapor-phase partitioning in the model accounted for vapor uptake by sorption onto moist mineral surfaces as well as sorption at the liquid-solid interface and dissolution into soil water. Under dry conditions, vapor-phase sorption of volatile organic pollutants was shown to have a retarding effect on transport of organic vapors. However, for shallow, contaminated soils, volatilization was controlled by vapor diffusion, even under dry conditions where vapor-phase sorption was high. The influence of Henry's law constant and of the aqueous-phase (solid-liquid) partition coefficient for volatile organic pollutants was considered in the simulations. Volatilization of organic vapors was shown to be favored for contaminants with high Henry's law constants and low aqueous-phase partitioning coefficients. Because of the interdependence of these two physical-chemical properties, individual properties of the contaminant should not be considered in isolation in the evaluation of vapor transport.     

The South Karelia Air Pollution Study: Relationship of Outdoor and Indoor Concentrations of Malodorous Sulfur Compounds Released by Pulp Mills

We studied the indoor penetration of ambient air malodorous sulfur compounds released by pulp mills. The indoor and outdoor concentrations were simultaneously measured with automatic SO₂ analyzers. The filtering effect of three different materials connected to a gaseous filter unit was tested during six study periods. The tested materials were Sorbixofil® based on gypsum impregnated by KMnO₄ Purafil® based on Al₂O₃, both absorbing sulfur compounds by oxidation, and carbonized tissue. The periods lasted from 14 to 88 days. The results indicated that malodorous sulfur air pollutants penetrated indoors effectively, but after some delay because the dilution was slow. In a comparison of different filter materials, Purafil® was the most effective, producing low indoor concentrations. The study concludes that people living near pulp mills are exposed to substantial amounts of malodorous air pollutants, both indoors and outdoors. This exposure can be reduced by using gaseous sulfur sensitive filter materials connected to a controlled ventilation system.     

A new detailed chemical model for indoor air pollution

A detailed chemical box model has been constructed based on a comprehensive chemical mechanism (the Master Chemical Mechanism) to investigate indoor air chemistry in a typical urban residence in the UK. Unlike previous modelling studies of indoor air chemistry, the mechanism adopted contains no simplifications such as lumping or the use of surrogate species, allowing more insight into indoor air chemistry than previously possible. The chemical mechanism, which has been modified to include the degradation reactions of key indoor air pollutants, contains around 15,400 reactions and 4700 species. The results show a predicted indoor OH radical concentration up to 4.0×10⁵ molecule cm⁻³, only a factor of 10–20 less than typically observed outdoors and sufficient for significant chemical cycling to take place. Concentrations of PAN-type species and organic nitrates are found to be important indoors, reaching concentrations of a few ppb. Sensitivity tests highlight that the most crucial parameters for modelling the concentration of OH are the light-intensity levels and the air exchange rate. Outdoor concentrations of O₃ and NO_X are also important in determining radical concentrations indoors. The reactions of ozone with alkenes and monoterpenes play a major role in producing new radicals, unlike outdoors where photolysis reactions are pivotal radical initiators. In terms of radical propagation, the reaction of HO₂ with NO has the most profound influence on OH concentrations indoors. Cycling between OH and RO₂ is dominated by reaction with the monoterpene species, whilst alcohols play a major role in converting OH to HO₂. Surprisingly, the absolute reaction rates are similar to those observed outdoors in a suburban environment in the UK during the summer. The results from this study highlight the importance of tailoring a model for its particular location and the need for future indoor air measurements of radical species, nitrated species such as PANs and organic nitrates, photolysis rates of key species over the range of wavelengths observed indoors and concurrent measurements of outdoor air pollutant concentrations.     

Dust build-up on surfaces in the indoor environment

The concentration and the composition of dust in the indoor environment has been associated with reported symptoms of the sick building syndrome. Levels of airborne concentrations of dust particles are well known. However, the relation to dust on surfaces for office environments are not well described. In this study, 662 measurements were performed of surface dust concentrations on hard surfaces in 19 buildings within Harvard University based on a sticking gelatine foil method. The measure is the dust covered area of the surface as a percentage. In three offices, the build-up of dust on surfaces was measured for a period of five days. Close to these surfaces the airborne PM_2.5 and PM₁₀ particle mass concentrations were measured simultanously. A significant correlation between the dust build-up and the difference between the PM₁₀ and the PM_2.5 was established. The particle size distribution was measured by means of an Aerodynamic Particle Sizer. The mean dust build-up normalized with the measured PM₁₀ was approximately four times higher than the equivalent calculated by a deposition model. This may in part be due to the effect of preferred orientation when particles settle to a surface. Different data for dust on surfaces and airborne particles in offices were compared. The levels of airborne particles in offices in Europe seem to be higher than the levels in the US.     

Measurement of fine particulate matter nonvolatile and semi-volatile organic material with the Sunset Laboratory Carbon Aerosol Monitor

Semi-volatile organic material (SVOM) in fine particles is not reliably measured with conventional semicontinuous carbon monitors because SVOM is lost from the collection media during sample collection. We have modified a Sunset Laboratory Carbon Aerosol Monitor to allow for the determination of SVOM. In a conventional Sunset monitor, gas-phase organic compounds are removed in the sampled airstream by a diffusion denuder employing charcoal-impregnated cellulose filter (CIF) surfaces. Subsequently, particles are collected on a quartz filter and the instrument then determines both the organic carbon and elemental carbon fractions of the aerosol using a thermal/optical method. However, some of the SVOM is lost from the filter during collection, and therefore is not determined. Because the interfering gas-phase organic compounds are removed before aerosol collection, the SVOM can be determined by filtering the particles at the instrument inlet and then replacing the quartz filter in the monitor with a charcoal-impregnated glass fiber filter (CIG), which retains the SVOM lost from particles collected on the inlet filter. The resulting collected SVOM is then determined in the analysis step by measurement of the carbonaceous material thermally evolved from the CIG filter. This concept was tested during field studies in February 2003 in Lindon, UT, and in July 2003 in Rubidoux, CA. The results obtained were validated by comparison with Particle Concentrator-Brigham Young University Organic Sampling System (PC-BOSS) results. The sum of nonvolatile organic material determined with a conventional Sunset monitor and SVOM determined with the modified Sunset monitor agree with the PC-BOSS results. Linear regression analysis of total carbon concentrations determined by the PC-BOSS and the Sunset resulted in a zero-intercept slope of 0.99 +/- 0.02 (R2 = 0.92) and a precision of sigma = +/- 1.5 microg C/m3 (8%).     

Air Pollution In Pittsburgh: A Historical Perspective

Sources and concentrations of indoor air pollutants and aeroallergens were evaluated in the arid Southwest community of Tucson, Arizona. One major purpose was to appraise the interaction of indoor and outdoor human exposures. A rough time budget study showed that 74% of adults spent 75% or more of their time in some indoor environment. Outdoor and indoor concentrations of TSP, RSP, CO, O₃ and aeroallergens were measured for 41 detached dwellings. Small area and basin monitoring occurred for TSP, CO, NO₂, O₃ and aeroallergens; ambient TSP frequently exceeds NAAQS and both CO and O3 do occasionally. Indoor TSP and RSP were lower than outdoors and were of a different composition. Outdoor infiltration falls rapidly for particles and pollen, related to distance Indoors. CO was low and O₃ was very low indoors. TSP and RSP correlated significantly with tobacco smoking and CO correlated with gas stove usage. Temperature varied minimally indoors and relative humidity indoors was similar to outdoor readings In this climate. It was concluded that better particle characterization and better estimates of total exposure are required.     

The influence of aerosol dynamics on indoor exposure to airborne DEHP

A mass-balance model was extended to investigate the influence of aerosol particles on the accumulation of indoor airborne DEHP, which allows the consideration of a variable particle concentration. The calculated gas-phase di-2-ethylhexyl phthalate (DEHP) concentration is consistent with those measured within residences in both the United States and Europe. Model predictions suggest that there are differences of more than 10% of particle-phase DEHP concentrations between the variable-particle-concentration case and the constant one for over half (578 days) within the calculation time of 1000 days. Airborne DEHP consists primarily of a particle phase. The exposure data indicate that the influence of particle dynamics remains significant throughout the calculation period, and the size fraction of 0–0.5 μm contributes the most, at 39.1%, to the total exposure to particle-phase DEHP as a result of a strong “source” effect which brings particles into the indoor air and a weak “sink” effect which removes particles from the indoor air. The sensitivity analysis indicates that deposition exhibits the most apparent influence, and particle emission from cooking is a significant factor, as cooking is the main source of particles in the size fraction of 0–0.5 μm. The sensitivity analysis also shows that particle penetration has a less obvious influence on the exposure to airborne DEHP because air exchange rate caused penetration introduces and removes particles simultaneously, thus having a limited influence on the airborne DEHP; while resuspension exhibits the weakest influence because it contributes little to the small particles which are the main component of aerosol particles indoors. Strategies for enhancing deposition and reducing particle emissions from cooking and penetration may be helpful to reduce residents’ exposure to airborne SVOCs.     

Exposure of population and microenvironmental distributions of volatile organic compound concentrations in the EXPOLIS study

Determination of volatile organic compounds (VOCs) formed one part of the EU-EXPOLIS project in which the exposure of European urban populations to particles and gaseous pollutants was studied. The EXPOLIS study concentrated on 30 target VOCs selected on the basis of environmental and health significance and usability of the compounds as markers of pollution sources. In the project, 201 subjects in Helsinki, 50 in Athens, 50 in Basel, 50 in Milan and, 50 in Oxford and 50 in Prague were selected for the final exposure sample. The microenvironmental and personal exposure concentrations of VOCs were the lowest in Helsinki and Basel, while the highest concentrations were measured in Athens and Milan; Oxford and Prague were in between. In all cities, home indoor air was the most significant exposure agent. Workplace indoor air concentrations measured in this study were generally lower than the home indoor concentrations and home outdoor air played a minor role as an exposure agent. When estimating the measured personal exposure concentrations using the measured concentrations and time fractions spent at home indoors, at home outdoors, and at the workplace, it could be concluded that these three microenvironments do not fully explain the personal exposure. Other important sources for personal exposure must be encountered, the most important being traffic/transportation and other indoor environments not measured in this study.     

VOCs in representative canadian residences

Stored extracts of passive samplers exposed in 757 randomly selected Canadian residences provided a unique opportunity for retrospective determination of the occurrence of airborne volatile organic compounds (VOCs). Aliquots of the individual extracts were pooled to form a composite exposure sample and a corresponding blank sample. To identify and quantitate potentially hazardous organics in the samples, GC-MS analyses were conducted by several approaches. The amounts of 52 target compounds in the the composite sample were estimated based on selected ion monitoring (SIM) results, extraction recoveries, average air volume sampled, and 3M OVM 3500 passive sampling rates. Forty of the organics were detected and were present in amounts equivalent to airborne concentrations ranging from <1 to 104 μg m⁻³. Several other compounds were also tentatively identified by full scan analysis. Many of the detected organics have been reported to be associated with activities such as tobacco smoking and the presence of consumer products and plastic materials indoors. The analytical results have been useful in risk assessments and establishment of a new Canadian priority substances list (PSL).     

Nicotine as a Marker for Environmental Tobacco Smoke: Implications of Sorption on Indoor Surface Materials

ABSTRACT

Recently developed models and data describing the interactions of gas-phase semi-volatile organic compounds with indoor surfaces are employed to examine the effects of sorption on nicotine's suitability as an environmental tobacco smoke (ETS) marker. Using parameters from our studies of nicotine sorption on carpet, painted wallboard, and stainless steel and previously published data on ETS particle deposition, the dynamic behavior of nicotine was modeled in two different indoor environments: a house and a stainless steel chamber. The results show that apparently contradictory observations of nicotine's behavior in indoor air can be understood by considering the effects of sorption under different experimental conditions. In indoor environments in which smoking has occurred regularly for an extended period, the sorbed mass of nicotine is very large relative to the mass emitted by a single cigarette. The importance of nicotine adsorption relative to ventilation as a gas-phase removal mechanism is reduced. Where smoking occurs less regularly or the indoor surfaces are cleaned prior to smoking (as in a laboratory chamber), nicotine deposition is more significant. Nicotine concentrations closely track the levels of other ETS constituents in environments with habitual smoking if the data are averaged over a period significantly longer than the period between cigarette combustion episodes. However, nicotine is not a suitable tracer for predicting ETS exposures at fine time scales or in settings where smoking occurs infrequently and irregularly.     

The Influences of Ambient Particle Composition and Size on Particle Infiltration in Los Angeles,CA, Residences

Abstract

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 (F_INF), for fine particles (PM_2.5), its nonvolatile (i.e., black carbon [BC]) and volatile (i.e., nitrate [NO₃ ^?]) components, and particle sizes ranging between 0.02 and 10 μm. F_INF was highest for BC (median = 0.84) and lowest for NO₃ ^? (median = 0.18). The low F_INF for NO₃ ^? was likely because of volatilization of NO₃ ^? particles once indoors, in addition to depositional losses upon building entry. The F_INF for PM_2.5 (median = 0.48) fell between those for BC and NO₃ ^?, reflecting the contributions of both particle components to PM_2.5. F_INF varied with particle size, air-exchange rate, and outdoor NO₃ ^? concentrations. The F_INF for particles between 0.7 and 2 μm 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 PM_2.5 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 PM_2.5 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.