Particle emission factors during cooking activities

Exposure to particles emitted by cooking activities may be responsible for a variety of respiratory health effects. However, the relationship between these exposures and their subsequent effects on health cannot be evaluated without understanding the properties of the emitted aerosol or the main parameters that influence particle emissions during cooking. Whilst traffic-related emissions, stack emissions and concentrations of ultrafine particles (UFPs, diameter < 100 nm) in urban ambient air have been widely investigated for many years, indoor exposure to UFPs is a relatively new field and in order to evaluate indoor UFP emissions accurately, it is vital to improve scientific understanding of the main parameters that influence particle number, surface area and mass emissions. The main purpose of this study was to characterise the particle emissions produced during grilling and frying as a function of the food, source, cooking temperature and type of oil. Emission factors, along with particle number concentrations and size distributions were determined in the size range 0.006–20 μm using a Scanning Mobility Particle Sizer (SMPS) and an Aerodynamic Particle Sizer (APS). An infrared camera was used to measure the temperature field. Overall, increased emission factors were observed to be a function of increased cooking temperatures. Cooking fatty foods also produced higher particle emission factors than vegetables, mainly in terms of mass concentration, and particle emission factors also varied significantly according to the type of oil used.     

Impact of particle emissions of new laser printers on modeled office room

In this study, we present how an indoor aerosol model can be used to characterize particle emitter and predict influence of the source on indoor air quality. Particle size-resolved emission rates were quantified and the source’s influence on indoor air quality was estimated by using office model simulations. We measured particle emissions from three modern laser printers in a flow-through chamber. Measured parameters were used as input parameters for an indoor aerosol model, which we then used to quantify the particle emission rates. The same indoor aerosol model was used to simulate the effect of the particle emission source inside an office model. The office model consists of a mechanically ventilated empty room and the particle source. The aerosol from the ventilation air was a filtered urban background aerosol. The effect of the ventilation rate was studied using three different ventilation ratios 1, 2 and 3 h^?1. According to the model, peak emission rates of the printers exceeded 7.0 × 10⁸ s^?1 (2.5 × 10¹² h^?1), and emitted mainly ultrafine particles (diameter less than 100 nm). The office model simulation results indicate that a print job increases ultrafine particle concentration to a maximum of 2.6 × 10⁵ cm^?3. Printer-emitted particles increased 6-h averaged particle concentration over eleven times compared to the background particle concentration.     

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).     

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).     

Deposition rates on smooth surfaces and coagulation of aerosol particles inside a test chamber

Because aerosol particle deposition is an important factor in indoor air quality, many empirical and theoretical studies have attempted to understand the process. In this study, we estimated the deposition rate of aerosol particles on smooth aluminum surfaces inside a test chamber. We investigated the influence of turbulent intensity due to ventilation and fan operation. We also investigated two important processes in particle deposition: turbophoresis, which is significant for micron particles, and coagulation, which is relevant to ultrafine particles (UFP diameter <0.1 μm) at high particle concentrations. Our analysis included semi-empirical estimates of the deposition rates that were compared to available deposition models and verified with simulations of an aerosol dynamics model. In agreement with previous studies, this study found that induced turbulent intensity greatly enhanced deposition rates of fine particles (FP diameter <1 μm). The deposition rate of FP was proportional to the ventilation rate, and it increased monotonically with fan speed. With our setup, turbophoresis was very important for coarse particles larger than 5 μm. The coagulation of aerosol particles was insignificant when the particle concentration was less than 10⁴ cm^?3 during fan operation. The model simulation results verified that the aerosol dynamics module incorporated in our Multi-Compartment and Size-Resolved Indoor Aerosol Model (MC-SIAM) was valid. The behavior of aerosol particles inside our chamber was similar to that found in real-life conditions with the same ventilation rates (0.018–0.39 h^?1) and similar air mixing modes. Therefore, our findings provide insight into indoor particle behavior.     

Modelling of indoor exposure to nitrogen dioxide in the UK

A dynamic multi-compartment computer model has been developed to describe the physical processes determining indoor pollutant concentrations as a function of outdoor concentrations, indoor emission rates and building characteristics. The model has been parameterised for typical UK homes and workplaces and linked to a time-activity model to calculate exposures for a representative homemaker, schoolchild and office worker, with respect to NO₂. The estimates of population exposures, for selected urban and rural sites, are expressed in terms of annual means and frequency of hours in which air quality standards are exceeded. The annual mean exposures are estimated to fall within the range of 5–21 ppb for homes with no source, and 21–27 ppb for homes with gas cooking, varying across sites and population groups. The contribution of outdoor exposure to annual mean NO₂ exposure varied from 5 to 24%, that of indoor penetration of outdoor air from 17 to 86% and that of gas cooking from 0 to 78%. The frequency of exposure to 1 h mean concentrations above 150 ppb was very low, except for people cooking with gas.     

Exposure assessment of air pollutants: a review on spatial heterogeneity and indoor/outdoor/personal exposure to suspended particulate matter,nitrogen dioxide and ozone

This review describes databases of small-scale spatial variations and indoor, outdoor and personal measurements of air pollutants with the main focus on suspended particulate matter, and to a lesser extent, nitrogen dioxide and photochemical pollutants. The basic definitions and concepts of an exposure measurement are introduced as well as some study design considerations and implications of imprecise exposure measurements. Suspended particulate matter is complex with respect to particle size distributions, the chemical composition and its sources. With respect to small-scale spatial variations in urban areas, largest variations occur in the ultrafine (<0.1 μm) and the coarse mode (PM_10–2.5, resuspended dust). Secondary aerosols which contribute to the accumulation mode (0.1–2 μm) show quite homogenous spatial distribution. In general, small-scale spatial variations of PM_2.5 were described to be smaller than the spatial variations of PM₁₀. Recent studies in outdoor air show that ultrafine particle number counts have large spatial variations and that they are not well correlated to mass data. Sources of indoor particles are from outdoors and some specific indoor sources such as smoking and cooking for fine particles or moving of people (resuspension of dust) for coarse particles. The relationships between indoor, outdoor and personal levels are complex. The finer the particle size, the better becomes the correlation between indoor, outdoor and personal levels. Furthermore, correlations between these parameters are better in longitudinal analyses than in cross-sectional analyses. For NO₂ and O₃, the air chemistry is important. Both have considerable small-scale spatial variations within urban areas. In the absence of indoor sources such as gas appliances, NO₂ indoor/outdoor relationships are strong. For ozone, indoor levels are quite small. The study hypothesis largely determines the choice of a specific concept in exposure assessment, i.e. whether personal sampling is needed or if ambient monitoring is sufficient. Careful evaluation of the validity and improvements in precision of an exposure measure reduce error in the measurements and bias in the exposure–effect relationship.     

Chamber studies on mass-transfer of di(2-ethylhexyl)phthalate (DEHP) and di-n-butylphthalate (DnBP) from emission sources into house dust

For a number of phthalates and especially for di(2-ethylhexyl)phthalate (DEHP), surprisingly high house dust concentrations are reported in the literature. Therefore, the uptake of the most prominent compounds DEHP and di-n-butylphthalate (DnBP) from plasticized indoor materials into house dust samples of different organic content has been experimentally determined. The experiments have been performed within 45 days which is sufficient for the more volatile phthalate (DnBP) to reach equilibrium conditions. DnBP reaches considerably higher concentrations in the chamber air compared to real room measurements and, thus, also elevated dust concentrations. In contrast, the mass transfer of DEHP in the dust via the gas phase was significantly lower. However, small chamber experiments showed elevated mass transfer of DEHP in case of direct contact between emission source and sink. This aspect is experimentally determined using an plasticized PVC polymer with and without direct contact to house dust. A transfer into the dust could be observed in dependence of the initial concentration in the material. However, the results do not allow the differentiation between the two uptake mechanisms via capillary forces and contact to the material’s boundary layer. The results illustrate that the reasons for elevated DEHP concentrations in dust indoors can be traced back to direct contact of source and sink, abrasion from the source, and transport via airborne particles.     

Indoor acrolein emission and decay rates resulting from domestic cooking events

Acrolein (2-propenal) is a common constituent of both indoor and outdoor air, can exacerbate asthma in children, and may contribute to other chronic lung diseases. Recent studies have found high indoor levels of acrolein and other carbonyls compared to outdoor ambient concentrations. Heated cooking oils produce considerable amounts of acrolein, thus cooking is likely an important source of indoor acrolein. A series of cooking experiments were conducted to determine the emission rates of acrolein and other volatile carbonyls for different types of cooking oils (canola, soybean, corn and olive oils) and deep-frying different food items. Similar concentrations and emission rates of carbonyls were found when different vegetable oils were used to deep-fry the same food product. The food item being deep-fried was generally not a significant source of carbonyls compared to the cooking oil. The oil cooking events resulted in high concentrations of acrolein that were in the range of 26.4–64.5 μg m^?3. These concentrations exceed all the chronic regulatory exposure limits and many of the acute exposure limits. The air exchange rate and the decay rate of the carbonyls were monitored to estimate the half-life of the carbonyls. The half-life for acrolein was 14.4 ± 2.6 h, which indicates that indoor acrolein concentrations can persist for considerable time after cooking in poorly-ventilated homes.     

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.     

The impact of building recirculation rates on secondary organic aerosols generated by indoor chemistry

Numerous investigators have documented increases in the concentrations of airborne particles as a consequence of ozone/terpene reactions in indoor environments. This study examines the effect of building recirculation rates on the concentrations of secondary organic aerosol (SOA) resulting from reactions between indoor limonene and ozone. The experiments were conducted in a large environmental chamber using four recirculation rates (11, 14, 19 and 24 air change per hour (ACH)) and a constant outdoor air exchange rate (1 ACH) as well as constant emission rates for limonene and ozone. As the recirculation rates increased, the deposition velocities of ozone and SOA increased. As a consequence of reduced production rates (due to less ozone) and larger surface removal rates, number and mass concentrations of SOA in different size ranges decreased significantly at higher recirculation rates. Enhanced coagulation at higher recirculation rates also reduced particle number concentrations, while shifting size-distributions towards larger particles. The results have health implications beyond changes in exposures, since particle size is a factor that determines where a particle deposits in the respiratory tract.     

Experimental evidence for a significant contribution of cellulose to indoor aerosol mass concentration

An apartment bedroom located in a residential area of Aveiro (Portugal) was selected with the aim of characterizing the cellulose content of indoor aerosol particles. Two sets of samples were taken: (1) PM₁₀ collected simultaneously in indoor and outdoor air; (2) PM₁₀ and PM_2.5 collected simultaneously in indoor air. The aerosol particles were concentrated on quartz fibre filters with low-volume samplers equipped with size selective inlets. The filters were weighed and then extracted for cellulose analysis by an enzymatic method. The average indoor cellulose concentration was 1.01 ± 0.24 μg m^?3, whereas the average outdoor cellulose concentration was 0.078 ± 0.047 μg m^?3, accounting for 4.0% and 0.4%, respectively, of the PM₁₀ mass. The corresponding average ratio between indoor and outdoor cellulose concentrations was 11.1 ± 4.9, indicating that cellulose particles were generated indoors, most likely due to the handling of cotton-made textiles as a result of routine daily activities in the bedroom. Indoor cellulose concentrations averaged 1.22 ± 0.53 μg m^?3 in the aerosol coarse fraction (determined from the difference between PM₁₀ and PM_2.5 concentrations) and averaged 0.38 ± 0.13 μg m^?3 in the aerosol fine fraction. The average ratio between the coarse and fine fractions of cellulose concentrations in the indoor air was 3.6 ± 2.1. This ratio is in line with the primary origin of this biopolymer. Results from this study provide the first experimental evidence in support of a significant contribution of cellulose to the mass of suspended particles in indoor air.     

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 relationship between indoor and outdoor airborne particles in the residential environment

The relationship between indoor and outdoor airborne particles was investigated for 16 residential houses located in a suburban area of Brisbane, Australia. The submicrometer particle numbers were measured using the Scanning Mobility Particle Sizer, the larger particle numbers using the Aerodynamic Particle Sizer and an approximation of PM_2.5 was also measured using a DustTrak. The measurements were conducted for normal and minimum ventilation conditions using simultaneous and non-simultaneous measurement methods designed for the purpose of the study. Comparison of the ratios of indoor to outdoor particle concentrations revealed that while temporary values of the ratio vary in a broad range from 0.2 to 2.5 for both lower and higher ventilation conditions, average values of the ratios were very close to one regardless of ventilation conditions and of particle size range. The ratios were in the range from 0.78 to 1.07 for submicrometer particles, from 0.95 to 1.0 for supermicrometer particles and from 1.01 to 1.08 for PM_2.5 fraction. Comparison of the time series of indoor to outdoor particle concentrations shows a clear positive relationship existing for many houses under normal ventilation conditions (estimated to be about and above 2 h⁻¹), but not under minimum ventilation conditions (estimated to be about and below 1 h⁻¹). These results suggest that for normal ventilation conditions, outdoor particle concentrations could be used to predict instantaneous indoor particle concentrations but not for minimum ventilation, unless air exchange rate is known, thus allowing for estimation of the “delay constant”.     

Continuous monitoring of ultrafine,fine, and coarse particles in a residence for 18 months in 1999-2000

Continuous monitors were employed for 18 months in an occupied townhouse to measure ultrafine, fine, and coarse particles; air change rates; wind speed and direction; temperature; and relative humidity (RH). A main objective was to document short-term and long-term variation in indoor air concentrations of size-resolved particles (0.01-20 microm) caused by (1) diumal and seasonal variation of outdoor air concentrations and meteorological variables, (2) indoor sources such as cooking and using candles, and (3) activities affecting air change rates such as opening windows and using fans. A second objective was to test and compare available instruments for their suitability in providing real-time estimates of particle levels and ancillary variables. Despite different measuring principles, the instruments employed in this study agreed reasonably well for particles less than 10 microm in diameter. The three instruments measuring fine and coarse particles (aerodynamic diameter between 0.3 and 20 microm) agreed to within 30% in their overall estimates of total volume. Two of these instruments employed optical scattering, and the third used an aerodynamic acceleration principle. However, several lines of evidence indicated that the instrument employing aerodynamic acceleration overestimated concentrations for particle diameters greater than 10 microm. A fourth instrument measuring ultrafine and accumulation-mode particles (0.01-1 microm) was operated with two different inlets providing somewhat different particle size ranges. The two inlets agreed in the ultrafine region (< 0.1 microm) but diverged increasingly for larger particles (up to 0.445 microm). Indoor sources affecting ultrafine particle concentrations were observed 22% of the time, and sources affecting fine and coarse particle concentrations were observed 12 and 15% of the time, respectively. When an indoor source was operating, particle concentrations for different sizes ranged from 2 to 20 times the average concentrations when no indoor source was apparent. Indoor sources, such as cooking with natural gas, and simple physical activities, such as walking, accounted for a majority (50-90%) of the ultrafine and coarse particle concentrations, whereas outdoor sources were more important for accumulation-mode particles between 0.1 and 1 microm in diameter. Averaged for the entire year and including no periods when indoor sources were apparent, the number distribution was bimodal, with a peak at approximately 10 nm (possibly smaller), a shallow minimum at approximately 14 nm, and a second broad peak at approximately 68 nm. The volume distribution was also bimodal, with a broad peak at approximately 200 nm, a minimum at approximately 1.2 microm, and then an upward slope again through the remaining size fractions. A database was created on a 5-min averaging time basis. It contains more than 90,000 measurements by two of the instruments and approximately 30,000 by the two optical scattering instruments. About 4500 hour-long average air change rates were also calculated throughout the year using a dedicated gas chromatograph with electron capture detection (GC/ECD). At high air change rates [> 0.8 air changes per hour (hr(-1))], particle concentrations were either elevated (when no source was present) or depressed (when an indoor source was operating) by factors of up to 2 compared with low air change rates.     

Effects of a constructional intervention on airborne and deposited particulate matter in the Portuguese National Tile Museum, Lisbon

In the 1970s, a large ambulatory of the National Tile Museum, Lisbon, was closed with glass panes on both ground and first floor. Although this design was meant to protect the museum collection from ambient air pollutants, small openings between the glass panes remain, creating a semi-enclosed corridor. The effects of the glass panes on the indoor air quality were evaluated in a comparative study by monitoring the airborne particle concentration and the extent of particle deposition at the enclosed corridor as well as inside the museum building. Comparison of the indoor/outdoor ratio of airborne particle concentration demonstrated a high natural ventilation rate in the enclosed corridor as well as inside the museum building. PM₁₀ deposition velocities on vertical surfaces were estimated in the order of 3?×?10^?4 m s^?1 for both indoor locations. Also, the deposition rates of dark-coloured and black particles in specific were very similar at both indoor locations, causing visual degradation. The effectiveness of the glass panes in protecting the museum collection is discussed.     

Characteristics of particulate matter emissions from toy cars with electric motors

Aerosol emissions from toy cars with electric motors were characterized. Particle emission rates from the toy cars, as high as 7.47 × 10⁷ particles/s, were measured. This emission rate is lower than other indoor sources such as smoking and cooking. The particles emitted from toy cars are generated from spark discharges inside the electric motors that power the toy cars. Size distribution measurements indicated that most particles were below 100 nm in diameter. Copper was the dominant inorganic species in these particles. By deploying aerosol mass spectrometers, high concentrations of particulate organic matter were also detected and characterized in detail. Several organic compounds were identified using a thermal desorption aerosol gas chromatography. The mass size distribution of particulate organic matter was bimodal. The formation mechanism of particulate organic matter from toy cars was elucidated.

Implications:?A possible new source of indoor air pollution, particles from electric motors in toy cars, was identified. This study characterized aerosol emissions from toy cars in detail. Most of these particles have a diameter less than 100 nm. Copper and some organics are the major components of these particles. Conditions that minimize these emissions were determined.     

Composition and mixing state of the urban background aerosol in the Rhein-Main area (Germany)

Size-resolved aerosol particle samples in the size range 0.1–10 μm aerodynamic diameter were collected in the years 2003 and 2004 at an urban background station in Mainz, Germany. Size, morphology, chemical composition and mixing state of more than 5400 individual particles of 7 selected sampling days were analyzed in detail by scanning electron microscopy and energy-dispersive X-ray microanalysis. In addition, transmission electron microscopy, aerosol mass spectrometry and atomic force microscopy were applied to obtain detailed information about the mixing state of the particles. The fine particle fraction (diameter<1 μm) is always dominated by complex secondary aerosol particles (⩾90% by number) independent from air mass origin. These particles are complex internal mixtures of ammonium and sodium sulfates, nitrates, and organic material. Between 20% and 40% of the complex secondary aerosol particles contain soot inclusions. The composition of the coarse particle fraction (>1 μm diameter) is strongly dependant on air mass history with variable abundances of complex secondary aerosol particles, aged sea salt, silicates, silicate mixtures, calcium sulfates, calcium sulfate/carbonate mixtures, calcium nitrate/carbonate mixtures, biological particles, and external soot.The dominance of complex secondary aerosol particles shows that reduction of the precursor gases is a major goal for successful reduction strategies for PM₁₀.     

Continuous Monitoring of Ultrafine,Fine, and Coarse Particles in a Residence for 18 Months in 1999-2000

Abstract

Continuous monitors were employed for 18 months in an occupied townhouse to measure ultrafine, fine, and coarse particles; air change rates; wind speed and direction; temperature; and relative humidity (RH). A main objective was to document short-term and long-term variation in indoor air concentrations of size-resolved particles (0.01-20 μm) caused by (1) diurnal and seasonal variation of outdoor air concentrations and meteorological variables, (2) indoor sources such as cooking and using candles, and (3) activities affecting air change rates such as opening windows and using fans. A second objective was to test and compare available instruments for their suitability in providing real-time estimates of particle levels and ancillary variables.

Despite different measuring principles, the instruments employed in this study agreed reasonably well for particles less than 10 μm in diameter. The three instruments measuring fine and coarse particles (aerodynamic diameter between 0.3 and 20 μm) agreed to within 30% in their overall estimates of total volume. Two of these instruments employed optical scattering, and the third used an aerodynamic acceleration principle. However, several lines of evidence indicated that the instrument employing aerodynamic acceleration overestimated concentrations for particle diameters greater than 10 μm. A fourth instrument measuring ultrafine and accumulation-mode particles (0.01-1 μm) was operated with two different inlets providing somewhat different particle size ranges. The two inlets agreed in the ultrafine region (<0.1 μm) but diverged increasingly for larger particles (up to 0.445 μm).

Indoor sources affecting ultrafine particle concentrations were observed 22% of the time, and sources affecting fine and coarse particle concentrations were observed 12 and 15% of the time, respectively. When an indoor source was operating, particle concentrations for different sizes ranged from 2 to 20 times the average concentrations when no indoor source was apparent. Indoor sources, such as cooking with natural gas, and simple physical activities, such as walking, accounted for a majority (50-90%) of the ultrafine and coarse particle concentrations, whereas outdoor sources were more important for accumulation-mode particles between 0.1 and 1 um in diameter. Averaged for the entire year and including no periods when indoor sources were apparent, the number distribution was bimodal, with a peak at ~10 nm (possibly smaller), a shallow minimum at ~14 nm, and a second broad peak at ~68 nm. The volume distribution was also bimodal, with a broad peak at ~200 nm, a minimum at ~1.2 μm, and then an upward slope again through the remaining size fractions.

A database was created on a 5-min averaging time basis. It contains more than 90,000 measurements by two of the instruments and approximately 30,000 by the two optical scattering instruments. About 4500 hour-long average air change rates were also calculated throughout the year using a dedicated gas chromatograph with electron capture detection (GC/ECD). At high air change rates [>0.8 air changes per hour (hr^?1)], particle concentrations were either elevated (when no source was present) or depressed (when an indoor source was operating) by factors of up to 2 compared with low air change rates.     

The Mass Distribution of Large Atmospheric Particles

This paper describes the results of a study to determine the total mass and the mass distribution of atmospheric aerosols, especially that mass associated with particles greater than 10 μm diameter. This study also determined what fraction of the total aerosol mass a standard high-volume air sampler collects and what fraction and size interval settle out on a dust fall plate. A special aerosol sampling system was designed for this study to obtain representative samples of large airborne particles. A suburban sampling site was selected because no local point sources of aerosols existed nearby. Samples were collected under various conditions of wind velocity and direction to obtain measurements on different types of aerosols.

Study measurements show that atmospheric particulate matter has a bimodal mass distribution. Mass associated with large particles mainly ranged from 5 to 100 μm in size, while mass associated with small particles ranged from an estimated 0.03 to 5 μm in size. Combined, these two distributions produced a bimodal mass distribution with a minimum around 5 μm diameter. The high-volume air sampler was found to collect most of the total aerosol mass, not just that fraction normally considered suspended particulate. Dust fall plates did not provide a good or very useful measure of total aerosol mass. The two fundamental processes of aerosol formation, condensation and dispersion appear to account for the formation of a bimodal mass distribution in both natural and anthropogenic aerosols. Particle size distribution measurements frequently are in error because representative samples of large airborne particles are not obtained. Considering this descrepancy, air pollution regulations should specify or be based upon an upper particle size limit.