Effects of physical/environmental factors on fine particle (PM(2.5)) exposure, outdoor-to-indoor transport and air exchange rate (AER) were examined. The fraction of ambient PM(2.5) found indoors (F(INF)) and the fraction to which people are exposed (alpha) modify personal exposure to ambient PM(2.5). Because F(INF), alpha, and AER are infrequently measured, some have used air conditioning (AC) as a modifier of ambient PM(2.5) exposure. We found no single variable that was a good predictor of AER. About 50% and 40% of the variation in F(INF) and alpha, respectively, was explained by AER and other activity variables. AER alone explained 36% and 24% of the variations in F(INF) and alpha, respectively. Each other predictor, including Central AC Operation, accounted for less than 4% of the variation. This highlights the importance of AER measurements to predict F(INF) and alpha. Evidence presented suggests that outdoor temperature and home ventilation features affect particle losses as well as AER, and the effects differ.Total personal exposures to PM(2.5) mass/species were reconstructed using personal activity and microenvironmental methods, and compared to direct personal measurement. Outdoor concentration was the dominant predictor of (partial R(2) = 30-70%) and the largest contributor to (20-90%) indoor and personal exposures for PM(2.5) mass and most species. Several activities had a dramatic impact on personal PM(2.5) mass/species exposures for the few study participants exposed to or engaged in them, including smoking and woodworking. Incorporating personal activities (in addition to outdoor PM(2.5)) improved the predictive power of the personal activity model for PM(2.5) mass/species; more detailed information about personal activities and indoor sources is needed for further improvement (especially for Ca, K, OC). Adequate accounting for particle penetration and persistence indoors and for exposure to non-ambient sources could potentially increase the power of epidemiological analyses linking health effects to particulate exposures.
The indoor environment is an important venue for exposure to fine particulate matter (PM2.5) of ambient (outdoor) origin. In this work, paired indoor and outdoor PM2.5 species concentrations from three geographically distinct cities (Houston, TX, Los Angeles County, CA, and Elizabeth, NJ) were analyzed using positive matrix factorization (PMF) and demonstrate that the composition and source contributions of ambient PM2.5 are substantially modified by outdoor-to-indoor transport. Our results suggest that predictions of "indoor PM2.5 of ambient origin" are improved when ambient PM2.5 is treated as a combination of four distinct particle types with differing infiltration behavior (primary combustion, secondary sulfate and organics, secondary nitrate, and mechanically generated PM) rather than as a "single internally mixed entity". Study-wide average infiltration factors (i.e., fraction of ambient PM2.5 found indoors) for Relationship of Indoor, Outdoor, and Personal Air (RIOPA) study homes were 0.51, 0.78, and 0.04 (consistent with P = 0.6, 0.9, and 0.09; k = 0.2, 0.1, and 0.6 h(-1)) for PM2.5 associated with primary combustion, secondary formation (excluding nitrate), and mechanical generation, respectively. Modification of the composition, properties, and source contributions of ambient PM2.5 in indoor environments has important implications for exposure mitigation strategies, development of health hypotheses, and evaluation of exposure error in epidemiological studies that use ambient central-site PM2.5 as a surrogate for PM2.5 exposure.
During the study Relationships of Indoor, Outdoor, and Personal Air (RIOPA*), 48-hour integrated indoor, outdoor, and personal air samples were collected between summer 1999 and spring 2001 in three different areas of the United States: Elizabeth NJ, Houston TX, and Los Angeles County CA. Air samples suitable for analyzing particulate matter 2.5 microm or smaller in aerodynamic diameter (PM2.5) were collected in 219 homes (twice in 169 homes). Indoor and outdoor air samples suitable for gas-phase and particle-phase organic analyses were collected in 152 homes (twice in 132 homes). Samples or subsets of samples were analyzed for PM2.5 mass, organic functional groups, elements, organic carbon (OC), elemental carbon (EC), gas-phase and particle-phase polycyclic aromatic hydrocarbons (PAHs), and chlordanes. Air exchange rate (AER), temperature, and relative humidity were measured for each residence; questionnaire data and time-activity information were collected from the participants. Median indoor, outdoor, and personal PM2.5 mass concentrations were 14.4, 15.5, and 31.4 microg/m3, respectively. Personal PM2.5 concentrations were significantly higher and more variable than indoor and outdoor concentrations. Several approaches were applied to quantify indoor PM2.5 of ambient (outdoor) and nonambient (indoor) origin, some using PM2.5 mass concentrations and others using PM2.5 species concentrations. PM of outdoor origin was estimated in three ways using increasingly accurate assumptions. Comparing estimates from the three approaches enabled us to quantify several types of errors that may be introduced when central-site PM concentrations are used as surrogate estimates for PM exposure. Estimates made using individual measurements produced broader distributions and higher means than those made using a single infiltration factor for all homes and days. The best estimate (produced by the robust regression approach) of the mean contribution of outdoor PM2.5 to the indoor mass concentration was 73% and to personal exposure was 26%. Possible implications of exposure error for epidemiologic assessments of PM are discussed below. Organic particulate matter was the major constituent of PM2.5 generated indoors. After correcting for artifacts, it constituted 48%, 55%, and 61% of PM2.5 mass inside study homes in Los Angeles, Elizabeth, and Houston, respectively. At least 40% but probably closer to 75% of this organic matter, on average, was emitted or formed indoors. Functional group analysis provided some insights into the composition and properties of the indoor-generated organic PM2.5. Chlordane, a very minor but mutagenic semivolatile organic mixture previously used as a termiticide, was found to be mostly of indoor origin. High emission rates were most frequently found in homes built from 1945 to 1959. Analysis of the change in gas-particle partitioning during transport of outdoor PAHs to indoor environments illustrated that chemical thermodynamics can alter the concentration and composition of outdoor PM as it is transported indoors. (This has been previously noted for nitrate [Lunden et al 2003].) In epidemiologic studies that rely on central-site monitoring data, such transformations may result in measurement error, and this possibility warrants further investigation.
The functional group (FG) composition of urban residential outdoor, indoor, and personal fine particle (PM2.5) samples is presented and used to provide insights relevant to organic PM2.5 exposure. PM2.5 samples (48 h) were collected during collected, and FG absorbances were quantified by partial least squares (PLS) regression, a multivariate calibration method.There is growing evidence in the literature that a large majority of indoor-generated PM2.5 is organic. The current research suggests that indoor-generated PM2.5 is enriched in aliphatic carbon-hydrogen (CH) FGs relative to ambient outdoor PM2.5. Indoor-generated CH exceeded outdoor-generated CH in 144 of the 167 homes for which indoor or outdoor CH was measurable; estimated indoor emission rates are provided. The strong presence of aliphatic CH FGs in indoor PM2.5 makes particulate organic matter substantially less polar indoors and in personal exposures than outdoors. This is a substantial new finding. Based on the quantified FGs, the average organic molecular weight (OM) per carbon weight (OC), a measure of the degree of oxygenation of organic PM, is in the range of 1.7-2.6 for outdoor samples and 1.3-1.7 for indoor and personal samples. Polarity or degree of oxygenation effects particle deposition in exposure environments and in the respiratory system. (C) 2007 Elsevier Ltd. All rights reserved.
Ambient volatile organic compound concentrations outside residences were measured in Elizabeth, New Jersey as part of the Relationship of Indoor, Outdoor, and Personal A:r (RIOPA) study to assess the influence of proximity of the residences to known ambient emissions sources. The closest distances between the outdoor samplers and emission sources were determined using Geographic Information Systems (GIS)techniques. Multiple regression models were developed for residential ambient concentrations of aromatic hydrocarbons (BTEX), methyl tert butyl ether (MTBE), and tetrachloroethylene (PCE). The natural log transformed ambient concentrations of BTEX were inversely associated with distances to major roadways with high traffic densities and gasoline stations, atmospheric stability, temperature, and wind speed. Ambient MTBE levels were associated with inverse distance to gas stations and interstate highways. Residential ambient PCE concentration was inversely associated with distance to dry cleaning facilities, atmospheric stability, temperature, wind speed, and relative humidity. The linear regression models that include proximity to emission sources and meteorological variables explained 16-45% of the overall variation of ambient residential VOC concentrations. Meteorological conditions, especially atmospheric stability and temperature, explained 60-90% of the total variation in the regression models. The residential ambient air concentrations were 1.5-4 times higher than the urban background levels outside homes very close (<50 m) to ambient emission sources where approximately 7% of the population live. However, the relative increase of risk for disease is small and variations in air concentration in the background urban atmosphere are greater than those from the proximity to roadways.
Residential indoor and outdoor fine particle (PM2.5) organic (OC) and elemental carbon (EC) concentrations (48 h) were measured at 173 homes in Houston, TX, Los Angeles County, CA, and Elizabeth, NJ as part of the Relationship of Indoor, Outdoor and Personal Air (RIOPA) study. The adsorption of organic vapors on the quartz fiber sampling filter (a positive artifact) was substantial indoors and out, accounting for 36% and 37% of measured OC at the median indoor (8.2 μg C/m3) and outdoor (5.0 μg C/m3) OC concentrations, respectively. Uncorrected, adsorption artifacts would lead to substantial overestimation of particulate OC both indoors and outdoors. After artifact correction, the mean particulate organic matter (OM=1.4 OC) concentration indoors (9.8 μg/m3) was twice the mean outdoor concentration (4.9 μg/m3). The mean EC concentration was 1.1 μg/m3 both indoors and outdoors. OM accounted for 29%, 30% and 29% of PM2.5 mass outdoors and 48%, 55% and 61% of indoor PM2.5 mass in Los Angeles Co., Elizabeth and Houston study homes, respectively. Indirect evidence provided by species mass balance results suggests that PM2.5 nitrate (not measured) was largely lost during outdoor-to-indoor transport, as reported by Lunden et al. This results in dramatic changes with outdoor-to-indoor transport in the mass and composition of ambient-generated PM2.5 at California homes. On average, 71% to 76% of indoor OM was emitted or formed indoors, calculated by (1) Random Component Superposition (RCS) model and (2) non-linear fit of OC and air exchange rate data to the mass balance model. Assuming that all particles penetrate indoors (P=1) and there is no particle loss indoors (k=0), a lower bound estimate of 41% of indoor OM was indoor-generated (mean). OM appears to be the predominant species in indoor-generated PM2.5, based on species mass balance results. Particulate OM emitted or formed indoors is substantial enough to alter the concentration, composition and behavior of indoor PM2.5. One interesting effect of increased indoor OM concentrations is a shift in the gas-particle partitioning of polycyclic aromatic hydrocarbons (PAHs) from the gas to the particle phase with outdoor-to-indoor transport.
This study on the relationships of indoor, outdoor, and personal air (RIOPA) was undertaken to collect data for use in evaluating the contribution of outdoor sources of air toxics and particulate matter (PM) to personal exposure. The study was not designed to obtain a population-based sample, but rather to provide matched indoor, outdoor, and personal concentrations in homes that varied in their proximity to outdoor pollution sources and had a wide range of air exchange rates (AERs). This design allowed examination of relations among indoor, outdoor, and personal concentrations of air toxics and PM across a wide range of environmental conditions; the resulting data set obtained for a wide range of environmental pollutants and AERs can be used to evaluate exposure models. Approximately 100 households with residents who do not smoke participated in each of three cities in distinct locations expected to have different climates and housing characteristics: Elizabeth, New Jersey; Houston, Texas; and Los Angeles County, California. Questionnaires were administered to characterize homes, neighborhoods, and personal activities that might affect exposures. The concentrations of a suite of volatile organic compounds (VOCs) and carbonyl compounds, as well as the fraction of airborne particulate matter with a mass median aerodynamic diameter < or = 2.5 microm (PM2.5), were measured during continuous 48-hour sessions in which indoor, outdoor, and personal air samples were collected simultaneously. During the same 48-hour period, the AER (exchanges/hr; x hr(-1)) was determined in each home, and carbonyl compounds were measured inside vehicle cabins driven by a subset of the participants. In most of the homes, measurements were made twice, during two different seasons, to obtain a wide distribution of AERs. This report presents in detail the data collection methods, quality control measures, and initial analyses of data distributions and relations among indoor, outdoor, and personal concentrations. The results show that indoor sources dominated personal and indoor air concentrations of many measured VOCs and carbonyl compounds. For several measured species, personal concentrations were higher than either indoor or outdoor concentrations, indicating the presence of some sources closely related to personal activities. For some species there were no significant indoor sources in the majority of the homes; thus indoor concentrations were mainly determined by outdoor concentrations in these homes. The range of distributions of air concentrations for the measured VOCs, formaldehyde and acetaldehyde, PM2.5, and AERs were generally consistent with values reported previously in the literature. Thus associations derived from or models based on this data set that may link the influence of outdoor sources with indoor air concentrations of air toxics and PM2.5 can be relevant to other urban settings. The simultaneous measurements of indoor concentrations, outdoor concentrations, AERs, and room volumes allowed the use of a mass balance model, under the steady-state approximation, to mechanistically examine the relative contributions of indoor and outdoor sources to measured indoor concentrations on a home-by-home basis. Estimated indoor source strengths for VOCs and carbonyl compounds varied widely from home to home, consistent with the indoor-outdoor concentration patterns, as shown in scatter plots. The indoor source estimations agreed with published values for PM2.5 and with the general understanding of sources of VOCs and carbonyl compounds. The source strengths reported here, derived from hundreds of homes, are an important contribution to the literature on exposure to air toxics. For the first time for many compounds, these estimates present a cohesive set of measurements across a range of air toxics in paired indoor, outdoor, and personal samples along with AER and questionnaire results that can be used for future analyses of indoor air quality. The estimation of outdoor contributions to measured indoor concentrations provides insights about the relative importance of indoor and outdoor sources in determining indoor concentrations, the main determinant of personal exposure for most of the measured compounds. In this report simple statistical tests mainly of the pooled data were used to analyze differences by sampling site, emission source type, season, home type, and home age. Paired adult-child personal concentrations within the same home were also compared using the pooled data set. These analyses generated some intriguing results that warrant more in-depth investigation in the future.
Real-time and integrated measurements of gaseous and particulate pollutants were conducted inside five conventional diesel school buses, a diesel bus with a particulate trap, and a bus powered by compressed natural gas (CNG) to determine the range of children's exposures during school bus commutes and conditions leading to high exposures. Measurements were made during 24 morning and afternoon commutes on two Los Angeles Unified School District bus routes from South to West Los Angeles, with seven additional runs on a rural/suburban route, and three runs to test the effect of window position. For these commutes, the mean concentrations of diesel vehicle-related pollutants ranged from 0.9 to 19 μg/m3 for black carbon, 23 to 400 ng/m3 for particle-bound polycyclic aromatic hydrocarbon (PB-PAH), and 64 to 220 μg/m3 for NO2. Concentrations of benzene and formaldehyde ranged from 0.1 to 11 μg/m3 and 0.3 to 5 μg/m3, respectively. The highest real-time concentrations of black carbon, PB-PAH and NO2 inside the buses were 52 μg/m3, 2000 ng/m3, and 370 μg/m3, respectively. These pollutants were significantly higher inside conventional diesel buses compared to the CNG bus, although formaldehyde concentrations were higher inside the CNG bus. Mean black carbon, PB-PAH, benzene and formaldehyde concentrations were higher when the windows were closed, compared with partially open, in part, due to intrusion of the bus's own exhaust into the bus cabin, as demonstrated through the use of a tracer gas added to each bus's exhaust. These same pollutants tended to be higher on urban routes compared to the rural/suburban route, and substantially higher inside the bus cabins compared to ambient measurements. Mean concentrations of pollutants with substantial secondary formation, such as PM2.5, showed smaller differences between open and closed window conditions and between bus routes. Type of bus, traffic congestion levels, and encounters with other diesel vehicles contributed to high exposure variability between runs.
The Relationship of Indoor, Outdoor and Personal Air (RIOPA) Study was undertaken to evaluate the contribution of outdoor sources of air toxics, as defined in the 1990 Clean Air Act Amendments, to indoor concentrations and personal exposures. The concentrations of 18 volatile organic compounds (VOCs), 17 carbonyl compounds, and fine particulate matter mass (PM 2.5 ) were measured using 48-h outdoor, indoor and personal air samples collected simultaneously. PM 2.5 mass, as well as several component species (elemental carbon, organic carbon, polyaromatic hydrocarbons and elemental analysis) were also measured; only PM 2.5 mass is reported here. Questionnaires were administered to characterize homes, neighborhoods and personal activities that might affect exposures. The air exchange rate was also measured in each home. Homes in close proximity (<0.5 km) to sources of air toxics were preferentially (2:1) selected for sampling. Approximately 100 non-smoking households in each of Elizabeth, NJ, Houston, TX, and Los Angeles, CA were sampled (100, 105, and 105 respectively) with second visits performed at 84, 93, and 81 homes in each city, respectively. VOC samples were collected at all homes, carbonyls at 90% and PM 2.5 at 60% of the homes. Personal samples were collected from nonsmoking adults and a portion of children living in the target homes. This manuscript provides the RIOPA study design and quality control and assurance data. The results from the RIOPA study can potentially provide information on the influence of ambient sources on indoor air concentrations and exposure for many air toxics and will furnish an opportunity to evaluate exposure models for these compounds.
Recent state and federal public school class-size reduction initiatives, increased elementary and pre-K enrollment driven by population growth and immigration, and limited resources for capital projects, modernization, and maintenance at aging schools have increased the prevalence of prefabricated, portable classrooms (portables). At present, approximately one of three California students are taught in portables, whose use is especially prevalent in more populated counties such as Los Angeles, home to the nation's second largest school district. Limited data existed on chemical compound air concentrations, and thus exposures, inside American public schools. Measurements have been limited, usually performed in complaint schools, and varied in sampling protocols and analysis methods. To address a school environment and children's health issue of present concern, an assessment of public school portables was conducted in Los Angeles County. Seven schools in two school districts were recruited, from which 20 classrooms — 13 portables, seven in main buildings — were randomly selected. We report indoor air concentrations of 21 target toxic and odorous volatile organic compounds (VOCs), including formaldehyde and acetaldehyde, measured with passive samplers (DNSH PAKS and 3M OVM 3500) in the cooling and heating seasons between June 2000 and June 2001. None of the measured indoor air formaldehyde concentrations exceeded the existing California Air Resources Board guideline (50 ppb, or 60 μg/m3). The main sources of aldehydes in classrooms, especially portables, were likely interior finish materials and furnishings made of particleboard without lamination. Indoor air VOC concentrations were generally low in this pilot study. The four most prevalent VOCs measured were toluene, m-/p-xylene, α-pinene, and δ-limonene; likely indoor sources were personal, teaching, and cleaning products. Future schools research should attempt larger samples over larger geographical areas.
The Relationship of Indoor, Outdoor and Personal Air (RIOPA) study was designed to investigate residential indoor, outdoor and personal exposures to several classes of air pollutants, including volatile organic compounds, carbonyls and fine particles (PM 2.5 ). Samples were collected from summer, 1999 to spring, 2001 in Houston (TX), Los Angeles (CA) and Elizabeth (NJ). Indoor, outdoor and personal PM 2.5 samples were collected at 212 nonsmoking residences, 162 of which were sampled twice. Some homes were chosen due to close proximity to ambient sources of one or more target analytes, while others were farther from sources. Median indoor, outdoor and personal PM 2.5 mass concentrations for these three sites were 14.4, 15.5 and 31.4 μ g/m 3 , respectively. The contributions of ambient (outdoor) and nonambient sources to indoor and personal concentrations were quantified using a single compartment box model with measured air exchange rate and a random component superposition (RCS) statistical model. The median contribution of ambient sources to indoor PM 2.5 concentrations using the mass balance approach was estimated to be 56% for all study homes (63%, 52% and 33% for California, New Jersey and Texas study homes, respectively). Reasonable variations in model assumptions alter median ambient contributions by less than 20%. The mean of the distribution of ambient contributions across study homes agreed well for the mass balance and RCS models, but the distribution was somewhat broader when calculated using the mass balance model with measured air exchange rates.
To investigate residential ozone (O-3) concentrations and their relationship to regional monitoring data, we studied 126 southern California homes between February and December 1994. Using a controlled flow sampler, 481 samples were collected over 24 h sampling periods, both inside (n = 241) and immediately outside (n = 240) residences. Indoor O-3 levels (13 +/- 12 ppb, arithmetic mean) were almost always below observed outdoor measurements (37 +/- 19 ppb). Low outdoor concentrations resulted in uniformly low indoor concentrations, but high outdoor levels resulted in a range of indoor levels. Indoor/outdoor ratios (0.37 +/- 0.25) were greater during the summer pollution period. Using information collected from interviews performed before and after sampling, we explored relationships between measured indoor O-3, home operating characteristics, and ambient O-3 reported at the closest regional monitoring station. Indoor O-3 levels were largely determined by outdoor O-3 levels and the duration of time that windows were kept open. Ozone measured adjacent to study homes predicted indoor levels no better than station ambient values. These data suggest that ambient O-3 measured at regional stations, coupled with information about how homes are operated, predictin-home O-3 levels moderately well and are potentially useful for future exposure assessment purposes.
The topics covered in this report are: describe the relationship between measured benzene, toluene, NO2, and radon concentrations with building characteristics, appliance factors, meteorological conditions, other measured pollutants, geographical locations, and sampling parameters; extrapolate the measured CO distributions from the three service territories to the entire State of California; develop a mass balance model to predict CO concentrations from air exchange rate, home volume and cooking/heating type; and explore the relationship among CO concentrations, measured benzene levels, and smoking behaviors.
This second volume provides a systematic evaluation of the data set focusing on the relationships of the recorded parameters with the following four outcome measures: indoor 48-hour average CO; net 48-hour average indoor minus outdoor CO; air exchange rates; and maximum 8-hour average indoor CO. Over 350 variables were measured and/or recorded for each house in the pilot study. These parameters included the concentrations of pollutants of interest (CO, benzene, NO2, toluene, radon, formaldehyde, and methane), housing characteristics (e.g., cooking fuel, burner adjustments, proper venting) and occupant practices (e.g., cigarette smoking, heating with the range/oven).
The indoor-outdoor relations of mutagenic compounds associated with airborne particles less than 10-mum aerodynamic diameter (PMIO) were studied in the homes of 10 nonsmokers located in southern California. Asthmatics lived in nine of the 10 homes studied. Low-volume samplers (4 and 2 L/min) fitted with PM10 and cyclone (5-mum nominal particle size cut) particle preselectros were used to collect 24-h air samples indoors and outdoors. In addition, three individuals carried personal samplers for 24-h periods. Filter extracts were tested for mutagenicity using a sensitive Salmonella microsuspension assay. The concentrations of particle-associated mutagens were significantly higher outdoors compared to indoors. For the PM10- and cyclone-collected samples, indoor-outdoor ratios averaged 0.46 and 0.49, respectively. There were significant correlations between indoor and outdoor mutagenicity (revertants/m3) for all samples (Spearman rank, R(s) = 0.74; n = 25 pairs; p < 0.001). Further, the indoor and outdoor correlation of specific-mass mutagenic activity [revertants per unit particle mass (revertants/mug)] was highly significant [p < 0.001; R(s) = 0.90 (n = 25 pairs)]. The mutagenic activity of personal samples was very similar to the fixed-site samples collected indoors. The results support the hypothesis that mutagen composition of the indoor and outdoor particles are similar and that outdoor particles which infiltrate into homes may be a significant source of respirable mutagenic particles in the homes of nonsmokers.
The volume of appendixes accompanies a report of the investigation of field and laboratory methods to measure the distribution of carbon monoxide and other pollutants, such as nitrogen dioxide, benzene, toluene, formaldehyde, radon, and methane, in California residences. The appendixes include field forms and questionnaires, instruction materials for the customer service representatives conducting the surveys, home plots for the contaminants, passive sampler field blanks results, and a summary of the interference testings.
As a component of a cross-sectional NO2 exposure study on 700 individuals living in the Los Angeles, California, area, a more detailed longitudinal study was carried out on 67 participants. Participants in the microenvironmental study were monitored for 24h and 48h NO2 exposures up to 8 times over a year. Participants wore personal NO2 passive sampling badges for 24h and exposed separate badges to sample indoor home and away-from-home NO2 concentrations. Seasonal variations in outdoor, indoor, and personal exposures were apparent. Concentrations away from home averaged 7 to 30 ppb, depending on the cycle, higher than the at-home concentrations. Personal exposures of participants who cooked with gas averaged 10ppb to 28 ppb higher than those without gas. Between 68 percent to 80 percent of the variations in personal exposures were predicted by linear regression models that included bedroom NO2 and outdoor (home) NO2 concentrations.