Jaymin Kwon

Influence of ambient (outdoor) sources on residential indoor and personal PM2.5 concentrations: Analyses of RIOPA data

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 (PM2.5). Samples were collected from summer, 1999 to spring, 2001 in Houston (TX), Los Angeles (CA) and Elizabeth (NJ). Indoor, outdoor and personal PM2.5 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 PM2.5 mass concentrations for these three sites were 14.4, 15.5 and 31.4 μg/m3, 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 PM2.5 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.

Relationship of Indoor, Outdoor and Personal Air (RIOPA) study: study design, methods and quality assurance/control results.

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 (PM2.5) were measured using 48-h outdoor, indoor and personal air samples collected simultaneously. PM2.5 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 PM2.5 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.

Fine organic particulate matter dominates indoor-generated PM2.5 in RIOPA homes

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.

Source proximity and residential outdoor concentrations of PM 2.5 , OC, EC, and PAHs

We examined the effect of proximity to specific mobile, area, and point sources on the residential outdoor concentrations of fine particulate matter PM (PM2.5) and several of its particle components. Integrated (48-h) PM2.5 samples were collected outside non-smoking residences in Elizabeth, NJ, between summer 1999 and spring 2001. Samples were analyzed for PM2.5 mass, organic and elemental carbon (OC and EC, respectively), trace elements, particle-phase polycyclic aromatic hydrocarbons (p-PAHs), and other important particle species. Information about the proximity of the study homes to potential mobile and area sources of OC, EC, p-PAHs, sulfur (S), and selenium (Se) (including urban interstate highways, local roadways, the Newark International Airport, the Elizabeth seaport, and a nearby refinery in Linden, NJ) were retrieved from a database that included detailed emissions, meteorological, and geographical data for the study area. The dependence of residential outdoor concentrations on source proximity and on various meteorological parameters was then examined for each species by multiple linear regression analysis. As expected, the predicted ambient air concentrations of all particle species (except S, Se) decreased with increasing distance from the sources. Although the enhancement in PM2.5 and OC levels outside the study homes closest to primary PM sources was modest (e.g., 1.6 and 2.5 times the background levels 37 m from interstate highways), the elevation of EC and p-PAH concentrations was substantial outside the closest study homes (i.e., about 20 times for p-PAHs 37 m from interstate highways and about 14 times for EC 192 m from the refinery in Linden, NJ). The predicted EC concentrations 192 and 500 m from the oil refinery were 22.8 and 3.0 μgC/m3, compared with an urban background of 1 μgC/m3. Thus, emissions from this source might dramatically affect EC exposure for residents living in its close proximity.

Concentrations and Source Characteristics of Airborne Carbonyl Compounds Measured Outside Urban Residences

Abstract This paper presents the analysis of ambient air concentrations of 10 carbonyl compounds (aldehydes and ketones) measured in the yards of 87 residences in the city of Elizabeth, NJ, throughout 1999–2001. Most of these residences were measured twice in different seasons; the sampling duration was 48 hr each time. The authors observed higher concentrations for most of the measured carbonyl compounds on warmer days, reflecting larger contributions of photochemical reactions on warmer days. The estimated contributions of photochemical production varied substantially across the measured carbonyl compounds and could be as high as 60%. Photochemical activity, however, resulted in a net loss for formaldehyde. The authors used stepwise multiple linear regression models to evaluate the impact of traffic sources and meteorological conditions on carbonyl concentrations using the data collected on colder days (with lower photochemical activities). They found that the concentrations of formal-dehyde, acetaldehyde, acrolein, propionaldehyde, crotonaldehyde, benzaldehyde, glyoxal, and methylglyoxal significantly decreased with increasing distance between a measured residence and one or more major roadways. They also found significant negative associations between concentrations for most of the measured carbonyl compounds and each of the following meteorological parameters: mixing height, wind speed, and precipitation.

Source proximity and meteorological effects on residential outdoor VOCs in urban areas: Results from the Houston and Los Angeles RIOPA studies

Concentrations of volatile organic compounds (VOCs) measured outside homes in Houston, TX and Los Angeles, CA were characterized by the effects of source proximity and meteorological factors. Benzene, toluene, ethylbenzene, m,p-xylene, o-xylene (BTEX), methyl tert butyl ether (MTBE), tetrachloroethylene (perchloroethylene, PCE), and carbon tetrachloride (CCl4) were examined. Multiple stepwise regression analysis converged the best-fit models with predictors from meteorological conditions and the proximity to specific point, area, and mobile sources on the residential outdoor VOC concentrations. Negative associations of wind speed with concentrations demonstrated the effect of dilution by high wind speed. Atmospheric stability increase was associated with concentration increase. Petrochemical source proximity was a significant predictor for BTEX and MTBE concentrations in Houston. Ethylbenzene and xylene source proximity was a significant predictor in Los Angeles. Close proximity to area sources such as scrap metal recycling or dry cleaning facilities increased the MTBE, PCE, and CCl4 concentrations in Houston and Los Angeles. Models for ethylbenzene, m,p-xylene, and MTBE in Houston, and benzene in Los Angeles explained that for the median values of the meteorological factors, homes closest to influential highways would have concentrations that were 1.7-2.2 fold higher than those furthest from these mobile emission sources. If the median distance to sources were used in the models, the VOC concentrations varied 1.7 to 6.6 fold as the meteorological conditions varied over the observed range. These results highlight that each urban area is unique and localized sources need to be carefully evaluated to understand potential contributions to VOC air concentrations near residences, which influence baseline indoor air concentrations and personal exposures. Results of this study could assist in the appropriate design of monitoring networks for community-level sampling. They may also improve the accuracy of exposure models linking emission sources with estimated pollutant concentrations at the residential level.