Christopher Godwin

Brominated flame retardants in offices in Michigan, U.S.A.

Brominated flame retardants (BFRs) are now ubiquitous contaminants with large reservoirs and high concentrations in buildings. Most of the information documenting BFR levels has been obtained in residences, and other environments that can lead to exposure have received relatively little attention, including offices that contain numerous BFR sources and where individuals spend considerable time. The aim of this study is to characterize BFR concentrations, potential emission sources, and migration pathways in office environments. We measure BFR levels in floor dust, indoor air, ventilation filter dust, and carpets in ten commercial and institutional buildings in Michigan, U.S.A. The median concentration of total BDEs in settled dust was 8754 ng g(-1), at the upper range of levels previously reported. Especially elevated levels were found in offices in buildings that contained known or likely BFR sources, e.g., computer servers. A trends analysis in a newly constructed building showed remarkable increases in concentrations of BFRs in settled dust and indoor air, and apparent steady-state levels were reached 5 to 8 months after building completion, a particularly striking finding given that the building was constructed and furnished several years after the voluntary phase-out of the penta- and octa-mixtures. Airborne particulate matter collected in a buildings HVAC system filters contained PBDEs, including BDE-209, at levels exceeding the concentration of floor dust. In conjunction with estimates of building air flow rates, filter efficiency and other parameters, mass balance calculations for this building were used to estimate the emission rates and reservoirs of PBDEs. The widespread distribution of BFRs found in offices in both new and old buildings suggests the significance of workplace exposures, the need for controls to minimize human exposure, intra-building migration, and environmental releases of these chemicals, and the need for monitoring in new buildings to confirm the effectiveness of the PBDE phase-out.

Particulate matter concentrations in residences: an intervention study evaluating stand‐alone filters and air conditioners

UNLABELLED This study, a randomized controlled trial, evaluated the effectiveness of free-standing air filters and window air conditioners (ACs) in 126 low-income households of children with asthma. Households were randomized into a control group, a group receiving a free-standing HEPA filter placed in the childs sleeping area, and a group receiving the filter and a window-mounted AC. Indoor air quality (IAQ) was monitored for week-long periods over three to four seasons. High concentrations of particulate matter (PM) and carbon dioxide were frequently seen. When IAQ was monitored, filters reduced PM levels in the childs bedroom by an average of 50%. Filter use varied greatly among households and declined over time, for example, during weeks when pollutants were monitored, filter use was initially high, averaging 84±27%, but dropped to 63±33% in subsequent seasons. In months when households were not visited, use averaged only 34±30%. Filter effectiveness did not vary in homes with central or room ACs. The study shows that measurements over multiple seasons are needed to characterize air quality and filter performance. The effectiveness of interventions using free-standing air filters depends on occupant behavior, and strategies to ensure filter use should be an integral part of interventions. PRACTICAL IMPLICATIONS Environmental tobacco smoke (ETS) increased particulate matter (PM) levels by about 14 μg/m3 and was often detected using ETS-specific tracers despite restrictions on smoking in the house as reported on questionnaires administered to caregivers. PM concentrations depended on season, filter usage, relative humidity, air exchange ratios, number of children, outdoor PM levels, sweeping/dusting, and presence of a central air conditioner (AC). Free-standing air filters can be an effective intervention that provides substantial reductions in PM concentrations if the filters are used. However, filter use was variable across the study population and declined over the study duration, and thus strategies are needed to encourage and maintain use of filters. The variability in filter use suggests that exposure misclassification is a potential problem in intervention studies using filters. The installation of a room AC in the bedroom, intended to limit air exchange ratios, along with an air filter, did not lower PM levels more than the filter alone.

Levels and sources of volatile organic compounds in homes of children with asthma

UNLABELLED Many volatile organic compounds (VOCs) are classified as known or possible carcinogens, irritants, and toxicants, and VOC exposure has been associated with the onset and exacerbation of asthma. This study characterizes VOC levels in 126 homes of children with asthma in Detroit, Michigan, USA. The total target VOC concentration ranged from 14 to 2274 μg/m(3) (mean = 150 μg/m(3); median = 91 μg/m(3)); 56 VOCs were quantified; and d-limonene, toluene, p, m-xylene, and ethyl acetate had the highest concentrations. Based on the potential for adverse health effects, priority VOCs included naphthalene, benzene, 1,4-dichlorobenzene, isopropylbenzene, ethylbenzene, styrene, chloroform, 1,2-dichloroethane, tetrachloroethene, and trichloroethylene. Concentrations varied mostly due to between-residence and seasonal variation. Identified emission sources included cigarette smoking, solvent-related emissions, renovations, household products, and pesticides. The effect of nearby traffic on indoor VOC levels was not distinguished. While concentrations in the Detroit homes were lower than levels found in other North American studies, many homes had elevated VOC levels, including compounds that are known health hazards. Thus, the identification and control of VOC sources are important and prudent, especially for vulnerable individuals. Actions and policies to reduce VOC exposures, for example, sales restrictions, improved product labeling, and consumer education, are recommended. PRACTICAL IMPLICATIONS Total target VOC concentrations in the Detroit homes ranged from 14 to 2274 lg/m3, generally lower than found in earlier studies. However, a subset of houses had elevated concentrations, and levels of 1,4-dichlorobenzene, naphthalene, and benzene reached levels commensurate with excess individual cancer risks of 10(-2), 10(-3), and 10(-4), respectively. VOC concentrations varied mostly due to between-residence and season effects. The most important sources included cigarette smoking, vehicle-related emissions, building renovation, solvents, household products, and pesticides.

Sources, concentrations, and risks of naphthalene in indoor and outdoor air

UNLABELLED Naphthalene is a ubiquitous pollutant, and very high concentrations are sometimes encountered indoors when this chemical is used as a pest repellent or deodorant. This study describes the distribution and sources of vapor-phase naphthalene concentrations in four communities in southeast Michigan, USA. Outdoors, naphthalene was measured in the communities and at a near-road site. Indoors, naphthalene levels were characterized in 288 suburban and urban homes. The median outdoor concentration was 0.15 μg/m(3), and a modest contribution from rush-hour traffic was noted. The median indoor long-term concentration was 0.89 μg/m(3), but concentrations were extremely skewed and 14% of homes exceeded 3 μg/m(3), the chronic reference concentration for non-cancer effects, 8% exceeded 10 μg/m(3), and levels reached 200 μg/m(3). The typical excess individual lifetime cancer risk was about 10(-4) and reached 10(-2) in some homes. Important sources include naphthalenes use as a pest repellent and deodorant, migration from attached garages and, to lesser extents, cigarette smoke and vehicle emissions. Excessive use as a repellent caused the highest concentrations. Naphthalene presents high risks in a subset of homes, and policies and actions to reduce exposures, for example, sales bans or restrictions, improved labeling, and consumer education, should be considered. PRACTICAL IMPLICATIONS Long-term average concentrations of naphthalene in most homes fell into the 0.2-1.7 μg/m(3) range reported as representative in earlier studies. The highly skewed distribution of concentrations results in a subset of homes with elevated concentrations and health risks that greatly exceed US EPA and World Health Organization (WHO) guidelines. The most important indoor source is the use of naphthalene as a pest repellant or deodorant; secondary sources include presence of an attached garage, cigarette smoking, and outdoor sources. House-to-house variation was large, reflecting differences among the residences and naphthalene use practices. Stronger policies and educational efforts are needed to eliminate or modify indoor usage practices of this chemical.

Air Change Rates and Interzonal Flows in Residences, and the Need for Multi-Zone Models for Exposure and Health Analyses

Air change rates (ACRs) and interzonal flows are key determinants of indoor air quality (IAQ) and building energy use. This paper characterizes ACRs and interzonal flows in 126 houses, and evaluates effects of these parameters on IAQ. ACRs measured using weeklong tracer measurements in several seasons averaged 0.73 ± 0.76 h−1 (median = 0.57 h−1, n = 263) in the general living area, and much higher, 1.66 ± 1.50 h−1 (median = 1.23 h−1, n = 253) in bedrooms. Living area ACRs were highest in winter and lowest in spring; bedroom ACRs were highest in summer and lowest in spring. Bedrooms received an average of 55 ± 18% of air from elsewhere in the house; the living area received only 26 ± 20% from the bedroom. Interzonal flows did not depend on season, indoor smoking or the presence of air conditioners. A two-zone IAQ model calibrated for the field study showed large differences in pollutant levels between the living area and bedroom, and the key parameters affecting IAQ were emission rates, emission source locations, air filter use, ACRs, interzonal flows, outdoor concentrations, and PM penetration factors. The single-zone models that are commonly used for residences have substantial limitations and may inadequately represent pollutant concentrations and exposures in bedrooms and potentially other environments other where people spend a substantial fraction of time.

Concentrations and Risks of p-Dichlorobenzene in Indoor and Outdoor Air

UNLABELLED p-dichlorobenzene (PDCB) is a chlorinated volatile organic compound that can be encountered at high concentrations in buildings owing to its use as pest repellent and deodorant. This study characterizes PDCB concentrations in four communities in southeast Michigan. The median concentration outside 145 homes was 0.04 μg/m(3), and the median concentration inside 287 homes was 0.36 μg/m(3). The distribution of indoor concentrations was extremely skewed. For example, 30% of the homes exceeded 0.91 μg/m(3), which corresponds to a cancer risk level of 10(-5) based on the California unit risk estimate, and 4% of homes exceeded 91 μg/m(3), equivalent to a 10(-3) risk level. The single highest measurement was 4100 μg/m(3). Estimates of whole-house emission rates were largely consistent with chamber test results in the literature. Indoor concentrations that exceed a few μg/m(3) indicate the use of PDCB products. PDCB concentrations differed among households and the four cities, suggesting the importance of locational, cultural, and behavioral factors in the use patterns of this chemical. The high PDCB levels found suggest the need for policies and actions to lower exposures, for example, sales or use restrictions, improved labeling, and consumer education. PRACTICAL IMPLICATIONS Distributions of p-dichlorobenzene concentrations in residences are highly right-skewed, and a subset of houses has very elevated concentrations that are equivalent to an excess cancer risk of 10(-3) or higher based on the California unit risk effect estimate. House-to-house variation is large, reflecting differences in use practices. Stronger policies and educational efforts are needed to eliminate or modify indoor usage practices of this chemical.

Experimental and modeling study of visible light responsive photocatalytic oxidation (PCO) materials for toluene degradation

Only limited research has examined the development and application of visible light responsive photocatalytic oxidation (PCO), although such materials have great potential for mitigating concentrations of volatile organic compounds (VOCs) when applied to building surfaces. This study evaluates the performance and characteristics of a visible light responsive photocatalyst, specially, a co-alloyed TiNbON compound with a band energy of 2.3 eV. The PCO material was developed using urea-glass synthesis, characterized by scanning electron microscopy (SEM), diffuse reflectance spectra (DRS), powder X-ray diffraction (PXRD), and Brunauer-Emmett-Teller (BET) methods, and VOC removal efficiency was measured under visible light for toluene (1-5 ppm) at room temperature (21.5°C) and a range of relative humidity (RH: 25 to 65%), flow rate (0.78 to 7.84 cm/s), and irradiance (42 to 95 W/m2). A systematic parametric evaluation of kinetic parameters was conducted. In addition, we compared TiNbON with a commercial TiO2-based material under black light, estimated TiNbONs long-term durability and stability, and tested its ability to thermally regenerate. Using mass transfer and kinetic analysis, three different Langmuir-Hinshelwood (LH) type reaction rate expressions were proposed and evaluated. A LH model considering one active site and competitive sorption of toluene and water was superior to others. The visible-light driven catalyst was able to remove up to 58 % of the toluene, generated less formaldehyde than the commercial TiO2, could be fully regenerated at 150°C, and had reasonable durability and stability. This evaluation of TiNbON shows the potential to remove VOCs and improve air quality for indoor applications. Further research is needed to evaluate the potential for harmful by-products, to identify optimal conditions, and to use field tests to show real-world performance.

Air exchange rates and migration of VOCs in basements and residences.

UNLABELLED Basements can influence indoor air quality by affecting air exchange rates (AERs) and by the presence of emission sources of volatile organic compounds (VOCs) and other pollutants. We characterized VOC levels, AERs, and interzonal flows between basements and occupied spaces in 74 residences in Detroit, Michigan. Flows were measured using a steady-state multitracer system, and 7-day VOC measurements were collected using passive samplers in both living areas and basements. A walk-through survey/inspection was conducted in each residence. AERs in residences and basements averaged 0.51 and 1.52/h, respectively, and had strong and opposite seasonal trends, for example, AERs were highest in residences during the summer, and highest in basements during the winter. Airflows from basements to occupied spaces also varied seasonally. VOC concentration distributions were right-skewed, for example, 90th percentile benzene, toluene, naphthalene, and limonene concentrations were 4.0, 19.1, 20.3, and 51.0 μg/m(3), respectively; maximum concentrations were 54, 888, 1117, and 134 μg/m(3). Identified VOC sources in basements included solvents, household cleaners, air fresheners, smoking, and gasoline-powered equipment. The number and type of potential VOC sources found in basements are significant and problematic, and may warrant advisories regarding the storage and use of potentially strong VOCs sources in basements. PRACTICAL IMPLICATIONS Few IAQ studies have examined basements. A sizable volume of air can flow between the basement and living area, and AERs in these two zones can differ considerably. In many residences, the basement contains significant emission sources and contributes a large fraction of VOC concentrations found in the living area. Exposures can be lowered by removing VOC sources from the basement; other exposure management options, such as local ventilation or isolation, are unlikely to be practical.

Design and performance evaluation of a medium flow sampler for airborne brominated flame retardants (BFRs)

Brominated flame retardants (BFRs), including polybrominated diphenyl ethers (PBDEs), have emerged as important and ubiquitous environmental pollutants, and there is a need to accurately measure airborne levels of these chemicals in both indoor and outdoor applications. We review and suggest performance criteria for BFR sampling systems, and then present the design of a new medium flow active sampler. The sampler uses a PTFE filter (47 mm, 1 microm pore size) in front of a polyurethane foam (PUF) adsorbent plug (22 mm dia, 76 mm length) with a nominal flow rate of 15 L min(-1) and a sampling period of one week, giving a sampling volume of 150 m(3). The sampler was evaluated using co-located systems to test precision, backup PUFs to test breakthrough, and distributed volume sampling to test linearity. Field experiments were conducted in five commercial buildings, one residence and outdoors at an urban site. A total of 20 BDE congeners were quantified. After appropriate cleaning of the PUF adsorbent, blank levels were negligible. Method detection limits (MDLs) were sufficiently low to quantify BDE congeners 17, 28, 71, 47, 100 and 99 in ambient air, and more than adequate to quantify these and other congeners in indoor air, where levels are typically much higher. The relative absolute deviation (RAD), based on distributed volume samples, ranged from 21% (BDE-71) to 81% (BDE-75) for indoor samples, and was somewhat higher for ambient samples. Only minimal breakthrough was detected in back-up samples, and over 80% of the samples had very low or negligible breakthrough. Humidity did not influence sampler performance. Overall, the medium-flow sampler can accurately measure PBDEs over a wide range of concentrations and applications.

Modeling Spatial and Temporal Variability of Residential Air Exchange Rates for the Near-Road Exposures and Effects of Urban Air Pollutants Study (NEXUS)

Air pollution health studies often use outdoor concentrations as exposure surrogates. Failure to account for variability of residential infiltration of outdoor pollutants can induce exposure errors and lead to bias and incorrect confidence intervals in health effect estimates. The residential air exchange rate (AER), which is the rate of exchange of indoor air with outdoor air, is an important determinant for house-to-house (spatial) and temporal variations of air pollution infiltration. Our goal was to evaluate and apply mechanistic models to predict AERs for 213 homes in the Near-Road Exposures and Effects of Urban Air Pollutants Study (NEXUS), a cohort study of traffic-related air pollution exposures and respiratory effects in asthmatic children living near major roads in Detroit, Michigan. We used a previously developed model (LBL), which predicts AER from meteorology and questionnaire data on building characteristics related to air leakage, and an extended version of this model (LBLX) that includes natural ventilation from open windows. As a critical and novel aspect of our AER modeling approach, we performed a cross validation, which included both parameter estimation (i.e., model calibration) and model evaluation, based on daily AER measurements from a subset of 24 study homes on five consecutive days during two seasons. The measured AER varied between 0.09 and 3.48 h−1 with a median of 0.64 h−1. For the individual model-predicted and measured AER, the median absolute difference was 29% (0.19 h‑1) for both the LBL and LBLX models. The LBL and LBLX models predicted 59% and 61% of the variance in the AER, respectively. Daily AER predictions for all 213 homes during the three year study (2010–2012) showed considerable house-to-house variations from building leakage differences, and temporal variations from outdoor temperature and wind speed fluctuations. Using this novel approach, NEXUS will be one of the first epidemiology studies to apply calibrated and home-specific AER models, and to include the spatial and temporal variations of AER for over 200 individual homes across multiple years into an exposure assessment in support of improving risk estimates.