科研成果 by Year: 2021

2021
Lunderberg, D. M. ; Misztal, P. K. ; Liu, Y. J. ; Arata, C. ; Tian, Y. ; Kristensen, K. ; Weber, R. J. ; Nazaroff, W. W. ; Goldstein, A. H. High-Resolution Exposure Assessment for Volatile Organic Compounds in Two California Residences. Environmental Science & Technology 2021. 访问链接Abstract
Time spent in residences substantially contributes to human exposure to volatile organic compounds (VOCs). Such exposures have been difficult to study deeply, in part because VOC concentrations and indoor occupancy vary rapidly. Using a fast-response online mass spectrometer, we report time-resolved exposures from multi-season sampling of more than 200 VOCs in two California residences. Chemical-specific source apportionment revealed that time-averaged exposures for most VOCs were mainly attributable to continuous indoor emissions from buildings and their static contents. Also contributing to exposures were occupant-related activities, such as cooking, and outdoor-to-indoor transport. Health risk assessments are possible for a subset of observed VOCs. Acrolein, acetaldehyde, and acrylic acid concentrations were above chronic advisory health guidelines, whereas exposures for other assessable species were typically well below the guideline levels. Studied residences were built in the mid-20th century, indicating that VOC emissions even from older buildings and their contents can substantially contribute to occupant exposures.
Qiu, J. ; Xie, D. ; Li, Y. ; Qu, Y. ; Liu, Y. ; Zhu, T. ; Liu, Y. J. Dibasic Esters Observed as Potential Emerging Indoor Air Pollutants in New Apartments in Beijing, China. Environmental Science & Technology Letters 2021. 访问链接Abstract
Volatile organic compounds (VOCs) emitted from building and furnishing materials represent a major concern of indoor air quality, in particular in new buildings. We carried out multiweek nontargeted VOC measurements in 10 new apartments in Beijing, China, using online chemical ionization mass spectrometry. Dimethyl esters of succinic, glutaric, and adipic acids, which are rarely known for their presence in indoor air, were identified in three apartments. The identification was confirmed using authentic standards and by gas chromatography/mass spectrometry analysis. Despite varying concentrations, the three compounds exhibited largely consistent ratios across the three apartments and throughout the observation periods. The observed ratios resemble chemical composition of dibasic esters (DBE), which are a solvent mixture of the three compounds and have been used in the coating industry. A field “sniffing” experiment further confirms DBE emissions from the coatings of some wooden furniture in at least one apartment. The average airborne DBE concentrations in the three apartments were 41, 5, and 4 $μ$g/m3, respectively, exceeding the screening level of 1 $μ$g/m3 recommended by the Michigan Department of Environmental Quality, United States. In the context of fast-growing DBE usage, the current results suggest that DBE might be emerging indoor air pollutants and merit further investigation.
Lunderberg, D. M. ; Liu, Y. J. ; Misztal, P. K. ; Arata, C. ; Tian, Y. ; Kristensen, K. ; Nazaroff, W. W. ; Goldstein, A. H. Intake Fractions for Volatile Organic Compounds in Two Occupied California Residences. Environmental Science & Technology Letters 2021, 8, 386–391. 访问链接Abstract
Experimental estimates of residential intake fractions for indoor volatile organic compound (VOC) releases are scarce. We evaluated individual intake fractions (iFi, mass inhaled by an individual per unit mass emitted) using approximately five months of time-resolved VOC measurements acquired at two residences. First, we directly estimated iFi using inert tracer gases that were released at fixed rates. Tracer gas iFi values were generally consistent between occupants and comparable across seasons. Furthermore, iFi for sources released on different floors of a residence were statistically indistinguishable, suggesting that source location within the living space was not strongly influential. Emissions from living space sources (iFi ∼ 0.3% = 3000 ppm) contributed to occupant exposures at rates 2–4 times higher than crawl space sources (iFi ∼ 1000 ppm) and greater than 40 times higher than attic sources (iFi < ∼70 ppm). Second, we indirectly estimated iFi for 251 VOCs using net emission rates estimated by indoor–outdoor material balance. Although emission patterns varied between compounds, all VOC-specific iFi estimates were clustered near the values of the living space tracer gases. These experimental observations substantiate the theoretical expectation that iFi values are largely independent of analyte characteristics, a useful simplification for exposure assessments.
Zhang, M. ; Xiong, J. ; Liu, Y. J. ; Misztal, P. K. ; Goldstein, A. H. Physical–Chemical Coupling Model for Characterizing the Reaction of Ozone with Squalene in Realistic Indoor Environments. Environmental Science & Technology 2021, 55, 1690–1698. 访问链接Abstract
Squalene can react with indoor ozone to generate a series of volatile and semi-volatile organic compounds, some of which may be skin or respiratory irritants, causing adverse health effects. Better understanding of the ozone/squalene reaction and product transport characteristics is thus important. In this study, we developed a physical–chemical coupling model to describe the behavior of ozone/squalene reaction products, that is, 6-methyl-5-hepten-2-one (6-MHO) and 4-oxopentanal (4-OPA) in the gas phase and skin, by considering the chemical reaction and physical transport processes (external convection, internal diffusion, and surface uptake). Experiments without intervention were performed in a single-family house in California utilizing time- and space-resolved measurements. The key parameters in the model were extracted from 5 day data and then used to predict the behaviors in some other days. Predictions from the present model can reproduce the concentration profiles of the three compounds (ozone, 6-MHO, and 4-OPA) well (R2 = 0.82–0.89), indicating high accuracy of the model. Exposure analysis shows that the total amount of 6-MHO and 4-OPA entering the blood capillaries in 4 days can reach 14.6 and 30.1 $μ$g, respectively. The contribution of different sinks to ozone removal in the tested realistic indoor environment was also analyzed.
Liu, Y. J. ; Misztal, P. K. ; Arata, C. ; Weschler, C. J. ; Nazaroff, W. W. ; Goldstein, A. H. Observing Ozone Chemistry in an Occupied Residence. Proceedings of the National Academy of Sciences 2021, 118, e2018140118. 访问链接Abstract
It has been suggested that indoor exposure to ozone oxidation products contributes materially to the apparent associations between outdoor ozone concentration and morbidity and mortality. Our current understanding of indoor ozone chemistry derives mainly from studies with test surfaces under controlled conditions. Little is known about the overall impact of ozone chemistry on air composition in dynamically changing indoor residential environments. The results presented here reflect a quantitative characterization of overall indoor ozone chemistry in a normally occupied home. Findings reveal a strong influence of off-body skin lipids on indoor ozone chemistry. Being able to elucidate indoor air pollutants derived from ozone chemistry facilitates the investigation of causal links between outdoor ozone concentrations and adverse health effects.Outdoor ozone transported indoors initiates oxidative chemistry, forming volatile organic products. The influence of ozone chemistry on indoor air composition has not been directly quantified in normally occupied residences. Here, we explore indoor ozone chemistry in a house in California with two adult inhabitants. We utilize space- and time-resolved measurements of ozone and volatile organic compounds (VOCs) acquired over an 8-wk summer campaign. Despite overall low indoor ozone concentrations (mean value of 4.3 ppb) and a relatively low indoor ozone decay constant (1.3 h−1), we identified multiple VOCs exhibiting clear contributions from ozone-initiated chemistry indoors. These chemicals include 6-methyl-5-hepten-2-one (6-MHO), 4-oxopentanal (4-OPA), nonenal, and C8-C12 saturated aldehydes, which are among the commonly reported products from laboratory studies of ozone interactions with indoor surfaces and with human skin lipids. These VOCs together accounted for ≥12% molecular yield with respect to house-wide consumed ozone, with the highest net product yield for nonanal (≥3.5%), followed by 6-MHO (2.7%) and 4-OPA (2.6%). Although 6-MHO and 4-OPA are prominent ozonolysis products of skin lipids (specifically squalene), ozone reaction with the body envelopes of the two occupants in this house are insufficient to explain the observed yields. Relatedly, we observed that ozone-driven chemistry continued to produce 6-MHO and 4-OPA even after the occupants had been away from the house for 5 d. These observations provide evidence that skin lipids transferred to indoor surfaces made substantial contributions to ozone reactivity in the studied house.All study data are included in the article and supporting information.