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1.
Environ Sci Process Impacts ; 26(2): 305-322, 2024 Feb 21.
Article in English | MEDLINE | ID: mdl-38108243

ABSTRACT

Indoor surfaces are coated with organic films that modulate thermodynamic interactions between the surfaces and room air. Recently published models can simulate film formation and growth via gas-surface partitioning, but none have statistically investigated film composition. The Indoor Model of Aerosols, Gases, Emissions, and Surfaces (IMAGES) was used here to simulate ten years of nonreactive film growth upon impervious indoor surfaces within a Monte Carlo procedure representing a sub-set of North American residential buildings. Film composition was resolved into categories reflecting indoor aerosol (gas + particle phases) factors from three sources: outdoor-originating, indoor-emitted, and indoor-generated secondary organic material. In addition to gas-to-film partitioning, particle deposition was modeled as a vector for organics to enter films, and it was responsible for a majority of the film mass after ∼1000 days of growth for the median simulation and is likely the main source of LVOCs within films. Therefore, the organic aerosol factor possessing the most SVOCs contributes most strongly to the composition of early films, but as the film ages, films become more dominated by the factor with the highest particle concentration. Indoor-emitted organics (e.g. from cooking) often constituted at least a plurality of the simulated mass in developed films, but indoor environments are diverse enough that any major organic material source could be the majority contributor to film mass, depending on building characteristics and indoor activities. A sensitivity analysis suggests that rapid film growth is most likely in both newer, more air-tight homes and older homes near primary pollution sources.


Subject(s)
Air Pollutants , Air Pollution, Indoor , Air Pollutants/analysis , Air Pollution, Indoor/analysis , Environmental Monitoring , Housing , Aerosols/analysis
2.
Environ Sci Technol ; 57(45): 17374-17383, 2023 11 14.
Article in English | MEDLINE | ID: mdl-37930106

ABSTRACT

Cooking activities emit myriad low-volatility, semivolatile, and highly volatile organic compounds that together form particles that can accumulate to large indoor concentrations. Absorptive partitioning thermodynamics governs the particle-phase organic aerosol concentration mainly via temperature and sorbing mass impacts. Cooking activities can increase the organic sorbing mass by 1-2 orders of magnitude, increasing particle-phase concentrations and affecting emission rate calculations. Although recent studies have begun to probe the volatility characteristics of indoor cooking particles, parametrizations of cooking particle mass emissions have largely neglected these thermodynamic considerations. Here, we present an improved thermodynamics-based model framework for estimating condensable organic material emission rates from a time series of observed concentrations, given that adequate measurements or assumptions can be made about the volatility of the emitted species. We demonstrate the performance of this methodology by applying data from stir-frying experiments performed during the House Observations of Microbial and Environmental Chemistry (HOMEChem) campaign to a two-zone box model representing the UTest House. Preliminary estimates of organic mass emitted on a per-stir-fry basis for three types of organic aerosol factors are presented. Our analysis highlights that using traditional nonvolatile particle models and emission characterizations for some organic aerosol emitting activities can incorrectly attribute concentration changes to emissions rather than thermodynamic effects.


Subject(s)
Air Pollutants , Air Pollution, Indoor , Volatile Organic Compounds , Air Pollutants/analysis , Volatile Organic Compounds/analysis , Aerosols/analysis , Cooking , Temperature , Air Pollution, Indoor/analysis , Environmental Monitoring/methods
3.
Environ Sci Process Impacts ; 25(9): 1464-1478, 2023 Sep 20.
Article in English | MEDLINE | ID: mdl-37560969

ABSTRACT

Indoor surfaces can act as reservoirs and reaction media influencing the concentrations and type of species that people are exposed to indoors. Mass accommodation and partitioning are impacted by the phase state and viscosity of indoor surface films. We developed the kinetic multi-layer model KM-FILM to simulate organic film formation and growth, but it is computationally expensive to couple such comprehensive models with indoor air box models. Recently, a novel effective mass accommodation coefficient (αeff) was introduced for efficient and effective treatments of gas-particle partitioning. In this study, we extended this approach to a film geometry with αeff as a function of penetration depth into the film, partitioning coefficient, bulk diffusivity, and condensed-phase reaction rate constant. Comparisons between KM-FILM and the αeff method show excellent agreement under most conditions, but with deviations before the establishment of quasi-equilibrium within the penetration depth. We found that the deposition velocity of species and overall film growth are impacted by bulk diffusivity in highly viscous films (Db ∼<10-15 cm2 s-1). Reactions that lead to non-volatile products can increase film thicknesses significantly, with the extent of film growth being dependent on the gas-phase concentration, rate coefficient, partitioning coefficient and diffusivity. Amorphous semisolid films with Db > ∼10-17-10-19 cm2 s-1 can be efficient SVOC reservoirs for compounds with higher partitioning coefficients as they can be released back to the gas phase over extended periods of time, while glassy solid films would not be able to act as reservoirs as gas-film partitioning is impeded.


Subject(s)
Air Pollutants , Air Pollution, Indoor , Volatile Organic Compounds , Humans , Viscosity , Volatile Organic Compounds/analysis , Air Pollution, Indoor/analysis , Kinetics , Air Pollutants/analysis
4.
PLoS One ; 18(1): e0272716, 2023.
Article in English | MEDLINE | ID: mdl-36608021

ABSTRACT

The Coronavirus Disease 2019 (COVID-19) pandemic renewed interest in infectious aerosols and reducing risk of airborne respiratory pathogen transmission, prompting development of devices to protect healthcare workers during airway procedures. However, there are no standard methods for assessing the efficacy of particle containment with these protective devices. We designed and built an aerosol bio-containment device (ABCD) to contain and remove aerosol via an external suction system and tested the aerosol containment of the device in an environmental chamber using a novel, quantitative assessment method. The ABCD exhibited a strong ability to control aerosol exposure in experimental and computational fluid dynamic (CFD) simulated scenarios with appropriate suction use and maintenance of device seals. Using a log-risk-reduction framework, we assessed device containment efficacy and showed that, when combined with other protective equipment, the ABCD can significantly reduce airborne clinical exposure. We propose this type of quantitative analysis serves as a basis for rating efficacy of aerosol protective enclosures.


Subject(s)
COVID-19 , Humans , COVID-19/prevention & control , Respiratory Aerosols and Droplets , Personal Protective Equipment , Protective Devices , Infectious Disease Transmission, Patient-to-Professional/prevention & control
5.
Environ Sci Process Impacts ; 24(12): 2310-2323, 2022 Dec 14.
Article in English | MEDLINE | ID: mdl-36314460

ABSTRACT

Reactive oxygen species (ROS) are among the species thought to be responsible for the adverse health effects of particulate matter (PM) inhalation. Field studies suggest that indoor sources of ROS contribute to measured ROS on PM in indoor air. We hypothesize that ozone reacts on indoor surfaces to form semi-volatile ROS, in particular organic peroxides (OPX), which partition to airborne particles. To test this hypothesis, we modeled ozone-induced formation of OPX, its decay and its partitioning to PM in a residential building and compared the results to field measurements. Simulations indicate that, while ROS of outdoor origin is the primary contributor to indoor ROS (in PM), a substantial fraction of ROS present in indoor PM is from ozone-surface chemistry. At an air change rate equal to 1/h, and an outdoor ozone mixing ratio of 35 ppb, 25% of the ROS concentration in air is due to indoor formation and partitioning of OPX to PM. For the same conditions, but with a modest indoor source of PM (1.5 mg h-1), 44% of indoor ROS on PM is of indoor origin. An indoor source of ozone, such as an electrostatic air cleaner, also increases OPX present in indoor PM. The results of the simulations support the hypothesis that ozone-induced formation of OPX on indoor surfaces, and subsequent partitioning to aerosols, is sufficient to explain field observations. Therefore, indoor sourced ROS could contribute meaningfully to total inhaled PM-ROS.


Subject(s)
Air Pollutants , Air Pollution, Indoor , Ozone , Reactive Oxygen Species/analysis , Air Pollution, Indoor/analysis , Aerosols , Particulate Matter/analysis , Air Pollutants/analysis , Particle Size , Environmental Monitoring/methods
6.
Environ Sci Process Impacts ; 24(10): 1678-1696, 2022 Oct 19.
Article in English | MEDLINE | ID: mdl-35920302

ABSTRACT

Ambient aerosols often experience temperature and humidity gradients following outdoor-to-indoor transport, causing organic aerosols (OA) to either gain or lose mass via gas-particle repartitioning. Recent models have sought to quantify these effects using equilibrium partitioning thermodynamics. However, evidence suggests some indoor OA may possess glassy or semisolid phase states with higher viscosities than liquid OA. Characteristic partitioning timescales of higher-viscosity particles are significantly longer than for liquid particles, which may either fully or partially inhibit repartitioning. For outdoor OA experiencing a temperature change during transport indoors, the ultimate repartitioning state depends on the relationship between the gas-particle partitioning rate coefficient (kgp) of semivolatile organics and the indoor particle loss rate coefficient (lp). That is, thermodynamic equilibrium partitioning may occur when semivolatile kgp ≫ lp, no repartitioning when semivolatile kgp ≪ lp, and partial repartitioning when their magnitudes are similar. Longer indoor particle lifetimes, higher particle number, and larger particle sizes all raise kgp (driving repartitioning towards equilibrium). For simulated U.S. residences, equilibrium condensation was likely reached in humid climate zones during warm meteorological conditions. In colder regions, the degree of evaporative repartitioning depended on whether organics could repartition before the particle phase state adjusts to indoor conditions, which is uncertain. When an appreciable temperature gradient exists, this study not only confirmed that all outdoor-originating OA that is liquid indoors will reach thermodynamic equilibrium, but also concluded that a plurality (46% for this domain) of such OA that is semisolid may also achieve thermodynamic equilibrium during its indoor lifetime.


Subject(s)
Air Pollutants , Air Pollution, Indoor , Air Pollutants/analysis , Temperature , Environmental Monitoring , Aerosols/analysis , Particle Size , Air Pollution, Indoor/analysis
7.
Indoor Air ; 32(7): e13075, 2022 07.
Article in English | MEDLINE | ID: mdl-35904391

ABSTRACT

Outdoor aerosols can transform and have their composition altered upon transport indoors. Herein, IMAGES, a platform that simulates indoor organic aerosol with the 2-dimensional volatility basis set (2D-VBS), was extended to incorporate the inorganic aerosol thermodynamic equilibrium model, ISORROPIA. The model performance was evaluated by comparing aerosol component predictions to indoor measurements from an aerosol mass spectrometer taken during the summer and winter seasons. Since ammonia was not measured in the validation dataset, outdoor ammonia was estimated from aerosol measurements using a novel pH-based algorithm, while nitric acid was held constant. Modeled indoor ammonia sources included temperature-based occupant and surface emissions. Sensitivity to the nitric acid indoor surface deposition rate ß g , HNO 3 , g was explored by varying it in model runs, which did not affect modeled sulfate due to its non-volatile nature, though the fitting of a filter efficiency was required for good correlations of modeled sulfate with measurements in both seasons. Modeled summertime nitrate well-matched measured observations when ß g , HNO 3 , g = 2.75 h - 1 , but wintertime comparisons were poor, possibly due to missing thermodynamic processes within the heating, ventilating, and air-conditioning (HVAC) system. Ammonium was consistently overpredicted, potentially due to neglecting thirdhand smoke impacts observed in the field campaign, as well as HVAC impacts.


Subject(s)
Air Pollutants , Air Pollution, Indoor , Aerosols/analysis , Air Pollutants/analysis , Air Pollution, Indoor/analysis , Ammonia , Environmental Monitoring/methods , Nitric Acid , Particulate Matter , Sulfates , Thermodynamics
8.
Environ Sci Technol ; 55(13): 9000-9011, 2021 07 06.
Article in English | MEDLINE | ID: mdl-34106692

ABSTRACT

Outdoor aerosols experience environmental changes as they are transported indoors, including outdoor-to-indoor temperature and mass-loading gradients, which can reduce or enhance their indoor concentrations due to repartitioning driven by changes in thermodynamic equilibrium states. However, the complexity required to model repartitioning typically hinders its inclusion in studies predicting indoor exposure to ambient aerosols. To facilitate exposure predictions, this work used an explicit thermodynamic indoor aerosol model to simulate outdoor-to-indoor aerosol repartitioning typical for residential and office buildings across the 16 U.S. climate zones over an annual time horizon. Results demonstrate that neglecting repartitioning when predicting indoor concentrations can produce errors of up to 80-100% for hydrocarbon-like organic aerosol, 40-60% for total organic aerosol, 400% for ammonium nitrate, and 60% (typically 3 µg/m3) for the total PM2.5 aerosol. Underpredictions were more likely for buildings in hotter than colder regions, and for residences than offices, since both cooler indoor air and more meaningful residential organic aerosol concentrations encourage condensation of semivolatile organics. Furthermore, a method for computing correction factors to more easily account for thermodynamic repartitioning is provided. Applying these correction factors to mechanical-only aerosol predictions significantly reduced errors to <0.5 µg/m3 for the total indoor PM2.5 while bypassing explicit thermodynamic simulations.


Subject(s)
Air Pollutants , Air Pollution, Indoor , Aerosols/analysis , Air Pollutants/analysis , Air Pollution, Indoor/analysis , Environmental Monitoring , Particle Size , Particulate Matter/analysis , Temperature
9.
Environ Sci Process Impacts ; 22(10): 2031-2057, 2020 Oct 01.
Article in English | MEDLINE | ID: mdl-33084679

ABSTRACT

Hygroscopic particulate matter (PM) constituents promote uptake of aerosol water (AW), depending on relative humidity (RH), which can constrain qualities such as organic aerosol (OA) phase state and inorganic aerosol (IA) deliquescence and efflorescence. This work provides a first incorporation of AW predictions into residential indoor PM simulations. The indoor model, IMAGES, which simulates factored OA concentrations and thermodynamics using the 2D-volatility basis set, was expanded to predict speciated IA concentrations, AW with κ-Köhler theory of hygroscopic growth, and OA phase state with glass transition temperatures. Since RH is the largest driver of AW and varies with meteorology, simulations were conducted using a database of historical ambient weather and pollution records spanning the sixteen U.S. climate zones, facilitating assessment of seasonal and regional trends. Over this diverse simulation set, the residential indoor AW mass was ∼10 to 100 times smaller than dry PM mass. This relative AW amount indoors was about ∼10 times smaller than outdoors, since indoor-emitted aerosol is likely less hygroscopic. The indoor OA phase state was typically semisolid, suggesting kinetic limitations might inhibit thermodynamic OA partitioning equilibrium from being established indoors. Residences in hot and humid climates during the summertime may have liquid indoor OA, while amorphous solid indoor OA can exist in cold climates. Deliquescence and efflorescence of recirculated IA within HVAC systems during cooling or heating, respectively, was also modeled. Oftentimes, two IA populations with different histories existing as wet or dry aerosol were generated by HVAC operation depending on indoor and outdoor environmental conditions and the HVAC operating mode.


Subject(s)
Air Pollutants , Air Pollution, Indoor , Aerosols/analysis , Air Pollutants/analysis , Air Pollution, Indoor/analysis , Environmental Monitoring , Humidity , Water
10.
Int Forum Allergy Rhinol ; 10(10): 1173-1179, 2020 10.
Article in English | MEDLINE | ID: mdl-32652898

ABSTRACT

The coronavirus disease-2019 (COVID-19) pandemic has heightened the awareness of aerosol generation by human expiratory events and their potential role in viral respiratory disease transmission. Concerns over high severe acute respiratory syndrome-coronavirus-2 (SARS-CoV-2) viral burden of mucosal surfaces has raised questions about the aerosol-generating potential and dangers of many otorhinolaryngologic procedures. However, the risks of aerosol generation and associated viral transmission by droplet or airborne routes for many otorhinolaryngology procedures are largely unknown. Indoor aerosol and droplet viral respiratory transmission risk is influenced by 4 factors: (1) aerosol or droplet properties; (2) indoor airflow; (3) virus-specific factors; and (4) host-specific factors. Herein we elaborate on known aerosol vs droplet properties, indoor airflow, and aerosol-generating events to provide context for risks of aerosol infectious transmission. We also provide simple but typically effective measures for mitigating the spread and inhalation of viral aerosols in indoor settings. Understanding principles of infectious transmission, aerosol and droplet generation, as well as concepts of indoor airflow, will assist in the integration of new data on SARS-CoV-2 transmission and activities that can generate aerosol to best inform on the need for escalation or de-escalation from current societal and institutional guidelines for protection during aerosol-generating procedures.


Subject(s)
Aerosols , COVID-19/transmission , Disease Transmission, Infectious/prevention & control , Otolaryngology/methods , SARS-CoV-2/physiology , Air Pollution, Indoor , COVID-19/prevention & control , Humans , Inhalation , Lipid Droplets , Pandemics
11.
Appl Environ Microbiol ; 86(17)2020 08 18.
Article in English | MEDLINE | ID: mdl-32591374

ABSTRACT

Identifying microbial indicators of damp and moldy buildings remains a challenge at the intersection of microbiology, building science, and public health. Sixty homes in New York City were assessed for moisture-related damage, and three types of dust samples were collected for microbiological analysis. We applied four approaches for detecting fungal signatures of moisture damage in these buildings. Two novel targeted approaches selected specific taxa, identified by a priori hypotheses, from the broad mycobiome as detected with amplicon sequencing. We investigated whether (i) hydrophilic fungi (i.e., requiring high moisture) or (ii) fungi previously reported as indicating damp homes would be more abundant in water-damaged rooms/homes than in nondamaged rooms/homes. Two untargeted approaches compared water-damaged to non-water-damaged homes for (i) differences between indoor and outdoor fungal populations or (ii) differences in the presence or relative abundance of particular fungal taxa. Strong relationships with damage indicators were found for some targeted fungal groups in some sampling types, although not always in the hypothesized direction. For example, for vacuum samples, hydrophilic fungi had significantly higher relative abundance in water-damaged homes, but mesophilic fungi, unexpectedly, had significantly lower relative abundance in homes with visible mold. Untargeted approaches identified no microbial community metrics correlated with water damage variables but did identify specific taxa with at least weak positive links to water-damaged homes. These results, although showing a complex relationship between moisture damage and microbial communities, suggest that targeting particular fungi offers a potential route toward identifying a fungal signature of moisture damage in buildings.IMPORTANCE Living or working in damp or moldy buildings increases the risk of many adverse health effects, including asthma and other respiratory diseases. To date, however, the particular environmental exposure(s) from water-damaged buildings that causes the health effects have not been identified. Likewise, a consistent quantitative measurement that would indicate whether a building is water damaged or poses a health risk to occupants has not been found. In this work, we tried to develop analytical tools that would find a microbial signal of moisture damage amid the noisy background of microorganisms in buildings. The most successful approach taken here focused on particular groups of fungi-those considered likely to grow in damp indoor environments-and their associations with observed moisture damage. With further replication and refinement, this hypothesis-based strategy may be effective in finding still-elusive relationships between building damage and microbiomes.


Subject(s)
Construction Materials/microbiology , Fungi/physiology , Housing , Humidity , Mycobiome , Dust/analysis , Fungi/isolation & purification , New York City
12.
Environ Sci Technol ; 54(2): 947-954, 2020 01 21.
Article in English | MEDLINE | ID: mdl-31834782

ABSTRACT

Fused filament fabrication three-dimensional (3D) printers have been shown to emit ultrafine particles (UFPs) and volatile organic compounds (VOCs). Previous studies have quantified bulk 3D printer particle and VOC emission rates, as well as described particle chemical composition via ex situ analysis. Here, we present size-resolved aerosol composition measurements from in situ aerosol mass spectrometry and ex situ transmission electron microscopy (TEM). Particles were sampled for in situ analysis during acrylonitrile butadiene styrene (ABS) and polylactic acid (PLA) 3D printing activities and ex situ analysis during ABS printing. We examined the effect of a high-efficiency particulate air filter attachment on ABS emissions and particle chemical composition and demonstrate that filtration was effective in preventing UFP emissions and that particles sampled during filtered prints did not have a high contribution (∼4% vs ∼10%) from aromatic ions in the mass spectrum. Ex situ analysis of particles collected during ABS printing was performed via TEM and electron energy loss spectroscopy, which indicated a high level of sp2 bonding type consistent with polymeric styrene. One 3D print with PLA resulted in an aerosol mass size distribution with a peak at ∼300 nm. Unfiltered ABS prints resulted in particle mass size distributions with peak diameters of ∼100 nm.


Subject(s)
Air Pollution, Indoor , Volatile Organic Compounds , Aerosols , Particle Size , Particulate Matter , Styrene
13.
Environ Sci Process Impacts ; 22(1): 227, 2020 Jan 01.
Article in English | MEDLINE | ID: mdl-31848558

ABSTRACT

Correction for 'Seasonal variation in aerosol composition and concentration upon transport from the outdoor to indoor environment' by Anita M. Avery et al., Environ. Sci.: Processes Impacts, 2019, 21, 528-547.

15.
J Expo Sci Environ Epidemiol ; 30(2): 253-261, 2020 03.
Article in English | MEDLINE | ID: mdl-31695112

ABSTRACT

Potted plants have demonstrated abilities to remove airborne volatile organic compounds (VOC) in small, sealed chambers over timescales of many hours or days. Claims have subsequently been made suggesting that potted plants may reduce indoor VOC concentrations. These potted plant chamber studies reported outcomes using various metrics, often not directly applicable to contextualizing plants' impacts on indoor VOC loads. To assess potential impacts, 12 published studies of chamber experiments were reviewed, and 196 experimental results were translated into clean air delivery rates (CADR, m3/h), which is an air cleaner metric that can be normalized by volume to parameterize first-order loss indoors. The distribution of single-plant CADR spanned orders of magnitude, with a median of 0.023 m3/h, necessitating the placement of 10-1000 plants/m2 of a building's floor space for the combined VOC-removing ability by potted plants to achieve the same removal rate that outdoor-to-indoor air exchange already provides in typical buildings (~1 h-1). Future experiments should shift the focus from potted plants' (in)abilities to passively clean indoor air, and instead investigate VOC uptake mechanisms, alternative biofiltration technologies, biophilic productivity and well-being benefits, or negative impacts of other plant-sourced emissions, which must be assessed by rigorous field work accounting for important indoor processes.


Subject(s)
Air Pollution, Indoor/analysis , Plants , Volatile Organic Compounds/analysis , Air Pollutants/analysis
16.
Environ Sci Technol ; 53(15): 8591-8598, 2019 Aug 06.
Article in English | MEDLINE | ID: mdl-31283200

ABSTRACT

Although ammonia (NH3) is usually found at outdoor concentrations of 1-5 ppb, indoor ammonia concentrations can be much higher. Indoor ammonia is strongly emitted from cleaning products, tobacco smoke, building materials, and humans. Because of ammonia's high reactivity, solubility in water, and tendency to sorb to a variety of surfaces, it is difficult to measure, and thus a comprehensive evaluation of indoor ammonia concentrations remains an understudied topic. During HOMEChem, which was a comprehensive indoor chemistry study occurring in a test house during June 2018, the real-time concentration of ammonia indoors was measured using cavity ring-down spectroscopy. A mean unoccupied background concentration of 32 ppb was observed, with further enhancements of ammonia occurring during cooking, cleaning, and occupancy activities, reaching maximum concentrations during these activities of 130, 1592, and 99 ppb, respectively. Furthermore, ammonia concentrations were strongly influenced by indoor temperatures and heating, ventilation, and air conditioning (HVAC) operation. In the absence of activity-based sources, the HVAC operation was the main modulator of ammonia concentration indoors.


Subject(s)
Air Pollutants , Air Pollution, Indoor , Ammonia , Environmental Monitoring , Humans , Ventilation
17.
Environ Sci Process Impacts ; 21(8): 1240-1254, 2019 Aug 14.
Article in English | MEDLINE | ID: mdl-31070639

ABSTRACT

We report on the development of a modelling consortium for chemistry in indoor environments that connects models over a range of spatial and temporal scales, from molecular to room scales and from sub-nanosecond to days, respectively. Our modeling approaches include molecular dynamics (MD) simulations, kinetic process modeling, gas-phase chemistry modeling, organic aerosol modeling, and computational fluid dynamics (CFD) simulations. These models are applied to investigate ozone reactions with skin and clothing, oxidation of volatile organic compounds and formation of secondary organic aerosols, and mass transport and partitioning of indoor species to surfaces. MD simulations provide molecular pictures of limonene adsorption on SiO2 and ozone interactions with the skin lipid squalene, providing kinetic parameters such as surface accommodation coefficient, desorption lifetime, and bulk diffusivity. These parameters then constrain kinetic process models, which resolve mass transport and chemical reactions in gas and condensed phases for analysis of experimental data. A detailed indoor chemical box model is applied to simulate α-pinene ozonolysis with improved representation of gas-particle partitioning. Application of 2D-volatility basis set reveals that OH-induced aging sometimes drives increases in indoor organic aerosol concentrations, due to organic mass functionalization and enhanced partitioning. CFD simulations show that concentrations of ozone and primary product change near the human surface rapidly, indicating non-uniform spatial distributions from the occupant surface to ambient air, while secondary ozone product is relatively well-mixed throughout the room. This development establishes a framework to integrate different modeling tools and experimental measurements, opening up an avenue for development of comprehensive and integrated models with representations of various chemistry in indoor environments.


Subject(s)
Air Pollutants/chemistry , Air Pollution, Indoor/analysis , Models, Theoretical , Ozone/chemistry , Volatile Organic Compounds/chemistry , Aerosols , Air Pollutants/analysis , Humans , Kinetics , Oxidation-Reduction , Ozone/analysis , Skin/chemistry , Spatio-Temporal Analysis , Surface Properties , Textiles/analysis , Volatile Organic Compounds/analysis
18.
Environ Sci Process Impacts ; 21(8): 1301-1312, 2019 Aug 14.
Article in English | MEDLINE | ID: mdl-30997458

ABSTRACT

Humans impact indoor air quality directly via emissions from skin, breath, or personal care products, and indirectly via reactions of oxidants with skin constituents, or with skin that has been shed. However, separating the influence of the many emissions and their oxidation products from the influence of outdoor-originated aerosols has been a challenge. Indoor and outdoor aerosols were alternatively sampled at 4 minute time resolution with a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) in a classroom with student occupants at regular intervals per university class schedule. Mass spectral analysis showed aerosol enhancements of oxidized and unoxidized hydrocarbon ion families during occupied periods, especially at ion fragments larger than m/z 100 and double bond equivalents consistent with squalene (C30H50) and its oxidized products from reaction with ozone, indicative of the secondary nature of the aerosol mass. Individual hydrocarbon mass fragments consistent with squalene fragmentation, including C5H9+, and C6H9+ were especially enhanced with room occupancy. Emissions of individual organic fragment ions were estimated using a model accounting for outdoor aerosols and air exchange. This showed occupancy related emissions at smaller fragments (C3H5+, C4H9+) that despite reflecting mostly outdoor-originated aerosols transported indoors, also show enhancements from occupant emissions indoors. Total emission of all fragments was 17.6 µg ß-1 h-1 above unoccupied levels, translating to approximately 25% increase in organic aerosol mass concentration in the classroom during an occupied hour with a median occupied ozone loss (ß). Human occupants, therefore, represent an additional mass burden of organic aerosol, especially in poorly ventilated or highly occupied indoor spaces.


Subject(s)
Aerosols/analysis , Air Pollutants/analysis , Air Pollution, Indoor/analysis , Environmental Monitoring/methods , Housing/standards , Humans , Hydrocarbons/analysis , Mass Spectrometry , Ozone/chemistry , Ventilation
19.
Indoor Air ; 29(4): 616-629, 2019 07.
Article in English | MEDLINE | ID: mdl-30861195

ABSTRACT

Organic aerosol (OA) is chemically dynamic, continuously evolving by oxidative chemistry, for instance, via hydroxyl radical (OH) reactions. Studies have explored this evolution (so-called OA aging) in the atmosphere, but none have investigated it indoors. Aging organic molecules in both particle and gas-phases undergo changes in oxygen content and volatility, which may ultimately either enhance or reduce the condensed-phase OA concentration (COA ). This work models OH-induced aging using the two-dimensional volatility basis set (2D-VBS) within an indoor model and explores its significance on COA relative to prior modeling methodologies which neglect aging transformations. Lagrangian, time-averaged, and transient indoor simulations were conducted. The time-averaged simulations included a Monte Carlo procedure and sensitivity analysis, using input distributions typical of U.S. residences. Results demonstrate that indoors, aging generally leads to COA augmentation. The extent to which this is significant is conditional upon several factors, most notably temperature, OH exposure, and OA mass loading. Time-averaged COA was affected minimally in typical residences (<5% increase). However, some plausible cases may cause stronger COA enhancements, such as in a sunlit room where photolysis facilitates significant OH production (~20% increase), or during a transient OH-producing cleaning event (~35% peak increase).


Subject(s)
Aerosols/analysis , Models, Chemical , Oxidation-Reduction , Ozone/analysis , Volatile Organic Compounds/analysis , Air Pollution, Indoor/analysis , Computer Simulation , Humans , Monte Carlo Method , Organic Chemicals , United States , Volatilization
20.
Environ Sci Process Impacts ; 21(3): 528-547, 2019 Mar 20.
Article in English | MEDLINE | ID: mdl-30698188

ABSTRACT

Outdoor-originated aerosols are an important component impacting indoor air quality. Since outdoor aerosols vary over short (diurnal) and long (seasonal) timescales, we examined how the variation in outdoor aerosol concentration and composition impact indoor aerosol. Measurements of both indoor and outdoor aerosol composition in real time in an urban classroom in winter and summer seasons were performed using an aerosol mass spectrometer (AMS), aethalometer, and a suite of gas phase instruments. Factor analysis of the organic aerosol components identified three factors in common between seasons, including hydrocarbon-like, cooking, and oxidized organic aerosol (HOA, COA, and OOA). Since sulfate is non-volatile, we report a sulfate-normalized indoor-outdoor ratio (I/O)i/SO4 for measured aerosol i components, allowing us to estimate aerosol component-based effects of seasonal and other variations in ventilation and HVAC operation, indoor emission sources, and chemically-based loss processes between outdoor and indoor environments. These chemical loss processes are interpreted in terms of changes in temperature and relative humidity (RH) between environments, which fluctuate on a daily and seasonal basis. The degree to which any effect is observed depends on the particular outdoor aerosol population and the magnitude of temperature or RH change. In wintertime, when aerosols were warmed upon transport indoors and loss of volatile components is favored, median (I/O)i/SO4 values for nitrate, total organics, HOA, and BC were smaller (0.35, 1.00, 1.24, and 1.18, respectively) than summertime values (0.75, 1.17, 1.96, and 1.80). For COA and OOA, however, (I/O)i/SO4 values were higher in the winter than in summer. Calculated aerosol liquid water (ALW), which is a function of temperature and RH and the relative contribution of hygroscopic components, varied significantly by season. Summertime ALW indoors provides a medium for aqueous processing, which is necessary for some hydrophilic gas phase reaction products that are important to indoor air quality and occupant exposure. This work describes the linkages between seasonal variability in aerosol composition outdoors and the subsequent chemically-specific variation observed when that aerosol is brought indoors.


Subject(s)
Air Pollutants/analysis , Air Pollution, Indoor/analysis , Environmental Monitoring/methods , Volatile Organic Compounds/analysis , Aerosols , Philadelphia , Seasons , Temperature
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