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1.
Environ Sci Technol ; 58(25): 11084-11095, 2024 Jun 25.
Artigo em Inglês | MEDLINE | ID: mdl-38860676

RESUMO

Ethylene oxide ("EtO") is an industrially made volatile organic compound and a known human carcinogen. There are few reliable reports of ambient EtO concentrations around production and end-use facilities, however, despite major exposure concerns. We present in situ, fast (1 Hz), sensitive EtO measurements made during February 2023 across the southeastern Louisiana industrial corridor. We aggregated mobile data at 500 m spatial resolution and reported average mixing ratios for 75 km of the corridor. Mean and median aggregated values were 31.4 and 23.3 ppt, respectively, and a majority (75%) of 500 m grid cells were above 10.9 ppt, the lifetime exposure concentration corresponding to 100-in-one million excess cancer risk (1 × 10-4). A small subset (3.3%) were above 109 ppt (1000-in-one million cancer risk, 1 × 10-3); these tended to be near EtO-emitting facilities, though we observed plumes over 10 km from the nearest facilities. Many plumes were highly correlated with other measured gases, indicating potential emission sources, and a subset was measured simultaneously with a second commercial analyzer, showing good agreement. We estimated EtO for 13 census tracts, all of which were higher than EPA estimates (median difference of 21.3 ppt). Our findings provide important information about EtO concentrations and potential exposure risks in a key industrial region and advance the application of EtO analytical methods for ambient sampling and mobile monitoring for air toxics.


Assuntos
Monitoramento Ambiental , Óxido de Etileno , Louisiana , Monitoramento Ambiental/métodos , Humanos , Poluentes Atmosféricos/análise
2.
Environ Res ; 257: 119220, 2024 May 24.
Artigo em Inglês | MEDLINE | ID: mdl-38797466

RESUMO

Brick kiln emissions adversely affect air pollution and the health of workers and individuals living near the kilns; however, evidence of their impacts remains limited. We conducted a systematic review of brick kiln pollution (emissions, source contributions and personal exposures) and its effects on health. We extracted articles from electronic databases and through manual citation searching. We estimated pooled, sample-size-weighted means and standard deviations for personal exposures by job type; computed mean emission factors and pollutant concentrations by brick kiln design; and meta-analyzed differences in means or proportions for health outcomes between brick kiln workers and controls or for participants living near or far away from kilns. We identified 104 studies; 74 were conducted in South Asia. The most evaluated pollutants were particulate matter (PM; n = 48), sulfur dioxide (SO2; n = 24) and carbon monoxide (CO; n = 22), and the most evaluated health outcomes were respiratory health (n = 34) and musculoskeletal disorders (n = 9). PM and CO emissions were higher among traditional than improved brick kilns. Mean respirable silica exposures were only measured in 4 (4%) studies and were as high as 620 µg/m3, exceeding the NIOSH recommended exposure limit by a factor of over 12. Brick kiln workers had consistently worse lung function, more respiratory symptoms, more musculoskeletal complaints, and more inflammation when compared to unexposed participants across studies; however, most studies had a small sample size and did not fully describe methods used for sampling or data collection. On average, brick kiln workers had worse health outcomes when compared to unexposed controls but study quality supporting the evidence was low. Few studies reported silica concentrations or personal exposures, but the few that did suggest that exposures are high. Further research is needed to better understand the relationship between brick kiln pollution and health among workers, and to evaluate exposure mitigation strategies.

3.
Environ Sci Technol ; 57(45): 17374-17383, 2023 11 14.
Artigo em Inglês | MEDLINE | ID: mdl-37930106

RESUMO

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.


Assuntos
Poluentes Atmosféricos , Poluição do Ar em Ambientes Fechados , Compostos Orgânicos Voláteis , Poluentes Atmosféricos/análise , Compostos Orgânicos Voláteis/análise , Aerossóis/análise , Culinária , Temperatura , Poluição do Ar em Ambientes Fechados/análise , Monitoramento Ambiental/métodos
4.
Environ Sci Technol ; 56(1): 109-118, 2022 01 04.
Artigo em Inglês | MEDLINE | ID: mdl-34910454

RESUMO

Reactive organic carbon (ROC) comprises a substantial fraction of the total atmospheric carbon budget. Emissions of ROC fuel atmospheric oxidation chemistry to produce secondary pollutants including ozone, carbon dioxide, and particulate matter. Compared to the outdoor atmosphere, the indoor organic carbon budget is comparatively understudied. We characterized indoor ROC in a test house during unoccupied, cooking, and cleaning scenarios using various online mass spectrometry and gas chromatography measurements of gaseous and particulate organics. Cooking greatly impacted indoor ROC concentrations and bulk physicochemical properties (e.g., volatility and oxidation state), while cleaning yielded relatively insubstantial changes. Additionally, cooking enhanced the reactivities of hydroxyl radicals and ozone toward indoor ROC. We observed consistently higher median ROC concentrations indoors (≥223 µg C m-3) compared to outdoors (54 µg C m-3), demonstrating that buildings can be a net source of reactive carbon to the outdoor atmosphere, following its removal by ventilation. We estimate the unoccupied test house emitted 0.7 g C day-1 from ROC to outdoors. Indoor ROC emissions may thus play an important role in air quality and secondary pollutant formation outdoors, particularly in urban and suburban areas, and indoors during the use of oxidant-generating air purifiers.


Assuntos
Poluentes Atmosféricos , Poluição do Ar em Ambientes Fechados , Poluentes Atmosféricos/análise , Poluição do Ar em Ambientes Fechados/análise , Monitoramento Ambiental/métodos , Cromatografia Gasosa-Espectrometria de Massas , Material Particulado/análise
5.
Environ Sci Technol ; 56(17): 12148-12157, 2022 09 06.
Artigo em Inglês | MEDLINE | ID: mdl-35952310

RESUMO

Analytical capabilities in atmospheric chemistry provide new opportunities to investigate indoor air. HOMEChem was a chemically comprehensive indoor field campaign designed to investigate how common activities, such as cooking and cleaning, impacted indoor air in a test home. We combined gas-phase chemical data of all compounds, excluding those with concentrations <1 ppt, with established databases of health effect thresholds to evaluate potential risks associated with gas-phase air contaminants and indoor activities. The chemical composition of indoor air is distinct from outdoor air, with gaseous compounds present at higher levels and greater diversity─and thus greater predicted hazard quotients─indoors than outdoors. Common household activities like cooking and cleaning induce rapid changes in indoor air composition, raising levels of multiple compounds with high risk quotients. The HOMEChem data highlight how strongly human activities influence the air we breathe in the built environment, increasing the health risk associated with exposure to air contaminants.


Assuntos
Poluentes Atmosféricos , Poluição do Ar em Ambientes Fechados , Poluentes Atmosféricos/análise , Poluição do Ar em Ambientes Fechados/análise , Culinária , Monitoramento Ambiental , Gases , Humanos , Material Particulado/análise
6.
Indoor Air ; 32(7): e13075, 2022 07.
Artigo em Inglês | MEDLINE | ID: mdl-35904391

RESUMO

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.


Assuntos
Poluentes Atmosféricos , Poluição do Ar em Ambientes Fechados , Aerossóis/análise , Poluentes Atmosféricos/análise , Poluição do Ar em Ambientes Fechados/análise , Amônia , Monitoramento Ambiental/métodos , Ácido Nítrico , Material Particulado , Sulfatos , Termodinâmica
7.
Environ Sci Technol ; 55(13): 9000-9011, 2021 07 06.
Artigo em Inglês | MEDLINE | ID: mdl-34106692

RESUMO

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.


Assuntos
Poluentes Atmosféricos , Poluição do Ar em Ambientes Fechados , Aerossóis/análise , Poluentes Atmosféricos/análise , Poluição do Ar em Ambientes Fechados/análise , Monitoramento Ambiental , Tamanho da Partícula , Material Particulado/análise , Temperatura
8.
Environ Sci Technol ; 55(8): 4532-4541, 2021 04 20.
Artigo em Inglês | MEDLINE | ID: mdl-33788543

RESUMO

Nitrogen oxides (NOX) and methane impact air quality through the promotion of ozone formation, and methane is also a strong greenhouse gas. Despite the importance of these pollutants, emissions in urban areas are poorly quantified. We present measurements of NOX, CH4, CO, and CO2 made at Drexel University in Philadelphia along with NOX and CO observations at two roadside monitors. Because CO2 concentrations in the winter result almost entirely from combustion with negligible influence from photosynthesis and respiration, we are able to infer fleet-averaged fuel-based emission factors (EFs) for NOX and CO, similar in some ways to how EFs are determined from tunnel studies. Comparison of the inferred NOX and CO fuel-based EF to the National Emissions Inventory (NEI) suggests errors in NEI emissions of either NOX, CO, or both. From the measurements of CH4 and CO2, which are not emitted by the same sources, we infer the ratio of CH4 emissions (from leaks in the natural gas infrastructure) to CO2 emissions (from fossil fuel combustion) in Philadelphia. Comparison of the CH4/CO2 emission ratios to emission inventories from the Environmental Protection Agency suggests underestimates in CH4 emissions by almost a factor of 4. These results demonstrate the need for the addition of long-term observations of CH4 and CO2 to existing monitoring networks in urban areas to better constrain emissions and complement existing measurements of NOX and CO.


Assuntos
Poluentes Atmosféricos , Monóxido de Carbono , Poluentes Atmosféricos/análise , Dióxido de Carbono/análise , Monóxido de Carbono/análise , Monitoramento Ambiental , Humanos , Metano/análise , Óxidos de Nitrogênio/análise , Philadelphia
9.
Environ Sci Technol ; 55(16): 10987-10993, 2021 08 17.
Artigo em Inglês | MEDLINE | ID: mdl-34342979

RESUMO

Water-soluble trace gas (WSTG) loss from indoor air via air conditioning (AC) units has been observed in several studies, but these results have been difficult to generalize. In the present study, we designed a box model that can be used to investigate and estimate WSTG removal due to partitioning to AC coil condensate. We compared the model output to measurements of a suite of organic acids cycling in an indoor environment and tested the model by varying the input AC parameters. These tests showed that WSTG loss via AC cycling is influenced by Henry's law constant of the compound in question, which is controlled by air and water temperatures and the condensate pH. Air conditioning unit specifications also impact WSTG loss through variations in the sensible heat ratio, the effective recirculation rate of air through the unit, and the timing of coil and fan operation. These findings have significant implications for indoor modeling. To accurately model the fate of indoor WSTGs, researchers must either measure or otherwise account for these unique environmental and operational characteristics.


Assuntos
Poluição do Ar em Ambientes Fechados , Ar Condicionado , Poluição do Ar em Ambientes Fechados/análise , Gases , Compostos Orgânicos , Água
10.
Indoor Air ; 31(1): 141-155, 2021 01.
Artigo em Inglês | MEDLINE | ID: mdl-32696534

RESUMO

Understanding the sources and composition of organic aerosol (OA) in indoor environments requires rapid measurements, since many emissions and processes have short timescales. However, real-time molecular-level OA measurements have not been reported indoors. Here, we present quantitative measurements, at a time resolution of five seconds, of molecular ions corresponding to diverse aerosol-phase species, by applying extractive electrospray ionization mass spectrometry (EESI-MS) to indoor air analysis for the first time, as part of the highly instrumented HOMEChem field study. We demonstrate how the complex spectra of EESI-MS are screened in order to extract chemical information and investigate the possibility of interference from gas-phase semivolatile species. During experiments that simulated the Thanksgiving US holiday meal preparation, EESI-MS quantified multiple species, including fatty acids, carbohydrates, siloxanes, and phthalates. Intercomparisons with Aerosol Mass Spectrometer (AMS) and Scanning Mobility Particle Sizer suggest that EESI-MS quantified a large fraction of OA. Comparisons with FIGAERO-CIMS shows similar signal levels and good correlation, with a range of 100 for the relative sensitivities. Comparisons with SV-TAG for phthalates and with SV-TAG and AMS for total siloxanes also show strong correlation. EESI-MS observations can be used with gas-phase measurements to identify co-emitted gas- and aerosol-phase species, and this is demonstrated using complementary gas-phase PTR-MS observations.


Assuntos
Aerossóis/análise , Poluição do Ar em Ambientes Fechados , Espectrometria de Massas por Ionização por Electrospray , Monitoramento Ambiental/métodos , Compostos Orgânicos
11.
Environ Sci Technol ; 54(12): 7107-7116, 2020 06 16.
Artigo em Inglês | MEDLINE | ID: mdl-32391692

RESUMO

It is important to improve our understanding of exposure to particulate matter (PM) in residences because of associated health risks. The HOMEChem campaign was conducted to investigate indoor chemistry in a manufactured test house during prescribed everyday activities, such as cooking, cleaning, and opening doors and windows. This paper focuses on measured size distributions of PM (0.001-20 µm), along with estimated exposures and respiratory-tract deposition. Number concentrations were highest for sub-10 nm particles during cooking using a propane-fueled stovetop. During some cooking activities, calculated PM2.5 mass concentrations (assuming a density of 1 g cm-3) exceeded 250 µg m-3, and exposure during the postcooking decay phase exceeded that of the cooking period itself. The modeled PM respiratory deposition for an adult residing in the test house kitchen for 12 h varied from 7 µg on a day with no indoor activities to 68 µg during a simulated day (including breakfast, lunch, and dinner preparation interspersed by cleaning activities) and rose to 149 µg during a simulated Thanksgiving day.


Assuntos
Poluentes Atmosféricos , Poluição do Ar em Ambientes Fechados , Adulto , Poluentes Atmosféricos/análise , Poluição do Ar em Ambientes Fechados/análise , Culinária , Monitoramento Ambiental , Habitação , Humanos , Tamanho da Partícula , Material Particulado/análise
12.
Environ Sci Technol ; 54(2): 947-954, 2020 01 21.
Artigo em Inglês | MEDLINE | ID: mdl-31834782

RESUMO

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.


Assuntos
Poluição do Ar em Ambientes Fechados , Compostos Orgânicos Voláteis , Aerossóis , Tamanho da Partícula , Material Particulado , Estireno
13.
Environ Sci Technol ; 54(11): 6751-6760, 2020 06 02.
Artigo em Inglês | MEDLINE | ID: mdl-32379430

RESUMO

Measurements by semivolatile thermal desorption aerosol gas chromatography (SV-TAG) were used to investigate how semivolatile organic compounds (SVOCs) partition among indoor reservoirs in (1) a manufactured test house under controlled conditions (HOMEChem campaign) and (2) a single-family residence when vacant (H2 campaign). Data for phthalate diesters and siloxanes suggest that volatility-dependent partitioning processes modulate airborne SVOC concentrations through interactions with surface-laden condensed-phase reservoirs. Airborne concentrations of SVOCs with vapor pressures in the range of C13 to C23 alkanes were observed to be correlated with indoor air temperature. Observed temperature dependencies were quantitatively similar to theoretical predictions that assumed a surface-air boundary layer with equilibrium partitioning maintained at the air-surface interface. Airborne concentrations of SVOCs with vapor pressures corresponding to C25 to C31 alkanes correlated with airborne particle mass concentration. For SVOCs with higher vapor pressures, which are expected to be predominantly gaseous, correlations with particle mass concentration were weak or nonexistent. During primary particle emission events, enhanced gas-phase emissions from condensed-phase reservoirs partitioned to airborne particles, contributing substantially to organic particulate matter. An emission event related to oven-usage was inferred to deposit siloxanes in condensed-phase reservoirs throughout the house, leading to the possibility of reemission during subsequent periods with high particle loading.


Assuntos
Poluentes Atmosféricos , Poluição do Ar em Ambientes Fechados , Compostos Orgânicos Voláteis , Poluentes Atmosféricos/análise , Poluição do Ar em Ambientes Fechados/análise , Habitação , Material Particulado/análise , Compostos Orgânicos Voláteis/análise , Volatilização
14.
Environ Sci Technol ; 54(3): 1730-1739, 2020 02 04.
Artigo em Inglês | MEDLINE | ID: mdl-31940195

RESUMO

We report elevated levels of gaseous inorganic chlorinated and nitrogenated compounds in indoor air while cleaning with a commercial bleach solution during the House Observations of Microbial and Environmental Chemistry field campaign in summer 2018. Hypochlorous acid (HOCl), chlorine (Cl2), and nitryl chloride (ClNO2) reached part-per-billion by volume levels indoors during bleach cleaning-several orders of magnitude higher than typically measured in the outdoor atmosphere. Kinetic modeling revealed that multiphase chemistry plays a central role in controlling indoor chlorine and reactive nitrogen chemistry during these periods. Cl2 production occurred via heterogeneous reactions of HOCl on indoor surfaces. ClNO2 and chloramine (NH2Cl, NHCl2, NCl3) production occurred in the applied bleach via aqueous reactions involving nitrite (NO2-) and ammonia (NH3), respectively. Aqueous-phase and surface chemistry resulted in elevated levels of gas-phase nitrogen dioxide (NO2). We predict hydroxyl (OH) and chlorine (Cl) radical production during these periods (106 and 107 molecules cm-3 s-1, respectively) driven by HOCl and Cl2 photolysis. Ventilation and photolysis accounted for <50% and <0.1% total loss of bleach-related compounds from indoor air, respectively; we conclude that uptake to indoor surfaces is an important additional loss process. Indoor HOCl and nitrogen trichloride (NCl3) mixing ratios during bleach cleaning reported herein are likely detrimental to human health.


Assuntos
Poluentes Atmosféricos , Poluição do Ar em Ambientes Fechados , Cloro , Gases , Humanos , Ácido Hipocloroso , Ventilação
15.
Environ Sci Technol ; 53(15): 8591-8598, 2019 Aug 06.
Artigo em Inglês | MEDLINE | ID: mdl-31283200

RESUMO

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.


Assuntos
Poluentes Atmosféricos , Poluição do Ar em Ambientes Fechados , Amônia , Monitoramento Ambiental , Humanos , Ventilação
16.
Environ Sci Technol ; 49(17): 10421-30, 2015 Sep 01.
Artigo em Inglês | MEDLINE | ID: mdl-26237368

RESUMO

The spatial distribution of PM1 components in the Barcelona metropolitan area was investigated using on-road mobile measurements of atmospheric particle- and gas-phase compounds during the DAURE campaign in March 2009. Positive matrix factorization (PMF) applied to organic aerosol (OA) data yielded 5 factors: hydrocarbon-like OA (HOA), cooking OA (COA), biomass burning OA (BBOA), and low volatility and semivolatile oxygenated OA (LV-OOA and SV-OOA). The area under investigation (∼500 km(2)) was divided into six zones (city center, harbor, industrial area, precoastal depression, 2 mountain ranges) for measurements and data analysis. Mean zonal OA concentrations are 4.9-9.5 µg m(-3). The area is heavily impacted by local primary emissions (HOA 14-38%, COA 10-18%, BBOA 10-12% of OA); concentrations of traffic-related components, especially black carbon, are biased high due to the on-road nature of the measurements. The formation of secondary OA adds more than half of the OA burden outside the city center (SV-OOA 14-40%, LV-OOA 17-42% of OA). A case study of one measurement drive from the shore to the precoastal mountain range furthest downwind of the city center indicates the importance of nonfossil over anthropogenic secondary OA based on OA/CO.


Assuntos
Aerossóis/análise , Poluentes Atmosféricos/análise , Modelos Teóricos , Compostos Orgânicos/análise , Biomassa , Cidades , Culinária , Geografia , Material Particulado/análise , Espanha , Volatilização
17.
Environ Sci Technol ; 49(11): 7012-20, 2015 Jun 02.
Artigo em Inglês | MEDLINE | ID: mdl-25897974

RESUMO

Limited direct measurements of criteria pollutants emissions and precursors, as well as natural gas constituents, from Marcellus shale gas development activities contribute to uncertainty about their atmospheric impact. Real-time measurements were made with the Aerodyne Research Inc. Mobile Laboratory to characterize emission rates of atmospheric pollutants. Sites investigated include production well pads, a well pad with a drill rig, a well completion, and compressor stations. Tracer release ratio methods were used to estimate emission rates. A first-order correction factor was developed to account for errors introduced by fenceline tracer release. In contrast to observations from other shale plays, elevated volatile organic compounds, other than CH4 and C2H6, were generally not observed at the investigated sites. Elevated submicrometer particle mass concentrations were also generally not observed. Emission rates from compressor stations ranged from 0.006 to 0.162 tons per day (tpd) for NOx, 0.029 to 0.426 tpd for CO, and 67.9 to 371 tpd for CO2. CH4 and C2H6 emission rates from compressor stations ranged from 0.411 to 4.936 tpd and 0.023 to 0.062 tpd, respectively. Although limited in sample size, this study provides emission rate estimates for some processes in a newly developed natural gas resource and contributes valuable comparisons to other shale gas studies.


Assuntos
Poluentes Atmosféricos/análise , Atmosfera/química , Sedimentos Geológicos/química , Gás Natural/análise , Monóxido de Carbono/análise , Íons , Limite de Detecção , Espectrometria de Massas , Metano/análise , Óxido Nitroso/análise , Pennsylvania , Fatores de Tempo , Compostos Orgânicos Voláteis/análise
18.
Proc Natl Acad Sci U S A ; 109(34): 13503-8, 2012 Aug 21.
Artigo em Inglês | MEDLINE | ID: mdl-22869714

RESUMO

The Multiple Chamber Aerosol Chemical Aging Study (MUCHACHAS) tested the hypothesis that hydroxyl radical (OH) aging significantly increases the concentration of first-generation biogenic secondary organic aerosol (SOA). OH is the dominant atmospheric oxidant, and MUCHACHAS employed environmental chambers of very different designs, using multiple OH sources to explore a range of chemical conditions and potential sources of systematic error. We isolated the effect of OH aging, confirming our hypothesis while observing corresponding changes in SOA properties. The mass increases are consistent with an existing gap between global SOA sources and those predicted in models, and can be described by a mechanism suitable for implementation in those models.


Assuntos
Aerossóis/química , Compostos Orgânicos/química , Atmosfera , Radicais Livres , Radical Hidroxila , Espectrometria de Massas/métodos , Modelos Químicos , Oxigênio/química , Ozônio , Reprodutibilidade dos Testes , Solventes/química , Raios Ultravioleta
19.
ACS EST Air ; 1(3): 175-187, 2024 Mar 08.
Artigo em Inglês | MEDLINE | ID: mdl-38482267

RESUMO

The oxidative potential (OP) of outdoor PM2.5 in wintertime Fairbanks, Alaska, is investigated and compared to those in wintertime Atlanta and Los Angeles. Approximately 40 filter samples collected in January-February 2022 at a Fairbanks residential site were analyzed for OP utilizing dithiothreitol-depletion (OPDTT) and hydroxyl-generation (OPOH) assays. The study-average PM2.5 mass concentration was 12.8 µg/m3, with a 1 h average maximum of 89.0 µg/m3. Regression analysis, correlations with source tracers, and contrast between cold and warmer events indicated that OPDTT was mainly sensitive to copper, elemental carbon, and organic aerosol from residential wood burning, and OPOH to iron and organic aerosol from vehicles. Despite low photochemically-driven oxidation rates, the water-soluble fraction of OPDTT was unusually high at 77%, mainly from wood burning emissions. In contrast to other locations, the Fairbanks average PM2.5 mass concentration was higher than Atlanta and Los Angeles, whereas OPDTT in Fairbanks and Atlanta were similar, and Los Angeles had the highest OPDTT and OPOH. Site differences were observed in OP when normalized by both the volume of air sampled and the particle mass concentration, corresponding to exposure and the intrinsic health-related properties of PM2.5, respectively. The sensitivity of OP assays to specific aerosol components and sources can provide insights beyond the PM2.5 mass concentration when assessing air quality.

20.
ACS EST Air ; 1(3): 188-199, 2024 Mar 08.
Artigo em Inglês | MEDLINE | ID: mdl-38482268

RESUMO

The indoor air quality of a residential home during winter in Fairbanks, Alaska, was investigated and contrasted with outdoor levels. Twenty-four-hour average indoor and outdoor filter samples were collected from January 17 to February 25, 2022, in a residential area with high outdoor PM2.5 concentrations. The oxidative potential of PM2.5 was determined using the dithiothreitol-depletion assay (OPDTT). For the unoccupied house, the background indoor-to-outdoor (I/O) ratio of mass-normalized OP (OPmDTT), a measure of the intrinsic health-relevant properties of the aerosol, was less than 1 (0.53 ± 0.37), implying a loss of aerosol toxicity as air was transported indoors. This may result from transport and volatility losses driven by the large gradients in temperature (average outdoor temperature of -19°C/average indoor temperature of 21 °C) or relative humidity (average outdoor RH of 78%/average indoor RH of 11%), or both. Various indoor activities, including pellet stove use, simple cooking experiments, incense burning, and mixtures of these activities, were conducted. The experiments produced PM2.5 with a highly variable OPmDTT. PM2.5 from cooking emissions had the lowest OP values, while pellet stove PM2.5 had the highest. Correlations between volume-normalized OPDTT (OPvDTT), relevant to exposure, and indoor PM2.5 mass concentration during experiments were much lower compared to those in outdoor environments. This suggests that mass concentration alone can be a poor indicator of possible adverse effects of various indoor emissions. These findings highlight the importance of considering both the quantity of particles and sources (chemical composition), as health metrics for indoor air quality.

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