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Direct-on-Filter (DoF) analysis of respirable crystalline silica (RCS) by Fourier Transform Infrared (FTIR) spectroscopy is a useful tool for assessing exposure risks. With the RCS exposure limits becoming lower, it is important to characterize and reduce measurement uncertainties. This study systematically evaluated two filter types (i.e., polyvinyl chloride [PVC] and polytetrafluoroethylene [PTFE]) for RCS measurements by DoF FTIR spectroscopy, including the filter-to-filter and day-to-day variability of blank filter FTIR reference spectra, particle deposition patterns, filtration efficiencies, and pressure drops. For PVC filters sampled at a flow rate of 2.5 L/min for 8 h, the RCS limit of detection (LOD) was 7.4 µg/m3 when a designated laboratory reference filter was used to correct the absorption by the filter media. When the spectrum of the pre-sample filter (blank filter before dust sampling) was used for correction, the LOD could be up to 5.9 µg/m3. The PVC absorption increased linearly with reference filter mass, providing a means to correct the absorption differences between the pre-sample and reference filters. For PTFE, the LODs were 12 and 1.2 µg/m3 when a designated laboratory blank or the pre-sample filter spectrum was used for blank correction, respectively, indicating that using the pre-sample blank spectrum will reduce RCS quantification uncertainty. Both filter types exhibited a consistent radially symmetric deposition pattern when particles were collected using 3-piece cassettes, indicating that RCS can be quantified from a single measurement at the filter center. The most penetrating aerodynamic diameters were around 0.1 µm with filtration efficiencies ≥ 98.8% across the measured particle size range with low-pressure drops (0.2-0.3 kPa) at a flow rate of 2.5 L/min. This study concludes that either the PVC or the PTFE filters are suitable for RCS analysis by DoF FTIR, but proper methods are needed to account for the variability of blank absorption among different filters.
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Politetrafluoretileno , Cloreto de Polivinila , Dióxido de Silício , Espectroscopia de Infravermelho com Transformada de Fourier/métodos , Cloreto de Polivinila/química , Dióxido de Silício/análise , Dióxido de Silício/química , Politetrafluoretileno/química , Filtração/instrumentação , Filtros de Ar , Poeira/análise , Exposição Ocupacional/análise , Poluentes Ocupacionais do Ar/análise , Monitoramento Ambiental/métodos , Monitoramento Ambiental/instrumentação , Limite de Detecção , Tamanho da Partícula , Exposição por Inalação/análiseRESUMO
The Guanzhong Basin (GZB) of northwest China is examined as a mega-region containing the mega-city of Xi'an. The concept of a "mega-region" is more accurate than that of a "mega-city" for air quality management as there is an interaction between urban and non-urban emissions. Parallels are drawn between the GZB and the San Joaquin Valley (SJV) mega-region of central California for excessive wintertime PM2.5 concentrations. Long-term chemical composition measurements show the usual high levels of organic and elemental carbon, minerals, sulfate, nitrate, and ammonium. Wintertime provides prolonged high pressure systems in both areas punctuated by unstable precipitation events. Sluggish nighttime winds allow pollutants such as ammonia from distant agricultural operations, to mix with urban pollutants, sometimes serving as a reactor to create secondary sulfates and nitrates, and possibly some secondary organic compounds. A shallow surface layer forms at night in the SJV and GZB that couples to an upper level inversion after sunrise, allowing pollutants accumulated aloft to mix to the surface. Although current air quality management strategies have focused on urban emissions, and PM2.5 levels are on a downward trend, future management efforts must consider reducing emissions from a variety of sources in the larger region of these basins. Agricultural emissions are important in the SJV, but are just being addressed in the GZB. Tactics developed for the SJV would probably be effective in other areas of the world with similar emissions, topography, and meteorology. Experiments related to agricultural NOx emissions, emission inventory enhancements, source apportionment, and estimates of precursor limitations for ammonium nitrate formation, have been conducted in the SJV that can be tested in the GZB.
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Poluentes Atmosféricos , Poluição do Ar , Poluentes Atmosféricos/análise , Poluição do Ar/análise , Monitoramento Ambiental , Material Particulado/análise , Estações do AnoRESUMO
Light-absorptivity of organic aerosol may play an important role in visibility and climate forcing, but it has not been assessed as extensively as black carbon (BC) aerosol. Based on multiwavelength thermal/optical analysis and spectral mass balance, this study quantifies BC for the U.S. Interagency Monitoring of Protected Visual Environments (IMPROVE) network while developing a brownness index (γBr) for non-BC organic carbon (OC*) to illustrate the spatiotemporal trends of light-absorbing brown carbon (BrC) content. OC* light absorption efficiencies range from 0 to 3.1 m2 gC-1 at 405 nm, corresponding to the lowest and highest BrC content of 0 and 100%, respectively. BC, OC*, and γBr explain >97% of the variability of measured spectral light absorption (405-980 nm) across 158 IMPROVE sites. Network-average OC* light absorptions at 405 nm are 50 and 28% those for BC over rural and urban areas, respectively. Larger organic fractions of light absorption occur in winter, partially due to higher organic brownness. Winter γBr exhibits a dramatic regional/urban-rural contrast consistent with anthropogenic BrC emissions from residential wood combustion. The spatial differences diminish to uniformly low γBr in summer, suggesting effective BrC photobleaching over the midlatitudes. An empirical relationship between BC, ambient temperature, and γBr is established, which can facilitate the incorporation of organic aerosol absorptivity into climate and visibility models that currently assume either zero or static organic light absorption efficiencies.
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Poluentes Atmosféricos , Aerossóis/análise , Poluentes Atmosféricos/análise , Biomassa , Carbono/análise , Monitoramento Ambiental , Material Particulado/análise , Fotodegradação , Estações do Ano , Estados UnidosRESUMO
In this study, 30 elements in fine particulate matter (PM2.5) were measured in 18 Chinese cities in 2013. Elemental pollution in northern, southwest, and central China were severe, attributing to excessive coal and biomass combustion in these regions. The concentrations of S, Cl, and K in these areas were 8.21 ± 3.90, 4.03 ± 1.96, and 1.59 ± 0.613 µg/m3, respectively, which were 1.6-2.7 times higher than those in other regions of China. In addition, the industrial emissions in northeast and north China were large, leading to the elevated heavy metal concentration of 1.32 ± 1.17 µg/m3, especially Zn, Pb, Cr, Cd, and Br. Soil dust was the highest in northwest China among the five regions with the concentration of crustal elements of 6.37 ± 4.51 µg/m3. Moreover, although the levels of elemental concentration in east and southeast China were relatively acceptable, regulators must pay attention to elevated level of V (0.009 ± 0.006 µg/m3) in these areas. Compared with 2003, several elements have deteriorated in some cities. For example, As increased by 70%, 18%, and 155% in Changchun, Beijing, and Jinchang, respectively. However, ~ 77% measured elements, e.g., Ti, Fe, and Pb markedly reduced in 2013, with reduction rates of 13-81%. These indicate that the government's policies related to particle-bound elements have shown certain positive environmental effects. For the health risks from the heavy metals in 2013, the non-cancer risks of As and Cd must not be neglected. The cancer risks of As and Pb were much higher than the international safety limit (10-4). More prominent health risks were found in southwest, central, and northwest China. Therefore, the government should accelerate the shift to cleaner energy in underdeveloped areas of China to obtain more environmental and health benefits.
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Poluentes Atmosféricos , Metais Pesados , Poluentes Atmosféricos/análise , China , Cidades , Poeira/análise , Monitoramento Ambiental , Metais Pesados/análise , Metais Pesados/toxicidade , Material Particulado/análise , Políticas , Medição de RiscoRESUMO
Intermediate volatility and semivolatile organic compounds (IVOC/SVOC) are important precursors of secondary organic aerosol (SOA) while SVOC is an important contributor to primary organic aerosol (POA). However, combustion emissions data for volatility classes are limited. This study reports the gas and particle emissions that were sampled with various dilution factors from a sewage sludge incinerator burning fuel oil. Volatility distributions were determined using measurements from online mass spectrometry and offline organic compound analyses. In the low volatility organic compound (LVOC) to IVOC range, volatility bins with organic saturation concentrations of 10-100 µg m-3 were most abundant, which was due to organic acids generated from sludge burning. Organic aerosol (OA) emission factors (EFOA) increased 1.4 times after cooling to ambient temperatures in comparison to those of the samples from the hot stack. Upon further isothermal dilution at 25 °C, the EFOA decreased while organic gas phase EFs increased with increasing dilution. Phase partitioning in volatility bins with saturation concentrations of 10-100 µg m-3 was sensitive to isothermal dilution that influenced the EFs. Therefore, gas- and particle-phase measurements alone cannot constrain EFs for these volatility classes. Low dilution factors may overestimate the particle phase and underestimate the gas phase EFs compared with real-world emission conditions.
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Poluentes Atmosféricos , Emissões de Veículos , Aerossóis/análise , Poluentes Atmosféricos/análise , Incineração , Esgotos , Emissões de Veículos/análise , VolatilizaçãoRESUMO
A newly developed dataset from the Interagency Monitoring of PROtected Visual Environments (IMPROVE) observation network, combined with a 3-D chemical transport model, is used to evaluate the spatial and temporal variability of brown carbon (BrC) in the United States. The model with BrC emitted from biomass burning and biofuel emissions agrees with the seasonal and spatial variability of BrC planetary boundary layer (PBL) absorption aerosol optical depth (AAOD) observations within a factor of 2. The model without whitening, the tendency for absorption to decrease with aerosol aging, overestimates the observed BrC PBL AAOD, and does not reflect the measured BrC PBL AAOD spatial variability. The model shows higher absorption direct radiative effects (DRE) from BrC at northern high latitudes than at mid-latitudes in spring and summer, due to boreal fire emissions, long whitening lifetimes and high surface albedos. These findings highlight the need to study BrC over the Arctic region.
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INTRODUCTION: Motor vehicle exhaust is an important source of air pollutants and greenhouse gases. Concerns over the health and climate effects of mobile-source emissions have prompted worldwide efforts to reduce vehicle emissions. Implementation of more stringent emission standards have driven advances in vehicle, engine, and exhaust after-treatment technologies as well as fuel formulations. On the other hand, vehicle numbers and travel distances have been increasing because of population and economic growth and changes in land use. These factors have resulted in changes to the amount and chemical composition of vehicle emissions.Roadway tunnel studies are a practical way to characterize real-world emissions from the on-road vehicle fleet in an environment isolated from other combustion pollution sources. Measurements in the same tunnel over time allow evaluation of vehicle emission changes and the effectiveness of emission reduction measures. Tunnel studies estimate the impacts of vehicle emissions on air quality and traffic-related exposures, generate source profile inputs for receptor-oriented source apportionment models, provide data to evaluate emission models, and serve as a baseline for future comparisons.The present study characterized motor vehicle emission factors and compositions in two roadway tunnels that were first studied over a decade ago. The specific aims were to (1) quantify current fleet air pollutant emission factors, (2) evaluate emission change over time, (3) establish source profiles for volatile organic compounds (VOCs) and particulate matter ≤2.5 µm in aerodynamic diameter (PM2.5), (4) estimate contributions of fleet components and non-tailpipe emissions to VOCs and PM2.5, and (5) evaluate the performance of the latest versions of mobile-source emission models (i.e., the EMission FACtors vehicle emission model used in Hong Kong [EMFAC-HK] and the MOtor Vehicle Emission Simulator used in the United States [MOVES]). METHODS: Measurements were conducted in the Shing Mun Tunnel (SMT) in Hong Kong and the Fort McHenry Tunnel (FMT) in Baltimore, Maryland, in the United States, representing the different fleet compositions, emission controls, fuels, and near-road exposure levels found in Hong Kong and the United States. These tunnels have extensive databases acquired in 2003-2004 for the SMT and 1992 for the FMT. The SMT sampling was conducted during the period from 1/19/2015 to 3/31/2015, and the FMT sampling occurred during the periods from 2/8/2015 to 2/15/2015 (winter) and 7/31/2015 to 8/7/2015 (summer). Concentrations of criteria pollutants (e.g., carbon monoxide [CO], nitrogen oxides [NOx], and particulate matter [PM]) were measured in real time, and integrated samples of VOCs, carbonyls, polycyclic aromatic hydrocarbons (PAHs), and PM2.5 were collected in canisters and sampling media for off-line analyses. Emission factors were calculated from the tunnel measurements and compared with previous studies to evaluate emission changes over time. Emission contributions by different vehicle types were assessed by source apportionment modeling or linear regression. Vehicle emissions were modeled by EMFAC-HK version 3.3 and MOVES version 2014a for the SMT and the FMT, respectively, and compared with measured values. The influences of vehicle fleet composition and environmental parameters (i.e., temperature and relative humidity) on emissions were evaluated. RESULTS: In the SMT, emissions of PM2.5, sulfur dioxide (SO2), and total non-methane hydrocarbons (NMHCs) markedly decreased from 2003-2004 to 2015: SO2 and PM2.5 were reduced by ~80%, and total NMHCs was reduced by ~44%. Emission factors of ethene and propene, key tracers for diesel vehicle (DV) emissions, decreased by ~65%. These reductions demonstrate the effectiveness of control measures, such as the implementation of low-sulfur fuel regulations and the phasing out of older DVs. However, the emission factors of isobutane and n-butane, markers for liquefied petroleum gas (LPG), increased by 32% and 17% between 2003-2004 and 2015, respectively, because the number of LPG vehicles increased. Nitrogen dioxide (NO2) to NOx volume ratios increased between 2003-2004 and 2015, indicating an increased NO2 fraction in primary exhaust emissions. Although geological mineral concentrations were similar between the 2003-2004 and 2015 studies, the contribution of geological materials to PM2.5 increased from 2% in 2003-2004 to 5% in 2015, signifying the continuing importance of non-tailpipe PM emissions as tailpipe emissions decrease. Emissions of CO, ammonia (NH3), nitric oxide (NO), NO2, and NOx, as well as carbonyls and PAHs in the SMT did not show statistically significant (at P < 0.05 based on Student's t-test) decreases from 2003-2004 to 2015. The reason for this is not clear and requires further investigation.A steady decrease in emissions of all measured pollutants during the past 23 years has been observed from tunnel studies in the United States, reflecting the effect of emission standards and new technologies that were introduced during this period. Emission reductions were more pronounced for the light-duty (LD) fleet than for the heavy-duty (HD) fleet. In comparison with the 1992 FMT study, the 2015 FMT study demonstrated marked reductions in LD emissions for all pollutants: emission factors for naphthalene were reduced the most, by 98%; benzene, toluene, ethylbenzene, and xylene (BTEX), by 94%; CO, NMHCs, and NOx, by 87%; and aldehydes by about 71%. Smaller reductions were observed for HD emission factors: naphthalene emissions were reduced by 95%, carbonyl emissions decreased by about 75%, BTEX by 60%, and NOx 58%.The 2015 fleet-average emission factors were higher in the SMT for CO, NOx, and summer PM2.5 than those in the FMT. The higher CO emissions in the SMT were possibly attributable to a larger fraction of motorcycles and LPG vehicles in the Hong Kong fleet. DVs in Hong Kong and the United States had similar emission factors for NOx. However, the non-diesel vehicles (NDVs), particularly LPG vehicles, had higher emission factors than those of gasoline cars, contributing to higher NOx emissions in the SMT. The higher PM2.5 emission factors in the SMT were probably attributable to there being more double-deck buses in Hong Kong.In both tunnels, PAHs were predominantly in the gas phase, with larger (four and more aromatic rings) PAHs mostly in the particulate phase. Formaldehyde, acetaldehyde, crotonaldehyde, and acetone were the most abundant carbonyl compounds in the SMT. In the FMT, the most abundant carbonyls were formaldehyde, acetone, acetaldehyde, and propionaldehyde. HD vehicles emitted about threefold more carbonyl compounds than LD vehicles did. In the SMT, the NMHC species were enriched with marker species for LPG (e.g., n-butane, isobutane, and propane) and gasoline fuel vapor (e.g., toluene, isopentane, and m/p-xylene), indicating evaporative losses. Source contributions to SMT PM2.5 mass were diesel exhaust (51.5 ± 1.8%), gasoline exhaust (10.0 ± 0.8%), LPG exhaust (5.0 ± 0.5%), secondary sulfate (19.9 ± 1.0%), secondary nitrate (6.3 ± 0.9%), and road dust (7.3 ± 1.3%). In the FMT, total NMHC emissions were 14% and 8% higher in winter than in summer for LD and HD vehicles, respectively. Elemental carbon (EC) and organic carbon (OC) were the major constituents of tunnel PM2.5. De-icing salt contributions to PM2.5 were observed in the FMT in winter.Emission estimates by the EMFAC-HK agreed with SMT measurements for CO2; the modeled emission factors for CO, NOx, and NMHCs were 1.5, 1.6, and 2.2 times the measurements, respectively; and the modeled emission factor for PM2.5 was 61% of the measured value in 2003. The EMFAC-HK estimates and SMT measurements for 2015 differed by less than 35%. The MOVES2014a model generally overestimated emissions of most of the pollutants measured in the FMT. No pollutants were significantly underestimated. The largest overestimation was observed for emissions measured during HD-rich driving conditions in winter. CONCLUSIONS: Significant reductions in SO2 and PM2.5 emissions between 2003 and 2015 were observed in the SMT, indicating the effectiveness of control measures on these two pollutants. The total NMHC emissions in the SMT were reduced by 44%, although isobutane and n-butane emissions increased because of the increase in the size of the LPG fleet. No significant reductions were observed for CO and NOx, results that differed from those for roadside ambient concentrations, emission inventory estimates, and EMFAC-HK estimates. In contrast, there was a steady decrease in emissions of most pollutants in the tunnels in the United States.
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Poluentes Atmosféricos/análise , Material Particulado/análise , Emissões de Veículos/análise , Compostos Orgânicos Voláteis/análise , Poluição do Ar/análise , Baltimore , Hong Kong , HumanosAssuntos
Poluentes Atmosféricos/normas , Poluição do Ar/legislação & jurisprudência , Material Particulado/normas , United States Environmental Protection Agency , Comitês Consultivos , Poluentes Atmosféricos/efeitos adversos , Saúde Ambiental , Regulamentação Governamental , Humanos , Material Particulado/efeitos adversos , Política Pública , Estados UnidosRESUMO
This study describes spatiotemporal patterns from October 2015 to September 2016 for PM2.5 mass and carbon measurements in rural (Kosmarra), urban (Raipur), and industrial (Bhilai) environments, in Chhattisgarh, Central India. Twenty-four-hour samples were acquired once every other week at the rural and industrial sites. Twelve-hour daytime and nighttime samples were acquired either a once a week or once every other week at the urban site. Each site was equipped with two portable, battery-powered, miniVol air samplers with PM2.5 inlets. Annual average PM2.5 mass concentrations were 71.8 ± 27 µg m-3 at the rural site, 133 ± 51 µg m-3 at the urban site, and 244.5 ± 63.3 µg m-3 at the industrial site, ~ 2-6 times higher than the Indian Annual National Ambient Air Quality Standard of 40 µg m-3. Average monthly nighttime PM2.5 and carbon concentrations at the urban site were consistently higher than those of daytime from November 2015 to April 2016, when temperatures were low. Annual average total carbon (TC = OC + EC) at the urban (46.8 ± 23.8 µg m-3) and industrial (98.0 ± 17.2 µg m-3) sites also exceeded the Indian PM2.5 NAAQS. TC accounted for 30-40% of PM2.5 mass. Annual average OC ranged from 17.8 ± 6.1 µg m-3 at the rural site to 64 ± 9.4 µg m-3 at the industrial site, with EC ranging from 4.51 ± 2.2 to 34.01 ± 7.8 µg m-3. The average OC/EC ratio at the industrial site (1.88) was 18% lower than that at the urban site and 52% lower than that at the rural site. OC was attributed to 43.0% of secondary organic carbon (SOC) at the rural site, twice that estimated for the urban and industrial sites. Mortality burden estimates for PM2.5 EC are 4416 and 6196 excess deaths at the urban and industrial sites, respectively, during 2015-2016.
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Poluentes Atmosféricos/análise , Carbono/análise , Monitoramento Ambiental/métodos , Material Particulado/análise , Baías , Índia , Tamanho da Partícula , Estações do Ano , TemperaturaRESUMO
UNLABELLED: Collocated comparisons for three PM(2.5) monitors were conducted from June 2011 to May 2013 at an air monitoring station in the residential area of Fort McMurray, Alberta, Canada, a city located in the Athabasca Oil Sands Region. Extremely cold winters (down to approximately -40°C) coupled with low PM(2.5) concentrations present a challenge for continuous measurements. Both the tapered element oscillating microbalance (TEOM), operated at 40°C (i.e., TEOM(40)), and Synchronized Hybrid Ambient Real-time Particulate (SHARP, a Federal Equivalent Method [FEM]), were compared with a Partisol PM(2.5) U.S. Federal Reference Method (FRM) sampler. While hourly TEOM(40) PM(2.5) were consistently ~20-50% lower than that of SHARP, no statistically significant differences were found between the 24-hr averages for FRM and SHARP. Orthogonal regression (OR) equations derived from FRM and TEOM(40) were used to adjust the TEOM(40) (i.e., TEOM(adj)) and improve its agreement with FRM, particularly for the cold season. The 12-year-long hourly TEOM(adj) measurements from 1999 to 2011 based on the OR equations between SHARP and TEOM(40) were derived from the 2-year (2011-2013) collocated measurements. The trend analysis combining both TEOM(adj) and SHARP measurements showed a statistically significant decrease in PM(2.5) concentrations with a seasonal slope of -0.15 µg m(-3) yr(-1) from 1999 to 2014. IMPLICATIONS: Consistency in PM(2.5) measurements are needed for trend analysis. Collocated comparison among the three PM(2.5) monitors demonstrated the difference between FRM and TEOM, as well as between SHARP and TEOM. The orthogonal regressions equations can be applied to correct historical TEOM data to examine long-term trends within the network.
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Poluentes Atmosféricos/química , Monitoramento Ambiental/métodos , Filtração/instrumentação , Material Particulado/química , Alberta , Filtração/métodosRESUMO
Inhalation exposure to indoor air pollutants and cigarette smoke increases the risk of developing tuberculosis (TB). Whether exposure to ambient air pollution particulate matter (PM) alters protective human host immune responses against Mycobacterium tuberculosis has been little studied. Here, we examined the effect of PM from Iztapalapa, a municipality of Mexico City, with aerodynamic diameters below 2.5 µm (PM2.5) and 10 µm (PM10) on innate antimycobacterial immune responses in human alveolar type II epithelial cells of the A549 cell line. Exposure to PM2.5 or PM10 deregulated the ability of the A549 cells to express the antimicrobial peptides human ß-defensin 2 (HBD-2) and HBD-3 upon infection with M. tuberculosis and increased intracellular M. tuberculosis growth (as measured by CFU count). The observed modulation of antibacterial responsiveness by PM exposure was associated with the induction of senescence in PM-exposed A549 cells and was unrelated to PM-mediated loss of cell viability. Thus, the induction of senescence and downregulation of HBD-2 and HBD-3 expression in respiratory PM-exposed epithelial cells leading to enhanced M. tuberculosis growth represent mechanisms by which exposure to air pollution PM may increase the risk of M. tuberculosis infection and the development of TB.
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Poluentes Atmosféricos/toxicidade , Poluição do Ar/análise , Mycobacterium tuberculosis/fisiologia , Material Particulado/toxicidade , Mucosa Respiratória/efeitos dos fármacos , Mucosa Respiratória/imunologia , Poluentes Atmosféricos/química , Linhagem Celular Tumoral , DNA Complementar/genética , Regulação da Expressão Gênica/efeitos dos fármacos , Regulação da Expressão Gênica/imunologia , Humanos , Imunidade Inata , México , Material Particulado/química , RNA Mensageiro/genética , RNA Mensageiro/metabolismo , beta-Defensinas/genética , beta-Defensinas/metabolismoRESUMO
Aerosol mass scattering efficiency (MSE), used for the scattering coefficient apportionment of aerosol species, is often studied under the condition of low aerosol mass loading in developed countries. Severe pollution episodes with high particle concentration frequently happened in eastern urban China in recent years. Based on synchronous measurement of aerosol physical, chemical, and optical properties at the megacity of Shanghai for two months during autumn 2012, we studied MSE characteristics at high aerosol mass loading. Their relationships with mass concentrations and size distributions were examined. It was found that MSE values from the original US IMPROVE algorithm could not represent the actual aerosol characteristics in eastern China. It results in an underestimation of the measured ambient scattering coefficient by 36%. MSE values in Shanghai were estimated to be 3.5 ± 0.55 m(2)/g for ammonia sulfate, 4.3 ± 0.63 m(2)/g for ammonia nitrate, and 4.5 ± 0.73 m(2)/g for organic matter, respectively. MSEs for three components increased rapidly with increasing mass concentration in low aerosol mass loading, then kept at a stable level after a threshold mass concentration of 1224 µg/m(3). During severe pollution episodes, particle growth from an initial peak diameter of 200300 nm to a peak diameter of 500600 nm accounts for the rapid increase in MSEs at high aerosol mass loading, that is, particle diameter becomes closer to the wavelength of visible lights. This study provides insights of aerosol scattering properties at high aerosol concentrations and implies the necessity of MSE localization for extinction apportionment, especially for the polluted regions.
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Aerossóis/análise , Poluentes Atmosféricos/análise , Monitoramento Ambiental/métodos , Algoritmos , China , Cidades , Nitratos/análise , Tamanho da Partícula , Análise de Regressão , Estações do AnoRESUMO
UNLABELLED: Geological samples were collected from 27 representative locations in the Athabasca Oil Sands Region (AOSR) in Alberta, Canada. These samples were resuspended onto filter substrates for PM2.5 and PM10 size fractions. Samples were analyzed for 229 chemical species, consisting of elements, ions, carbon, and organic compounds. These chemical species are normalized to gravimetric mass to derive individual source profiles. Individual profiles were grouped into six categories typical of those used in emission inventories: paved road dust, unpaved road dust close to and distant from oil sand operations, overburden soil, tailings sands, and forest soils. Consistent with their geological origin, the major components are minerals, organic and elemental carbon, and ions. The sum of five major elements (i.e., Al, Si, K, Ca, and Fe) and their oxidized forms account for 25-40% and 45-82% of particulate matter (PM) mass, respectively. Si is the most abundant element, averaging 17-18% in the Facility (oil sand operations) and 23-27% in the Forest profiles. Organic carbon is the second most abundant species, averaging 9-11% in the Facility and 5-6% in the Forest profiles. Elemental carbon abundance is 2-3 times higher in Facility than Forest profiles. Sulfate abundance is ~7 times higher in the Facility than in the Forest profiles. The ratios of cation/anion and base cation (sum of Na+, Mg2+, K+, and Ca2+)/nitrogen- and sulfur-containing ions (sum of NH4+, NO2-, NO3-, and SO4(2-)) exceed unity, indicating that the soils are basic. Lead (Pb) isotope ratios of facility soils are similar to the AOSR stack and diesel emissions, while those of forest soils have much lower 206Pb/207Pb and 208Pb/207Pb ratios. High-molecular-weight n-alkanes (C25-C40), hopanes, and steranes are more than an order of magnitude more abundant in Facility than Forest profiles. These differences may be useful for separating anthropogenic from natural sources of fugitive dust at receptors. IMPLICATIONS: Several organic compounds typical of combustion emissions and bitumen are enriched relative to forest soils for fugitive dust sources near oil sands operations, consistent with deposition uptake by biomonitors. AOSR dust samples are alkaline, not acidic, indicating that potential acid deposition is neutralized. Chemical abundances are highly variable within emission inventory categories, implying that more specific subcategories can be defined for inventory speciation.
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Poluentes Atmosféricos/química , Poeira/análise , Tamanho da Partícula , Material Particulado/química , Canadá , Carbono/química , Monitoramento Ambiental , Chumbo/química , Metais Terras Raras/química , Compostos Orgânicos/química , PetróleoRESUMO
UNLABELLED: Positive matrix factorization (PMF) and effective variance (EV) solutions to the chemical mass balance (CMB) were applied to PM(2.5) (particulate matter with an aerodynamic diameter <2.5 µm) mass and chemically speciated measurements for samples taken from 2008 to 2010 at the Atlanta, Georgia, and Birmingham, Alabama, sites. Commonly measured PM(2.5) mass, elemental, ionic, and thermal carbon fraction concentrations were supplemented with detailed nonpolar organic speciation by thermal desorption-gas chromatography/mass spectrometry (TD-GC/MS). Source contribution estimates were calculated for motor vehicle exhaust, biomass burning, cooking, coal-fired power plants, road dust, vegetative detritus, and secondary sulfates and nitrates for Atlanta. Similar sources were found for Birmingham, with the addition of an industrial source and the separation of biomass burning into open burning and residential wood combustion. EV-CMB results based on conventional species were qualitatively similar to those estimated by PMF-CMB. Secondary ammonium sulfate was the largest contributor, accounting for 27-38% of PM(2.5), followed by biomass burning (21-24%) and motor vehicle exhaust (9-24%) at both sites, with 4-6% of PM(2.5) attributed to coal-fired power plants by EV-CMB. Including organic compounds in the EV-CMB reduced the motor vehicle exhaust and biomass burning contributions at both sites, with a 13-23% deficit for PM(2.5) mass. The PMF-CMB solution showed mixing of sources within the derived factors, both with and without the addition of speciated organics, as is often the case with complex source mixtures such as those at these urban-scale sites. The nonpolar TD-GC/MS compounds can be obtained from existing filter samples and are a useful complement to the elements, ions, and carbon fractions. However, they should be supplemented with other methods, such as TD-GC/MS on derivitized samples, to obtain a wider range of polar compounds such as sterols, sugars, and organic acids. The PMF and EV solutions to the CMB equations are complementary to, rather than replacements for, each other, as comparisons of their results reveal uncertainties that are not otherwise evident. IMPLICATIONS: Organic markers can be measured on currently acquired PM(2.5) filter samples by thermal methods. These markers can complement element, ion, and carbon fraction measurements from long-term speciation networks. Applying the positive matrix factorization and effective variance solutions for the chemical mass balance equations provides useful information on the accuracy of the source contribution estimates. Nonpolar compounds need to be complemented with polar compounds to better apportion cooking and secondary organic aerosol contributors.
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Poluentes Atmosféricos/análise , Monitoramento Ambiental , Material Particulado/análise , Alabama , Cidades , Cromatografia Gasosa-Espectrometria de Massas , Georgia , Tamanho da PartículaRESUMO
PM2.5 (particulate matter with an aerodynamic diameter <2.5 microm) samples (n = 58) collected every sixth day in Xi'an, China, from 5 July 2008 to 27 June 2009 are analyzed for levoglucosan (1,6-anhydro-beta-D-glucopyranose) to evaluate the impacts of biomass combustion on ambient concentrations. Twenty-four-hour levoglucosan concentrations displayed clear summer minima and winter maxima that ranged from 46 to 1889 ng m(-3), with an average of 428 +/- 399 ng m(-3). Besides agricultural burning, biomass/biofuel combustion for household heating with straws and branches appears to be of regional importance during the heating season in northwestern China. Good correlations (0.70 < R < 0.91) were found between levoglucosan relative to water- soluble K+, Cl-, organic carbon (OC), elemental carbon (EC), and glyoxal. The highest levoglucosan/OC ratio of2.3% wasfound in winter, followed by autumn (1.5%). Biomass burning contributed to 5.1-43.8% of OC (with an average of 17.6 +/- 8.4%).
Assuntos
Poluentes Atmosféricos/química , Monitoramento Ambiental/métodos , Glucose/análogos & derivados , Material Particulado/química , China , Incêndios , Glucose/química , Tamanho da Partícula , Estações do AnoRESUMO
Particulate Matter (PM) concentrations near highways are influenced by vehicle tailpipe and non-tailpipe emissions, other emission sources, and urban background aerosols. This study collected PM2.5 and PM10 filter samples near two southern California highways (I-5 and I-710) over two weeks in winter 2020. Samples were analyzed for chemical source markers. Mean PM2.5 and PM10 concentrations were approximately 10-15 and 30 µg/m3, respectively. Organic matter, mineral dust, and elemental carbon (EC) were the most abundant PM components. EC and polycyclic aromatic hydrocarbons at I-710 were 19-26% and 47% higher than those at the I-5 sites, respectively, likely due to a larger proportion of diesel vehicles. High correlations were found for elements with common sources, such as markers for brake wear (e.g., Fe, Ba, Cu, and Zr) and road dust (e.g., Al, Si, Ca, and Mn). Based on rubber abundances, the contributions of tire tread particles to PM2.5 and PM10 mass were approximately 8.0% at I-5 and 5.5% at I-710. Two different tire brands showed significantly different Si, Zn, carbon, and natural rubber abundances.
Assuntos
Poluentes Atmosféricos , Material Particulado , Material Particulado/análise , Poluentes Atmosféricos/análise , Emissões de Veículos/análise , Monitoramento Ambiental , Poeira/análise , California , Tamanho da PartículaRESUMO
As the importance of non-tailpipe particles (NTP) over tailpipe emissions from urban traffic has been increasing, there is a need to evaluate NTP contributions to ambient particulate matter (PM) using representative source profiles. The Brake and Tire Wear Study conducted in Los Angeles, California in the winter of 2020 collected 64 PM2.5 and 64 PM10 samples from 32 pairs of downwind-upwind measurements at two near-road locations (I-5 in Anaheim and I-710 in Long Beach). These samples were characterized for inorganic and organic markers and, along with locally-developed brake wear, tire wear, and road dust source profiles, subject to source apportionment using the effective-variance chemical mass balance (EV-CMB) model. Model results highlighted the dominance of resuspended dust in both PM2.5 (23-33%) and PM10 (32-53%). Brake and tire wear contributed more to PM2.5 than tailpipe exhausts (diesel + gasoline) for I-5 (29-30% vs. 19-21%) while they were comparable for I-710 (15-17% vs. 15-19%). For PM10, the brake and tire wear contributions were 2-3 times the exhaust contributions. Different fleet compositions on and near I-5 and I-710 appeared to influence the relative importance of NTP and exhaust sources. The downwind-upwind differences in source contributions were often insignificant, consistent with small and/or nearly equal impacts of adjacent highway traffic emissions on the downwind and upwind sites. The utility of sole markers, such as barium and zinc, to predict brake and tire wear abundances in ambient PM is evaluated.
Assuntos
Poluentes Atmosféricos , Poluentes Atmosféricos/análise , Monitoramento Ambiental , Material Particulado/análise , Emissões de Veículos/análise , PoeiraRESUMO
Exposure atmospheres for rodent inhalation toxicology studies were generated to enable the evaluation of biological responses to a simulated downwind coal combustion atmosphere. A composition representing a single test case of emissions components as they may exist tens to hundreds of miles from a coal-fired power plant was developed. The particulate matter (PM) was 99% sulfate (partially neutralized) and 1% ash. Sulfate was present in equimolar concentrations to sulfur dioxide (SO2). Gaseous nitrogen species included nitrogen monoxide (NO), nitrogen dioxide (NO2), and nitric acid (HNO3). At the high-exposure level, the gaseous species target concentrations were 0.2 ppm SO2, 0.6 ppm NO, 0.3 ppm NO2, and 0.1 ppm HNO3. The test atmosphere was produced by combining effluent from a laboratory coal combustor with sulfate generated through an evaporation-condensation generator. These atmospheres were used to conduct inhalation toxicology studies that have been previously reported.
Assuntos
Poluentes Atmosféricos , Carvão Mineral , Material Particulado , Centrais Elétricas , Testes de Toxicidade/métodos , Administração por Inalação , Poluentes Atmosféricos/análise , Amônia/análise , Metais/análise , Óxidos de Nitrogênio/análise , Material Particulado/análise , Sulfatos/análise , Dióxido de Enxofre/análise , Compostos Orgânicos Voláteis/análiseRESUMO
The 2012 Critical Review Discussion complements Wilson, (2012), provides pointers to more detailed treatments of different topics and adds additional dimensions to the area of "energy". These include broader aspects of technologies driven by fuel resources and environmental issues, the concept of energy technology innovation, evolution in transportation resources, and complexities of energy policies addressing carbon taxes or carbon trading. National and global energy data bases are identified and evaluated and conversion factors are given to allow their comparability.