RESUMO
Shipping is the main source of anthropogenic particle emissions in large areas of the globe, influencing climate, air quality, and human health in open seas and coast lines. Here, we determined, by laboratory and on-board measurements of ship engine exhaust, fuel-specific particle number (PN) emissions for different fuels and desulfurization applied in shipping. The emission factors were compared to ship exhaust plume observations and, furthermore, exploited in the assessment of global PN emissions from shipping, utilizing the STEAM ship emission model. The results indicate that most particles in the fresh ship engine exhaust are in ultrafine particle size range. Shipping PN emissions are localized, especially close to coastal lines, but significant emissions also exist on open seas and oceans. The global annual PN produced by marine shipping was 1.2 × 1028 (±0.34 × 1028) particles in 2016, thus being of the same magnitude with total anthropogenic PN emissions in continental areas. The reduction potential of PN from shipping strongly depends on the adopted technology mix, and except wide adoption of natural gas or scrubbers, no significant decrease in global PN is expected if heavy fuel oil is mainly replaced by low sulfur residual fuels. The results imply that shipping remains as a significant source of anthropogenic PN emissions that should be considered in future climate and health impact models.
Assuntos
Poluentes Atmosféricos , Navios , Poluentes Atmosféricos/análise , Humanos , Oceanos e Mares , Material Particulado/análise , Enxofre/análise , Emissões de Veículos/análiseRESUMO
Coal combustion is one of the most significant anthropogenic CO2 and air pollution sources globally. This paper studies the atmospheric emissions of a power plant fuelled with a mixture of industrial pellets (10.5%) and coal (89.5%). Based on the stack measurements, the solid particle number emission, which was dominated by sub-200 nm particles, was 3.4×1011 MJ-1 for the fuel mixture when electrostatic precipitator (ESP) was cleaning the flue gas. The emission factor was 50 mg MJ-1 for particulate mass and 11 740 ng MJ-1 for the black carbon with the ESP. In the normal operation situation of the power plant, i.e., including the flue-gas desulphurisation and fabric filters (FGD and FF), the particle number emission factor was 1.7×108 MJ-1, particulate mass emission factor 2 mg MJ-1 and black carbon emission factor 14 ng MJ-1. Transmission electron microscopy (TEM) analysis supported the particle number size distribution measurement in terms of particle size and the black carbon concentration. The TEM images of the particles showed variability of the particle sizes, morphologies and chemical compositions. The atmospheric measurements, conducted in the flue-gas plume, showed that the flue-gas dilutes closed to background concentrations in 200 sec. However, an increase in particle number concentration was observed when the flue gas aged. This increase in particle number concentration was interpret as formation of new particles in the atmosphere. In general, the study highlights the importance of detailed particle measurements when utilizing new fuels in existing power plants. Implications: CO2 emissions of energy production decrease when substituting coal with biofuels. The effects of fuels changes on particle emission characteristics have not been studied comprehensively. In this study conducted for a real-scale power plant, co-combustion of wood pellets and coal caused elevated black carbon emissions. However, it was beneficial from the total particle number and particulate mass emission point of view. Flue-gas cleaning can significantly decrease the pollutant concentrations but also changes the characteristics of emitted particles. Atmospheric measurements implicated that the new particle formation in the atmospheric flue-gas plume should be taken into account when evaluating all effects of fuel changes." Are implication statements part of the manuscript?
Assuntos
Poluentes Atmosféricos/análise , Poluição do Ar , Monitoramento Ambiental/métodos , Poluição Ambiental , Combustíveis Fósseis/análise , Centrais Elétricas/normas , Poluição do Ar/análise , Poluição do Ar/prevenção & controle , Carvão Mineral/análise , Cinza de Carvão/análise , Saúde Ambiental/métodos , Saúde Ambiental/normas , Poluição Ambiental/análise , Poluição Ambiental/prevenção & controle , Temperatura Alta , Humanos , Tamanho da Partícula , Madeira/análise , Madeira/químicaRESUMO
Inexpensive aerosol sensors have been considered as a complementary option to address the issue of expensive but low spatial coverage air quality monitoring networks. However, the accuracy and response characteristics of these sensors is poorly documented. In this study, inexpensive Shinyei PPD42NS and PPD60PV sensors were evaluated using a novel laboratory evaluation method. A continuously changing monodisperse size distribution of particles was generated using a Vibrating Orifice Aerosol Generator. Furthermore, the laboratory results were validated in a field experiment. The laboratory tests showed that both of the sensors responded to particulate mass (PM) concentration stimulus, rather than number concentration. The highest detection efficiency for the PPD42NS was within particle size range of 2.5-4 µm, and the respective optimal size range for the PPD60PV was 0.7-1 µm. The field test yielded high PM correlations (R² = 0.962 and R² = 0.986) for viable detection ranges of 1.6-5 and 0.3-1.6 µm, when compared to a medium cost optical dust monitor. As the size distribution of atmospheric particles tends to be bimodal, it is likely that indicatively valid results could be obtained for the PM10-2.5 size fraction (particulate mass in size range 2.5-10 µm) with the PPD42NS sensor. Respectively, the PPD60PV could possibly be used to measure the PM2.5 size fraction (particulate mass in size below 2.5 µm).
RESUMO
In densely populated areas, traffic is a significant source of atmospheric aerosol particles. Owing to their small size and complicated chemical and physical characteristics, atmospheric particles resulting from traffic emissions pose a significant risk to human health and also contribute to anthropogenic forcing of climate. Previous research has established that vehicles directly emit primary aerosol particles and also contribute to secondary aerosol particle formation by emitting aerosol precursors. Here, we extend the urban atmospheric aerosol characterization to cover nanocluster aerosol (NCA) particles and show that a major fraction of particles emitted by road transportation are in a previously unmeasured size range of 1.3-3.0 nm. For instance, in a semiurban roadside environment, the NCA represented 20-54% of the total particle concentration in ambient air. The observed NCA concentrations varied significantly depending on the traffic rate and wind direction. The emission factors of NCA for traffic were 2.4·1015 (kgfuel)-1 in a roadside environment, 2.6·1015 (kgfuel)-1 in a street canyon, and 2.9·1015 (kgfuel)-1 in an on-road study throughout Europe. Interestingly, these emissions were not associated with all vehicles. In engine laboratory experiments, the emission factor of exhaust NCA varied from a relatively low value of 1.6·1012 (kgfuel)-1 to a high value of 4.3·1015 (kgfuel)-1 These NCA emissions directly affect particle concentrations and human exposure to nanosized aerosol in urban areas, and potentially may act as nanosized condensation nuclei for the condensation of atmospheric low-volatile organic compounds.
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Exhaust emissions of 23 individual city buses at Euro III, Euro IV and EEV (Enhanced Environmentally Friendly Vehicle) emission levels were measured by the chasing method under real-world conditions at a depot area and on the normal route of bus line 24 in Helsinki. The buses represented different technologies from the viewpoint of engines, exhaust after-treatment systems (ATS) and fuels. Some of the EEV buses were fueled by diesel, diesel-electric, ethanol (RED95) and compressed natural gas (CNG). At the depot area the emission factors were in the range of 0.3-21 × 10(14) # (kg fuel)(-1), 6-40 g (kg fuel)(-1), 0.004-0.88 g (kg fuel)(-1), 0.004-0.56 g (kg fuel)(-1), 0.01-1.2 g (kg fuel)(-1), for particle number (EFN), nitrogen oxides (EFNOx), black carbon (EFBC), organics (EFOrg), and particle mass (EFPM1), respectively. The highest particulate emissions were observed from the Euro III and Euro IV buses and the lowest from the ethanol and CNG-fueled buses, which emitted BC only during acceleration. The organics emitted from the CNG-fueled buses were clearly less oxidized compared to the other bus types. The bus line experiments showed that lowest emissions were obtained from the ethanol-fueled buses whereas large variation existed between individual buses of the same type indicating that the operating conditions by drivers had large effect on the emissions.
Assuntos
Poluentes Atmosféricos/análise , Poluentes Atmosféricos/química , Veículos Automotores , Emissões de Veículos/análise , Cidades , Finlândia , Peso MolecularRESUMO
The chemical and microbial composition of urban air particulate matter (PM) displays seasonal variation that may affect its harmfulness on human health. We studied the in vitro inflammatory and cellular metabolic activity/cytotoxicity of urban air particulate samples collected in four size-ranges (PM10-2.5, PM2.5-1, PM1-0.2, PM0.2) during four seasons in relatively clean urban environment in Helsinki, Finland. The composition of the same samples were analyzed, including ions, elements, PAH compounds and endotoxins. In addition, microbial contribution on the detected responses was studied by inhibiting the endotoxin-induced responses with Polymyxin B both in the PM samples and by two different bacterial strains representing Gram-positive and -negative bacteria. Macrophage cell line (RAW 264.7) was exposed to the size segregated particulate samples as well as to microbe samples for 24h and markers of inflammation and cytotoxicity were analyzed. The toxicological responses were dependent on the dose as well as size range of the particles, PM10-2.5 being the most potent and smaller size ranges having significantly smaller responses. Samples collected during spring and autumn had in most cases the highest inflammatory activity. Soil components and other non-exhaust particulate emissions from road traffic correlated with inflammatory responses in coarse particles. Instead, PAH-compounds and K(+) had negative associations with the particle-induced inflammatory responses in fine particles, suggesting the role of incomplete biomass combustion. Endotoxin content was the highest in PM10-2.5 samples and correspondingly, the largest decrease in the responses by Polymyxin B was seen with the very same samples. We found also that inhibitory effect of Polymyxin B was not completely specific for Gram-negative bacteria. Thus, in addition to endotoxin, also other microbial components may have a significant effect on the toxicological responses by ambient particulate matter.
Assuntos
Poluentes Atmosféricos/química , Poluentes Atmosféricos/toxicidade , Macrófagos/efeitos dos fármacos , Material Particulado/química , Material Particulado/toxicidade , Animais , Linhagem Celular , Sobrevivência Celular/efeitos dos fármacos , Relação Dose-Resposta a Droga , Endotoxinas/toxicidade , Finlândia , Humanos , Técnicas In Vitro , Interleucina-6/metabolismo , Macrófagos/imunologia , Camundongos , Tamanho da Partícula , Polimixina B/farmacologia , Estações do Ano , Fator de Necrose Tumoral alfa/metabolismo , Saúde da População UrbanaRESUMO
Little information is available on the concentrations of ambient fine particles (PM2.5) in residential areas where wood combustion is common for recreational purposes and secondary heating. Further, the validity of central site measurements of PM2.5 as a measure of exposure is unclear. Therefore, outdoor PM2.5 samples were repeatedly collected at a central site and home outdoor locations from a panel of 29 residents in a suburb in Kuopio, Finland. Source apportionment results from the central site were used to estimate the contributions from local sources, including wood combustion, to PM2.5 and absorption coefficient (ABS) at home outdoor locations. Correlations between the central and home outdoor concentrations of PM2.5, ABS, and their local components were analyzed for each home. At the central site, the average PM2.5 was 6.0 µg m(-)(3) during the heating season, and the contribution from wood combustion (16%) was higher than the contribution from exhaust emissions (12%). Central site measurements predicted poorly daily variation in PM2.5 from local sources. In conclusion, wood combustion significantly affects air quality also in areas where it is not the primary heating source. In epidemiological panel studies, central site measurements may not sufficiently capture daily variation in exposure to PM2.5 from local wood combustion.
Assuntos
Poluição do Ar/análise , Calefação , Fumaça/análise , Finlândia , Habitação , Humanos , Tamanho da Partícula , Material Particulado/análise , Recreação , Emissões de Veículos/análise , Madeira/químicaRESUMO
OBJECTIVE: To compare short-term effects of fine particles (PM2.5; aerodynamic diameter <2.5â µm) from different sources on the blood levels of markers of systemic inflammation. METHODS: We followed a panel of 52 ischaemic heart disease patients from 15 November 2005 to 21 April 2006 with clinic visits in every second week in the city of Kotka, Finland, and determined nine inflammatory markers from blood samples. In addition, we monitored outdoor air pollution at a fixed site during the study period and conducted a source apportionment of PM2.5 using the Environmental Protection Agency's model EPA PMF 3.0. We then analysed associations between levels of source-specific PM2.5 and markers of systemic inflammation using linear mixed models. RESULTS: We identified five source categories: regional and long-range transport (LRT), traffic, biomass combustion, sea salt, and pulp industry. We found most evidence for the relation of air pollution and inflammation in LRT, traffic and biomass combustion; the most relevant inflammation markers were C-reactive protein, interleukin-12 and myeloperoxidase. Sea salt was not positively associated with any of the inflammatory markers. CONCLUSIONS: Results suggest that PM2.5 from several sources, such as biomass combustion and traffic, are promoters of systemic inflammation, a risk factor for cardiovascular diseases.
Assuntos
Poluição do Ar/efeitos adversos , Exposição Ambiental/efeitos adversos , Isquemia Miocárdica/epidemiologia , Material Particulado/toxicidade , Poluição do Ar/análise , Biomarcadores/sangue , Doenças Cardiovasculares/etiologia , Causalidade , Citocinas/sangue , Exposição Ambiental/análise , Ensaio de Imunoadsorção Enzimática , Finlândia/epidemiologia , Humanos , Inflamação/sangue , Inflamação/epidemiologia , Luminescência , Isquemia Miocárdica/sangue , Nefelometria e Turbidimetria , Material Particulado/análise , Fatores de RiscoRESUMO
Vehicle engines produce submicrometer exhaust particles affecting air quality, especially in urban environments. In on-road exhaust studies with a heavy duty diesel vehicle and in laboratory studies with two gasoline-fueled passenger cars, we found that as much as 20-30% of the number of exhaust particles larger than 3 nm may be formed during engine braking conditions-that is, during decelerations and downhill driving while the engine is not fueled. Particles appeared at size ranges extending even below 7 nm and at high number concentrations. Their small size and nonvolatility, coupled with the observation that these particles contain lube-oil-derived metals zinc, phosphorus, and calcium, are suggestive of health risks at least similar to those of exhaust particles observed before. The particles' characteristics indicate that their emissions can be reduced using exhaust after-treatment devices, although these devices have not been mandated for all relevant vehicle types. Altogether, our findings enhance the understanding of the formation vehicle emissions and allow for improved protection of human health in proximity to traffic.
Assuntos
Gasolina/análise , Veículos Automotores , Nanopartículas/química , Emissões de Veículos/análise , Condução de Veículo , Nanopartículas/ultraestrutura , Tamanho da Partícula , Espectrometria por Raios XRESUMO
Particle emissions affect radiative forcing in the atmosphere. Therefore, it is essential to know the physical and chemical characteristics of them. This work studied the chemical, physical, and optical characteristics of particle emissions from small-scale wood combustion, coal combustion of a heating and power plant, as well as heavy and light fuel oil combustion at a district heating station. Fine particle (PM1) emissions were the highest in wood combustion with a high fraction of absorbing material. The emissions were lowest from coal combustion mostly because of efficient cleaning techniques used at the power plant. The chemical composition of aerosols from coal and oil combustion included mostly ions and trace elements with a rather low fraction of absorbing material. The single scattering albedo and aerosol forcing efficiency showed that primary particles emitted from wood combustion and some cases of oil combustion would have a clear climate warming effect even over dark earth surfaces. Instead, coal combustion particle emissions had a cooling effect. Secondary processes in the atmosphere will further change the radiative properties of these emissions but are not considered in this study.
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Aerossóis/análise , Aerossóis/química , Carvão Mineral/análise , Óleos Combustíveis/análise , Temperatura Alta , Fenômenos Ópticos , Madeira/química , Poluição do Ar/análise , Tamanho da Partícula , Material Particulado/químicaRESUMO
Heavy fuel oil (HFO) is a commonly used fuel in industrial heating and power generation and for large marine vessels. In this study, the fine particle emissions of a 47 MW oil-fired boiler were studied at 30 MW power and with three different fuels. The studied fuels were HFO, water emulsion of HFO, and water emulsion of HFO mixed with light fuel oil (LFO). With all the fuels, the boiler emitted considerable amounts of particles smaller than 200 nm in diameter. Further, these small particles were quite hygroscopic even as fresh and, in the case of HFO+LFO emulsion, the hygroscopic growth of the particles was dependent on particle size. The use of emulsions and the addition of LFO to the fuel had a reducing effect on the hygroscopic growth of particles. The use of emulsions lowered the sulfate content of the smallest particles but did not affect significantly the sulfate content of particles larger than 42 nm and, further, the addition of LFO considerably increased the black carbon content of particulate matter. The results indicate that even the fine particles emitted from HFO based combustion can have a significant effect on cloud formation, visibility, and air quality.
Assuntos
Poluentes Atmosféricos/análise , Óleos Combustíveis , Calefação , Tamanho da Partícula , Material Particulado/química , Molhabilidade , Material Particulado/análiseRESUMO
BACKGROUND: One of the major areas for increasing the use of renewable energy is in traffic fuels e.g. bio-based fuels in diesel engines especially in commuter traffic. Exhaust emissions from fossil diesel fuelled engines are known to cause adverse effects on human health, but there is very limited information available on how the new renewable fuels may change the harmfulness of the emissions, especially particles (PM). We evaluated the PM emissions from a heavy-duty EURO IV diesel engine powered by three different fuels; the toxicological properties of the emitted PM were investigated. Conventional diesel fuel (EN590) and two biodiesels were used - rapeseed methyl ester (RME, EN14214) and hydrotreated vegetable oil (HVO) either as such or as 30% blends with EN590. EN590 and 100% HVO were also operated with or without an oxidative catalyst (DOC + POC). A bus powered by compressed natural gas (CNG) was included for comparison with the liquid fuels. However, the results from CNG powered bus cannot be directly compared to the other situations in this study. RESULTS: High volume PM samples were collected on PTFE filters from a constant volume dilution tunnel. The PM mass emission with HVO was smaller and with RME larger than that with EN590, but both biofuels produced lower PAH contents in emission PM. The DOC + POC catalyst greatly reduced the PM emission and PAH content in PM with both HVO and EN590. Dose-dependent TNFα and MIP-2 responses to all PM samples were mostly at the low or moderate level after 24-hour exposure in a mouse macrophage cell line RAW 264.7. Emission PM from situations with the smallest mass emissions (HVO + cat and CNG) displayed the strongest potency in MIP-2 production. The catalyst slightly decreased the PM-induced TNFα responses and somewhat increased the MIP-2 responses with HVO fuel. Emission PM with EN590 and with 30% HVO blended in EN590 induced the strongest genotoxic responses, which were significantly greater than those with EN590 + cat or 100% HVO. The emission PM sample from the CNG bus possessed the weakest genotoxic potency but had the strongest oxidative potency of all the fuel and catalyst combinations. The use of 100% HVO fuel had slightly weaker and 100% RME somewhat stronger emission PM induced ROS production, when compared to EN590. CONCLUSIONS: The harmfulness of the exhaust emissions from vehicle engines cannot be determined merely on basis of the emitted PM mass. The study conditions and the engine type significantly affect the toxicity of the emitted particles. The selected fuels and DOC + POC catalyst affected the PM emission from the heavy EURO IV engine both qualitative and quantitative ways, which influenced their toxicological characteristics. The plain HVO fuel performed very well in emission reduction and in lowering the overall toxicity of emitted PM, but the 30% blend of HVO in EN590 was no better in this respect than the plain EN590. The HVO with a DOC + POC catalyst in the EURO IV engine, performed best with regard to changes in exhaust emissions. However some of the toxicological parameters were significantly increased even with these low emissions.
Assuntos
Poluentes Atmosféricos/toxicidade , Biocombustíveis , Macrófagos/efeitos dos fármacos , Gás Natural/toxicidade , Material Particulado/toxicidade , Emissões de Veículos/toxicidade , Poluentes Atmosféricos/química , Animais , Apoptose/efeitos dos fármacos , Ciclo Celular/efeitos dos fármacos , Linhagem Celular , Permeabilidade da Membrana Celular/efeitos dos fármacos , Sobrevivência Celular/efeitos dos fármacos , Citocinas/metabolismo , Ácidos Graxos Monoinsaturados , Hidrogenação , Macrófagos/metabolismo , Camundongos , Material Particulado/química , Óleos de Plantas/toxicidade , Óleo de Brassica napus , Espécies Reativas de Oxigênio/metabolismo , Emissões de Veículos/análiseRESUMO
Short-term exposure to ambient air pollution is associated with increased cardiovascular mortality and morbidity. This adverse health effect is suggested to be mediated by inflammatory processes. The purpose of this study was to determine if low levels of particulate matter, typical for smaller cities, are associated with acute systemic inflammation. Fifty-two elderly individuals with ischemic heart disease were followed for six months with biweekly clinical visits in the city of Kotka, Finland. Blood samples were collected for the determination of inflammatory markers interleukin (IL)-1ß, IL-6, IL-8, IL-12, interferon (IFN)γ, C-reactive protein (CRP), fibrinogen, myeloperoxidase and white blood cell count. Particle number concentration and fine particle (particles with aerodynamic diameters <2.5 µm (PM(2.5))) as well as thoracic particle (particles with aerodynamic diameters <10 µm (PM(10))) mass concentration were measured daily at a fixed outdoor measurement site. Light-absorbance of PM(2.5) filter samples, an indicator of combustion derived particles, was measured with a smoke-stain reflectometer. In addition, personal exposure to PM(2.5) was measured with portable photometers. During the study period, wildfires in Eastern Europe led to a 12-day air pollution episode, which was excluded from the main analyses. Average ambient PM(2.5) concentration was 8.7 µg/m(3). Of the studied pollutants, PM(2.5) and absorbance were most strongly associated with increased levels of inflammatory markers; most notably with C-reactive protein and IL-12 within a few days of exposure. There was also some evidence of an effect of particulate air pollution on fibrinogen and myeloperoxidase. The concentration of IL-12 was considerably (227%) higher during than before the forest fire episode. These findings show that even low levels of particulate air pollution from urban sources are associated with acute systemic inflammation. Also particles from wildfires may exhibit pro-inflammatory effects.
Assuntos
Poluentes Atmosféricos/análise , Exposição por Inalação/efeitos adversos , Exposição por Inalação/análise , Isquemia Miocárdica/etiologia , Isquemia Miocárdica/imunologia , Material Particulado/análise , Idoso , Idoso de 80 Anos ou mais , Biomarcadores/sangue , Proteína C-Reativa/análise , Citocinas/sangue , Monitoramento Ambiental/métodos , Feminino , Fibrinogênio/análise , Finlândia , Humanos , Contagem de Leucócitos , Leucócitos , Masculino , Pessoa de Meia-Idade , Isquemia Miocárdica/sangue , Peroxidase/sangueRESUMO
Several studies have shown that combustion-derived fine particles cause adverse health effects. Previous toxicological studies on combustion-derived fine particles have rarely involved multiple endpoints and a detailed characterization of chemical composition. In this study, we developed a novel particle sampling system for toxicological and chemical characterization (PSTC), consisting of the Dekati Gravimetric Impactor (DGI) and a porous tube diluter. Physico-chemical and toxicological properties of the particles emitted from various combustion sources were evaluated in two measurement campaigns. First, the DGI was compared with the High-Volume Cascade Impactor (HVCI) and to the Dekati Low-Pressure Impactor (DLPI), using the same dilution system and the same sampling conditions. Only small differences were observed in the mass size distributions, total particulate matter (PM), and particulate matter with diameter smaller than 1 um (PM(1)) concentrations and geometric mass mean diameters (GMMD) between these three impactors. Second, the PSTC was compared with the HVCI sampling system, which has been optimal for collection of particulate samples for toxicological and chemical analyses. Differences were observed in the mass size distributions, total PM and PM(1) emissions, and GMMDs, probably due to the different sampling and dilution methods as well as different sampling substrates which affected the behavior of semi-volatile and volatile organic compounds. However, no significant differences were detected in the in vitro measurements of cytotoxicity between the samples collected with the PSTC and the HVCI systems. In measurements of genotoxicity, significant differences between the two sampling systems were seen only with the particles emitted from the sauna stove. In conclusion, due to compact size, PSTC is an applicable method for use in particle sampling as part of the toxicological and chemical characterization of particulate emissions from different combustion sources. It offers some advantages compared to the previously used high-volume sampling methods including compactness for field measurements, simple preparation of sample substrates and high extraction efficiency.
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Poluentes Atmosféricos/química , Métodos Analíticos de Preparação de Amostras/métodos , Material Particulado/química , Emissões de Veículos/análise , Poluentes Atmosféricos/toxicidade , Métodos Analíticos de Preparação de Amostras/instrumentação , Animais , Ciclo Celular/efeitos dos fármacos , Linhagem Celular , Sobrevivência Celular/efeitos dos fármacos , Monitoramento Ambiental , Humanos , Camundongos , Testes de Mutagenicidade , Material Particulado/toxicidadeRESUMO
Biomass burning has a strong influence on the atmospheric aerosol composition through particulate organic, inorganic, and soot emissions. When biomass burns, cellulose and hemicelluloses degrade, producing monosaccharide anhydrides (MAs) such as levoglucosan, mannosan, and galactosan. Therefore, these compounds have been commonly used as tracers for biomass burning. In this study, a fast water-based method was developed for the routine analysis of MAs, based on high-performance anion-exchange chromatography with electrospray ionization mass spectrometry detection. This method combines simple sample preparation, fast separation, and the advantages of the selective detection with MS. Analysis run was optimized to the maximum separation of levoglucosan, mannosan, and galactosan with 15-min analysis. The validation results indicated that the method showed good applicability for determination of MA isomer concentrations in ambient samples. The limit of detection was 100 pg for levoglucosan and 50 pg for mannosan and galactosan. Wide determination ranges enabled the analysis of samples of different concentration levels. The method showed good precision, both for standard solutions (3.9-5.9% RSD) and for fine particle samples (4.3-8.5% RSD). Co-elution of internal standard (carbon-13-labeled levoglucosan) and sugar alcohols with levoglucosan decreased the sensitivity of levoglucosan determination. The method was used to determine the MA concentrations in ambient fine particle samples from urban background (Helsinki) and rural background (Hyytiälä) in Finland. The average levoglucosan, mannosan, and galactosan concentrations were 77, 8.8, and 4.2 ng m(-3) in Helsinki (winter 2008-2009) and 17, 2.3, and 1.4 ng m(-3) in Hyytiälä (spring 2007), respectively. The interrelation of the three MA isomers was fairly constant in the ambient fine particle samples.
Assuntos
Cromatografia/métodos , Monitoramento Ambiental/métodos , Galactose/análogos & derivados , Glucose/análogos & derivados , Manose/análogos & derivados , Material Particulado/análise , Cromatografia Líquida de Alta Pressão/métodos , Galactose/análise , Glucose/análise , Manose/análise , Espectrometria de Massas/métodosRESUMO
This study was conducted at three sites of different characteristics in São Paulo State: São Paulo (SPA), Piracicaba (PRB) and Mata Atlântica Forest (MAT). PM(10), n-alkanes, pristane and phytane, PAHs, water-soluble ions and biomass burning tracers like levoglucosan and retene, were determined in quartz fiber filters. Samplings occurred on May 8th to August 8th, 2007 at the MAT site; on August 15th to 29th in 2007 and November 10th to 29th in 2008 at the PRB site and, March 13th to April 4th in 2007 and August 7th to 29th in 2008 at the SPA site. Aliphatic compounds emitted biogenically were less abundant at the urban sites than at the forest site, and its distribution showed the influence of tropical vascular plants. Air mass transport from biomass burning regions is likely to impact the sites with specific molecular markers. The concentrations of all species were variable and dependent of seasonal changes. In the most dry and polluted seasons, n-alkane and cation total concentrations were similar between the megacity and the biomass burning site. PAHs and inorganic ion abundances were higher at São Paulo than Piracicaba, yet, the site influenced by biomass burning seems to be the most impacted by the organic anion abundance in the atmosphere. Pristane and phytane confirm the contamination by petroleum residues at urban sites; at the MAT site, biological activity and long range transport of pollutants might influence the levels of pristane.
Assuntos
Aerossóis/análise , Poluentes Atmosféricos/análise , Atmosfera/química , Monitoramento Ambiental , Material Particulado/análise , Biomassa , Brasil , Cidades , Diterpenos/análise , Glucose/análogos & derivados , Glucose/análise , Incineração , Fenantrenos/análise , Hidrocarbonetos Policíclicos Aromáticos/análise , Terpenos/análise , ÁrvoresRESUMO
A series of smoke plumes was detected in Helsinki, Finland, during a one-month-lasting period in August 2006. The smoke plumes originated from wildfires close to Finland, and they were short-term and had a high particulate matter (PM) concentration. Physical and chemical properties of fine particles in those smokes were characterised by a wide range of real-time measurements that enabled the examination of individual plume events. Concurrently PM(1) filter samples were collected and analysed off-line. Satellite observations employing MODIS sensor on board of NASA EOS Terra satellite with the dispersion model SILAM and the Fire Assimilation System were used for evaluation of the emission fluxes from wildfires. The model predicted well the timing of the plumes but the predicted PM concentrations differed from the observed. The measurements showed that the major growth in PM concentration was caused by submicrometer particles consisting mainly of particulate organic matter (POM). POM had not totally oxidised during the transport based on the low WSOC-to-OC ratio. The fresh plumes were compared to another major smoke episode that was observed in Helsinki during April-May 2006. The duration and the source areas of the two episode periods differed. The episode in April-May was a period of nearly constantly upraised level of long-range transported PM and it was composed of aged particles when arriving in Helsinki. The two episodes had differences also in the chemical composition of PM. The mass concentrations of biomass burning tracers (levoglucosan, potassium, and oxalate) increased during both the episodes but different concentration levels of elemental carbon and potassium indicated that the episodes differed in the form of burning as well as in the burning material. In spring dry crop residue and hay from the previous season were burnt whereas in August smokes from smouldering and incomplete burning of fresh vegetation were detected.
Assuntos
Atmosfera/química , Incêndios , Material Particulado/química , Fumaça/análise , Monitoramento Ambiental , FinlândiaRESUMO
Epidemiological studies show heterogeneities in the particulate pollution-related exposure-effect relationships among cardiorespiratory patients, but the connection to chemical composition and toxic properties of the inhaled particles is largely unknown. To identify the chemical constituents and sources responsible for the diverse inflammatory and cytotoxic effects of urban air, fine (PM(2.5-0.2)) and coarse (PM(10-2.5)) particulate samples were collected during contrasting air pollution situations. We exposed mouse RAW 246.7 macrophages for 24 hrs to PM(2.5-0.2) and PM(10-2.5) samples from six European cities. The concentrations of proinflammatory cytokines (IL-6, TNFalpha), chemokine (MIP-2), and nitric oxide were measured from the cell culture medium, and the cytotoxicity was assayed. Spearman's correlations between the chemical constituents and cellular responses were analyzed. In the PM(2.5-0.2) size range, the tracers of photo-oxidation of organics in the atmosphere (oxalate, succinate, malonate), some transition metals (Ni, V, Fe, Cu, Cr), and insoluble soil constituents (Ca, Al, Fe, Si) correlated positively with the response parameters. In contrast, the tracers of incomplete biomass (monosaccharide anhydrides) and coal (As) combustion, and polycyclic aromatic hydrocarbons (PAHs), had negative correlations with the inflammatory activity. The compositions of PM(10-2.5) samples were more uniform and there were only occasional high correlations between the chemical constituents, endotoxin, and the response parameters. The present results suggest that the local sources of incomplete combustion and resuspended road dust are important producers of harmful fine particulate constituents that may, however, operate via diverse toxicity mechanisms. The results agree well with our recent findings in the mouse lung.
Assuntos
Poluentes Atmosféricos/toxicidade , Inflamação/induzido quimicamente , Macrófagos/efeitos dos fármacos , Material Particulado/toxicidade , Poluentes Atmosféricos/análise , Animais , Linhagem Celular , Sobrevivência Celular/efeitos dos fármacos , Quimiocinas/biossíntese , Corantes , Citocinas/biossíntese , Europa (Continente) , Inflamação/patologia , Camundongos , Óxido Nítrico/biossíntese , Tamanho da Partícula , Material Particulado/química , Hidrocarbonetos Policíclicos Aromáticos/análise , Sais de Tetrazólio , Tiazóis , Fator de Necrose Tumoral alfa/metabolismo , Água/análiseRESUMO
This study investigates commuter and driver exposure to aerosol particles in buses and trams in Helsinki, Finland. Particle number and PM(2.5) concentrations were determined in the cabin and the driver's compartment. In addition, the <2.5 microm black carbon concentration was measured in the driver's compartment and PM(2.5) was collected for elemental analysis in the cabin. The measurements were repeated on two generations of buses and trams including two measurement days in each vehicle type. Fine particle number and mass concentrations in the driver's compartments were only slightly increased compared to Helsinki background air. Daily average ratios of number and mass to the background varied in range 0.8-4.3 and 1.0-2.9, respectively, both being the highest in the older bus type. However, the drivers were exposed to elevated levels of black carbon, which some studies have addressed to be strongly correlated with adverse health effects. The daily average ratio of black carbon to the background varied between 2.4 and 11.4. Additionally, the black carbon concentration had spatial variation. The drivers were exposed to higher peak concentrations of black carbon in downtown area. Particle concentrations were smaller in the driver's compartment than in the cabin. The newer technology in the newer model of the tram and bus seemed to decrease driver exposure to aerosol particles.
Assuntos
Aerossóis/análise , Poluentes Atmosféricos/análise , Monitoramento Ambiental , Veículos Automotores , Material Particulado/análise , Condução de Veículo , Finlândia , Tamanho da Partícula , Fuligem/análiseRESUMO
Inflammation is regarded as an important mechanism in mortality and morbidity associated with exposures of cardiorespiratory patients to urban air particulate matter. We investigated the association of the chemical composition and sources of urban air fine (PM(2.5-0.2)) and coarse (PM(10-2.5)) particulate samples with the inflammatory activity in the mouse lung. The particulate samples were collected during selected seasons in six European cities using a high-volume cascade impactor. Healthy C57BL/6J mice were intratracheally instilled with a single dose (10 mg/kg) of the particulate samples. At 4, 12, and 24 h after the exposure, the lungs were lavaged and the bronchoalveolar lavage fluid (BALF) was assayed for indicators of inflammation and tissue damage: cell number, total protein, and cytokines (tumor necrosis factor [TNF]-alpha, interleukin [IL]-6, and KC). Dicarboxylic acids and transition metals, especially Ni and V, in PM(2.5-0.2) correlated positively and some secondary inorganic ions (NO3(-), NH4(+)) negatively with the inflammatory activity. Total organic matter and SO4(2-) had no consistent correlations. In addition, the soil-derived constituents (Ca2+, Al, Fe, Si) showed positive correlations with the PM(2.5-0.2)-induced inflammatory activity, but their role in PM(10-2.5) remained obscure, possibly due to largely undefined biogenic material. Markers of poor biomass and coal combustion, i.e., monosaccharide anhydrides and As, were associated with elevated PAH contents in PM(2.5-0.2) and a consistent immunosuppressive effect. Overall, our results support epidemiological findings that the local sources of incomplete combustion and resuspended road dust are important in urban air particulate pollution-related health effects.