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1.
Three mercury (Hg) species (gaseous elemental mercury (GEM), gaseous oxidized mercury (GOM), and fine particulate-bound mercury (PBM2.5)) were measured in the stack of a small scale wood combustion chamber at 400 °C, in the stack of an advanced wood boiler, and in two areas influenced by wood combustion. The low temperature process (lab-scale) emitted mostly GEM (∼99% when burning wood pellets and ∼95% when burning unprocessed wood). The high temperature wood boiler emitted a greater proportion of oxidized Hg (approximately 65%) than the low temperature system. In field measurements, mean PBM2.5 concentrations at the rural and urban sites in winter were statistically significantly higher than in warmer seasons and were well correlated with Delta-C concentrations, a wood combustion indictor measured by an aethalometer (UV-absorbable carbon minus black carbon). Overall the results suggest that wood combustion may be an important source of oxidized mercury (mostly in the particulate phase) in northern climates in winter.  相似文献   

2.
The bilinear receptor model positive matrix factorization (PMF) was used to apportion particulate matter with an aerodynamic diameter of 1–10 μm (PM1–10) sources in a village, B?ezno, situated in an industrial region of northern Bohemia in Central Europe. The receptor model analyzed the data sets of 90- and 60-min integrations of PM1–10 mass concentrations and elemental composition for 27 elements. The 14-day sampling campaigns were conducted in the village in summer 2008 and winter 2010. Also, to ensure seasonal and regional representativeness of the data sets recorded in the village, the spatial-temporal variability of the 24-hr PM10 and PM1–10 within 2008–2010 in winter and summer across the multiple sites was evaluated. There were statistically significant interseasonal differences of the 24-hr PM data, but not intrasummer or intrawinter differences of the 24-hr PM1–10 data across the multiple sites. PMF resolved seven sources of PM1–10. They were high-temperature coal combustion; combustion in local heating boilers; marine aerosol; mineral dust; primary biological/wood burning; road dust, car brakes; and gypsum. The main summer factors were assigned to mineral dust (38.2%) and primary biological/wood burning (33.1%). In winter, combustion factors dominated (80%) contribution to PM1–10. The conditional probability function (CPF) helped to identified local sources of PM1–10. The source of marine aerosol from the North Sea and English Channel was indicated by the Hybrid Single Particle Lagrangian Integrated Trajectory Model (HYSPLIT).

Implications: This is the first application of PMF to highly time/size resolved PM data in Czech Republic. The coarse aerosol fraction, PM1–10, was chosen with regard to industrial character of the region, sampling site near the coal strip mine and coal power stations. Contrary to expectation, source apportionment did not show dominance of emissions from the coal strip mine. The results will enable local authorities and state bodies responsible for air quality assessment to focus on sources most responsible for air pollution in this industrial region.

Supplemental Materials:?Supplemental materials are available for this paper. Go to the publisher's online edition of the Journal of the Air & Waste Management Association for (1) details of measurement campaigns; (2) CPF for each of the sources contributing to PM1–10; (3) factors contribution to PM1–10 resolved by PMF; (4) diurnal pattern of road dust, car brake factor in summer and winter; (5) trajectories during the marine aerosol episode in winter 2010; and (6) temporal temperature, concentration, and wind speed relationships during the summer 2008 campaign and winter 2010 campaign.  相似文献   

3.
This study reports a general assessment of the organic composition of the PM2.5 samples collected in the city of Augsburg, Germany in a summer (August-September 2007) and a winter (February-March 2008) campaign of 36 and 30 days, respectively. The samples were directly submitted to in-situ derivatisation thermal desorption gas chromatography coupled with time of flight mass spectrometry (IDTD-GC-TOFMS) to simultaneously determine the concentrations of many classes of molecular markers, such as n-alkanes, iso- and anteiso-alkanes, polycyclic aromatic hydrocarbons (PAHs), oxidized PAHs, n-alkanoic acids, alcohols, saccharides and others.The PCA analysis of the data identified the contributions of three emission sources, i.e., combustion sources, including fossil fuel emissions and biomass burning, vegetative detritus, and oxidized PAHs. The PM chemical composition shows seasonal trend: winter is characterized by high contribution of petroleum/wood combustion while the vegetative component and atmospheric photochemical reactions are predominant in the hot season.  相似文献   

4.
PM2.5 (particulate matter with an aerodynamic diameter <2.5 μm) 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-β-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 of 2.3% was found 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%).

Implications:?PM2.5 levoglucosan concentrations and the correlation between levoglucosan relative to other compounds during four seasons in Xi’an showed that the influence of biomass burning is maximum during the residential heating season (winter), although some important influences may be detected in spring (field preparation burnings) and autumn (corn stalks and wheat straw burning, fallen dead leaves burning) at Xi’an and surrounding areas. Household heating with biomass during winter was quite widespread in Guanzhong Plain. Therefore, the control of biomass/biofuel combustion could be an effective method to reduce pollutant emission on a regional scale.  相似文献   

5.
Polycyclic aromatic hydrocarbons (PAHs) in PM2.5 and cloud/fog water samples were collected at Mount Taishan in an autumn–winter period, and were analyzed by GS-MS. Higher molecular weight PAHs (4–6 rings) predominated in PM2.5 samples, whereas lighter PAH compounds contributed 61.71% of the total PAH concentration in cloud/fog samples. Particles tended to contain more PAHs and have a more intensive influence on the atmospheric environment on colder days. During cloud/fog events, the scavenging ratio based on PAHs associated with particles was estimated to be about 13.45%. PAHs in PM2.5 samples had a significant positive relationship with CO and SO2, suggesting that PAHs, SO2, and CO may originated from the same sources, such as residential coal combustion activities. Diagnostic ratio analysis and factor analysis indicated that the sources of PAHs were mainly from coal combustion during this period.  相似文献   

6.
Organic aerosol is the least understood component of ambient fine particulate matter (PM2.5). In this study, organic and elemental carbon (OC and EC) within ambient PM2.5 over a three-year period at a forested site in the North Carolina Piedmont are presented. EC exhibited significant weekday/weekend effects and less significant seasonal effects, in contrast to OC, which showed strong seasonal differences and smaller weekend/weekday effects. Summer OC concentrations are about twice as high as winter concentrations, while EC was somewhat higher in the winter. OC was highly correlated with EC during cool periods when both were controlled by primary combustion sources. This correlation decreased with increasing temperature, reflecting higher contributions from secondary organic aerosol, likely of biogenic origin. PM2.5 radiocarbon data from the site confirms that a large fraction of the carbon in PM2.5 is indeed of biogenic origin, since modern (non-fossil fuel derived) carbon accounted for 80% of the PM2.5 carbon over the course of a year. OC and EC exhibited distinct diurnal profiles, with summertime OC peaking in late evening and declining until midday. During winter, OC peaked during the early morning hours and again declined until midday. Summertime EC peaked during late morning hours except on weekends. Wintertime EC often peaked in late PM or early AM hours due to local residential wood combustion emissions. The highest short term peaks in OC and EC were associated with wildfire events. These data corroborate recent source apportionment studies conducted within 20 km of our site, where oxidation products of isoprene, α-pinene, and β-caryophyllene were identified as important precursors to organic aerosols. A large fraction of the carbon in rural southeastern ambient PM2.5 appears to be of biogenic origin, which is probably difficult to reduce by anthropogenic controls.  相似文献   

7.
Abstract

Approximately 750 total suspended particulates (TSPs) and coarse particulate matter (PM10) filter samples from six urban sites and a background site and >210 source samples were collected in Jiaozuo City during January 2002 to April 2003. They were analyzed for mass and abundances of 25 chemical components. Seven contributive sources were identified, and their contributions to ambient TSP/PM10 levels at the seven sites in three seasons (spring, summer, and winter days) and a “whole” year were estimated by a chemical mass balance (CMB) receptor model. The spatial TSP average was high in spring and winter days at a level of approximately 530 ~g/m3 and low in summer days at 456 ~g/m3; however, the spatial PM10 average exhibited little variation at a level of approximately 325 ~g/m3, and PM10-to-TSP ratios ranged from 0.58 to 0.81, which suggested heavy particulate matter pollution existing in the urban areas. Apportionment results indicated that geological material was the largest contributor to ambient TSP/PM10 concentrations, followed by dust emissions from construction activities, coal combustion, secondary aerosols, vehicle movement, and other industrial sources. In addition, paved road dust and re-entrained dust were also apportioned to the seven source types and found soil, coal combustion, and construction dust to be the major contributors.  相似文献   

8.
Continuous observation of PM2.5 was conducted in Taiyuan, a heavily polluted city in China, during high pollution season from December 2005 to February 2006. The results of this study showed that PM2.5 and carbonaceous species pollution were serious during winter in Taiyuan. The organic carbon (OC) and element carbon (EC) were accounted for 18.6±11.2% and 2.9±1.6% of PM2.5, respectively, which indicated that carbonaceous aerosols were key components for control fine particles pollution in Taiyuan. Coal combustion was a dominant source of OC and EC of PM2.5 in the urban area of Taiyuan during winter. The impact of local and remote particle sources on urban air quality was assessed using PM2.5 concentration rose and 3-day back trajectories of air masses arriving at Taiyuan. The meteorological conditions were found to affect the ambient concentrations of PM2.5, OC, EC and OC/EC ratio.  相似文献   

9.
The atmosphere of the Lake Tahoe air basin is contaminated with high molecular weight (> C12) petroleum hydrocarbons. Aerosol samples were collected by high-volume filtration and the solvent-soluble organic matter was analyzed. The relative concentrations of petroleum residues found were as follows: winter > summer and day > night. This contamination is primarily due to the poorer combustion of diesel and home heating fuels at that altitude and during periods of colder climate.  相似文献   

10.
Abstract

Source types or source regions contributing to the concentration of atmospheric fine particles measured at Brigantine National Wildlife Refuge, NJ, were identified using a factor analysis model called Positive Matrix Factorization (PMF). Cluster analysis of backward air trajectories on days of high- and low-factor concentrations was used to link factors to potential source regions. Brigantine is a Class I visibility area with few local sources in the center of the eastern urban corridor and is therefore a good location to study Mid-Atlantic regional aerosol. Sulfate (expressed as ammonium sulfate) was the most abundant species, accounting for 49% of annual average fine mass. Organic compounds (22%; expressed as 1.4 × organic carbon) and ammonium nitrate (10%) were the next abundant species. Some evidence herein suggests that secondary organic aerosol formation is an important contributor to summertime regional aerosol.

Nine factors were identified that contributed to PM2.5 mass concentrations: coal combustion factors (66%, summer and winter), sea salt factors (9%, fresh and aged), motor vehicle/mixed combustion (8%), diesel/Zn-Pb (6%), incinerator/industrial (5%), oil combustion (4%), and soil (2%). The aged sea salt concentrations were highest in springtime, when the land breeze-sea breeze cycle is strongest. Comparison of backward air trajectories of high- and low-concentration days suggests that Brigantine is surrounded by sources of oil combustion, motor vehicle/mixed combustion, and waste incinerator/industrial emissions that together account for 17% of PM2.5 mass. The diesel/Zn-Pb factor was associated with sources north and west of Brigantine. Coal combustion factors were associated with coal-fired power plants west and southwest of the site. Particulate carbon was associated not only with oil combustion, motor vehicle/mixed combustion, waste incinerator/industrial, and diesel/Pb-Zn, but also with the coal combustion factors, perhaps through common transport.  相似文献   

11.
This study identifies major contributing sources of high particulate matter (PM) days in Hong Kong and conducive meteorological conditions leading to high PM. The PM10 chemical composition of 3393 ambient samples collected at ten monitoring stations in Hong Kong during 1998–2005 were used as input for positive matrix factorization (PMF) modeling to identify and quantify the aerosol sources in Hong Kong. Days with PM10 levels exceeding 56 μg m?3, the average plus one standard deviation of the mass concentration of all samples, are defined as high PM days. A total of 401 samples fell in the high PM category during the study period. Biomass burning, secondary sulfate and secondary nitrate were found to be the major contributors leading to high PM, responsible for 68–73% of PM10 mass on high PM days. The contributions by these sources on high PM days were 140–180% higher than their respective average concentration contributions. These sources were identified to be regional sources on the grounds of little spatial variation in their concentrations among the monitoring stations and a temporal pattern of higher in the winter and lower in the summer. Sampling days of high PM in 2004 and 2005 were individually examined for weather charts and regional surface wind maps. Weak high pressures over mainland China were the most important synoptic event leading to high PM days in the fall and winter, while typhoon episodes were responsible for most summer cases. Approximately 80% of the high PM days were in the fall and winter months (September–February). Almost all the high PM days were associated with northwesterly, northerly or northeasterly regional transport. Anthropogenic primary sources (coal combustion, vehicular exhaust, and residue oil combustion) showed the highest contributions associated with northwesterly wind, indicating the strong influence of the more urbanized areas to the northwest of Hong Kong in the Pearl River Delta region.  相似文献   

12.
Mössbauer spectroscopy was applied to analyze the iron compounds present in atmospheric aerosol. As a significant part of air pollution, especially in winter months, iron appeared in the form of iron sulfides (FeS2, FeS and Fe1−xS), which were products of coal combustion. Also, iron oxyhydroxides and iron oxides, mostly α-Fe2O3 (bulk) and in the form of ultra fine particles in superparamagnetic state were observed. The concentration of iron in atmospheric air was calculated from the experimental spectra. Seasonal variations of iron concentration in atmospheric air measured over twenty years in the mountain region of Poland are discussed.  相似文献   

13.
PM2.5 sampling was conducted at a curbside location in Delhi city for summer and winter seasons, to evaluate the effect of PM2.5 and its chemical components on the visibility impairment. The PM2.5 concentrations were observed to be higher than the National Ambient Air Quality Standards (NAAQS), indicating poor air quality. The chemical constituents of PM2.5 (the water-soluble ionic species SO42-, NO3?, Cl?, and NH4+, and carbonaceous species: organic carbon, elemental carbon) were analyzed to study their impact on visibility impairment by reconstructing the light extinction coefficient, bext. The visibility was found to be negatively correlated with PM2.5 and its components. The reconstructed bext showed that organic matter was the largest contributor to bext in both the seasons which may be attributed to combustion sources. In summer season, it was followed by elemental carbon and ammonium sulfate; however, in winter, major contributions were from ammonium nitrate and elemental carbon. Higher elemental carbon in both seasons may be attributed to traffic sources, while lower concentrations of nitrate during summer, may be attributed to volatility because of higher atmospheric temperatures.

Implications: The chemical constituents of PM2.5 that majorly effect the visibility impairment are organic matter and elemental carbon, both of which are products of combustion processes. Secondary formations that lead to ammonium sulfate and ammonium nitrate production also impair the visibility.  相似文献   

14.
The seasonal variability in the mass concentration and chemical composition of atmospheric particulate matter (PM10 and PM2.5) was studied during a 2-year field study carried out between 2010 and 2012. The site of the study was the area of Ferrara (Po Valley, Northern Italy), which is characterized by frequent episodes of very stable atmospheric conditions in winter. Chemical analyses carried out during the study allowed the determination of the main components of atmospheric PM (macro-elements, ions, elemental carbon, organic matter) and a satisfactory mass closure was obtained. Accordingly, chemical components could be grouped into the main macro-sources of PM: soil, sea spray, inorganic compounds from secondary reactions, vehicular emission, organics from domestic heating, organics from secondary formation, and other sources. The more significant seasonal variations were observed for secondary inorganic species in the fine fraction of PM; these species were very sensitive to air mass age and thus to the frequency of stable atmospheric conditions. During the winter ammonium nitrate, the single species with the highest concentration, reached concentrations as high as 30 μg/m3. The intensity of natural sources was fairly constant during the year; increases in natural aerosols were linked to medium and long-range transport episodes. The ratio of winter to summer concentrations was roughly 2 for combustion product, close to 3 for secondary inorganic species, and between 2 and 3 for organics. The winter increase of organics was due to poorer atmospheric dispersion and to the addition of the emission from domestic heating. A similar winter to summer ratio (around 3) was observed for the fine fraction of PM.  相似文献   

15.
The aerosol samples were collected from a high elevation mountain site, Nainital, in India (1958 m asl) during September 2006 to June 2007 and were analyzed for water-soluble inorganic species, total carbon, nitrogen, and their isotopic composition (δ13C and δ15N, respectively). The chemical and isotopic composition of aerosols revealed significant anthropogenic influence over this remote free-troposphere site. The amount of total carbon and nitrogen and their isotopic composition suggest a considerable contribution of biomass burning to the aerosols during winter. On the other hand, fossil fuel combustion sources are found to be dominant during summer. The carbon aerosol in winter is characterized by greater isotope ratios (av. ?24.0?‰), mostly originated from biomass burning of C4 plants. On the contrary, the aerosols in summer showed smaller δ13C values (?26.0?‰), indicating that they are originated from vascular plants (mostly of C3 plants). The secondary ions (i.e., SO4 2?, NH4 +, and NO3 ?) were abundant due to the atmospheric reactions during long-range transport in both seasons. The water-soluble organic and inorganic compositions revealed that they are aged in winter but comparatively fresh in summer. This study validates that the pollutants generated from far distant sources could reach high altitudes over the Himalayan region under favorable meteorological conditions.  相似文献   

16.
A 5-yr record of continuous high-frequency carbon dioxide CO2 observations over the 1995–1999 period for the Mace Head Atmospheric Research Station has been examined to reveal a complex interplay between local- and regional-scale sources and sinks. During the winter months, an additional CO2 source, over and above fossil fuel combustion, is required to support the observed concentrations of CO2 in European regionally polluted air masses. During the summer months, an additional CO2 sink is required. Over the entire study period, the additional net European ecosystem exchange source–sink required is –0.36±0.4 Gtonne C yr−1.  相似文献   

17.
Ambient aerosol samples, collected from Mangalore region in the southwest coast of India during the period of late winter (February and March) to early summer (April and May), have been analysed for water-soluble ionic species. Their abundance pattern is dominated by HCO3, SO42−, Na+, Cl, with minor contribution from NO3, Ca2+, NH4+, K+ and Mg2+ indicating the contribution from not only sea salt, but also from anthropogenic and dust sources; with pronounced seasonal variability. The suspended particulate matter concentration varied from 35 to 160 μg m−3, with consistently higher values during the late winter. Back trajectory analysis suggests the origin of the air masses shifting from Indo-Gangetic Plains (during late winter) to those from the Arabian Sea and the area around Persian Gulf during April–May. Air masses passing over Northern India (Indo-Gangetic Plains) impart characteristic contribution of ionic species from fossil fuel combustion, biomass burning and eolian dust as asserted by the factor analysis. A detailed study on characterisation of aerosols from south Asian region is rather sparse but essential for modelling the effect of tropospheric aerosols on climate.  相似文献   

18.
From December to April, the Arctic air mass is polluted by man-made mid-latitudinal emissions from fossil fuel combustion, smelting and industrial processes. In the rest of the year, pollution levels are much lower. This is the outcome of less efficient pollutant removal processes and better south (S) to north (N) transport during winter. In winter, the Arctic air mass covers much of Eurasia and N. America. Meteorological flow fields and the distribution of anthropogenic SO2 emissions in the northern hemisphere favor northern Eurasia as the main source of visibility reducing haze. Observations of SO42− concentrations in the atmosphere throughout the Arctic yield, depending on location and year, a January–April mean of 1.5–3.9 μg m−3 in the Norwegian Arctic to 1.2–2.2 μg m−3 in the N. American Arctic. An estimate of the mean vertical profile of fine particle aerosol mass during March and April shows that, on average, pollution is concentrated in the lower 5 km of the atmosphere. Not only are anthropogenic particles present in the Arctic atmosphere but also gases such as SO2, perfluorocarbons and pesticides. The acidic nature and seasonal variation of Arctic pollution is reflected in precipitation, the snowpack and glacier snow in the Arctic. A pH of 4.9–5.2 in winter and ~ 5.6 in summer is expected in the absence of calcareous wind blown soil. Glacial records indicate that Arctic air pollution has undergone a marked increase since the mid 1950s paralleling a marked increase in SO2 and NOx emissions in Europe. Effects of Arctic pollution include a reduction in visibility and perturbation of the solar radiation budget in April–June. Potential effects are the acidification and toxification of sensitive ecosystems.  相似文献   

19.
The nitrogen oxides (NOx) reduction technology by combustion modification which has economic benefits as a method of controlling NOx emitted in the combustion process, has recently been receiving a lot of attention. Especially, the moderate or intense low oxygen dilution (MILD) combustion which applied high temperature flue gas recirculation has been confirmed for its effectiveness with regard to solid fuel as well. MILD combustion is affected by the flue gas recirculation ratio and the composition of recirculation gas, so its NOx reduction efficiency is determined by them. In order to investigate the influence of factors which determine the reduction efficiency of NOx in MILD coal combustion, this study changed the flow rate and concentration of nitrogen (N2), carbon dioxide (CO2) and steam (H2O) which simulate the recirculation gas during the MILD coal combustion using our lab-scale drop tube furnace and performed the combustion experiment. As a result, its influence by the composition of recirculation gas was insignificant and it was shown that flue gas recirculation ratio influences the change of NOx concentration greatly. Implications: We investigated the influence of factors determining the nitrogen oxides (NOx) reduction efficiency in MILD coal combustion, which applied high-temperature flue gas recirculation. Using a lab-scale drop tube furnace and simulated recirculation gas, we conducted combustion testing changing the recirculation gas conditions. We found that the flue gas recirculation ratio influences the reduction of NOx emissions the most.  相似文献   

20.
Contribution of pollution from different types of sources in Jamshedpur, the steel city of India, has been estimated in winter 1993 using two approaches in order to delineate and prioritize air quality management strategies for the development of region in an environmental friendly manner. The first approach mainly aims at preparation of a comprehensive emission inventory and estimation of spatial distribution of pollution loads in terms of SO2 and NO2 from different types of industrial, domestic and vehicular sources in the region. The results indicate that industrial sources account for 77% and 68% of the total emissions of SO2 and NO2, respectively, in the region, whereas vehicular emissions contributed to about 28% of the total NO2 emissions. In the second approach, contribution of these sources to ambient air quality levels to which the people are exposed to, was assessed through air pollution dispersion modelling. Ambient concentration levels of SO2 and NO2 have been predicted in winter season using the ISCST3 model. The analysis indicates that emissions from industrial sources are responsible for more than 50% of the total SO2 and NO2 concentration levels. Vehicular activities contributed to about 40% of NO2 pollution and domestic fuel combustion contributed to about 38% of SO2 pollution. Predicted 24-h concentrations were compared with measured concentrations at 11 ambient air monitoring stations and good agreement was noted between the two values. In-depth zone-wise analysis of the above indicates that for effective air quality management, industrial source emissions should be given highest priority, followed by vehicular and domestic sources in Jamshedpur region.  相似文献   

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