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1.
Particulate matter (PM) sources at two different sites in a rural town in New Zealand were investigated on an hourly time-scale. Streaker samplers were used to collect hourly, size-segregated PM(10-2.5) and PM(2.5) samples that were analyzed for elemental content using ion beam analysis techniques. Black carbon concentrations were determined using light reflection and PM(10) concentrations were recorded using colocated continuous PM monitors. PM(10) concentrations at both sites displayed a diurnal pattern, with hourly PM(10) concentration maxima in the evening (7 pm-midnight) and in the morning (7-9 am). One of the monitoring sites experienced consistently higher average PM(10) concentrations during every hour and analysis indicated that katabatic flows across the urban area contributed to the increased concentrations observed. Source apportionment using positive matrix factorization on the hourly data revealed four primary PM(10) sources for each site: biomass burning, motor vehicles, marine aerosol and crustal matter. Biomass burning was the most dominant source at both sites and was responsible for both the evening and morning PM(10) concentration peaks. The use of elemental speciation combined with PM(10) concentrations for source apportionment on an hourly time-scale has never been reported and provides unique and useful information on PM sources for air quality management.  相似文献   

2.
Size-fractionated (equivalent to ambient PM2.5 and PM10) local soil, plant, and spore samples were collected in the Sonoran Desert near Phoenix, AZ and measured for saccharide content with the goal of characterizing ambient particulate matter sources including soil and primary biological aerosol particles (PBAPs) from plants and fungi. Different saccharide compositions were observed among soil, plant, and spore samples and between PM2.5 and PM10 fractions. The total measured nonlevoglucosan saccharide content relative to PM mass in ambient aerosols collected in a Phoenix suburb (Higley) was much higher compared to the local soil samples but much lower compared to the PBAP. The enrichment of saccharides from two saccharide-dominated PM source factors resolved by a positive matrix factorization model is also higher than the saccharide content in the size-fractionated local soil samples, but lower than that measured in the size-segregated PBAP samples. This indicates that ambient concentration of particulate saccharides at Higley was dominated by contributions from PBAPs directly injected into the atmosphere from plants and spores rather than from soil and associated biota. Our results also suggest the contribution to the fine size fraction of ambient PM from the primary biologically derived sources may be greater than previously acknowledged.  相似文献   

3.
A new approach for determining the contributions of emission sources to concentrations of particulate matter and gases is developed using the chemical mass balance (CMB) method and the U.S. EPA's National Emission Inventory (NEI). The approach apportions combined gas-phase and condensed-phase concentrations of individual compounds as well as PM(2.5) mass. Because the NEI is used to provide source emission profiles for CMB analysis, the method generates information on the consistency of the NEI with ambient monitoring data. The method also tracks secondary species to primary source emissions, permitting a more complete accounting of the impact of aggregated source types on PM(2.5) mass concentrations. An example application is presented using four years of monitoring data collected at eight sites in the Southeastern Aerosol Research and Characterization (SEARCH) network. Including both primary and secondary species, area sources contributed 2.0-3.7 μg m(-3) (13-26%), point sources contributed 3.0-4.6 μg m(-3) (22-33%), and mobile sources contributed 1.0-6.0 μg m(-3) (9-42%) to mean PM(2.5) mass concentrations. Whereas the NEI generally accounts for the ambient concentrations of gases and particles, certain anomalies are identified, especially related to carbonaceous compounds and dust.  相似文献   

4.
Combustion of wood and other biomass fuels produces source-specific organic compounds arising from pyrolysis of lignin, including substantial amounts of 4-substituted methoxylated phenolic compounds (methoxyphenols). These compounds have been used as atmospheric markers to determine the contribution of wood smoke to ambient atmospheric fine particulate matter (PM). However, reliable quantification of methoxyphenols represents an analytical challenge because these compounds are polar, semi-volatile, and somewhat reactive. We reportherein an improved gas chromatographic-mass spectrometric (GC/MS) method for the sensitive and reliable determination of methoxyphenols in low-volume ambient PM samples. Deuterated standard compounds are added to the environmental samples prior to extraction to determine analyte recoveries in each sample. Analytical figures of merit for the assay, as applied to ambient PM2.5 and PM10 samples are as follows: recovery = 63-100%; precision = 2-6%; analytical limit of detection (S/N 2) = 0.002 microg/mL; limit of quantitation = 0.07-0.45 ng/m3 (assuming a 14 m3 sample). The improved method was applied to ambient PM samples collected between 1999 and 2000 in Seattle, WA. Particle-bound methoxyphenol concentrations in the range <0.1 to 22 ng/m3 were observed and the methoxyphenols were present almost exclusively in the fine (PM2.5) size fraction. We also demonstrated that XRF analysis of samples of atmospheric PM collected on Teflon filters significantly reduced the levels of methoxyphenols measured in the PM samples in subsequent assay of the same filters. Therefore, XRF analysis of filters, commonly undertaken to obtain trace element concentrations for use in source apportionment analyses, would preclude the subsequent analysis of those filters for methoxyphenols and other similarly semivolatile or reactive organic chemicals.  相似文献   

5.
Published emission factors (EFs) often vary significantly, leading to high uncertainties in emission estimations. There are few reliable EFs from field measurements of residential wood combustion in China. In this study, 17 wood fuels and one bamboo were combusted in a typical residential stove in rural China to measure realistic EFs of particulate matter (PM), organic carbon (OC), and elemental carbon (EC), as well as to investigate the influence of fuel properties and combustion conditions on the EFs. Measured EFs of PM, OC, and EC (EF(PM), EF(OC), and EF(EC), respectively) were in the range of 0.38-6.4, 0.024-3.0, and 0.039-3.9 g/kg (dry basis), with means and standard derivation of 2.2 ± 1.2, 0.62 ± 0.64, and 0.83 ± 0.69 g/kg, respectively. Shrubby biomass combustion produced higher EFs than tree woods, and both species had lower EFs than those of indoor crop residue burning (p < 0.05). Significant correlations between EF(PM), EF(OC), and EF(EC) were expected. By using a nine-stage cascade impactor, it was shown that size distributions of PM emitted from tree biomass combustions were unimodal with peaks at a diameter less than 0.4 μm (PM(0.4)), much finer than the PM from indoor crop residue burning. Approximately 79.4% of the total PM from tree wood combustion was PM with a diameter less than 2.1 μm (PM(2.1)). PM size distributions for shrubby biomasses were slightly different from those for tree fuels. On the basis of the measured EFs, total emissions of PM, OC, and EC from residential wood combustion in rural China in 2007 were estimated at about 303, 75.7, and 92.0 Gg.  相似文献   

6.
Size-resolved particulate matter emissions from heavy-duty diesel vehicles (HDDVs) and light-duty gasoline vehicles (LDGVs) operated under realistic driving cycles were analyzed for elemental carbon (EC), organic carbon (OC), hopanes, steranes, and polycyclic aromatic hydrocarbons. Measured hopane and sterane size distributions did not match the total carbon size distribution in most cases, suggesting that lubricating oil was not the dominant source of particulate carbon in the vehicle exhaust. A regression analysis using 17alpha(H)-21beta(H)-29-norhopane as a tracer for lubricating oil and benzo[ghi/perylene as a tracer for gasoline showed that gasoline fuel and lubricating oil both make significant contributions to particulate EC and OC emissions from LDGVs. A similar regression analysis performed using 17alpha(H)-21beta(H)-29-norhopane as a tracer for lubricating oil and flouranthene as a tracerfor diesel fuel was able to explain the size distribution of particulate EC and OC emissions from HDDVs. The analysis showed that EC emitted from all HDDVs operated under relatively high load conditions was dominated by diesel fuel contributions with little EC attributed to lubricating oil. Particulate OC emitted from HDDVs was more evenly apportioned between fuel and oil contributions. EC emitted from LDGVs operated underfuel-rich conditions was dominated by gasoline fuel contributions. OC emitted from visibly smoking LDGVs was mostly associated with lubricating oil, but OC emitted from all other categories of LDGVs was dominated by gasoline fuel. The current study clearly illustrates that fuel and lubricating oil make separate and distinct contributions to particulate matter emissions from motor vehicles. These particles should be tracked separately during ambient source apportionment studies since the atmospheric evolution and ultimate health effects of these particles may be different. The source profiles for fuel and lubricating oil contributions to EC and OC emissions derived in this study provide a foundation for future source apportionment calculations.  相似文献   

7.
Extended field measurements of particle number (size distribution of particle diameters, D, in the range between 18 nm and 10 microm), surface area concentrations, and PM1 and PM10 mass concentrations were performed in Switzerland to determine traffic emissions using a comprehensive set of instruments. Measurements took place at roads with representative traffic regimes: at the kerbside of a motorway (120 km h(-1)), a highway (80-100 km h(-1)), and in an urban area with stop-and-go traffic (0-50 km h(-1)) regulated by light signals. Mean diurnal variations showed that the highest pollutant concentrations were during the morning rush hours, especially of the number density in the nanoparticle size range (D <50 nm). From the differences between up- and downwind concentrations (or differences between kerbside and background concentrations for the urban site), "real-life" emission factors were derived using NOx concentrations to calculate dilution factors. Particle number and volume emission factors of different size ranges (18-50 nm, 18-100 nm, and 18-300 nm) were derived for the total vehicle fleet and separated into a light-duty (LDV) and a heavy-duty vehicle (HDV) contribution. The total particle number emissions per vehicle were found to be about 11.7-13.5 x 10(14) particles km(-1) for constant speed (80-120 km h(-1) and 3.9 x 10(14) particles km(-1) for urban driving conditions. LDVs showed higher emission factors at constant high speed than under urban disturbed traffic flow. In contrast, HDVs emitted more air pollutants during deceleration and acceleration processes in stop-and-go traffic than with constant speed of about 80 km h(-1). On average, one HDV emits a 10-30 times higher amount of particulate air pollutants (in terms of both number and volume) than one LDV.  相似文献   

8.
9.
Kitchen-area 22-h gravimetric PM2.5 and passive diffusion stain-tube carbon monoxide (CO) concentrations were measured in homes with open fire and improved wood cookstoves in two studies. In the first study (Guat-2), which also studied homes with gas cookstoves, three samples were collected per stove condition from each of three test houses. In the second study (Guat-3), one sample was collected per house from 15 open fire and 25 improved-stove houses. CO personal samples were also taken for mother and child in both studies. Spearman correlation coefficients (R) between kitchen-area CO and PM2.5 levels in homes using open fires or impoved wood cookstoves were high ranging from 0.92 (Guat-2) to 0.94 (Guat-3), as were those between the personal samples for mother and child ranging from 0.85 (Guat-3) to 0.96 (Guat-2). In general, the correlations were lower for less-polluted conditions. The study found that CO is a good proxy for PM2.5 in homes using open fires or planchas (improved wood cookstove with chimney) but not under gas stove use conditions. It also determined that mother personal CO is a good proxy for child's (under 2 years of age) personal CO and that area CO measurements are not strongly representative of personal CO measurements. These results generally support the use of Draeger CO passive diffusion tubes as a proxy for PM2.5 in such cases where a single type of emission source is the predominant source for CO and PM2.5.  相似文献   

10.
Previously published results for emission factors of medical waste incineration do not include enough information about the incinerated waste composition. This paper reports the first emission factors estimated for particulate matter, As, Cd, Cr, Pb, Mn, Hg, and Ni, considering that medical waste is segregated in different types according to Portuguese legislation. The main purpose was to evaluate the influence of incinerated waste composition and segregation practice on emission factors. One "controlled-air" incinerator without air pollution control devices was used for the incineration either of mixtures with a defined composition or of a specific waste type. Previously published emission factors are not associated with the composition of the incinerated mixture, and the results showed that the usefulness of those emission factors is very doubtful. The existence of different waste classifications also reduces the usefulness of previously published results. To protect human health, appropriate equipment to control atmospheric pollutants must be used, since the legal limits for pollutant concentrations were strongly surpassed (226 times higher than the limit for Hg), with risks for patients and workers of the hospital and exposed population. It was concluded that rigorous segregation practices and adequate management methodologies allow reducing 80% of the amount of wastes that must be incinerated, practically eliminating Hg and Pb emissions and reducing those of PM, As, Cd, Cr, Mn, and Ni, respectively, 98, 90, 92, 84, 77, and 92%.  相似文献   

11.
Current regulation aimed at reducing inorganic atmospheric fine particulate matter (PM2.5) is focused on reductions in sulfur dioxide (SO2) and oxides of nitrogen (NO(x) = NO + NO2); however, controls on these pollutants are likely to increase in cost and decrease in effectiveness in the future. A supplementary strategy is reduction in ammonia (NH3) emissions, yet an evaluation of controls on ammonia has been limited by uncertainties in emission levels and in the cost of control technologies. We use state of the science emission inventories, an emission-based regional air quality model, and an explicit treatment of uncertainty to estimate the cost-effectiveness and uncertainty of ammonia emission reductions on inorganic particulate matter in the Eastern United States. Since a paucity of data on agricultural operations precludes a direct calculation of the costs of ammonia control, we calculate the "ammonia savings potential", defined as the minimum cost of applying SO2 and NO(x) emission controls in order to achieve the same reduction in ambient inorganic PM2.5 concentration as obtained from a 1 ton decrease in ammonia emissions. Using 250 scenarios of NH3, SO2, and NO(x) emission reductions, we calculate the least-cost SO2 and NO(x) control scenarios that achieve the same reduction in ambient inorganic PM2.5 concentration as a decrease in ammonia emissions. We find that the lower-bound ammonia savings potential in the winter is $8,000 per ton NH3; therefore, many currently available ammonia control technologies are cost-effective compared to current controls on SO2 and NO(x) sources. Larger reductions in winter inorganic particulate matter are available at lower cost through controls on ammonia emissions.  相似文献   

12.
为提高基于ImageJ的卷烟包灰值测定方法的准确度和重复性,分别从卷烟燃烧面选择、燃烧灰柱高度及图像选择区域宽度三方面对该方法进行优化研究,形成了如下方案:(1)当烟支燃烧至距离接装纸1cm处时进行拍照;(2)采用高度25mm、宽度6.46 mm的矩形选择框以灰柱底部为起点选择图片区域进行分析;(3)取3支卷烟、3个燃烧面(正对、背对、侧对搭口面)的平均值为一次测量结果。该方案较好控制了卷烟纸搭口、灰柱弯曲、外翻灰片等对测量结果的影响,因而测量结果可以更全面地反映卷烟的裂纹情况,重复性也得到了改善。与改进前相比,4个参试样品重复测量结果的RSD由26.18%~34.52%下降到了15.3%~20.6%。  相似文献   

13.
Size-fractionated samples of airborne particulate matter have been collected in a number of campaigns at Marylebone Road, London and simultaneously at background sites either in Regents Park or at North Kensington. Analysis of these samples has enabled size distributions of total mass and of a number of elements to be determined, and roadside increments attributable to nonexhaust emissions arising from traffic activity have been calculated. Taking a novel approach, the combined use of size distribution information and tracer elements has allowed the separate estimation of the contributions of brake dust, tire dust, and resuspension to particle mass in the range 0.9-11.5 μm aerodynamic diameter and mean contributions (± s.e.) at the Marylebone Road sampling site are estimated as resuspended dust 38.1 ± 9.7%, brake dust 55.3 ± 7.0%, and tire dust 10.7 ± 2.3%, (accounting for a total of 104.1% of coarse particle mass in the traffic increment above background).  相似文献   

14.
Source tests were conducted to analyze and characterize diagnostic key tracers for emissions from burning of coals with various ranks. Ambient aerosol particulate matter was also collected in three areas of China and a background area in Corvallis, OR (U.S.) to confirm the presence of tracers specific for coal smoke. The results showed a series of aliphatic and aromatic hydrocarbons and phenolic compounds, including PAHs and hydroxy-PAHs as the major tracers, as well as a significant unresolved complex mixture (UCM) of compounds. The tracers that were found characteristic of coal combustion processes included hydroxy-PAHs and PAHs. Atmospheric ambient samples from Beijing and Taiyuan, cities where coal is burned in northern China, revealed that the hydroxy-PAH tracers were present during the wintertime, but not in cities where coal is not commonly used (e.g., Guangzhou, South China). Thus, the mass of hydroxy-PAHs can be apportioned to coal smoke and the source strength modeled by summing the proportional contents of EC (elemental carbon), PAHs, UCM and alkanes with the hydroxy-PAHs.  相似文献   

15.
The purpose of this study is to characterize manganese oxidation states and speciation in airborne particulate matter (PM) and describe how these potentially important determinants of PM toxicity vary by location. Ambient PM samples were collected from five counties across the US using a high volume sequential cyclone system that collects PM in dry bulk form segregated into "coarse" and "fine" size fractions. The fine fraction was analyzed for this study. Analyses included total Mn using ICP-MS and characterization of oxidation states and speciation using X-ray absorption spectroscopy (XAS). XAS spectra of all samples and ten standard compounds of Mn were obtained at the National Synchrotron Light Source. XAS data was analyzed using Linear Combination Fitting (LCF). Results of the LCF analysis describe differences in composition between samples. Mn(II) acetate and Mn(II) oxide are present in all samples, while Mn(II) carbonate and Mn(IV) oxide are absent. To the best of our knowledge, this is the first paper to characterize Mn composition of ambient PM and examine differences between urban sites in the US. Differences in oxidation state and composition indicate regional variations in sources and atmospheric chemistry that may help explain differences in health effects identified in epidemiological studies.  相似文献   

16.
A novel approach to determine size-segregated particle number emission factors for traffic is presented. It was proven that using limited data sets (800-2000 samples) statistically significant emission factors from road traffic can be extracted. In this study data from four sites were used for calculating emission factors (rural and urban roadside, urban rooftop, and urban background). The measurements were performed using SMPS/DMPS (scanning or differential particle sizers) from TSI and commercial gas analyzers. Describing the particle concentration as a ratio to an exhaust trace gas, e.g. NOx, the dilution effect will be minimized. This ratio is easily compared among different studies. By knowledge of the emission factor of the chosen trace gas the emission ratio can be converted to an emission factor for particle numbers of defined particle sizes. For the presented method only one measurement site is needed, where the difference between high and low (background) traffic exposure is used. To define high and low traffic exposure, the best result was obtained using high ratio of [NO] to [NO2] and low [NOx], respectively. Emission ratios for 10-100-nm particles at two road sites, one high-speed 90-kmph rural case and one urban, slower, and more congested situation, were determined to (35 +/- 15) x 10(14) and (24 +/- 8) x 10(14) particles per mole NOx, respectively.  相似文献   

17.
Wintertime PM10 samples from two New Zealand cities (Christchurch and Auckland) have been characterized using gas chromatography - mass spectrometry for biomass burning tracers, hopanes, n-alkanes, fatty acids, n-alkanols and sugars. The aerosol samples of Christchurch, which were heavily influenced by residential wood and coal burning, showed substantially higher ambient concentrations for most of the organic compounds than those of Auckland, where major sources of aerosols were vehicular emissions and sea-salt. Mass ratios between the biomass burning tracers studied were found to be significantly different (e.g., beta-sitosterol to nssK+ ratios were more than three times higher in Christchurch than in Auckland), although levoglucosan to nssK+ ratios were similar at the both sites. We also estimated, for the first time using stereochemical configurations of hopanes, that 60% of fossil fuel emissions came from petroleum utilization with the remaining 40% being from coal burning in Christchurch. In contrast, contribution of coal burning was negligible in Auckland. Moreover, contributions of most biomass burning tracers to organic carbon (OC) were significantly higher in Christchurch than in Auckland. On the other hand, saccharides (excluding levoglucosan) and hopanes accounted for larger fractions of OC in Auckland. This study demonstrates that intensive wood and coal burning can significantly affect organic aerosol composition in an urban environment.  相似文献   

18.
Short-term monitoring of individual particulate matter (PM) exposures on subjects and inside residences in health effect studies have been sparse due to the lack of adequate monitoring devices. The recent development of small and portable light scattering devices, including the Radiance nephelometer (neph) and the personal DataRAM (pDR) has made this monitoring possible. This paper evaluates the performance of both the passive pDR and neph (without any size fractionation inlet) against measurements from both Harvard impactors (HI2.5) and Harvard personal environmental monitors (HPEM2.5) for PM2.5 in indoor, outdoor, and personal settings. These measurements were taken at the residences and on the person of nonsmoking elderly subjects across the metropolitan Seattle area and represent a wide range of light scattering measurements directly related to exposures and health effects. At low PM levels, nephs provided finer resolution and more precise measurements (precision = 3-8% and uncertainty = 2.8 x 10(-7) m(-1) or <1 microg/m3) than the pDRs. The unbiased precision of pDRs above 10 microg/m3 is around 5% (with an unbiased uncertainty of 4.4 microg/m3). The 24-h average responses of the pDR and neph, as compared to 24-h integrated gravimetric measurements, are not affected by indoor sources of PM. When regressed against 24-h gravimetric measurements, nephs showed higher coefficients of determination (R2 = 0.81-0.93) than pDRs (R2 = 0.77-0.84). The default mass calibration on the pDRs generally overestimated indoor HI2.5 measurements by 56%. When carried by subjects, the pDR overestimated the HPEM2.5 measurements by approximately 27%. Collocated real-time indoor nephs and pDRs at diverse residential sites had varied coefficients of determination across homes (R2 = 0.75-0.96), and the difference between pDR and neph responses increased during cooking hours. This difference was larger during baking or frying episodes than during other cooking or cleaning activities. Relative humidity, ranging between 25% and 64% indoors in our study, was not a significant factor affecting the differences in neph or pDR response. In summary, for nonsmoking residences, the mass scattering efficiency (m2/g) of a stationary indoor neph on a 24-h basis does not vary by residence, including residences with and without cooking activities. This is also true forthe pDR. These same stationary indoor pDRs and nephs correlate well with each other, even on a 10-min basis, in the absence of indoor source activities. The fact that these activities comprised a relatively small percentage (cooking + cleaning = 2.3%) of the overall sampling time meant that the overall correlation between these two instruments for all time periods was good. However, when examining the cooking and cleaning periods separately, the correlation was not very good. Thus, during these short-term PM episodes, the 24-h average calibrations versus gravimetric mass should be used with caution. Both devices should be potentially useful in future exposure assessment and health effects studies.  相似文献   

19.
Exposure to increased levels of ambient particulate matter (PM) are associated with several health effects, including cardiopulmonary diseases. The formation of reactive oxygen species (ROS) is thought to play an important role in the induction of these health effects. To quantify the ROS generating capacityof PM,we developed an improved electron spin resonance (ESR) spectrometry-based method. ROS formation was measured directly on PM-containing filters, thereby avoiding the selective extraction of components and loss of material or reactivity, which is likely to occur during filter extraction. Also, ascorbic acid was added to stimulate ROS formation. This method was applied to PM10 samples originating from different sources. The radical generating capacity of PM10 from both gasoline and diesel engine exhaust was significantly higher as compared to that of PM10 from ambient or indoor air. Furthermore, in urban PM10 and PM2.5, ROS-generating capacity significantly correlated with concentrations of polycyclic aromatic hydrocarbon content and particular transition metals. This indicates thatthis improved ESR method may be a valuable tool for evaluating the relationship between ROS formation by PM and the adverse health effects associated with this type of air pollution.  相似文献   

20.
Subterranean termites are a major factor in the biodegradation of wood construction products. In this study the efficacy of wood treated with micronized copper, zinc oxide and their mixture was compared to that of wood treated with soluble amine copper oxide against subterranean termites in a laboratory test. All of the formulations tested were effective in controlling wood degradation by the termites, with copper being slightly more effective than zinc and micronized copper being slightly more effective than amine copper.  相似文献   

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