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1.
On November 18, 1997, above-road particulate matter (PM) lidar (light detection and ranging) signals and heavy-duty (HD) and light-duty (LD) vehicle counts were simultaneously collected for 894 10-sec sampling periods at the Caldecott Tunnel in Orinda, CA, for the purpose of measuring the relative contributions of LD and HD vehicles to the PM lidar signal under real-world driving conditions. The relationship between the PM lidar signal and traffic activity (i.e., LD and HD traffic volumes) was examined using a time-series analysis technique, multilagged regression. The time-series model results indicate that the PM lidar signal in the current sampling period (PMt) depended on the level recorded in the previous three sampling periods (i.e., PMt-1, PMt-2, and PMt-3), the number of LD vehicles in the seventh past sampling period (LDt-7), and the number of HD vehicles measured 80 sec previous to the current sampling period (HDt-8). On a 10-sec period basis, the model results indicate that HD vehicles contributed, on average, 3 times more to above-road PM lidar signals than did LD vehicles. The observed lag in the relationship between vehicle types and the lidar signal 20 m above the road suggests that resuspended road dust, rather than tailpipe exhaust emissions, was the main source of the detected PM. Detection of road dust at such heights above the road suggests the need for investigating the processes governing the vertical transport and recycling of PM over the road as a function of vehicle dynamics under a range of meteorological conditions.  相似文献   

2.
ABSTRACT

On November 18, 1997, above-road particulate matter (PM) lidar (light detection and ranging) signals and heavy-duty (HD) and light-duty (LD) vehicle counts were simultaneously collected for 894 10-sec sampling periods at the Caldecott Tunnel in Orinda, CA, for the purpose of measuring the relative contributions of LD and HD vehicles to the PM lidar signal under real-world driving conditions. The relationship between the PM lidar signal and traffic activity (i.e., LD and HD traffic volumes) was examined using a time-series analysis technique, multilagged regression. The time-series model results indicate that the PM lidar signal in the current sampling period (PMt) depended on the level recorded in the previous three sampling periods (i.e., PMt-1, PMt-2, and PMt-3), the number of LD vehicles in the seventh past sampling period (LDt-7), and the number of HD vehicles measured 80 sec previous to the current sampling period (HDt-8). On a 10-sec period basis, the model results indicate that HD vehicles contributed, on average, 3 times more to above-road PM li-dar signals than did LD vehicles. The observed lag in the relationship between vehicle types and the lidar signal 20 m above the road suggests that resuspended road dust, rather than tailpipe exhaust emissions, was the main source of the detected PM. Detection of road dust at such heights above the road suggests the need for investigating the processes governing the vertical transport and recycling of PM over the road as a function of vehicle dynamics under a range of meteorological conditions.  相似文献   

3.
Individuals are exposed to particulate matter from both indoor and outdoor sources. The aim of this study was to compare the relative contributions of three sources of personal exposure to fine particles (PM2.5) by using chemical tracers. The study design incorporated repeated 24-hr personal exposure measurements of air pollution from 28 cardiac-compromised residents of Toronto, Ontario, Canada. Each study participant wore the Rupprecht & Patashnick ChemPass Personal Sampling System 1 day a week for a maximum of 10 weeks. During their individual exposure measurement days the subjects reported to have spent an average of 89% of their time indoors. Particle phase elemental carbon, sulfate, and calcium personal exposure data were used in a mixed-effects model as tracers for outdoor PM2.5 from traffic-related combustion, regional, and local crustal materials, respectively. These three sources were found to contribute 13% +/- 10%, 17% +/- 16%, and 7% +/- 6% of PM2.5 exposures. The remaining fraction of the personal PM2.5 is hypothesized to be predominantly related to indoor sources. For comparison, central site outdoor PM2.5 measurements for the same dates as personal measurements were used to construct a receptor model using the same three tracers. In this case, traffic-related combustion, regional, and local crustal materials were found to contribute 19% +/- 17%, 52% +/- 22%, and 10% +/- 7%, respectively. Our results indicate that the three outdoor PM2.5 sources considered are statistically significant contributors to personal exposure to PM2.5. Our results also suggest that among the Toronto subjects, who spent a considerable amount of time indoors, exposure to outdoor PM2.5 includes a greater relative contribution from combustion sources compared with outdoor PM2.5 measurements where regional sources are the dominant contributor.  相似文献   

4.
5.
The objective of this project is to demonstrate how the ambient air measurement record can be used to define the relationship between O3 (as a surrogate for photochemistry) and secondary particulate matter (PM) in urban air. The approach used is to develop a time-series transfer-function model describing the daily PM10 (PM with less than 10 microm aerodynamic diameter) concentration as a function of lagged PM and current and lagged O3, NO or NO2, CO, and SO2. Approximately 3 years of daily average PM10, daily maximum 8-hr average O3 and CO, daily 24-hr average SO2 and NO2, and daily 6:00 a.m.-9:00 a.m. average NO from the Aerometric Information Retrieval System (AIRS) air quality subsystem are used for this analysis. Urban areas modeled are Chicago, IL; Los Angeles, CA; Phoenix, AZ; Philadelphia, PA; Sacramento, CA; and Detroit, MI. Time-series analysis identified significant autocorrelation in the O3, PM10, NO, NO2, CO, and SO2 series. Cross correlations between PM10 (dependent variable) and gaseous pollutants (independent variables) show that all of the gases are significantly correlated with PM10 and that O3 is also significantly correlated lagged up to two previous days. Once a transfer-function model of current PM10 is defined for an urban location, the effect of an O3-control strategy on PM concentrations is estimated by calculating daily PM10 concentrations with reduced O3 concentrations. Forecasted summertime PM10 reductions resulting from a 5 percent decrease in ambient O3 range from 1.2 microg/m3 (3.03%) in Chicago to 3.9 microg/m3 (7.65%) in Phoenix.  相似文献   

6.
Environmental epidemiology and more specifically time-series analysis have traditionally used area-averaged pollutant concentrations measured at central monitors as exposure surrogates to associate health outcomes with air pollution. However, spatial aggregation has been shown to contribute to the overall bias in the estimation of the exposure-response functions. This paper presents the benefit of adding features of the spatial variability of exposure by using concentration fields modeled with a chemistry transport model instead of monitor data and accounting for human activity patterns. On the basis of county-level census data for the city of Paris, France, and a Monte Carlo simulation, a simple activity model was developed accounting for the temporal variability between working and evening hours as well as during transit. By combining activity data with modeled concentrations, the downtown, suburban, and rural spatial patterns in exposure to nitrogen dioxide, ozone, and PM2.5 (particulate matter [PM] < or = 10 microm in aerodynamic diameter) were captured and parametrized. Exposures predicted with this model were used in a time-series study of the short-term effect of air pollution on total nonaccidental mortality for the 4-yr period from 2001 to 2004. It was shown that the time series of the exposure surrogates developed here are less correlated across co-pollutants than in the case of the area-averaged monitor data. This led to less biased exposure-response functions when all three co-pollutants were inserted simultaneously in the same regression model. This finding yields insight into pollutant-specific health effects that are otherwise masked by the high correlation among co-pollutants.  相似文献   

7.
Statistical analyses of time-series or spatial data have been widely used to investigate the behavior of ambient air pollutants. Because air pollution data are generally collected in a wide area of interest over a relatively long period, such analyses should take into account both spatial and temporal characteristics. The objective of this study is 2-fold: (1) to identify an efficient way to characterize the spatial variations of fine particulate matter (PM2.5) concentrations based solely upon their temporal patterns, and (2) to analyze the temporal and seasonal patterns of PM2.5 concentrations in spatially homogenous regions. This study used 24-hr average PM2.5 concentrations measured every third day during a period between 2001 and 2005 at 522 monitoring sites in the continental United States. A k-means clustering algorithm using the correlation distance was used to investigate the similarity in patterns between temporal profiles observed at the monitoring sites. A k-means clustering analysis produced six clusters of sites with distinct temporal patterns that were able to identify and characterize spatially homogeneous regions of the United States. The study also presents a rotated principal component analysis (RPCA) that has been used for characterizing spatial patterns of air pollution and discusses the difference between the clustering algorithm and RPCA.  相似文献   

8.
The influence of sea-land breezes (SLBs) on the spatial distribution and temporal variation of particulate matter (PM) in the atmosphere was investigated over coastal Taiwan. PM was simultaneously sampled at inland and offshore locations during three intensive sampling periods. The intensive PM sampling protocol was continuously conducted over a 48-hr period. During this time, PM2.5 and PM(2.5-10) (PM with aerodynamic diameters < 2.5 microm and between 2.5 and 10 microm, respectively) were simultaneously measured with dichotomous samplers at four sites (two inland and two offshore sites) and PM10 (PM with aerodynamic diameters < or =10 microm) was measured with beta-ray monitors at these same 4 sites and at 10 sites of the Taiwan Air Quality Monitoring Network. PM sampling on a mobile air quality monitoring boat was further conducted along the coastline to collect offshore PM using a beta-ray monitor and a dichotomous sampler. Data obtained from the inland sites (n=12) and offshore sites (n=2) were applied to plot the PM10 concentration contour using Surfer software. This study also used a three-dimensional meteorological model (Pennsylvania State University/National Center for Atmospheric Research Meteorological Model 5) and the Comprehensive Air Quality Model with Extensions to simulate surface wind fields and spatial distribution of PM10 over the coastal region during the intensive sampling periods. Spatial distribution of PM10 concentration was further used in investigating the influence of SLBs on the transport of PM10 over the coastal region. Field measurement and model simulation results showed that PM10 was transported back and forth across the coastline. In particular, a high PM10 concentration was observed at the inland sites during the day because of sea breezes, whereas a high PM10 concentration was detected offshore at night because of land breezes. This study revealed that the accumulation of PM in the near-ocean region because of SLBs influenced the tempospatial distribution of PM10 over the coastal region.  相似文献   

9.
Improving knowledge on the apportionment of airborne particulate matter will be useful to handle and fulfill the legislation regarding this pollutant. The main aim of this work was to assess the influence of markers in the source apportionment of airborne PM10, in particular, whether the use of particle polycyclic aromatic hydrocarbon (PAH) and ions provided similar results to the ones obtained using not only the mentioned markers but also gas phase PAH and trace elements. In order to reach this aim, two receptor models: UNMIX and positive matrix factorization were applied to two sets of data in Zaragoza city from airborne PM10, a previously reported campaign (2003–2004) (Callén et al. Chemosphere 76:1120-1129, 2009), where PAH associated to the gas and particle phases, ions and trace elements were used as markers and a long sampling campaign (2001–2009), where only PAH in the particle phase and ions were analyzed. For both campaigns, positive matrix factorization was able to explain a higher number of sources than the UNMIX model. Independently of the sampling campaign and the receptor model used, soil resuspension was the main PM10 source, especially in the warm period (21st March–21st September), where most of the PM10 exceedances were produced. Despite some of the markers of anthropogenic sources were different for both campaigns, common sources associated to different combustion sources (coal, light-oil, heavier-oil, biomass, and traffic) were found and PAH in particle phase and ions seemed to be good markers for the airborne PM10 apportionment.  相似文献   

10.
To investigate the chemical characteristics of fine particles in the Sihwa area, Korea, atmospheric aerosol samples were collected using a dichotomous PM10 sampler and two URG PM2.5 cyclone samplers during five intensive sampling periods between February 1998 and February 1999. The Inductively Coupled Plasma (ICP)-Atomic Emission Spectrometry (AES)/ICP-Mass Spectrometry (MS), ion chromatograph (IC), and thermal manganese dioxide oxidation (TMO) methods were used to analyze the trace elements, ionic species, and carbonaceous species, respectively. Backward trajectory analysis, factor analysis, and a chemical mass balance (CMB) model were used to estimate quantitatively source contributions to PM2.5 particles collected in the Sihwa area. The results of PM2.5 source apportionment using the CMB7 receptor model showed that (NH4)2SO4 was, on average, the major contributor to PM2.5 particles, followed by nontraffic organic carbon (OC) emission, NH4NO3, agricultural waste burning, motor vehicle emission, road dust, waste incineration, marine aerosol, and others. Here, the nontraffic OC sources include primary anthropogenic OC emitted from the industrial complex zone, secondary OC, and organic species from distant sources. The source impact of waste incineration emission became significant when the dominant wind directions were from southwest and west sectors during the sampling periods. It was found that PM2.5 particles in the Sihwa area were influenced mainly by both anthropogenic local sources and long-range transport and transformation of air pollutants.  相似文献   

11.
12.
The time-series correlation between ambient levels, indoor levels, and personal exposure to PM2.5 was assessed in panels of elderly subjects with cardiovascular disease in Amsterdam, the Netherlands, and Helsinki, Finland. Subjects were followed for 6 months with biweekly clinical visits. Each subject's indoor and personal exposure to PM2.5 was measured biweekly, during the 24-hr period preceding the clinical visits. Outdoor PM2.5 concentrations were measured at fixed sites. The absorption coefficients of all PM2.5 filters were measured as a marker for elemental carbon (EC). Regression analyses were conducted for each subject separately, and the distribution of the individual regression and correlation coefficients was investigated. Personal, indoor, and ambient concentrations were highly correlated within subjects over time. Median Pearson's R between personal and outdoor PM2.5 was 0.79 in Amsterdam and 0.76 in Helsinki. For absorption, these values were 0.93 and 0.81 for Amsterdam and Helsinki, respectively. The findings of this study provide further support for using fixed-site measurements as a measure of exposure to PM2.5 in epidemiological time-series studies.  相似文献   

13.
Source apportionment with site specific source profiles   总被引:1,自引:0,他引:1  
A receptor modeling study was performed to identify and apportion the sources of PM10 mass in Granite City, Illinois, an area of historic TSP nonattainment. Samples of the ambient aerosol were collected using a dichotomous sampler. Each sample was analyzed by x-ray fluorescence and instrumental neutron activation analysis. To begin the study, a factor analysis was performed. Two different chemical mass balance (CMB) analyses were then made. The first CMB analysis used only source profiles available from the literature while the second included twelve source profiles developed from dust samples collected in Granite City. Both CMB analyses used 20 of the 33 analyzed elements since many of the source profiles in the literature did not include the other thirteen elements. The results from both sets of CMB analyses were grouped by the predominate wind direction at the site during the time each sample was taken to identify the direction of each source relative to the sampler. It was found that regional sources were the primary contributors to the fine fraction while the coarse fraction was composed of material from local industries. These sources were generally the ones identified during the Regional Air Pollution Study previously conducted in the area. However, the emission profiles from these sources were observed to have changed between the studies. It was also found that the use of the locally generated profiles greatly improved the results of the CMB analysis.  相似文献   

14.
Version 4.10s of the comprehensive air-quality model with extensions (CAMx) photochemical grid model has been developed, which includes two options for representing particulate matter (PM) size distribution: (1) a two-section representation that consists of fine (PM2.5) and coarse (PM2.5-10) modes that has no interactions between the sections and assumes all of the secondary PM is fine; and (2) a multisectional representation that divides the PM size distribution into N sections (e.g., N = 10) and simulates the mass transfer between sections because of coagulation, accumulation, evaporation, and other processes. The model was applied to Southern California using the two-section and multisection representation of PM size distribution, and we found that allowing secondary PM to grow into the coarse mode had a substantial effect on PM concentration estimates. CAMx was then applied to the Western United States for the 1996 annual period with a 36-km grid resolution using both the two-section and multisection PM representation. The Community Multiscale Air Quality (CMAQ) and Regional Modeling for Aerosol and Deposition (REMSAD) models were also applied to the 1996 annual period. Similar model performance was exhibited by the four models across the Interagency Monitoring of Protected Visual Environments (IMPROVE) and Clean Air Status and Trends Network monitoring networks. All four of the models exhibited fairly low annual bias for secondary PM sulfate and nitrate but with a winter overestimation and summer underestimation bias. The CAMx multisectional model estimated that coarse mode secondary sulfate and nitrate typically contribute <10% of the total sulfate and nitrate when averaged across the more rural IMPROVE monitoring network.  相似文献   

15.
Source identification of atlanta aerosol by positive matrix factorization   总被引:3,自引:0,他引:3  
Data characterizing daily integrated particulate matter (PM) samples collected at the Jefferson Street monitoring site in Atlanta, GA, were analyzed through the application of a bilinear positive matrix factorization (PMF) model. A total of 662 samples and 26 variables were used for fine particle (particles < or = 2.5 microm in aerodynamic diameter) samples (PM2.5), and 685 samples and 15 variables were used for coarse particle (particles between 2.5 and 10 microm in aerodynamic diameter) samples (PM10-2.5). Measured PM mass concentrations and compositional data were used as independent variables. To obtain the quantitative contributions for each source, the factors were normalized using PMF-apportioned mass concentrations. For fine particle data, eight sources were identified: SO4(2-) -rich secondary aerosol (56%), motor vehicle (22%), wood smoke (11%), NO(3-) -rich secondary aerosol (7%), mixed source of cement kiln and organic carbon (OC) (2%), airborne soil (1%), metal recycling facility (0.5%), and mixed source of bus station and metal processing (0.3%). The SO4(2-) -rich and NO(3-) -rich secondary aerosols were associated with NH(4+). The SO4(2-) -rich secondary aerosols also included OC. For the coarse particle data, five sources contributed to the observed mass: airborne soil (60%), NO(3-)-rich secondary aerosol (16%), SO4(2-) -rich secondary aerosol (12%), cement kiln (11%), and metal recycling facility (1%). Conditional probability functions were computed using surface wind data and identified mass contributions from each source. The results of this analysis agreed well with the locations of known local point sources.  相似文献   

16.
Fine particulate matter (PM2.5) concentrations associated with 202 24-hr samples collected at the National Energy Technology Laboratory (NETL) particulate matter (PM) characterization site in south Pittsburgh from October 1999 through September 2001 were used to apportion PM2.5 into primary and secondary contributions using Positive Matrix Factorization (PMF2). Input included the concentrations of PM2.5 mass determined with a Federal Reference Method (FRM) sampler, semi-volatile PM2.5 organic material, elemental carbon (EC), and trace element components of PM2.5. A total of 11 factors were identified. The results of potential source contributions function (PSCF) analysis using PMF2 factors and HYSPLIT-calculated back-trajectories were used to identify those factors associated with specific meteorological transport conditions. The 11 factors were identified as being associated with emissions from various specific regions and facilities including crustal material, gasoline combustion, diesel combustion, and three nearby sources high in trace metals. Three sources associated with transport from coal-fired power plants to the southeast, a combination of point sources to the northwest, and a steel mill and associated sources to the west were identified. In addition, two secondary-material-dominated sources were identified, one was associated with secondary products of local emissions and one was dominated by secondary ammonium sulfate transported to the NETL site from the west and southwest. Of these 11 factors, the four largest contributors to PM2.5 were the secondary transported material (dominated by ammonium sulfate) (47%), local secondary material (19%), diesel combustion emissions (10%), and gasoline combustion emissions (8%). The other seven factors accounted for the remaining 16% of the PM2.5 mass. The findings are consistent with the major source of PM2.5 in the Pittsburgh area being dominated by ammonium sulfate from distant transport and so decoupled from local activity emitting organic pollutants in the metropolitan area. In contrast, the major local secondary sources are dominated by organic material.  相似文献   

17.
The lognormal, Weibull, and type V Pearson distributions were selected to fit the concentration frequency distributions of particulate matter with an aerodynamic diameter of < or = 10 microm (PM10) and SO2 in the Taiwan area. Air quality data from three stations, Hsin-Chu, Shalu, and Gain-Jin, were fitted with three distributions and compared with the measured data. The parameters of unimodal and bimodal fitted distributions were obtained by the methods of maximum likelihood and nonlinear least squares, respectively. Moreover, the root mean square error (RMSE), index of agreement (d), and Kolmogorov-Smirnov (K-S) test were used as criteria to judge the goodness-of-fit of these three distributions. These results show that the frequency distributions of PM10 concentration at the Hsin-Chu and Shalu stations are unimodal, but the distribution at Gain-Jin is bimodal. The distribution type of PM10 concentration varied greatly in different areas and could be influenced by local meteorological conditions. For SO2 concentration distribution, the distributions were all unimodal. The results also show that the lognormal distribution is the more appropriate to represent the PM10 distribution, while the Weibull and lognormal distributions are more suitable to represent the SO2 distribution. Moreover, the days exceeding the air quality standard (AQS) (PM10 > 125 microg/ m3) for the Hsin-Chu, Shalu, and Gain-Jin stations in the coming year are successfully predicted by the theoretic distributions.  相似文献   

18.
Data from the U.S. Environmental Protection Agency's Aerometric Information Retrieval System (now known as the Air Quality System) database for 1999 and 2000 have been used to characterize the spatial variability of concentrations of particulate matter with aerodynamic diameter < or = 2.5 microg (PM2.5) in 27 urban areas across the United States. Different measures were used to quantify the degree of uniformity of PM2.5 concentrations in the urban areas characterized. It was observed that PM2.5 concentrations varied to differing degrees in the urban areas examined. Analyses of several urban areas in the Southeast indicated high correlations between site pairs and spatial uniformity in concentration fields. Considerable spatial variation was found in other regions, especially in the West. Even within urban areas in which all site pairs were highly correlated, a variable degree of heterogeneity in PM2.5 concentrations was found. Thus, even though concentrations at pairs of sites were highly correlated, their concentrations were not necessarily the same. These findings indicate that the potential for exposure misclassification errors in time-series epidemiologic studies exists.  相似文献   

19.
The origin of the daily exceedances of 50 μg PM10 m−3 (daily limit value or DLV of the EU air quality directive) and of an arbitrary daily value (DV) 35 μg PM2.5 m−3 recorded in 2001–2003 in 13 regional background stations of the Iberian Peninsula were interpreted. This was carried out by means of back-trajectory analysis, available PM model outputs, satellite data and meteorological maps. This allows the detection of high PM episodes on a regional scale and the study of their seasonal and geographical variability.The number of exceedances of the PM10 DLV ranged in 2001–2003 from 6 to 41 depending on the monitoring site. For the selected PM2.5 DV, the range of daily exceedances was 0–10 in the study period.The majority of the PM10 (>70% in most stations) and PM2.5 (17–55% in most stations) exceedances in regional background monitoring stations are caused by African dust outbreaks. These exceedances were less frequent in winter than in summer due to: (a) the frequent long range transport of dust in the warm seasons over Iberia, (b) the re-suspension associated with convective atmospheric dynamics, and (c) the relative low rainfall favouring re-suspension and high residence time of PM. Moreover, a regional contribution of secondary aerosols derived from the efficient photochemical transformation of gaseous precursors may coincide with African transport in summer.Episodes with lack of advective conditions caused 2–29% and 20–50% of the PM10 and PM2.5 exceedances. These occurred mainly in summer due to poor renovation of air masses, increased convective re-suspension, dispersion of pollutants towards rural areas and regional re-circulation and aging of air masses which result in the proliferation of secondary inorganic species.Long-range transport of PM from continental Europe caused exceedances (9–40% and 18–38% of the PM10 and PM2.5 exceedances, respectively), only in northern Iberia because, as the European air masses evolve towards the south, the pollutants suffer dispersion/dilution. Local exceedances are associated with the advection of the clean Atlantic air masses, which cannot increase PM levels to a great extent without the influence of a local source of PM. The proportion of local exceedances of PM10 and PM2.5 ranged 6–33% and 17–40%, respectively.  相似文献   

20.
In this work, the effect of meteorological parameters and local topography on mass concentrations of fine (PM2.5) and coarse (PM2.5-10) particles and their seasonal behavior was investigated. A total of 236 pairs of samplers were collected using an Anderson Dichotomous sampler between December 2004 and October 2005. The average mass concentrations of PM2.5, PM2.5-10, and particulate matter less than 10 microm in aerodynamic diameter (PM10) were found to be 29.38, 23.85, and 53.23 microg/m3, respectively. The concentrations of PM2.5 and PM10 were found to be higher in heating seasons (December to May) than in summer. The increase of relative humidity, cloudiness, and lower temperature was found to be highly related to the increase of particulate matter (PM) episodic events. During non-rainy days, the episodic events for PM2.5 and PM10 were increased by 30 and 10.7%, respectively. This is a result of the extensive use of fuel during winter for heating purposes and also because of stagnant air masses formed because of low temperature and low wind speed over the study area.  相似文献   

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