共查询到20条相似文献,搜索用时 15 毫秒
1.
UNMIX and Positive Matrix Factorization (PMF) solutions to the Chemical Mass Balance (CMB) equations were applied to chemically speciated PM2.5 measurements from 23 sites in California's San Joaquin Valley to estimate source contributions. Six and seven factors were determined by UNMIX for the low_PM2.5 period (February to October) and high_PM2.5 period (November to January), respectively. PMF resolved eightfactors for each period that corresponded with the UNMIX factors in chemical profiles and time series. These factors are attributed to marine sea salt, fugitive dust, agriculture-dairy, cooking, secondary aerosol, motor vehicle, and residential wood combustion (RWC) emissions, with secondary aerosol and RWC accounting for over 70% of PM2.5 mass during the high_PM2.5 period. A zinc factor was only resolved by PMF. The contribution from motor vehicles was between 10 and 25% with higher percentages occurring in summer. The PMF model was further evaluated by examining (1) site-specific residuals between the measured and calculated concentrations, (2) comparability of motor vehicle and RWC factors against source profiles obtained from recent emission tests, (3) edges in bi-plots of key indicator species, and (4) spatiotemporal variations of the factors' strengths. These evaluations support the compliance with model assumptions and give a higher confidence level to source apportionment results for the high_PM2.5 period. 相似文献
2.
The formation of secondary ammonium nitrate during the 1995 Integrated Monitoring Study (IMS95) in San Joaquin Valley, CA was investigated using a box model that simulates the atmospheric chemistry and gas/particle partition of inorganic compounds. The concentration of particulate matter (PM) nitrate was found to be sensitive to reductions in VOC emissions. Nitric acid, rather than ammonia, was the limiting reagent in the formation of PM nitrate. The formation of nitric acid was more sensitive to the availability of oxidants than that of NOx. Oxidant chemistry in wintertime conditions in the San Joaquin Valley was shown to be VOC-sensitive. In fact, a decrease in NOx emissions may have the counter-intuitive effect of increasing PM nitrate. 相似文献
3.
Positive matrix factorization (PMF) was applied to synthetic datasets that simulate personal exposures to airborne PM2.5 from 12 sources. Three differentfilter analysis scenarios using different analytical chemistry techniques were considered. The full suite scenario quantified elemental carbon, organic carbon, inorganic ions, trace elements, and trace organic species including carboxylic acids and organic compounds with -OH functionality. A second scenario excluded trace elements and a third assumed that derivatization steps to quantify polar organic compounds were not performed. Similar errors in source apportionment were seen with all three scenarios. In most cases, PMF failed to separate out factors corresponding to road dust and vegetative debris, two sources that made relatively uniform contributions to the synthetic exposures. Factors representing wood smoke, natural gas combustion, and meat cooking sources were difficult to identify due to a lack of unique tracers with concentrations reliably above the detection limits assumed in the study. Factors representing cigarette smoke, candle smoke, gasoline exhaust, and secondary aerosols were comparatively easy to identify. When contributions from a pair of sources, such as diesel and gasoline exhaust, were highly correlated in the synthetic datasets, a single factor corresponding to both sources was usually found. 相似文献
4.
Gillies JA Gertler AW Sagebiel JC Dippel WA 《Environmental science & technology》2001,35(6):1054-1063
Total and speciated particulate matter (PM2.5 and PM10) emission factors from in-use vehicles were measured for a mixed light- (97.4% LD) and heavy-duty fleet (2.6% HD) in the Sepulveda Tunnel, Los Angeles, CA. Seventeen 1-h test runs were performed between July 23, 1996, and July 27, 1996. Emission factors were calculated from mass concentration measurements taken at the tunnel entrance and exit, the volume of airflow through the tunnel, and the number of vehicles passing through the 582 m long tunnel. For the mixed LD and HD fleet, PM2.5 emission factors in the Sepulveda Tunnel ranged from 0.016 (+/-0.007) to 0.115 (+/-0.019) g/vehicle-km traveled with an average of 0.052 (+/-0.027) g/vehicle.km. PM10 emission factors ranged from 0.030 (+/-0.009) to 0.131 (+/-0.024) g/vehicle. km with an average of 0.069 (+/-0.030) g/vehicle.km. The PM2.5 emission factor was approximately 74% of the PM10 factor. Speciated emission rates and chemical profiles for use in receptor modeling were also developed. PM2.5 was dominated by organic carbon (OC) (31.0 +/- 19.5%) and elemental carbon (EC) (48.5 +/- 20.5%) that together account for 79% (+/-24%) of the total emissions. Crustal elements (Fe, Mg, Al, Si, Ca, and Mn) contribute approximately 7.8%, and the ions Cl-, NO3-, NH3+, SO4(2-), and K+ together constitute another 9.8%. In the PM10 size fraction the particulate emissions were also dominated by OC (31 +/- 12%) and EC (35 +/- 13%). The third most prominent species was Fe (18.5 +/- 9.0%), which is greater than would be expected from purely geological sources. Other geological components (Mg, Al, Si, K, Ca, and Mn) accounted for an additional 12.6%. PM10 emission factors showed some dependence on vehicle speed, whereas PM2.5 did not. For test runs in which the average vehicle speed was 42.6 km/h a 1.7 times increase in PM10 emission factor was observed compared to those runs with an average vehicle speed of 72.6 km/h. Speciated emissions were similar. However, there is significantly greater mass attributable to geological material in the PM10, indicative of an increased contribution from resuspended road dust. The PM2.5 shows relatively good correlation with NOx emissions, which indicates that even at the low percent of HD vehicles, which emit significantly more NOx than LD vehicles, they may also have a significant impact on the PM2.5 levels. 相似文献
5.
Gotschi T Oglesby L Mathys P Monn C Manalis N Koistinen K Jantunen M Hanninen O Polanska L Kunzli N 《Environmental science & technology》2002,36(6):1191-1197
Recent studies on separated particle-size fractions highlight the health significance of particulate matter smaller than 2.5 microm (PM2.5), but gravimetric methods do not identify specific particle sources. Diesel exhaust particles (DEP) contain elemental carbon (EC), the dominant light-absorbing substance in the atmosphere. Black smoke (BS) is a measure for light absorption of PM and, thus, an alternative way to estimating EC concentrations, which may serve as a proxy for diesel exhaust emissions. We analyzed PM2.5 and BS data collected within the EXPOLIS study (Air Pollution Exposure Distribution within Adult Urban Populations in Europe) in Athens, Basel, Helsinki, and Prague. 186 indoor/outdoor filter pairs were sampled and analyzed. PM2.5 and BS levels were lowest in Helsinki, moderate in Basel, and remarkably higher in Athens and Prague. In each city, Spearman correlation coefficients of indoor versus outdoor were higher for BS (range rspearman: 0.57-0.86) than for PM2.5 (0.05-0.69). In a BS linear regression model (all data), outdoor levels explained clearly more of indoor variation (86%) than in the corresponding PM2.5 model (59%). In conclusion, ambient BS seizes a health-relevant fraction of fine particles to which people are exposed indoors and outdoors and exposure to which can be assessed by monitoring outdoor concentrations. BS measured on PM2.5 filters can be recommended as a valid and cheap additional indicator in studies on combustion-related air pollution and health. 相似文献
6.
Some nitrogen-containing organic compounds (NOCs) in PM2.5 aerosols in forest, tunnel, urban, rural, and mixed forest/ urban areas in the Lower Fraser Valley (LFV), British Columbia, Canada, were measured to assess their chemical characteristics, temporal and spatial distributions, and origins. The levels of E-caprolactam, isoindole-1,3-dione, benzothiazolone, and N-butyl-benzensulfonamide showed significant differences among the sites, with the highest level at the mixed forest/urban site, indicating that aerosols at this site were impacted by chemical manufacturing activities. N,N-diethyl-m-toluamide (deet) was detected at all locations but was highest in the forest area, demonstrating a widespread usage as an insect repellent in the LFV and at camps at the forest site. Alkyl amides, tracers from wood burning and cooking, ranging from C6 to C20 including two unsaturated amides, hexadecenamide, and 9-octa-decenamide, were detected at all sites. Three patterns of carbon number distributions of alkyl amides varied with location and time, and were mainly impacted by biomass burning or cooking compared to levoglucosan and cholesterol in the LFV. Ratio of oleamide to stearamide (C18:1/C18:0) was discussed as a potential indicator for determining "age" or transport range of biomass combustion plumes. 相似文献
7.
McKone TE Castorina R Harnly ME Kuwabara Y Eskenazi B Bradman A 《Environmental science & technology》2007,41(9):3233-3240
We characterize cumulative intakes of organophosphorus (OP) pesticides in an agricultural region of California by drawing on human biomonitoring data, California pesticide use reporting (PUR) data, and limited environmental samples together with outputs from the CalTOX multimedia, multipathway, source-to-dose model. The study population is the CHAMACOS cohort of almost 600 pregnant Latina women in the Salinas Valley region. We use model estimates of OP intake and urinary dialkylphosphate (DAP) metabolite excretion to develop premises about relative contributions from different exposure sources and pathways. We evaluate these premises by comparing the magnitude and variation of DAPs in the CHAMACOS cohort with those of the whole U.S. population using data from the National Health and Nutrition Examination Survey (NHANES). This comparison supports the premise that diet is the common and dominant exposure pathway in both populations. Biomarker comparisons and model results support the observation that, relative to NHANES, the CHAMACOS population has a statistically significant (p < 0.001) added intake of OP pesticides with low inter-individual variability. We attribute the magnitude and small variance of this intake to residential nondietary exposures from local agricultural OP uses. These results show that mass-balance models can estimate exposures for OP pesticides within the range measured by biological monitoring. 相似文献
8.
A study of personal, indoor, and outdoor exposure to PM2.5 and associated elements has been carried out for 37 residents of the Research Triangle Park area in North Carolina. Participants were selected from persons expected to be at elevated risk from exposure to particles, and included 29 persons with hypertension and 8 cardiac patients with implanted defibrillators. Participants were monitored for 7 consecutive days in each of four seasons. One goal of the study was to estimate the contribution of outdoor PM2.5 to indoor concentrations. This depends on the infiltration factor Finf, the fraction of outdoor PM2.5 remaining airborne after penetrating indoors. After confirming with our measurements the findings of previous studies that sulfur has few indoor sources, we estimated an average Finf for each house based on indoor/outdoor sulfur ratios. These estimates ranged from 0.26 to 0.87, with a median value of 0.55. Since these estimates apply only to particles of size similar to that of sulfur particles (0.06-0.5 microm diameter), and since larger particles (0.5-2.5 microm) have lower penetration rates and higher deposition rates, these estimates are likely to be higher than the true infiltration factors for PM2.5 as a whole. In summer when air conditioners were in use, the sulfur-based infiltration factor was at its lowest (averaging 0.50) for most homes, whereas the average Finf for the other three seasons was 0.62-0.63. Using the daily estimated infiltration factor for each house, we calculated the contribution of outdoor PM2.5 to indoor air concentrations. The indoor-generated contributions to indoor PM2.5 had a wider range (0-33 microg/m3) than the outdoor contributions (5-22 microg/m3). However, outdoor contributions exceeded the indoor-generated contributions in 27 of 36 homes. A second goal of the study was to determine the contribution of outdoor particles to personal exposure. This is determined by the "outdoor exposure factor" Fpex, the fraction of outdoor PM2.5 contributing to personal exposure. As with Finf, we estimated Fpex by the personal/outdoor sulfur ratios. The estimates ranged from 0.33 to 0.77 with a median value of 0.53. Outdoor air particles were less important for personal exposures than for indoor concentrations, with the median outdoor contribution to personal exposure just 49%. We regressed the outdoor contributions to personal exposures on measured outdoor PM2.5 at the central site. The regressions had R2 values ranging from 0.19 to 0.88 (median = 0.73). These values provide an indication of the extent of misclassification error in epidemiological estimates of the effect of outdoor particles on health. 相似文献
9.
Technical note: Contribution of ammonia emitted from livestock to atmospheric fine particulate matter (PM2.5) in the United States 总被引:1,自引:0,他引:1
Hristov AN 《Journal of dairy science》2011,94(6):3130-3136
Ammonia emitted from animal feeding operations is an air pollutant contributing to the formation of fine particulate matter (PM2.5), considered a major environmental risk to human health. In the United States, farm animals are the greatest contributor to gaseous ammonia emissions. Ammonia reacts with atmospheric nitric and sulfuric acids to form PM2.5 (nitrate and sulfate), but the proportion of PM2.5 attributable to ammonia emitted from animal farming operations has not been quantified. Thus, the objective of this analysis was to estimate the contribution of ammonia emitted from farm animals to PM2.5 in the United States. The following approach was used: (1) the amount of ammonium in sulfate and nitrate PM2.5 was calculated based on chemically speciated measurements published by the United States Environmental Protection Agency; and (2) the amount of ammonium in sulfate and nitrate PM2.5 originating from livestock was assumed equal to the fraction of the total ammonia emissions attributable to livestock. Across different regions of the United States and under different weather conditions, PM2.5 formed from ammonia emitted from livestock operations were estimated to contribute on average from 5 to 11% of the total PM2.5 concentrations. In certain areas (North Central, for example) and in cool weather, farm animal contribution to atmospheric PM2.5 concentration may be as much as 20%. 相似文献
10.
Lee PK Brook JR Dabek-Zlotorzynska E Mabury SA 《Environmental science & technology》2003,37(21):4831-4840
The chemical composition of Toronto PM2.5 was measured daily from Feb 2000 to Feb 2001, and source apportionment was undertaken using positive matrix factorization (PMF). In Toronto, PM2.5 levels were influenced both by local urban activities and also by regional-scale transport. Although several PMF solutions were possible, an eight-source model for explaining the observed Toronto PM2.5 was found to provide realistic results and interesting insights into sources. The four main sources were coal combustion related to regional transport and secondary sulfate (26%), secondary nitrate related to both local and upwind sources of NOx and NH3 (36%), secondary organic aerosols (SOA) formed from a variety of precursor organic emissions (15%), and motor vehicle traffic (10%). The other detectable sources were road salt (winter) and three types of primary PM2.5 hypothesized to be associated with smelters, coal and oil combustion, industry, and local construction. Overall, motor vehicle-related emissions (including road salt and nitrate) were estimated to be responsible for about 40% of the PM2.5. In the summer, the SOA mass was estimated to contribute approximately 20% to the PM2.5. Inclusion of water-soluble, low-molecular-weight organic acids led to identification of this component, thus providing a significant improvement in PMF's ability to resolve sources. Without organic acid measurements the SOA portion of the observed PM2.5 was assigned to the secondary coal component, increasing its contribution and resulting in a source profile with an unrealistic amount of organic mass. This suggests that in the northeastern part of North America, there are physical and/or chemical processes that lead to close interaction between secondary organic and inorganic aerosols. 相似文献
11.
12.
Watershed sources of disinfection byproduct precursors in the Sacramento and San Joaquin Rivers, California 总被引:2,自引:0,他引:2
High levels of dissolved organic carbon (DOC) and bromide (Br) in the Sacramento and San Joaquin River waterways are of concern because DOC and Br are organic and inorganic precursors, respectively, of carcinogenic and mutagenic disinfection byproducts (DBPs). The Sacramento and San Joaquin Rivers are the two major rivers supplying water to the San Francisco Bay Delta, but sources and loads of DBP precursors into the Delta are still uncertain. The major objectives of this study were to evaluate both the quantity (DOC and Br fluxes) and the quality (reactivity in forming DBPs) of DBP precursors from the Sacramento and San Joaquin watersheds. Water samples were collected every 2 weeks at up to 35 locations along the Sacramento and San Joaquin Rivers and selected tributaries and analyzed for DOC (4 years), Br (1 year), and ultraviolet absorbance at 254 nm (1 year). Selected water samples were also tested for THM formation potential. Estimated fluxes for the Sacramento River were 39 000 +/- 12 000 Mg DOC year(-1) and 59 Mg of Br year(-1) as compared to 9000 +/- 5000 Mg of DOC year(-1) and 1302 Mg of Br year(-1) for the San Joaquin River. The THM formation potential was higher in the San Joaquin River (441 +/- 49 microg L(-1)) than the Sacramento River (176 +/- 20 microg L(-1)) because of higher concentrations of both organic (DOC = 3.62 +/- 0.14 vs 1.92 +/- 0.09 mg L(-1)) and inorganic DBP (Br = 0.80 +/- 0.07 vs < 0.03 +/- 0.01 mg L(-1)) precursors. The Sacramento River's greater DOC load despite lower DOC concentrations is due to its discharge being about 5 times greater than the San Joaquin River (50 x 10(9) vs 10 x 10(9) L day(-1)). The DOC concentration was significantly correlated with several land-cover types, including agriculture; however, no relationship was found between DOC quality and land-cover at the watershed scale. 相似文献
13.
Yli-Tuomi T Lanki T Hoek G Brunekreef B Pekkanen J 《Environmental science & technology》2008,42(12):4440-4446
Daily PM2.5 samples were repeatedly collected (1-8 times) in the homes of elderly nonsmoking individuals with coronary heart disease in Amsterdam, The Netherlands (33 individuals) and Helsinki, Finland (44 individuals). Sources of indoor PM2.5 were evaluated using a two-way multilinear engine model. Because the indoor elemental data lacked a traffic marker, separation of traffic related PM was attempted by combining the indoor data with fixed site outdoor data that also contained NO. Six outdoor sources, including long-range transport (LRT), urban mixture, oil combustion, traffic, sea-salt, and soil were identified, and three indoor sources were resolved: resuspension, potassium-rich and copper-rich sources. The average contribution of the indoor factors was 6% (1.1 microg m(-3)) and 22% (2.4 microg m(-3)) in Amsterdam and Helsinki, respectively. The highest longitudinal correlations between source-specific outdoor and indoor PM2.5 concentrations were found for LRT and urban mixture; the median R was above 0.6 for most sources. The longitudinal correlations were lower in Helsinki than in Amsterdam. Indoor-generated PM2.5 was not related to ambient concentrations. We conclude that using outdoor and indoor data together improved the source apportionment of indoor PM2.5. The results support the use of fixed site outdoor measurements in epidemiological time-series studies on outdoor air pollution. 相似文献
14.
The research presented here was conducted within the scope of an experiment investigating technical feasibility and environmental impacts of tire combustion in a coal-fired power station. Previous work has shown that combustion of a coal+tire blend rather than pure coal increased bulk emissions of various elements (e.g., Zn, As, Sb, Pb). The aim of this study is to characterize the chemical and structural properties of emitted single particles with dimensions <2.5 microm (PM2.5). This transmission electron microscope (TEM)-based study revealed that, in addition to phases typical of coal fly ash (e.g., aluminum-silicate glass, mullite), the emitted PM2.5 contains amorphous selenium particles and three types of crystalline metal sulfates never reported before from stack emissions. Anglesite, PbSO4, is ubiquitous in the PM2.5 derived from both fuels and contains nearly all Pb present in the PM. Gunningite, ZnSO4-H2O, is the main host for Zn and only occurs in the PM derived from the coal+tire blend, whereas yavapaiite, KFe3+(SO4)2, is present only when pure coal was combusted. We conclude that these metal sulfates precipitated from the flue gas, may be globally abundant aerosols, and have, through hydration or dissolution, a major environmental and health impact. 相似文献
15.
We measured exposure to fine particles (PM2.5) and polycyclic aromatic hydrocarbons (PAHs), including carcinogenic PAHs, in multiple locations for a diverse population of participants who resided in Shizuoka, Japan. In summer and winter 2002 we surveyed personal concentrations, those of four primary indoor microenvironments-living room, bedroom, kitchen (summer only), and workplace--and those outside the subjects' houses. Concentrations of PM2.5 and PAHs tended to be higher during winter. Median PM2.5 concentration was highest in living room samples during winter but in personal samples during summer. The median PAH concentrations normalized to the cancer potency equivalence factor of benzo[a]pyrene (BaP-TEQ) was highest in the bedroom during winter but outdoors in summer. Personal exposure level profiles differed markedly between smokers and nonsmokers. Personal exposures to BaP ([BaP]p) and BaP-TEQ ([BaP-TEQ]P) in nonsmokers were strongly correlated. Personal exposures of nonsmokers, as calculated from the corresponding time-weighted indoor and outdoor concentrations, were consistent with measured levels of BaP but not PM2.5. Personal exposure of nonsmokers to BaP, as calculated from the time-weighted living room, bedroom, and either workplace or outdoor concentrations, accounted for 92-107% of the measured levels of BaP-TEQ. 相似文献
16.
While particulate matter (PM) in the atmosphere can lead to a wide array of negative health effects, the cause of toxicity is largely unknown. One aspect of PM that likely affects health is the chemical composition, in particular the transition metals within the particles. Chromium is one transition metal of interest due to its two major oxidation states, with Cr(III) being much less toxic compared to Cr(VI). Using microfocused X-ray absorption near edge structure (micro-XANES), we analyzed the Cr speciation in fine particles (diameters < or = 2.5 microm) collected at three sites in the Sacramento Valley of northern California. The microfocused X-ray beam enables us to look at very small areas on the filter with a resolution of typically 5-7 micrometers. With XANES we are able to not only distinguish between Cr(VI) and Cr(III), but also to identify different types of Cr(III) and more reduced Cr species. At all of our sampling sites the main Cr species were Cr(III), with Cr(OH)3 or a Cr-Fe, chromite-like, phase being the dominant species. Cr(VI)-containing particles were found only in the most urban site. All three sites contained some reduced Cr species, either Cr(0) or Cr3C2, although these were minor components. This work demonstrates that micro-XANES can be used as a minimally invasive analytical tool to investigate the composition of ambient PM. 相似文献
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18.
Salmonella senftenberg was detected in association with persistent contamination events in mussel processing facilities between 1998 and 2002 in Spain. A total of 110 isolates from 8 facilities were subjected to molecular typing by Pulsed-Field Gel Electrophoresis (PFGE). Additionally, a selection of epidemiologically unrelated isolates of this serovar originating from human, animal, feed and environmental sources was included in the study. PFGE analysis proved to be a useful tool for studying the persistence and dissemination of S. senftenberg in factory environments. Facilities that used brine in their processing lines had greater genetic diversity among their S. senftenberg populations, which supports the hypothesis that imported salt used for brine preparation could have been the origin of the contamination. The XbaI type X19 was the most prevalent among the panel, and it was found persisting exclusively in one facility during the 5-year study. In general, isolates from mussel processing plants were clearly different from those of clinical and environmental sources. However, one of the human isolates showed an indistinguishable restriction pattern to an isolate from a frozen mussel sample, this could indicate the potential for food-borne transmission of this serovar via consumption of contaminated seafood products. Isolates in the study were largely sensitive to antimicrobials. Only 9 isolates (6 from mussel processing facilities, 1 from soy flour and 2 from meat meal) showed antimicrobial resistance. 相似文献
19.
The development of Lactobacillus and Staphylococcus strains used as starter cultures throughout the ripening of Galician chorizo, a traditional dry fermented sausage from the north-west of Spain, was monitored combining different molecular-based techniques. The bacterial diversity occurring in the inoculated sausages at the beginning and the end of the ripening was also studied and compared to the indigenous population in an uninoculated control batch. 相似文献
20.
The relative roles of natural and anthropogenic sources in determining ozone and fine particle concentrations over the continental United States (U.S.) are investigated using an expanded emissions inventory of natural sources and an updated version of the Community Multiscale Air Quality (CMAQ) model. Various 12-month CMAQ simulations for the year 2002 using different sets of input emissions data are combined to delineate the contributions of background pollutants (i.e., model boundary conditions), natural emissions, anthropogenic emissions, as well as the specific impacts of lightning and wildfires. Results are compared with observations and previous air quality model simulations. Wildfires and lightning are both identified as contributing significantly to ozone levels with lightning NO(x) adding as much as 25-30 ppbV (or up to about 50%) to surface 8-h average natural O(3) mixing ratios in the southeastern U.S. Simulated wildfire emissions added more than 50 ppbV (in some cases >90%) to 8-h natural O(3) at several locations in the west. Modeling also indicates that natural emissions (including biogenic, oceanic, geogenic and fires) contributed ≤ 40% to the annual average of total simulated fine particle mass over the eastern two-thirds of the U.S. and >40% across most of the western U.S. Biogenic emissions are the dominant source of particulate mass over the entire U.S. and wildfire emissions are secondary. Averaged over the entire modeling domain, background and natural ozone are dominant with anthropogenically derived ozone contributing up to a third of the total only during summer. Background contributions to fine particle levels are relatively insignificant in comparison. Model results are also contrasted with the U.S. Environmental Protection Agency (EPA) default values for natural light scattering particle concentrations to be used for regional haze regulatory decision-making. Regional differences in EPA guidance are not supported by the modeling and EPA uncertainty estimates for default values are far smaller than the modeled variability in natural particle concentrations. 相似文献