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1.
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   

2.
Atmospheric particulate matter (PM) is an air-suspended mixture of solid and liquid particles that vary in size, shape, and chemical composition. Long-term exposure to elevated concentrations of fine atmospheric particles is considered to pose a health threat to humans and animals. In this context, it has been hypothesized that toxic chemicals such as polycyclic aromatic hydrocarbons (PAHs) play an important role. Some PAHs are known to be carcinogenic and it has been shown that carcinogenic effects of PAHs are mediated by the aryl hydrocarbon receptor (AhR). In this study, PM1 was collected at a rural and an urban traffic site during an intense winter smog period, in which concentration of PM1 often exceeded 50 μg m?3. We applied an in vitro reporter gene assay (DR-CALUX) to detect and quantify PM1-associated chemicals that induce AhR-mediated gene expression. This activity was expressed as CALUX equivalents of 2,3,7,8-tetrachlorodibenzodioxin (PM-TCDD-CEQs). In addition, concentrations of PAHs in the PM1 extracts were determined using gas chromatography/high-resolution mass spectrometry. Concentrations of PM-TCDD-CEQs ranged from 10 to 85 pg m?3 and from 19 to 87 pg m?3 at the urban and rural site, respectively. By the use of known relative potency factors, the measured concentration of a PAH was converted into a PAH-TCDD-CEQ concentration. ΣPAH-TCDD-CEQ and PM-TCDD-CEQ were highly correlated at both sites (r2 = 0.90 and 0.69). The calculated ΣPAH-TCDD-CEQs explain between 2% and 20% of the measured PM-TCDD-CEQs. Benzo[k]fluoranthene was the most important PAH causing approximately 60% of the total ΣPAH-TCDD-CEQ activity. In contrast to NO, CO, PM10, and PM1, the concentration of PM-TCDD-CEQs showed no significant difference between the two sites. No indications were found that road traffic emissions caused elevated concentrations of PM-TCDD-CEQs at the urban traffic site.  相似文献   

3.
The light extinction and direct forcing properties of the atmospheric aerosol were investigated for a midwestern rural site (Bondville, IL) using field measurements, a semi-empirical light extinction model, and a radiative transfer code. Model inputs were based on the site measurements of the physical and chemical characteristics of atmospheric aerosol during the spring, summer, fall and winter of 1994. The light scattering and extinction coefficients were calculated and apportioned using the elastic light scattering interactive efficiency (ELSIE) model (Sloane and Wolff, 1985, Atmospheric Environment 19(4), 669–680). The average efficiencies calculated for organic carbon (OC, carbon measured as organic multiplied by 1.2) ranged from 3.81 m2/g OC at lower relative humidities (<63%) to 6.90 m2/g OC at higher relative humidities (>75%) while sulfate (assumed as ammonium sulfate) efficiencies ranged from 1.23 m2/g (NH4)2SO4 to 5.78 m2/g (NH4)2SO4 for the same range of relative humidities. Radiative transfer calculations showed that the rural aerosol at Bondville is most likely to have an overall negative (cooling) forcing effect on climate. Elemental carbon (EC), however, acts to counter sulfate forcing to a degree that has a significant seasonal variation, primarily due to the seasonal variation in the sulfate concentrations. Taking the loading to be the mean summer EC+ammonium sulfate loading and assuming [EC]/[(NH4)2SO4] to be zero in one case (i.e. no soot present) and 0.025 (summer mean at Bondville) in another leads to a 37% difference in calculated forcing.  相似文献   

4.
A microanalytical method suitable for the quantitative determination of the sugar anhydride levoglucosan in low-volume samples of atmospheric fine particulate matter (PM) has been developed and validated. The method incorporates two sugar anhydrides as quality control standards. The recovery standard sedoheptulosan (2,7-anhydro-beta-D-altro-heptulopyranose) in 20 microL solvent is added onto samples of the atmospheric fine PM and aged for 1 hr before ultrasonic extraction with ethylacetate/ triethylamine. The extract is reduced in volume, an internal standard is added (1,5-anhydro-D-mannitol), and a portion of the extract is derivatized with 10% by volume N-trimethylsilylimidazole. The derivatized extract is analyzed by gas chromatography/mass spectrometry (GC/MS). The recovery of levoglucosan using this procedure was 69 +/- 6% from five filters amended with 2 microg levoglucosan, and the reproducibility of the assay is 9%. The limit of detection is approximately 0.1 microg/mL, which is equivalent to approximately 3.5 ng/m3 for a 10 L/min sampler or approximately 8.7 ng/m3 for a 4 L/min personal sampler (assuming 24-hr integrated samples). We demonstrated that levoglucosan concentrations in collocated samples (expressed as ng/m3) were identical irrespective of whether samples were collected by PM with aerodynamic diameter < or = 2.5 microm or PM with aerodynamic diameter < or = 10 microm impactors. It was also demonstrated that X-ray fluorescence analysis of samples of atmospheric PM, before levoglucosan determinations, did not alter the levels of levoglucosan.  相似文献   

5.
Composition of exhaust from a ship diesel engine using heavy fuel oil (HFO) was investigated onboard a large cargo vessel. The emitted particulate matter (PM) properties related to environmental and health impacts were investigated along with composition of the gas-phase emissions. Mass, size distribution, chemical composition and microphysical structure of the PM were investigated. The emission factor for PM was 5.3 g (kg fuel)?1. The mass size distribution showed a bimodal shape with two maxima: one in the accumulation mode with mean particle diameter DP around 0.5 μm and one in the coarse mode at DP around 7 μm. The PM composition was dominated by organic carbon (OC), ash and sulphate while the elemental carbon (EC) composed only a few percent of the total PM. Increase of the PM in exhaust upon cooling was associated with increase of OC and sulphate. Laser analysis of the adsorbed phase in the cooled exhaust showed presence of a rich mixture of polycyclic aromatic hydrocarbon (PAH) species with molecular mass 178–300 amu while PM collected in the hot exhaust showed only four PAH masses.Microstructure and elemental analysis of ship combustion residuals indicate three distinct morphological structures with different chemical composition: soot aggregates, significantly metal polluted; char particles, clean or containing minerals; mineral and/or ash particles. Additionally, organic carbon particles of unburned fuel or/and lubricating oil origin were observed. Hazardous constituents from the combustion of heavy fuel oil such as transitional and alkali earth metals (V, Ni, Ca, Fe) were observed in the PM samples.Measurements of gaseous composition in the exhaust of this particular ship showed emission factors that are on the low side of the interval of global emission factors published in literature for NOx, hydrocarbons (HC) and CO.  相似文献   

6.
A receptor model of positive matrix factorization (PMF) was used to identify the emission sources of fine and coarse particulates in Bandung, a city located at about 150 km south-east of Jakarta. Total of 367 samples were collected at urban mixed site, Tegalega area, in Bandung City during wet and dry season in the period of 2001–2007. The samples of fine and coarse particulate matter were collected simultaneously using dichotomous samplers and mini-volume samplers. The Samples from dichotomous Samplers were analyzed for black carbon and elements while samples from mini-volume samplers were analyzed for ions. The species analyzed in this study were Na, Mg, Al, Si, K, Ca, Ti, Cr, Mn, Fe, Ni, Cu, Pb, Cl?, NO3?, SO42?, and NH4+. The data were then analyzed using PMF to determine the source factors. Different numbers of source factors were found during dry and wet season. During dry season, the main source factors for fine particles were secondary aerosol (NH4)2SO4, electroplating industry, vehicle emission, and biomass burning, while for coarse particles, the dominant source factors were electroplating industry, followed by aged sea salt, volcanic dust, soil dust, and lime dust. During the wet season, the main source factors for fine particulate matter were vehicle emission and secondary aerosol. Other sources detected were biomass burning, lime dust, soil and volcanic dust. While for coarse particulate matter, the main source factors were sulphate-rich industry, followed by lime dust, soil dust, industrial emission and construction dust.  相似文献   

7.
The organic carbon (OC)/elemental carbon (EC) tracer method is applied to the Pittsburgh, PA, area to estimate the contribution of secondary organic aerosol (SOA) to the monthly average concentration of organic particulate matter (PM) during 1995. An emissions inventory is constructed for the primary emissions of OC and EC in the area of interest. The ratio of primary emissions of OC to those of EC ranges between 2.4 in the winter months and 1.0 in the summer months. A mass balance model and ambient measurements were used to assess the accuracy of the emissions inventory. It is estimated to be accurate to within 50%. The results from this analysis show a strong monthly dependence of the SOA contribution to the total organic PM concentration, varying from near zero during winter months to as much as 50% of the total OC concentration in the summer.  相似文献   

8.
This paper discusses the evaluation and application of a new generation of particulate matter (PM) emission factor model (MicroFacPM). MicroFacPM that was evaluated in Tuscarora Mountain Tunnel, Pennsylvania Turnpike, PA shows good agreement between measured and modeled emissions. MicroFacPM application is presented to the vehicle traffic on the main approach road to the Ambassador Bridge, which is one of the most important international border entry points in North America, connecting Detroit, MI, with Windsor, Ontario, Canada. An increase in border security has forced heavy-duty diesel vehicles to line up for several kilometers through the city of Windsor causing concern about elevated concentrations of ambient PM. MicroFacPM has been developed to model vehicle-generated PM (fine [PM2.5] and coarse < or = 10 microm [PM10]) from the on-road vehicle fleet, which in this case includes traffic at very low speeds (10 km/h). The Windsor case study gives vehicle generated PM2.5 sources and their breakdown by vehicle age and class. It shows that the primary sources of vehicle-generated PM2.5 emissions are the late-model heavy-duty diesel vehicles. We also applied CALINE4 and AERMOD in conjunction with MicroFacPM, using Canadian traffic and climate conditions, to describe the vehicle-generated PM2.5 dispersion near this roadway during the month of May in 2003.  相似文献   

9.
Atmospheric particulate matter (PM) is hypothesized to increase the risk of myocardial infarction (MI). However, the epidemiological evidence is inconsistent. We identified 33 studies with more than 4 million MI patients and applied meta-analysis and meta-regression to assess the available evidence. Twenty-five studies presented the effects of the PM level on hospitalization for MI patients, while eight studies showed the effects on mortality. An increase in PM10 was associated with hospitalization and mortality in myocardial infarction patients (RR per 10 μg/m3?=?1.011, 95 % CI 1.006–1.016; RR per 10 μg/m3?=?1.008, 95 % CI 1.004–1.012, respectively); PM2.5 also increased the risk of hospitalization and mortality in MI patients (RR per 10 μg/m3?=?1.024, 95 % CI 1.007–1.041 for hospitalization and RR per 10 μg/m3?=?1.012, 95 % CI 1.010–1.015 for mortality). The results of the cumulative meta-analysis indicated that PM10 and PM2.5 were associated with myocardial infarctionwith the addition of new studies each year. In conclusion, short-term exposure to high PM10 and PM2.5 levels revealed to increase risk of hospitalization and mortality for myocardial infarction. Policy support of pollution control and individual protection was strongly recommended.  相似文献   

10.
PM2.5 samples were collected during an annual monitoring campaign (January 2012–January 2013) in the urban area of Naples, one of the major cities in Southern Italy. Samples were collected by means of a standard gravimetric sampler (Tecora Echo model) and characterized from a chemical point of view by ion chromatography. As a result, 143 samples together with their ionic composition have been collected. We extend traditional source apportionment techniques, usually based on multivariate factor analysis, interpreting the chemical analysis results within a Lagrangian framework. The Hybrid Single-Particle Lagrangian Integrated Trajectory Model (HYSPLIT) model was used, providing linkages to the source regions in the upwind areas. Results were analyzed in order to quantify the relative weight of different source types/areas. Model results suggested that PM concentrations are strongly affected not only by local emissions but also by transboundary emissions, especially from the Eastern and Northern European countries and African Saharan dust episodes.  相似文献   

11.
An arsenic speciation study has been performed in PM10 samples collected on a fortnight basis in the city of Huelva (SW Spain) during 2001 and 2002. The arsenic species were extracted from the PM10 filters using a NH2OH x HCl solution and sonication, and determined by HPLC-HG-AFS. The mean bulk As concentration of the samples analyzed during 2001 and 2002 slightly exceed the mean annual 6 ng m(-3) target value proposed by the European Commission for 2013, arsenate [As(V)] being responsible for the high level of arsenic. The speciation analyses showed that As(V) was the main arsenic species found, followed by arsenite [As(III)] (mean 6.5 and 7.8 ng m(-3) for As(V), mean 1.2 and 2.1 ng m(-3) for As(III), in 2001 and 2002, respectively). The high levels of arsenic species found in PM10 in Huelva have a predominant industrial origin, such as the one from a nearby copper smelter, and do not present a seasonal pattern. The highest daily levels of arsenic species correspond to synoptic conditions in which the winds with S and SW components transport the contaminants from the main emission source. The frequent African dust outbreaks over Huelva may result in an increment of mass levels of PM10, but do not represent a significant input of arsenic in comparison to the anthropogenic source. The rural background levels of arsenic around Huelva are rather high, in comparison to other rural or urban areas in Spain, showing a relatively high atmosphere residence time of arsenic. This work shows the importance of arsenic speciation in studies of aerosol chemistry, due to the presence of arsenic species [As(III) and As(V)] with distinct toxicity.  相似文献   

12.
Twenty four-hour averaged concentrations of fine particulate matter were collected at Athens, OH between March 2004 and November 2005 in an effort to characterize the nature of PM2.5 and apportion its sources. PM2.5 samples were chemically analyzed and positive matrix factorization was applied to this speciation data to identify the probable sources. PMF arrived at a 7-factor model to most accurately apportion sources of the PM2.5 observed at Athens. Conditional probability function (CPF) and potential source contribution function (PSCF) were applied to the identified sources to investigate the geographical location of these sources. Secondary sulfate source dominated the contributions with a total contribution of 62.6% with the primary and secondary organic source following second with 19.9%. Secondary nitrate contributed a total of 6.5% with the steel production source and Pb- and Zn-source coming in at 3.1% and 2.9%, respectively. Crustal and mobile sources were small contributors (2.5% each) of PM2.5 to the Athens region. The secondary sulfate, secondary organic and nitrate portrayed a clear seasonal nature with the sulfate and secondary organic peaking in the warm months and the nitrate reaching a high in the cold months. The high percentage of secondary sulfate observed at a rural site like Athens suggests the involvement of regional transport mechanisms.  相似文献   

13.
The externally-mixed source-oriented UCD/CIT air quality model was applied to determine the significance of inter-regional transport for primary and secondary particulate matter (PM) in California's Central Valley during a severe wintertime PM pollution episode from December 15, 2000 to January 7, 2001. The gases and primary PM emitted from eight different geographical sub-regions were tracked separately in a model simulation that included transport, physical and chemical transformation and deposition processes. The model results directly predict the contribution that each sub-region makes to PM concentrations throughout the entire model domain. The boundary layer was relatively stagnant during the simulated 3-week air quality episode, and no consistent transport pattern for primary PM was predicted. Several significant inter-regional transport events were identified that each lasted a few days. Each of these inter-regional events was characterized by transport of gas-phase precursors of nitrate that combined with local emissions of ammonia to produce particulate nitrate. Nitrate already in the particle phase was not transported efficiently due to higher dry deposition rates for particles relative to gas-phase nitrogen oxides. The distinctive pattern of transport for nitrate precursors reflects the relatively long timescales required to convert NOx emissions to nitrate during winter conditions characterized by low temperatures, weak photolysis rates, and low oxidant concentrations. The equilibrium partitioning of nitrate and ammonia to the particle phase is relatively fast once the nitrate has been produced. The most-likely transport distance for nitrate during the current episode varied from 130–140 km for the northern portion of the Central Valley to 50–60 km in the southern portion of the Central Valley. Sub-regions further south in the Valley have smaller transport distances because of slower wind speeds and the greater abundance of ammonia in these areas, leading to faster conversion of gas-phase reactive nitrogen into particulate nitrate, which has a higher dry deposition rate than the gas-phase species. The most-likely transport distance for primary organic compounds (OC) was found to be less than that for nitrate, varying from 50 to 60 km for the northern portion of the Valley to 20–30 km for southern portion of the Valley. Overall, 68% of the particulate nitrate formed in the most polluted sub-regions of the Central Valley originates from emissions in those same sub-regions. Local emissions controls should therefore provide an effective strategy to reduce airborne particulate matter concentrations to acceptable levels.  相似文献   

14.
A ten-month field study aimed to determine the contribution of natural events (i.e. sea-salt and mineral dust events) to urban PM concentration was carried out at six sampling sites in Central Italy (Lazio region). Four indicators have been used to identify natural events during the period of the study. The first one is constituted by the ratio between number of particles in the coarse to the accumulation mode. It is simple, cheap, and the information are given in quasi-real time, but the nature of the event (sea-salt or mineral dust) is not detectable. The second indicator relies on the chemical analysis of the collected PM by X-ray fluorescence (XRF) and allows a robust identification of sea-salt and crustal components. The third one is based on diagnostic ratios of elemental fractions: Mgextractable/Tiresidue for sea-salt and Tiresidue/Sbresidue for mineral dust. It requires skilled staff but it is most accurate and sensible. The last indicator, constructed on the basis of natural radioactivity data, is not diagnostic for the nature of the event but it is able to estimate the increase in PM concentration with respect to the expected concentration in the absence of natural events.The relevance of natural events and the variations in PM concentration and composition during the study are discussed. The joined use of the four indicators allowed the identification of about 20 natural PM episodes. In general, sea-salt aerosol events did not cause exceedance of the daily EU limit value for PM10. Saharan dust events, instead, were in most cases responsible for the exceedance of the limit value at all stations.  相似文献   

15.
Three 2-wk seasonal field campaigns were performed in 2003 and 2004 at a sampling site on the southern Tyrrhenian coast of Italy with the aim to investigate the dynamics and characteristics of particle-bound pollutants in the Mediterranean area. Fine (PM(2.5)) and coarse particulate matter (PM(10-2.5)) size fractions were collected by a manual dichotomous sampler on 37-mm Teflon filters over a 24-hr sampling period. On average, 70% of the total PM(10) (PM(2.5) + PM(10-2.5)) mass was associated with the coarse fraction and 30% with the fine fraction during the three campaigns. The ambient concentrations of Pb, Ni, Cr, Zn, Mn, V, Cd, Fe, Cu, Ca, and Mg associated with both size fractions were determined by atomic absorption spectrometry. Ambient concentrations showed differences in their absolute value, ranging from few ng x m(-3) to microg x m(-3), as well as in their variability within the PM(2.5) and PM(10-2.5) size fractions. PM(10) levels were well below the European Union (EU) limit value during the study period with the exception of three events during the first campaign (fall) and five events during the third campaign (spring). Two main sources were identified as the major contributors including mineral dust, transported from North Africa, and sea spray from the Tyrrhenian Sea. Comparing the results with backward trajectories, calculated using the Hybrid Single-Particle Lagrangian Integrated Trajectory Model (HYSPLIT) and Total Ozone Mapping Spectrometer-National Aeronautics and Space Administration (TOMS-NASA) maps, it was observed that in central and eastern Europe, the Tyrrhenian Sea and North Africa were the major emission source regions that affected the temporal variations and daily averages of PM(2.5) and PM(10-2.5) concentrations.  相似文献   

16.
为研究成都市降水对大气颗粒物(以下简称颗粒物)的湿清除作用,对2014—2016年成都市的颗粒物(PM2.5、PM10)和气象观测数据进行分析。结果表明:月、季尺度下,降水对PM2.5、PM10均有削减作用。降水时段的PM2.5、PM10浓度较非降水时段分别降低17.1%和15.8%,且冬季降幅最为明显。考察472次降水过程对颗粒物的湿清除作用,发现单次降水过程后PM2.5、PM10浓度增长频次(243、234次)和削减频次(229、238次)接近,但颗粒物浓度总体呈削减趋势。对于单次降水过程,颗粒物的初始浓度与降水对颗粒物的湿清除作用关系密切,特别是降水持续时间超过8h后,颗粒物初始浓度越高,削减效果越好。  相似文献   

17.
Environmental Science and Pollution Research - Dhaka and its neighboring areas suffer from severe air pollution, especially during dry season (November–April). We investigated temporal and...  相似文献   

18.
Particulate matter (PM) has become a major research issue receiving increasing attention because of its significant negative impact on human health. There are main indicators that next to the morphological characteristics of the particle, also the chemical composition plays an important role in the adverse health effects of PM. In this context, the rather polar organic fraction of PM is expected to play a major role, and advanced analytical techniques are developed to improve the knowledge on the molecular composition of this fraction. One component class that deserves major attention consists of the oxygenated polycyclic aromatic hydrocarbons (PAHs). Those compounds are considered to be among the key compounds in PM toxicity. This paper presents a comprehensive review focusing on the analysis, fate and behavior of oxygenated PAHs in the atmosphere. The first part of the paper briefly introduces (i) the main sources and atmospheric pathways of oxygenated PAHs, (ii) available physical–chemical properties and (iii) their health effects. The second and main part of this paper gives a thorough discussion on the entire analytical sequence necessary to identify and quantify oxygenated PAHs on atmospheric PM. Special attention is given to critical parameters and innovations related to (i) sampling, (ii) sample preparation including both extraction and clean-up, and (iii) separation and detection. Third, the state-of-the-art knowledge about the atmospheric occurrence of oxygenated PAHs is discussed, including an extended overview of reported concentrations presented as a function of sampling season and geographical location. A clear seasonal effect is observed with the median of the oxygenated PAHs concentrations during winter being a factor of 3–4 higher than during summer. However, the oxygenated PAH/parent PAH ratio is about 20 times higher during summer, indicating the importance of photochemical activity in the atmosphere.  相似文献   

19.
Air quality field data, collected as part of the fine particulate matter Supersites Program and other field measurements programs, have been used to assess the degree of intraurban variability for various physical and chemical properties of ambient fine particulate matter. Spatial patterns vary from nearly homogeneous to quite heterogeneous, depending on the city, parameter of interest, and the approach or method used to define spatial variability. Secondary formation, which is often regional in nature, drives fine particulate matter mass and the relevant chemical components toward high intraurban spatial homogeneity. Those particulate matter components that are dominated by primary emissions within the urban area, such as black carbon and several trace elements, tend to exhibit greater spatial heterogeneity. A variety of study designs and data analysis approaches have been used to characterize intraurban variability. High temporal correlation does not imply spatial homogeneity. For example, there can be high temporal correlation but with spatial heterogeneity manifested as smooth spatial gradients, often emanating from areas of high emissions such as the urban core or industrial zones.  相似文献   

20.
通过酸缓冲能力的测定实验,研究杭州市主城区大气颗粒物的酸缓冲能力,并利用二重源解析技术,解析了大气颗粒物中碱性组分的来源.结果表明,杭州市主城区大气颗粒物呈弱碱性,对降水酸度有一定的缓冲作用,但作用较小.总体而言,TSP与PM10的酸缓冲能力与其浓度呈负相关,但相关关系不明显,TSP的酸缓冲能力比PM10强.Ca是影响大气颗粒物酸缓冲能力的关键化学组分.TSP的酸缓冲能力主要来自建筑水泥尘.  相似文献   

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