Fine Particulate Chemical Composition and Light Extinction at Meadview,AZ

Abstract

The concentration of fine particulate nitrate, sulfate, and carbonaceous material was measured for 12-hr day-night samples using diffusion denuder samplers during the Project Measurement of Haze and Visibility Effects (MOHAVE) July to August 1992 Summer Intensive study at Meadview, AZ, just west of Grand Canyon National Park. Organic material was measured by several techniques. Only the diffusion denuder method measured the semivolatile organic material. Fine particulate sulfate and nitrate (using denuder technology) determined by various groups agreed. Based on the various collocated measurements obtained during the Project MOHAVE study, the precision of the major fine particulate species was ±0.6 μg/m³ organic material, ±0.3 μg/m³ ammonium sulfate, and ±0.07 μg/m³ ammonium nitrate. Data were also available on fine particulate crustal material, fine and coarse particulate mass from the Interagency Monitoring of Protected Visual Environments sampling system, and relative humidity (RH), light absorption, particle scattering, and light extinction measurements from Project MOHAVE. An extinction budget was obtained using mass scattering coefficients estimated from particle size distribution data. Literature data were used to estimate the change in the mass scattering coefficients for the measured species as a function of RH and for the absorption of light by elemental carbon. Fine particulate organic material was the principal particulate contributor to light extinction during the study period, with fine particulate sulfate as the second most important contributor. During periods of highest light extinction, contributions from fine particulate organic material, sulfate, and light-absorbing carbon dominated the extinction of light by particles. Particle light extinction was dominated by sulfate and organic material during periods of lowest light extinction. Combination of the extinction data and chemical mass balance analysis of sulfur oxides sources in the region indicate that the major anthropogenic contributors to light extinction were from the Los Angeles, CA, and Las Vegas, NV, urban areas. Mohave Power Project associated secondary sulfate was a negligible contributor to light extinction.     

Indoor-outdoor relationship of suspended particulate matter and its chemical composition at different sizes

The indoor-outdoor concentration relationship of particulate matter PM_9.0 (aerodynamic diameter 9 μm or smaller) and its chemical composition (sulfate, nitrate, chloride and ammonium) has been studied. Samples were collected using four identical Anderson impactors, each one collecting nine size ranges by eight impactor stages (9, 5.8, 4.7, 3.3, 2.1, 1.1, 0.65 and 0.43 μm) plus a back-up filter representing particles finer than 0.45 μm. Concentrations of sulfate, nitrate and chloride were determined by ion chromatography, and an ammonium-selective ion electrode plus a Corning pH ion meter were used to determine ammonium ion. The results revealed that sulfate was the predominant component and chloride the least abundant. The size distribution of sulfate, nitrate and ammonium very strongly peaked near 0.65 μm and with very little at the larger sizes. The chloride concentration was depleted in the fine particles and enhanced in the relatively coarser particles, with the peak at 3.3 μm. All these concentrations had a significant linear relationship with mass concentrations in outdoor samples. In indoor samples, the same relation was observed only for sulfate and ammonium, which were also significantly correlated with each other. Furthermore, indoor sulfate, chloride and ammonium concentrations were higher towards the finest particle sizes, indicating a higher potential inhalation health hazard. The study also confirmed that indoor air quality depends on outdoor atmospheric pollution level, indoor activities and virtually on the particle size. Finally, the study would assist in selecting the type of collector required to reduce the level of particulates to an acceptable level for indoor ambient air.     

A review on morphology,nanostructure, chemical composition,and number concentration of diesel particulate emissions

Environmental Science and Pollution Research - Particulate matter (PM) emitted from compression ignition (CI) engines (diesel engines) has a detrimental effect on human health and the environment....     

Fine particulate matter and visibility in the Lake Tahoe Basin: chemical characterization, trends, and source apportionment

Speciated PM2.5 (particulate matter with an aerodynamic diameter相似文献   

Aerosol chemical composition and light scattering in Portland,Oregon: The role of carbon

Measurements of light scattering and the chemical composition of the fine aerosol from the Portland (Oregon) Aerosol Characterization Study (PACS) of 1977–1978 are reported. Scattering coefficients for sulfate, nitrate, carbonaceous aerosol and residual mass were determined by stepwise multiple linear regression. Unlike other cities the scattering efficiencies for sulfate, nitrate and carbonaceous aerosol were approximately the same. Carbonaceous aerosol was found to account for about 50% of both the fine aerosol mass and the light scattering.     

Particulate contributions to light extinction and local forcing at a rural Illinois site

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.     

Diurnal and seasonal patterns in light scattering,extinction, and relative humidity

Since 1988, several federal and state governmental agencies in the US have coordinated efforts to operate the interagency monitoring of protected visual environments (IMPROVE) network at sites in remote areas. Most IMPROVE sites are equipped with either a transmissometer to measure light extinction (B_ext) or a nephelometer to measure particle scattering (B_sp). Optical, temperature, and relative humidity (RH) measurements are made hourly at these sites. The diurnal and seasonal patterns in these data are examined and discussed here. At many IMPROVE sites the diurnal patterns in RH and therefore B_ext or B_sp are as expected based on average temperature. On average, RH is higher at night and during the winter than during warmer times of the day and year. Also as expected, based on RH alone, at many sites hourly mean B_ext or B_sp values are either in phase with RH or weakly dependent on time of day. Usually, the diurnal differences are not as large as the seasonal differences. Another group of IMPROVE sites have mean RH patterns similar to those described above but have a different diurnal pattern in measured scattering or extinction. At these sites, the highest mean B_sp or B_ext occurs during mid-day rather than at night. At several of these sites, especially those on ridge tops, it is hypothesized that this is because the diurnal shifts in mixing height only allow the surface layer of the atmosphere to reach the monitor during mid-day. Several other sites have unique diurnal or seasonal patterns in average B_sp or B_ext that can usually be linked to emissions in nearby source regions or local meteorology and terrain.     

Fine and coarse particulate matter chemical characterization in a heavily industrialized city in central Mexico during Winter 2003

This paper presents the results of the first reported study on fine particulate matter (PM) chemical composition at Salamanca, a highly industrialized urban area of Central Mexico. Samples were collected at six sites within the urban area during February and March 2003. Several trace elements, organic carbon (OC), elemental carbon (EC), and six ions were analyzed to characterize aerosols. Average concentrations of PM with aerodynamic diameter of less than 10 microm (PM10) and fine PM with aerodynamic diameter of less than 2.5 microm (PM2.5) ranged from 32.2 to 76.6 [g m(-3) and 11.1 to 23.7 microg m(-3), respectively. OC (34%), SO4= (25.1%), EC (12.9%), and geological material (12.5%) were the major components of PM2.5. For PM10 geological material (57.9%), OC (17.3%), and SO4= (9.7%) were the major components. Coarse fraction (PM,, -PM2.5), geological material (81.7%), and OC (8.6%) were the dominant species, which amounted to 90.4%. Correlation analysis showed that sulfate in PM2.5 was present as ammonium sulfate. Sulfate showed a significant spatial variation with higher concentrations to the north resulting from predominantly southwesterly winds above the surface layer and by major SO2 sources that include a power plant and refinery. At the urban site of Cruz Roja it was observed that PM2.5 mass concentrations were similar to the submicron fraction concentrations. Furthermore, the correlation between EC in PM2.5 and EC measured from an aethalometer was r(2) = 0.710. Temporal variations of SO2 and nitrogen oxide were observed during a day when the maximum concentration of PM2.5 was measured, which was associated with emissions from the nearby refinery and power plant. From cascade impactor measurements, the three measured modes of airborne particles corresponded with diameters of 0.32, 1.8, and 5.6 microm.     

Source apportionment of fine particulate matter in Phoenix, AZ, using positive matrix factorization

Speciated particulate matter (PM)2.5 data collected as part of the Interagency Monitoring of Protected Visual Environments (IMPROVE) program in Phoenix, AZ, from April 2001 through October 2003 were analyzed using the multivariate receptor model, positive matrix factorization (PMF). Over 250 samples and 24 species were used, including the organic carbon and elemental carbon analytical temperature fractions from the thermal optical reflectance method. A two-step approach was used. First, the species excluding the carbon fractions were used, and initially eight factors were identified; non-soil potassium was calculated and included to better refine the burning factor. Next, the mass associated with the burning factor was removed, and the data set rerun with the carbon fractions. Results were very similar (i.e., within a few percent), but this step enabled a separation of the mobile factor into gasoline and diesel vehicle emissions. The identified factors were burning (on average 2% of the mass), secondary transport (7%), regional power generation (13%), dust (25%), nitrate (9%), industrial As/Pb/Se (2%), Cu/Ni/V (7%), diesel (9%), and general mobile (26%). The overall contribution from mobile sources also increased, as some mass (OC and nitrate) from the nitrate and regional power generation factors were apportioned with the mobile factors. This approach allowed better apportionment of carbon as well as total mass. Additionally, the use of multiple supporting analyses, including air mass trajectories, activity trends, and emission inventory information, helped increase confidence in factor identification.     

Size-segregated measurements of particulate elemental carbon and aerosol light absorption at remote arctic locations

Size-segregated aerosol samples were taken during 2 winter pollution periods and in clean summer air at different remote locations in the European Arctic > 74°N. By means of a newly developed integrating sphere photometer these filter samples have been analysed for aerosol light absorption coefficients and particulate elemental carbon (PEC). The relatively high PEC concentrations in winter confirm other findings about the Arctic winter atmosphere having an aged continental aerosol burden. In summer very low light absorption coefficients of 4.5 × 10⁻⁸ m⁻¹ were measured, similar to upper tropospheric background values. For the climatically important months of March-May the key optical aerosol properties (extinction coefficient, single scattering albedo and absorption to backscatter ratio) were determined. Based on the approach of J.M. Mitchell (1971, in Man's Impact on Climate. MIT Press, Cambridge, MA) the Arctic haze aerosol is found to contribute to atmospheric heating, even in the summer. A first PEC size distribution was determined in a clean polar summer air. The results show systematic variations in the PEC size distribution from urban to remote locations and seasonal variations in the sink region which may be exploited to quantify aerosol removal process in long distance transport studies.     

Day-of-week patterns of particulate matter and its chemical components at selected sites in California

This paper analyzes day-of-week variations in concentrations of particulate matter (PM) in California. Because volatile organic compounds (VOCs) and oxides of nitrogen (NOx) are not only precursors of ozone (O3) but also of secondary PM, it is useful to know whether the variations by day of week in these precursors are also evident in PM data. Concentrations of PM < or = 10 microm (PM10) and < or = 2.5 microm in aerodynamic diameter (PM2.5) were analyzed. PM concentrations exhibit a general weekly pattern, with the maximum occurring late in the workweek and the minimum occurring on weekends (especially Sunday); however, this pattern does not prevail at all sites and areas. PM nitrate (NO3-) data from Size Selective Inlet (SSI) samplers in the South Coast Air Basin (SoCAB) tend to be somewhat lower on weekends compared with weekdays. During 1988-1991, the weekend average was lower than the weekday average at 8 of 13 locations, with an average decrease of 1%. During 1997-2000, the weekend average was lower than the weekday average at 10 of 13 locations, with an average decrease of 6%. The weekend averages are generally lower than weekday averages for sulfates, organic carbon, and elemental carbon. Because heavy-duty trucks typically represent a major source of elemental carbon, the weekend decrease in heavy-duty truck traffic may also result in a decrease in ambient elemental carbon concentrations.     

Fine particulate matter source apportionment for the Chemical speciation Trends Network site at Birmingham, Alabama, using Positive Matrix Factorization

The Positive Matrix Factorization (PMF) receptor model version 1.1 was used with data from the fine particulate matter (PM2.5) Chemical Speciation Trends Network (STN) to estimate source contributions to ambient PM2.5 in a highly industrialized urban setting in the southeastern United States. Model results consistently resolved 10 factors that are interpreted as two secondary, five industrial, one motor vehicle, one road dust, and one biomass burning sources. The STN dataset is generally not corrected for field blank levels, which are significant in the case of organic carbon (OC). Estimation of primary OC using the elemental carbon (EC) tracer method applied on a seasonal basis significantly improved the model's performance. Uniform increase of input data uncertainty and exclusion of a few outlier samples (associated with high potassium) further improved the model results. However, it was found that most PMF factors did not cleanly represent single source types and instead are "contaminated" by other sources, a situation that might be improved by controlling rotational ambiguity within the model. Secondary particulate matter formed by atmospheric processes, such as sulfate and secondary OC, contribute the majority of ambient PM2.5 and exhibit strong seasonality (37 +/- 10% winter vs. 55 +/- 16% summer average). Motor vehicle emissions constitute the biggest primary PM2.5 mass contribution with almost 25 +/- 2% long-term average and winter maximum of 29 +/- 11%. PM2.5 contributions from the five identified industrial sources vary little with season and average 14 +/- 1.3%. In summary, this study demonstrates the utility of the EC tracer method to effectively blank-correct the OC concentrations in the STN dataset. In addition, examination of the effect of input uncertainty estimates on model results indicates that the estimated uncertainties currently being provided with the STN data may be somewhat lower than the levels needed for optimum modeling results.     

Morphological and chemical composition characteristics of summertime atmospheric particles collected at Tokchok Island,Korea

Determination of the chemical compositions of atmospheric single particles in the Yellow Sea region is critical for evaluating the environmental impact caused by air pollutants emitted from mainland China and the Korean peninsula. After ambient aerosol particles were collected by the Dekati PM10 cascade impactor on July 17–23, 2007 at Tokchok Island (approximately 50 km west of the Korean coast nearby Seoul), Korea, overall 2000 particles (on stage 2 and 3 with cut-off diameters of 2.5–10 μm and 1.0–2.5 μm, respectively) in 10 samples were determined by using low-Z particle electron probe X-ray microanalysis. X-ray spectral and secondary electron image (SEI) data showed that soil-derived and sea-salt particles which had reacted or were mixed with SO₂ and NO_x (or their acidic products) outnumbered the primary and “genuine” ones (59.2% vs. 19.2% in the stage 2 fraction and 41.3% vs. 9.9% in the stage 3 fraction). Moreover, particles containing nitrate in the secondary soil-derived species greatly outnumbered those containing sulfate. Organic particles, mainly consisting of marine biogenic species, were more abundant in the stage 2 fraction than in the stage 3 fraction (11.6% vs. 5.1%). Their relative abundance was greater than the sum of carbon-rich, K-containing, Fe-containing, and fly ash particles, which exhibited low frequencies in all the samples. In addition, many droplets rich in C, N, O, and S were observed. They tended to be small, exhibiting a dark round shape on SEI, and generally included 8–20 at.% C, 0–12 at.% N, 60–80 at.% O, and 4–10 at.% S (sometimes with <3 at.% Mg and Na). They were attributed to be a mixture of carbonaceous matter, H₂SO₄, and NH₄HSO₄/(NH₄)₂SO₄, mostly from the reaction of atmospheric SO₂ with NH₃ under high relative humidity. The analysis of the relationship between the aerosol particle compositions and 72-h backward air-mass trajectories suggests that ambient aerosols at Tokchok Island are strongly affected not only by seawater from the Yellow Sea but also by anthropogenic pollutants emitted from China and the Seoul–Incheon metropolis, resulting in the dominance of complex secondary aerosol particles.     

PM2.5 mass and light extinction reconstruction in IMPROVE

Compliance under the Regional Haze Rule of 1999 is based on Interagency Monitoring of Protected Visual Environments (IMPROVE) protocols for reconstructing aerosol mass and light extinction from aerosol chemical concentrations measured in the IMPROVE network. The accuracy, consistency, and potential biases in these formulations were examined using IMPROVE aerosol chemistry and light extinction data from 1988-1999. Underestimation of particulate matter with an aerodynamic diameter < 2.5 microm (PM2.5) by the IMPROVE mass reconstruction formula by 12%, on average, appears to be related to the exclusion of sodium, chlorine, and other elements and to artifacts associated with the measurement of organic carbon, but not to absorption of water by sulfates and nitrates on IMPROVE Teflon filters during weighing. Light scattering measured by transmissometry is not consistent with nephelometer scattering or single-scatter albedos expected for remote locations. Light scattering was systematically overestimated by 34%, on average, with the IMPROVE particle scattering (Bsp) reconstruction formula. The use of climatologically based hygroscopic growth factors f(RH) suggested for compliance with the Haze Rule contributes significantly to this overestimation and increases the amount of light extinction attributable to sulfates for IMPROVE samples between 1993 and 1999 by 5 percentage points.     

Fine particulate phase PAHs in ambient atmosphere of Chennai metropolitan city,India

Background  

Airborne fine particulates (PM 2.5) and its associated polycyclic aromatic hydrocarbons (PAHs) are reportedly hazardous in urban environment due to the presence of multiple emission sources.     

Open-path,closed-path,and reconstructed aerosol extinction at a rural site

The Handix Scientific open-path cavity ringdown spectrometer (OPCRDS) was deployed during summer 2016 in Great Smoky Mountains National Park (GRSM). Extinction coefficients from the relatively new OPCRDS and from a more well-established extinction instrument agreed to within 7%. Aerosol hygroscopic growth (f(RH)) was calculated from the ratio of ambient extinction measured by the OPCRDS to dry extinction measured by a closed-path extinction monitor (Aerodyne’s cavity-attenuated phase shift particulate matter extinction monitor [CAPS PMex]). Derived hygroscopicity (relative humidity [RH] < 95%) from this campaign agreed with data from 1995 at the same site and time of year, which is noteworthy given the decreasing trend for organics and sulfate in the eastern United States. However, maximum f(RH) values in 1995 were less than half as large as those recorded in 2016—possibly due to nephelometer truncation losses in 1995. Two hygroscopicity parameterizations were investigated using high-time-resolution OPCRDS+CAPS PMex data, and the κ_ext model was more accurate than the gamma model. Data from the two ambient optical instruments, the OPCRDS and the open-path nephelometer, generally agreed; however, significant discrepancies between ambient scattering and extinction were observed, apparently driven by a combination of hygroscopic growth effects, which tend to increase nephelometer truncation losses and decrease sensitivity to the wavelength difference between the two instruments as a function of particle size. There was not a statistically significant difference in the mean reconstructed extinction values obtained from the original and the revised IMPROVE (Interagency Monitoring of Protected Visual Environments) equations. On average, IMPROVE reconstructed extinction was ~25% lower than extinction measured by the OPCRDS, which suggests that the IMPROVE equations and 24-hr aerosol data are moderately successful in estimating current haze levels at GRSM. However, this conclusion is limited by the coarse temporal resolution and the low dynamic range of the IMPROVE reconstructed extinction.

Implications: Although light extinction, which is directly related to visibility, is not directly measured in U.S. National Parks, existing IMPROVE protocols can be used to accurately infer visibility for average humidity conditions, but during the large fraction of the year when humidity is above or below average, accuracy is reduced substantially. Furthermore, nephelometers, which are used to assess the accuracy of IMPROVE visibility estimates, may themselves be biased low when humidity is very high. Despite reductions in organic and sulfate particles since the 1990s, hygroscopicity, particles’ affinity for water, appears unchanged, although this conclusion is weakened by the previously mentioned nephelometer limitations.     

Molecular composition of organic fine particulate matter in Houston,TX

Organic fine particulate matter collected in Houston, TX between March 1997 and March 1998 was analyzed to determine the concentration of individual organic compounds. Samples from four sites were analyzed including two industrial locations (Houston Regional Monitoring Corporation (HRM-3) site in Channelview and Clinton Drive site near the Ship Channel Turning Basin), one suburban location (Bingle Drive site in Northwest Houston) and one background site (Galveston Island). At the three urban locations, samples were divided into three seasonal sample aggregates (spring, summer and winter), while at the background site a single annual average sample pool was used. Between 10 and 16 individual samples were pooled to get aggregate samples with enough organic carbon mass for analysis. Overall, 82 individual organic compounds were quantified. These include molecular markers which are compounds unique to specific fine particle sources and can be used to track the relative contribution of source emissions to ambient fine particle levels. The differences both spatially and temporally in these tracers can be used to evaluate the variability in emission source strengths.     

An investigation of interurban variations in the chemical composition and mutagenic activity of airborne particulate organic matter using an integrated chemical class/bioassay system

Previous investigations in this laboratory have demonstrated that the mutagenic activities of extractable particulate organic matter (EOM) from cities which differ in their principal fuels and meteorology can vary significantly. To gain a better understanding of these interurban variations, an Integrated Chemical Class/Biological Screening System was developed and used for a more detailed examination of differences in the chemical composition and mutagenic activity of EOM. The screening system involved coupling in situ Ames mutagenicity determinations on high performance thin layer chromatography (HPTLC) plates with class specific chemical analyses on a second set of plates. The system was used to screen for mutagenic activity and selected chemical classes (including PAH, nitro-PAH, phenols, carboxylic acids, carbonyls, aza-arenes and alkylating agents) in EOM from the following sites: New York City; Elizabeth, N.J.; Mexico City; Beijing, China; Philadelphia, PA; and the Caldecott Tunnel (CA).The results of this study demonstrated mutagenic activity and chemical compositional differences in HPTLC subfractions of particulate organic matter from these cities and from the Caldecott Tunnel. The greatest interurban differences in chemical classes were observed for the phenols, carbonyl compounds and alkylating agents. Interurban variations in mutagenic activities were greatest for EOM subfractions of intermediate polarity. These differences are probably related to interurban differences in the fuels used, types of sources and atmospheric conditions. The relationships between these variables are not well understood at present.     

Fine particle concentrations and composition during wintertime inversions in Logan,Utah, USA

During Winter 2004, a series of elevated PM_2.5 events occurred in Logan, Utah, coinciding with strong winter inversions. This period resulted in 17 exceedances of the 24-h PM_2.5 standard, and some of the highest PM_2.5 mass loadings recorded in the United States, including 9 days of 24-h PM_2.5 measurements over 100 μg m⁻³. During the 3-month period, we monitored the size and mass concentrations of airborne particles using an aerosol mass spectrometer. PM_2.5 concentrations were dominated by the formation of ammonium nitrate, accounting for over 50% of the non-refractory aerosol matter throughout the study and 80% on the highest pollution days. Another 15–20% of the particulate matter was composed of organic carbon. The high particle concentration loadings in Utah's Cache Valley result from a combination of unfavorable meteorology dominated by a severe cold-temperature inversion, a mix of rural and urban emission sources, and a confined geographical area. As a rapidly growing formerly rural area, the Cache Valley is representative of future air pollution problems facing areas of the interior west undergoing rapid urbanization.