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Gaseous and particulate pollutant concentrations associated with five samples per day collected during a July 2001 summer intensive study at the Pittsburgh Carnegie Mellon University (CMU) Supersite were used to apportion fine particulate matter (PM2.5) into primary and secondary contributions using PMF2. Input to the PMF2 analysis included the concentrations of PM2.5 nonvolatile and semivolatile organic material, elemental carbon (EC), ammonium sulfate, trace element components, gas-phase organic material, and NO(x), NO2, and O3 concentrations. A total of 10 factors were identified. These factors are associated with emissions from various sources and facilities including crustal material, gasoline combustion, diesel combustion, and three nearby sources high in trace metals. In addition, four secondary sources were identified, three of which were associated with secondary products of local emissions and were dominated by organic material and one of which was dominated by secondary ammonium sulfate transported to the CMU site from the west and southwest. The three largest contributors to PM2.5 were secondary transported material (dominated by ammonium sulfate) from the west and southwest (49%), secondary material formed during midday photochemical processes (24%), and gasoline combustion emissions (11%). The other seven sources accounted for the remaining 16% of the PM2.5. Results obtained at the CMU site were comparable to results previously reported at the National Energy Technology Laboratory (NETL), located approximately 18 km south of downtown Pittsburgh. The major contributor at both sites was material transported from the west and southwest. Some difference in nearby sources could be attributed to meteorology as evaluated by HYSPLIT model back-trajectory calculations. These findings are consistent with the majority of the secondary ammonium sulfate in the Pittsburgh area being the result of contributions from distant transport, and thus decoupled from local activity involving organic pollutants in the metropolitan area. In contrast, the major local secondary sources were dominated by organic material.

Apportionment of primary and secondary pollutants during a July 2001 intensive study at the National Energy Technology Laboratory is reported. PM2.5 was apportioned into primary and secondary contributions using PMF2, and results were compared with apportionment based on UNMIX 2.3. Input to PMF2 included PM2.5 mass data from four per 24 hour PC-BOSS filters and TEOM, NOx, NO2, O3, non-volatile, semi-volatile, and volatile organic material, elemental carbon, sulfate, and PIXE determined trace metals. Nine factors were identified in the PMF analysis. Six factors were associated with primary particles from crustal, mobile (gasoline and diesel), and three local sources high in trace metals. Three factors were associated with secondary sources. Two were associated with local emissions dominated by organic material, one was dominated by transported ammonium sulfate. UNMIX was able to identify the two major mobile sources, major local secondary source and transported secondary source. The three major sources of ...

Lichens are known to accumulate airborne elements. This characteristic makes them useful as biomonitors of air quality. However, direct correlations of element concentrations in the air with element concentrations in lichen thalli are generally unavailable. The purpose of this study was to quantitatively examine the relationship between concentrations of copper in ambient air samples and thalli of foliose and fruticose lichens. Lichen samples from four sites along an air copper gradient were collected and analyzed. Foliose specimens consistently accumulated more than twice as much copper as fruticose specimens at all four sites. The relationship between copper concentrations in foliose and fruticose lichens and ambient air samples along an airborne copper gradient was examined using a stepwise regression model. An R2 value of (0.84) and an F-statistic of (182.5, p

Lichen samples were collected and observations about lichen communities were recorded at sites in the intermountain western United States. Specifically the states of Idaho, Montana, Wyoming, Nevada, Utah, Colorado, Arizona, and New Mexico were included in this study. The minor and trace-element concentrations in many of the lichens collected were determined by proton induced X-ray emission (PIXE). These data are part of a base line assessment of current air pollution conditions in this region. These data also provide an opportunity to study some aspects of lichen physiology. Using the data from 508 foliose and fruticose lichens, frequency distributions for concentrations of phosphorus and calcium are considered. Phosphorus has a closely-spaced, bimodal distribution: one mode for foliose lichens and one mode for fruticose lichens. This suggests that all lichen genera in this study have similar requirements and absorption mechanisms for phosphorus. Calcium has a complex frequency distribution and concentrations that range from 450 mg/kg to 14 % dry weight. Contributions to this complex distribution pattern can be understood if the data are resolved into growth form, genera within each growth form, and in some cases species within a given genus. This complex dependence on calcium is strong evidence that lichens develop specific calcium-related adaptations in order to accommodate various habitat conditions.

Air pollutants were collected in Logan, Cache County, UT, in February 1993 during two periods of atmospheric inversion accompanied by fog. The following atmospheric species were determined: (1) gaseous SO2, NO2 (semi-quantitatively),HNO3, NH3, and HF; (2) fine particulate SO4 =, NO3 -, NH4 +, F–, H+, C, Si, S, K, Ca, Ti, Mn, Fe, Ni, Cu, Zn, Pb, Se, Br, and Sr, and; (3) fine particulate mass, which was calculated. The major components of fine particulate matter were carbonaceous material, ammonium nitrate, and ammonium sulfate, while the soil component was small. Calculated, fine particulate mass averaged 80 μg/m3 and reached concentrations as high as 120 μg/m3. SO2/Sox and NO2/NOy mole ratios generally varied between 0.2 and 0.1 during inversions. These ratios also showed moderate but consistent diurnal patterns. The emission inventory for Cache County indicates sources of SO2 and NOx but not significant amounts of primary sulfate and nitrate. The observations reported here indicate there is sign...

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.

Lichens have been shown to be effective biomonitors of air quality. They are currently being used to characterize background element levels and to identify air pollution effects on federally administered lands in the Rocky Mountain region of the western United States. PIXE analysis for twenty elements has been performed on over two hundred lichen specimens collected from various national forests, national monuments, and national parks in the region. This paper reports on patterns of iron and titanium accumulation in lichen tissues. Data show a strong relationship between concentrations of iron and titanium. The Fe/Ti ratios agree well with values reported in similar lichen studies; however, our values for both iron and titanium concentrations are ten times greater than other reports. A distribution function for the log of iron concentrations is distinctly bimodal. The lower concentration mode contains fruticose lichens from bark substrates and the higher concentration mode contains foliose lichens from rock substrates. High iron concentrations in fruticose lichens along the Wasatch Front suggest air pollution impact from a local steel plant.Lichens have been shown to be effective biomonitors of air quality. They are currently being used to characterize background element levels and to identify air pollution effects on federally administered lands in the Rocky Mountain region of the western United States. PIXE analysis for twenty elements has been performed on over two hundred lichen specimens collected from various national forests, national monuments, and national parks in the region. This paper reports on patterns of iron and titanium accumulation in lichen tissues. Data show a strong relationship between concentrations of iron and titanium. The Fe/Ti ratios agree well with values reported in similar lichen studies; however, our values for both iron and titanium concentrations are ten times greater than other reports. A distribution function for the log of iron concentrations is distinctly bimodal. The lower concentration mode contains fruticose lichens from bark substrates and the higher concentration mode contains foliose lichens from ro...

Sulfur transformation chemistry was studied in the plume of the Utah smelter of Kennecott Copper Corporation from April to October 1977. Samples were taken at up to four locations from 4 to 60 km from the stacks. Data collected at each station included: SO2 concentration, low-volume collected total paniculate matter, high-volume collected size fractionated paniculate matter, wind velocity and direction, temperature, and relative humidity. Paniculate samples were analyzed for S(IV). sulfate, strong acid, anions, cations, and elemental concentrations using calorimetric, ion Chromatographie, FIXE, ESCA, ion microprobe, and SEM-ion microprobe techniques. The concentration of As in the paniculate matter was used as a conservative plume tracer. The ratios Mo/As, Pb/As, and Zn/As were constant in particulate matter collected at all sampling sites for any particle size. Strong mineral acid was neutralized by background metal oxide and/or carbonate particulates within 40km of the smelter. This neutralization process is limited only by the rate of incorporation of basic material into the plume. Two distinct metal-S(IV) species similar to those observed in laboratory aerosol experiments were found in the plume. The formation of paniculate S(IV) species occurs by interaction of SO2 (g) with both ambient and plume derived aerosol and is equilibrium controlled. The extent of formation of S(IV) complexes in the aerosol is directly proportional to the SO2(g) and paniculate (Cu + Fe) concentration and inversely proportional to the paniculate acidity. S(IV) species were stable in collected paniculate matter only in the neutralized material, but with proper sampling techniques could be demonstrated to also be present in very acidic particles at high ambient SO2(g) concentrations. Reduction of arsenate to arsenite by the aerosol S(IV) complexes during plume transport is suggested. The SO2(g)-sulfate conversion process in the plume is described by a mechanism which is first order in SO2(g). Equations are derived describing sulfur chemistry when both S(IV) and sulfate formation occur in a plume. The formation of sulfate results primarily in the formation of < 0.5 μm particulates. The formation process is not correlated with plume expansion, paniculate acidity, metal content, or S(IV) species. Due to meteorological restrictions on sampling, data were collected only during periods of maximum insolation. The formation of sulfate from SO2(g) in the plume during periods of high insolation is temperature dependent with an apparent activation energy of 16.6 ± 1.4 kcal mol−1 and a k1, value of 0.039h−1 at 25°C.

Etude de la conversion SO 2 en sulfate dans le panache d'une centrale electrique chauffee au petrole situee pres de la cote Pacifique

Recent epidemiological and animal lexicological studies indicate that reactions between SO2 and metal containing aerosols result in the formation of respiratory irritants. These studies point out the importance of understanding in detail the chemical species formed by such interactions. Using a combination of thermometric, ESCA and PIXE analysis techniques, it has been demonstrated that both inorganic and organic S(IV) species are stable constituents of aerosols associated with pollution sources containing SO2 and transition metals or with pollution sources resulting from the combustion of fossil fuels. The data indicate the inorganic sulfite species are present as complexes with Fe(III), Cu(II), Zn(II) and possibly Pb(II). The concentration of these inorganic sulfite species is 10 to 30% of the sulfate concentration in primary aerosols produced by smelters. These inorganic sulfite species tend to be evenly distributed over the various particle sizes. In contrast, the inorganic sulfite in primary aerosols produced by fossil fuel burning sources tends to exist in the

Effluents from a high temperature, high pressure, entrained flow gasifier were analysed for possible inorganic and organic pollutants. The effluents and product gases from this type of reactor are very clean compared to those produced in established commercial gasification processes. The only major potential pollutants are the particulate matter and NH4+ in the scrubber water, the bottom ash, and the H2S and HCN in the product and flash gases. All of the non-volatile organic compounds produced are quantitatively adsorbed by the particulate matter in the scrubber water. Increasing the pressure and decreasing the O2coal ratio tended to reduce pollutants in the effluents and increase coal conversion efficiency.

Fly ash samples were collected from the flue lines of two different oil-fired power plants and analyzed by a variety of analytical procedures designed to determine the V cations extractable from the samples. Both VO/sub 2//sup +/ and VO/sup 2 +/ were shown to be present in the samples. The V(V) cation, VO/sub 2//sup +/, was the principal species extracted from these samples.