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1.
Abstract

Nylon filters are a popular medium to collect atmospheric fine particles in different aerosol monitoring networks, including those operated by the U.S. Environmental Protection Agency and the Interagency Monitoring of Protected Visual Environments (IMPROVE) program. Extraction of the filters by deionized water or by a basic aqueous solution (typically a mixture of sodium carbonate and sodium bicarbonate) is often performed to permit measurement of the inorganic ion content of the collected particles. Whereas previous studies have demonstrated the importance of using a basic solution to efficiently extract gaseous nitric acid collected using nylon filters, there has been a recent movement to the use of deionized water for extraction of particles collected on nylon filters to eliminate interference from sodium ion (Na+) during ion chromatographic analysis of inorganic aerosol cations. Results are reported here from a study designed to investigate the efficiency of deionized water extraction of aerosol nitrate (NO3 ?) and sulfate from nylon filters. Data were obtained through the conduct of five field experiments at selected IMPROVE sites. Results indicate that the nylon filters provide superior retention of collected fine particle NO3 ?, relative to Teflon filters, and that deionized water extraction (with ultrasonication) of collected NO3 ? and sulfate is as efficient, for the situations studied, as extraction using a basic solution of 1.7 mM sodium bicarbonate and 1.8 mM sodium carbonate.  相似文献   

2.
A method is described to estimate light scattering (Bsp) by sea-salt aerosols at coastal locations in the Interagency Monitoring of Protected Visual Environments (IMPROVE) network. Dry mass scattering efficiencies for fine and coarse sea-salt particles were based on previously measured dry sea-salt size distributions. Enhancement of sea-salt particle scattering by hygroscopic growth was based on NaCl water activity data. Sea-salt aerosol mass at the IMPROVE site in the Virgin Islands (VIIS) was estimated from strontium (Sr) concentrations in IMPROVE aerosol samples. Estimated Bsp, including contributions from sea-salt mass based on Sr, agreed well with measured Bsp at the VIIS IMPROVE site. On average, sea salt accounted for 52% of estimated Bsp at this site. Sea-salt aerosol mass cannot be reliably estimated from Sr unless its crustal enrichment factor exceeds 10. Sodium (Na) concentrations are not accurately determined by X-ray fluorescence analysis in IMPROVE samples. It is recommended that Na be measured in the fine and coarse modes by a more appropriate method, such as atomic absorption spectroscopy or ion chromatography, to account for scattering by sea-salt particles at IMPROVE sites where such contributions may be significant.  相似文献   

3.
The mass size distribution of atmospheric aerosol particles was determined by means of an electric low pressure impactor (ELPI) in rural air in Hungary. The particles captured on different stages of the impactor were chemically analyzed by capillary zone electrophoresis to quantify ionic components as well as by catalytic combustion method to detect total carbon in the samples. The results show that fine aerosol consists mainly of ammonium sulfate and organic carbon. These two species have rather different size distributions since very small particles are composed almost of carbon compounds. The analysis of fine aerosol samples collected simultaneously on filters indicates that an important part of organics is soluble in water. The mass balance of fine particles as a function of their size is estimated by taking into account the liquid water adsorbed by ammonium sulfate and by converting the mass of carbon to the mass of carbon compounds. Finally, the size resolved mass balance of fine aerosol particles is presented and discussed as a function of the origin of air masses.  相似文献   

4.
Abstract

A method is described to estimate light scattering (Bsp) by sea-salt aerosols at coastal locations in the Interagency Monitoring of Protected Visual Environments (IMPROVE) network. Dry mass scattering efficiencies for fine and coarse sea-salt particles were based on previously measured dry sea-salt size distributions. Enhancement of sea-salt particle scattering by hygroscopic growth was based on NaCl water activity data. Sea-salt aerosol mass at the IMPROVE site in the Virgin Islands (VIIS) was estimated from strontium (Sr) concentrations in IMPROVE aerosol samples. Estimated Bsp, including contributions from sea-salt mass based on Sr, agreed well with measured Bsp at the VIIS IMPROVE site. On average, sea salt accounted for 52% of estimated Bsp at this site. Sea-salt aerosol mass cannot be reliably estimated from Sr unless its crustal enrichment factor exceeds 10. Sodium (Na) concentrations are not accurately determined by X-ray fluorescence analysis in IMPROVE samples. It is recommended that Na be measured in the fine and coarse modes by a more appropriate method, such as atomic absorption spectroscopy or ion chromatography, to account for scattering by sea-salt particles at IMPROVE sites where such contributions may be significant.  相似文献   

5.
An annular denuder system, which consisted of a cyclone separator; two diffusion denuders coated with sodium carbonate and citric acid, respectively; and a filter pack consisting of Teflon and nylon filters in series, was used to measure acid gases, ammonia (NH3), and fine particles in the atmosphere from April 1998 to March 1999 in eastern North Carolina (i.e., an NH3-rich environment). The sodium carbonate denuders yielded average acid gas concentrations of 0.23 microg/m3 hydrochloric acid (standard deviation [SD] +/- 0.2 microg/m3); 1.14 microg/m3 nitric acid (SD +/- 0.81 microg/m3), and 1.61 microg/m3 sulfuric acid (SD +/- 1.58 microg/m3). The citric acid denuders yielded an average concentration of 17.89 microg/m3 NH3 (SD +/- 15.03 microg/m3). The filters yielded average fine aerosol concentrations of 1.64 microg/m3 ammonium (NH4+; SD +/- 1.26 microg/m3); 0.26 microg/m3 chloride (SD +/- 0.69 microg/m3), 1.92 microg/m3 nitrate (SD +/- 1.09 microg/m3), and 3.18 microg/m3 sulfate (SO4(2-); SD +/- 3.12 microg/m3). From seasonal variation, the measured particulates (NH4+, SO4(2-), and nitrate) showed larger peak concentrations during summer, suggesting that the gas-to-particle conversion was efficient during summer. The aerosol fraction in this study area indicated the domination of ammonium sulfate particles because of the local abundance of NH3, and the long-range transport of SO4(2-) based on back trajectory analysis. Relative humidity effects on gas-to-particle conversion processes were analyzed by particulate NH4+ concentration originally formed from the neutralization processes with the secondary pollutants in the atmosphere.  相似文献   

6.
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.  相似文献   

7.
Concentrations and distributions of three major water-soluble ion species (sulfate, nitrate, and ammonium) contained in ambient particles were measured at three sampling sites in the Kao-ping ambient air quality basin, Taiwan. Ambient particulate matter (PM) samples were collected in a Micro-orifice Uniform Deposit Impactor from February to July 2003 and were analyzed for water-soluble ion species with an ion chromatograph. The PM1/ PM2.5 and PM1/PM10 concentration ratios at the emission source site were 0.73 and 0.53 and were higher than those (0.68 and 0.48) at the background site because there are more combustion sources (i.e., industrial boilers and traffic) around the emission source site. Mass-size distributions of PM NO3- were found in both the fine and coarse modes. SO4(2-)and NH4+ were found in the fine particle mode (PM2.5), with significant fractions of submicron particles (PM1). The source site had higher PM1/PM10(79, 42, and 90%) and PM1/PM2.5 concentration ratios (90, 58, and 93%) for the three major inorganic secondary aerosol components (SO4(2-), NO3-, and NH4+) than the receptor site (65, 27, and 65% for PM1/PM10, 69, 51, and 70% for PM1/PM2.5. Results obtained in this study indicate that the PM1 (submicron aerosol particles) fraction plays an important role in the ambient atmosphere at both emission source and receptor sites. Further studies regarding the origin and formation of ambient secondary aerosols are planned.  相似文献   

8.
Frequency distributions of the major chemical components of aerosol fine mass are shown to illustrate the respective species’ contributions to the range of observed fine particle mass concentration. The magnitude of a species’ contribution to the upper extremes of aerosol fine mass is relevant to control scenarios that seek to improve worst day fine particle conditions, or in many cases worst day visibility. We summarize the relative contributions of fine particle sulfate, nitrate, carbon, and soil plus sea salt to the upper extremes of aerosol fine mass based on Interagency Monitoring of PROtected Visual Environments (IMPROVE) data collected at monitoring locations across the United States during 1995 through 1999. The data show that the spatial pattern of a given chemical species’ contribution to the upper extremes of aerosol fine mass is often quite different than at lower fine mass concentrations. In some cases, the monitoring data suggest a casual relationship between specific aerosol source regions and the magnitude in which a species’ contribution to the upper extremes of fine mass is elevated above the contribution to median fine mass concentrations.  相似文献   

9.
Size-resolved aerosol particle samples in the size range 0.1–10 μm aerodynamic diameter were collected in the years 2003 and 2004 at an urban background station in Mainz, Germany. Size, morphology, chemical composition and mixing state of more than 5400 individual particles of 7 selected sampling days were analyzed in detail by scanning electron microscopy and energy-dispersive X-ray microanalysis. In addition, transmission electron microscopy, aerosol mass spectrometry and atomic force microscopy were applied to obtain detailed information about the mixing state of the particles. The fine particle fraction (diameter<1 μm) is always dominated by complex secondary aerosol particles (⩾90% by number) independent from air mass origin. These particles are complex internal mixtures of ammonium and sodium sulfates, nitrates, and organic material. Between 20% and 40% of the complex secondary aerosol particles contain soot inclusions. The composition of the coarse particle fraction (>1 μm diameter) is strongly dependant on air mass history with variable abundances of complex secondary aerosol particles, aged sea salt, silicates, silicate mixtures, calcium sulfates, calcium sulfate/carbonate mixtures, calcium nitrate/carbonate mixtures, biological particles, and external soot.The dominance of complex secondary aerosol particles shows that reduction of the precursor gases is a major goal for successful reduction strategies for PM10.  相似文献   

10.
The ratio of organic mass (OM) to organic carbon (OC) in PM(2.5) aerosols at US national parks in the IMPROVE network was estimated experimentally from solvent extraction of sample filters and from the difference between PM(2.5) mass and chemical constituents other than OC (mass balance) in IMPROVE samples from 1988 to 2003. Archived IMPROVE filters from five IMPROVE sites were extracted with dichloromethane (DCM), acetone and water. The extract residues were weighed to determine OM and analyzed for OC by thermal optical reflectance (TOR). On average, successive extracts of DCM, acetone, and water contained 64%, 21%, and 15%, respectively, of the extractable OC, respectively. On average, the non-blank-corrected recovery of the OC initially measured in these samples by TOR was 115+/-42%. OM/OC ratios from the combined DCM and acetone extracts averaged 1.92 and ranged from 1.58 at Indian Gardens, AZ in the Grand Canyon to 2.58 at Mount Rainier, WA. The average OM/OC ratio determined by mass balance was 2.07 across the IMPROVE network. The sensitivity of this ratio to assumptions concerning sulfate neutralization, water uptake by hygroscopic species, soil mass, and nitrate volatilization were evaluated. These results suggest that the value of 1.4 for the OM/OC ratio commonly used for mass and light extinction reconstruction in IMPROVE is too low.  相似文献   

11.
First-time measurements of the potentially toxic inorganic species of arsenic (arsenite arid arsenate) have been obtained in fine (<2.5 µm AD) and coarse (>2.5 µm AD) atmospheric particles in the Los Angeles area. A recently developed method that includes procedures for sample collection, preparation, and analysis was used in this study. Size-fractlonated aerosol samples were collected with a high-volume dichotomous virtual impactor that employed polytetrafluoroethylene filters. Results were obtained for the recovery of arsenic standards added to unexposed and collected filters. Data from this study, indicated that the recently developed speciation method can be used to determine concentrations of As(lll) and As(V) In atmospheric particulate matter samples.

Size-fractionated aerosol samples were collected in the city of Industry during January and February 1987. In most samples, As(lll) and As( V) were above the detection limit (approximately 1 ng m-3 of either species) in both aerosol size fractions. A greater portion (about 75 percent) of the two species were observed in the fine particles. The As(lll)/As(V) ratio for both particle sizes was close to 1 (I.e., an equal mixture of both species). Comparison of total suspended particulate arsenic measured by the speciation method to that measured by a routine California Air Resources Board-approved procedure showed good agreement (r = 0.94), indicating both methods were approximately equivalent for the collection and analysis of aerosol arsenic.  相似文献   

12.
In an attempt to identify the ionic imbalance, hydrogen carbonate, HCO3 (bicarbonate), was determined together with the commonly determined nine major ions because the imbalance was frequently encountered in the chemical analysis of samples with high pHs. Titration method was applied for the determination of the samples with pH higher than 5.6. These samples amounted to 102 of the 1536 samples collected in Hokkaido, Northern Japan, from April 1998 to December 2002. Of the 102 samples, 74 (Group A) showed an acceptable ion balance without including HCO3. In the other 28 (Group B), however, inclusion of HCO3 successfully improved the ion balance. These results suggested that hydrogen carbonate was a potential candidate for explaining the imbalance. The hydrogen carbonate concentrations showed a strong correlation with the corresponding non-sea salt calcium (nss-Ca2+) concentrations, which implied that hydrogen carbonate was derived from calcium carbonate particles incorporated into falling raindrops or cloud droplets. For Group A, the relationship between hydrogen carbonate and the nss-calcium ion concentration was very similar to that for commonly suspended particles in Hokkaido. On the other hand, Group B exhibited a stronger but significantly different correlation. To the samples of Group B, a back-trajectory analysis was applied to demonstrate that the samples were associated with aerosol travelling from Northern China or Mongolia, which indicated that alkaline aerosol affected the chemistry. In consideration of these findings, the current standard of the ion balance should be critically reviewed for modification in regard to the contribution of hydrogen carbonate not only in source areas but also in receptor areas of alkaline aerosol.  相似文献   

13.
Acidic aerosol concentrations measured by an annular denuder system (ADS) and a honeycomb denuder system (HDS) in Hsinchu, Taiwan, were compared. Aerosols were also sampled by a MOUDI (micro-orifice uniform deposit impactor) and analyzed by an ion chromatograph to determine the size distributions of different species. Using the measured aerosol size distribution, theoretical analysis showed that positive HNO3 artifact due to volatilization of NH4NO3 is generally negligible for both samplers. Comparing two different denuder samplers, the average concentration of HNO3 measured by the ADS was found to be lower than that measured by the HDS, while the difference between the two samplers for the average concentration of other species was found to be within +/- 15%. A possible cause of the difference in HNO3 concentrations is due to a greater loss of HNO3 in the cyclone used by the ADS than in the impactor used by the HDS. The study also showed incomplete absorption of the evaporated HCl and HNO3 from the particles on the Teflon filter by the first nylon filter in the filter pack of the ADS. Collection efficiency and capacity of HCl and HNO3 by the nylon filters need further investigation.  相似文献   

14.
Beck M  Radke M 《Chemosphere》2006,64(7):1134-1140
Concentrations of steroids and inorganic ions were measured in waste water of an aerated sand trap as well as in aerosol particles emitted from this tank at the waste water treatment plant (WWTP) of Bayreuth, Germany, in January and February 2003. The investigations comprised seven sterols, two estrogens, and several inorganic ions. Since an appropriate method for the determination of sterols in waste water was not available, a new method based on solid phase extraction was developed. The concentrations of the sterols coprostanol and cholesterol amounted to 30-180 microg l(-1) in waste water and to 400-5000 pg m(-3) in aerosol particles. All other sterols were present in markedly lower concentrations. The mean concentrations of the two estrogens estrone and 17beta-estradiol were about 165 pg m(-3) in aerosol particles. The steroid concentrations in both waste water and aerosol particles varied greatly over time, however with the exception of coprostanol, no clear correlation was detected between concentrations in waste water and aerosol particles.  相似文献   

15.
Hydroxymethanesulfonate (HMS), a product of the heterogeneous reaction between S(IV) and HCHO, was measured in atmospheric aerosol samples collected at two locations indicating it can exist outside of clouds. Sampling was performed through collection with filters and analysis using ion chromatography with a treatment step to distinguish between HMS and uncomplexed S(IV). Concentrations of HMS were found to range from below the detection limit to 6.5 ng m-3 for samples collected in central New Mexico in the summer and around 30 ng m-3 for two samples collected in Seattle, Washington in the spring. Higher concentrations were associated with greater occurrence of clouds, which is the presumed source of the HMS. In the samples collected in Seattle, about half of the HMS was found associated with fine particles. In the central New Mexico samples, molar ratios of HMS to sulfate in particulate matter were found to be less than 0.002 indicating that HMS was a minor contributor of aerosol sulfur under the conditions of the measurements.  相似文献   

16.
The Interagency Monitoring of Protected Visual Environments (IMPROVE) particle monitoring network consists of approximately 160 sites at which fine particulate matter (PM2.5) mass and major species concentrations and course particulate matter (PM10) mass concentrations are determined by analysis of 24-hr duration sampling conducted on a 1-day-in-3 schedule A simple algorithm to estimate light extinction from the measured species concentrations was incorporated in the 1999 Regional Haze Rule as the basis for the haze metric used to track haze trends. A revised algorithm was developed that is more consistent with the recent atmospheric aerosol literature and reduces bias for high and low light extinction extremes. The revised algorithm differs from the original algorithm in having a term for estimating sea salt light scattering from Cl(-) ion data, using 1.8 instead of 1.4 for the mean ratio of organic mass to measured organic carbon, using site-specific Rayleigh scattering based on site elevation and mean temperature, employing a split component extinction efficiency associated with large and small size mode sulfate, nitrate and organic mass species, and adding a term for nitrogen dioxide (NO2) absorption for sites with NO2 concentration information. Light scattering estimates using the original and the revised algorithms are compared with nephelometer measurements at 21 IMPROVE monitoring sites. The revised algorithm reduces the underprediction of high haze periods and the overprediction of low haze periods compared with the performance of the original algorithm. This is most apparent at the hazier monitoring sites in the eastern United States. For each site, the PM10 composition for days selected as the best 20% and the worst 20% haze condition days are nearly identical regardless of whether the basis of selection was light scattering from the original or revised algorithms, or from nephelometer-measured light scattering.  相似文献   

17.
Abstract

An annular denuder system, which consisted of a cyclone separator; two diffusion denuders coated with sodium carbonate and citric acid, respectively; and a filter pack consisting of Teflon and nylon filters in series, was used to measure acid gases, ammonia (NH3), and fine particles in the atmosphere from April 1998 to March 1999 in eastern North Carolina (i.e., an NH3?rich environment). The sodium carbonate denuders yielded average acid gas concentrations of 0.23 μg/m3 hydrochloric acid (standard deviation [SD] ± 0.2 μg/m3); 1.14 μg/m3 nitric acid (SD ± 0.81 μg/m3), and 1.61 μg/m3 sulfuric acid (SD ± 1.58 μg/m3). The citric acid denuders yielded an average concentration of 17.89 μg/m3 NH3 (SD ± 15.03 μg/m3). The filters yielded average fine aerosol concentrations of 1.64 μg/m3 ammonium (NH4 +;SD ± 1.26 μg/m3); 0.26 μg/m3 chloride (SD ± 0.69 μg/m3), 1.92 μg/m3 nitrate (SD ± 1.09 μg/m3), and 3.18 μg/m3 sulfate (SO4 2?; SD ± 3.12 μg/m3). From seasonal variation, the measured particulates (NH4 +,SO4 2?, and nitrate) showed larger peak concentrations during summer, suggesting that the gas-to-particle conversion was efficient during summer. The aerosol fraction in this study area indicated the domination of ammonium sulfate particles because of the local abundance of NH3, and the long-range transport of SO4 2? based on back trajectory analysis. Relative humidity effects on gas-to-particle conversion processes were analyzed by particulate NH4 + concentration originally formed from the neutralization processes with the secondary pollutants in the atmosphere.  相似文献   

18.
The [revised] IMPROVE Equation for estimating light extinction from aerosol chemical composition was evaluated considering new measurements at U.S. national parks. Compared with light scattering (Bsp) measured at seven IMPROVE sites with nephelometer data from 2003–2012, the [revised] IMPROVE Equation over- and underestimated Bsp in the lower and upper quintiles, respectively, of measured Bsp. Underestimation of the worst visibility cases (upper quintile) was reduced by assuming an organic mass (OM)/organic carbon (OC) ratio of 2.1 and hygroscopic growth of OM, based on results from previous field studies. This assumption, however, tended to overestimate low Bsp even more. Assuming that sulfate was present as ammonium bisulfate rather than as ammonium sulfate uniformly reduced estimated Bsp. The split-mode model of concentration- and size-dependent dry mass scattering efficiencies in the [revised] IMPROVE Equation does not eliminate systematic biases in estimated Bsp. While the new measurements of OM/OC and OM hygroscopicity should be incorporated into future iterations of the IMPROVE Equation, the problem is not well constrained due to a lack of routine measurements of sulfate neutralization and the water-soluble fraction of OM in the IMPROVE network.

Implications: Studies in U.S. national parks showed that aerosol organics contain more mass and absorb more water as a function of relative humidity than is currently assumed by the IMPROVE Equation for calculating chemical light extinction. Consideration of these results could significantly shift the apportionment of light extinction to water-soluble organic aerosols and therefore better inform pollution control strategies under the U.S. Environmental Protection Agency Regional Haze Rule.  相似文献   


19.
采用水族箱生态模拟方法,利用碳酸钠和碳酸氢钠作为碱度调节剂设置不同碱度水平,研究了氮磷营养相对充足的试验水体中藻类各相关指标对无机碳的响应,并对试验过程中所测得的理化指标和生物指标进行统计分析.研究表明:富营养水体无机碳含量与藻类叶绿素水平存在着正相关关系;适当增加水体中的无机碳浓度能够改变蓝、绿藻门种类比例;当碱度水平达到一定程度时,铜绿微囊藻可以逐渐成为优势种,并从体系中上升,演替成为水华.  相似文献   

20.
The ionic compositions of particulate matter with aerodynamic diameter < or = 2.5 microm (PM2.5) and size-resolved aerosol particles were measured in Big Bend National Park, Texas, during the 1999 Big Bend Regional Aerosol and Visibility Observational study. The ionic composition of PM2.5 aerosol was dominated by sulfate (SO4(2-)) and ammonium (NH4+). Daily average SO4(2-) and NH4+ concentrations were strongly correlated (R2 = 0.94). The molar ratio of NH4+ to SO4(2-) averaged 1.54, consistent with concurrent measurements of aerosol acidity. The aerosol was observed to be comprised of a submicron fine mode consisting primarily of ammoniated SO4(2-) and a coarse particle mode containing nitrate (NO3-). The NO3- appears to be primarily associated with sea salt particles where chloride has been replaced by NO3-, although formation of calcium nitrate (Ca(NO3)2) is important, too, on several days. Size-resolved aerosol composition results reveal that a size cut in particulate matter with aerodynamic diameter < or = 1 microm would have provided a much better separation of fine and coarse aerosol modes than the standard PM2.5 size cut utilized for the study. Although considerable nitric acid exists in the gas phase at Big Bend, the aerosol is sufficiently acidic and temperatures sufficiently high that even significant future reductions in PM2.5 SO4(2-) are unlikely to be offset by formation of particulate ammonium nitrate in summer or fall.  相似文献   

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