Sources of fine particulate species in ambient air over lake Champlain Basin, VT

This study is a part of an ongoing investigation of the types and locations of emission sources that contribute fine particulate air contaminants to Underhill, VT. The air quality monitoring data used for this study are from the Interagency Monitoring of Protected Visual Environments network for the period of 2001-2003 for the Underhill site. The main source-receptor modeling techniques used are the positive matrix factorization (PMF) and potential source contribution function (PSCF). This new study is intended as a comparison to a previous study of the 1988-1995 Underhill data that successfully revealed a total of 11 types of emission sources with significant contributions to this rural site. This new study has identified a total of nine sources: nitrate-rich secondary aerosol, wood smoke, East Coast oil combustion, automobile emission, metal working, soil/dust, sulfur-rich aerosol type I, sulfur-rich aerosol type II, and sea salt/road salt. Furthermore, the mass contributions from the PMF identified sources that correspond with sampling days with either good or poor visibility were analyzed to seek possible correlations. It has been shown that sulfur-rich aerosol type I, nitrate aerosol, and automobile emission are the most important contributors to visibility degradation. Soil/dust and sea salt/road salt also have an added effect.     

Health Effects of Fine Particulate Air Pollution: Lines that Connect

Abstract

Efforts to understand and mitigate the health effects of particulate matter (PM) air pollution have a rich and interesting history. This review focuses on six substantial lines of research that have been pursued since 1997 that have helped elucidate our understanding about the effects of PM on human health. There has been substantial progress in the evaluation of PM health effects at different time-scales of exposure and in the exploration of the shape of the concentration-response function. There has also been emerging evidence of PM-related cardiovascular health effects and growing knowledge regarding interconnected general pathophysiological pathways that link PM exposure with cardiopulmonary morbidity and mortality. Despite important gaps in scientific knowledge and continued reasons for some skepticism, a comprehensive evaluation of the research findings provides persuasive evidence that exposure to fine particulate air pollution has adverse effects on cardiopulmonary health. Although much of this research has been motivated by environmental public health policy, these results have important scientific, medical, and public health implications that are broader than debates over legally mandated air quality standards.     

Source Identification and Trends in Concentrations of Gaseous and Fine Particulate Principal Species in Seoul,South Korea

Abstract

Ambient measurements were made using two sets of annular denuder system during the four seasons (April 2001 to February 2002) and were then compared with the results during the period of 1996–1997 to estimate the trends and seasonal variations in concentrations of gaseous and fine particulate matter (PM_2.5) principal species. Annual averages of gaseous HNO₃ and NH₃ increased by 11% and 6%, respectively, compared with those of the previous study, whereas HONO and SO₂ decreased by 11% and 136%, respectively. The PM_2.5 concentration decreased by ～17%, 35% for SO₄ ^2?, and 29% for NH₄ ⁺, whereas NO₃ ^? increased by 21%. Organic carbon (OC) and elemental carbon (EC) were 12.8 and 5.98 μg/m^-3, accounting for ～26 and 12% of PM_2.5 concentration, respectively. The species studied accounted for 84% of PM_2.5 concentration, ranging from 76% in winter to 97% in summer.

Potential source contribution function (PSCF) analysis was used to identify possible source areas affecting air pollution levels at a receptor site in Seoul. High possible source areas in concentrations of PM_2.5, NO₃ ^?, SO₄ ^2?, NH₄ ⁺, and K⁺ were coastal cities of Liaoning province (possibly emissions from oil-fired boilers on ocean liners and fishing vessels and industrial emissions), inland areas of Heibei/Shandong provinces (the highest density areas of agricultural production and population) in China, and typical port cities (Mokpo, Yeosu, and Busan) of South Korea. In the PSCF map for OC, high possible source areas were also coastal cities of Liaoning province and inland areas of Heibei/Shandong provinces in China. In contrast, high possible source areas of EC were highlighted in the south of the Yellow Sea, indicating possible emissions from oil-fired boilers on large ships between South Korea and Southeast Asia. In summary, the PSCF results may suggest that air pollution levels in Seoul are affected considerably by long-range transport from external areas, such as the coastal zone in China and other cities in South Korea, as well as Seoul itself.     

Sources of Atmospheric Carbonaceous Particulate Matter in Pittsburgh,Pennsylvania

Abstract

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 particu-late 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 on SOA contribution to the total organic PM concentration, varying from near zero during winter months to 50% or more of the total OC concentration in the summer.     

Removal of Ultrafine and Fine Particulate Matter from Air by a Granular Bed Filter

Abstract

The removal efficiency of granular filters packed with lava rock and sand was studied for collection of airborne particles 0.05–2.5 μm in diameter. The effects of filter depth, packing wetness, grain size, and flow rate on collection efficiency were investigated. Two packing grain sizes (0.3 and 0.15 cm) were tested for flow rates of 1.2, 2.4, and 3.6 L/min, corresponding to empty bed residence times (equal to the bulk volume of the packing divided by the airflow rate) in the granular media of 60, 30, and 20 sec, respectively. The results showed that at 1.2 L/min, dry packing with grains 0.15 cm in diameter removed more than 80% (by number) of the particles. Particle collection efficiency decreased with increasing flow rate. Diffusion was identified as the predominant collection mechanism for ultrafine particles, while the larger particles in the accumulation mode of 0.7–2.5 μm were removed primarily by gravitational settling. For all packing depths and airflow rates, particle removal efficiency was generally higher on dry packing than on wet packing for particles smaller than 0.25 μm. The results suggest that development of biological filters for fine particles is possible.     

The Formation of Reactive Oxygen Species Catalyzed by Neutral,Aqueous Extracts of NIST Ambient Particulate Matter and Diesel Engine Particles

ABSTRACT

It is important to characterize the chemical properties of particulate matter in order to understand how low doses, inhaled by a susceptible population, might cause human health effects. The formation of reactive oxygen species catalyzed by neutral, aqueous extracts of two ambient par-ticulate samples, National Institute of Standards & Technology (NIST) Standard Reference Materials (SRM) 1648 and 1649, and two diesel particulate samples, NIST SRM 1650 and SRM 2975, were measured. The formation of reactive oxygen species was estimated by measuring the formation of malondialdehyde from 2-deoxyribose in the presence of ascorbic acid; H₂O₂ was not added to this assay. SRM 1649, ambient particulate matter collected from Washington, DC, generated the most malondialdehyde, while SRM 2975, diesel particulate matter collected from a forklift, yielded the least amount. Desferrioxamine inhibited the formation of malondialdehyde from the par-ticulate samples providing additional data to support the observation that transition metals were involved in the generation of reactive oxygen species. Six transition metal sulfates (iron sulfate, copper sulfate, vanadyl sulfate, cobalt sulfate, nickel sulfate, and zinc sulfate) were assayed     

Characterization and Identification of Trends in Average Ambient Ozone and Fine Particulate Matter Levels through Trajectory Cluster Analysis in Eastern Canada

Abstract

In many locations in Eastern Canada, ambient levels of fine particulate matter (PM_2.5) and surface ozone (O₃) depend on airflow direction and synoptic scale meteorological conditions. In this study, a cluster analysis was performed on 10 yr (1994 –2003) of back-trajectory data for 11 locations in Eastern Canada, resulting in the identification of 10 unique back-trajectory clusters (or airflows) for each location. The airflows were then used to characterize and identify spatial and temporal trends in the daily maximum 8-hr average O₃ (dmax 8-hr O₃) and the daily average PM_2.5 levels. Results showed that airflows from the southwest passing over Michigan and Southern Ontario were associated, on average, with the highest O₃ levels at most locations in Eastern Canada.For PM_2.5, the highest levels occurred with airflows from the Eastern Ohio River Valley. At major urban locations in Ontario and Quebec, the warm season mean (May to September) dmax 8-hr O₃ and the annual mean PM_2.5 were, on average, 12 parts per billion and 7.6 μg/m³ higher, respectively, than airflows from the north. Elevated levels of O₃ and PM_2.5 also occurred under light airflows, and, on average, the levels under light airflows were higher than their nonlight counterparts. At several locations in Canada, including Toronto, Montreal, Quebec City, and Kejimkujik, the annual warm season mean dmax 8-hr O₃ experienced a statistically significant (95% confidence) increasing trend over the 10-yr period. When airflow direction was considered, a number of locations experienced statistically significant upward trends in O₃ for airflow from the north and northwest. Several locations also showed significant upward trends associated with airflow from the southwest passing over Michigan and Southwestern Ontario. Although there are no statistically significant downward trends, airflows from the southwest have shown a reduction in O₃ levels in Southwestern Ontario in more recent years.     

Measurement of Particulate Bound Mercury,Gaseous Elemental Mercury,and Reactive Gaseous Mercury Concentrations by Using an Ambient Air Mercury Collection System

In this investigation, the concentrations of gaseous elemental mercury (GEM), reactive gaseous mercury (RGM) and particulate bound mercury (PBM) in ambient air were measured at the Hung Kuang (traffic) sampling site during September 27 to October 6, 2014. An ambient air mercury collection system (AAMCS) was utilized to measure simultaneously PBM, GEM, and RGM concentrations in ambient air. The results thus obtained demonstrate that the mean concentrations of PBM, GEM, and RGM were 38.57 ± 11.4 (pg/m³), 17.67 ± 5.56 (ng/m³) and 10.78 ± 2.8 (pg/m³), respectively, at this traffic-sampling site. The mean GEM/PBM and GEM/RGM concentration ratios were 458 and 1639, respectively. The results obtained herein demonstrate that AAMCS can be utilized to collect three phases of mercury simultaneously. The mean PBM, GEM, and RGM concentrations herein were compared with others found in Asia, America, Europe and Antarctica. The mean PBM, GEM, and RGM concentrations were found to be lowest in Asia and Antarctica. The mean PBM concentration in Europe was approximately eight times that in this investigation. The mean GEM and RGM concentrations in this study were 1.21 and 170 times those found in the United States.     

Determination of Levoglucosan in Atmospheric Fine Particulate Matter

Abstract

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-β-D-altro-heptulopyranose) in 20 μL 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 μg levoglu-cosan, and the reproducibility of the assay is 9%. The limit of detection is ～0.1 μg/mL, which is equivalent to ～3.5 ng/m³ for a 10 L/min sampler or ～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 ≤2.5 μm or PM with aerodynamic diameter ≤10 μm 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.     

Exposure of Chronic Obstructive Pulmonary Disease Patients to Particulate Matter: Relationships between Personal and Ambient Air Concentrations

ABSTRACT

Most time-series studies of particulate air pollution and acute health outcomes assess exposure of the study population using fixed-site outdoor measurements. To address the issue of exposure misclassification, we evaluate the relationship between ambient particle concentrations and personal exposures of a population expected to be at risk of particle health effects.

Sampling was conducted within the Vancouver metropolitan area during April-September 1998. Sixteen subjects (non-smoking, ages 54-86) with physician-diagnosed chronic obstructive pulmonary disease (COPD) wore personal PM_{2 5} monitors for seven 24-hr periods, randomly spaced approximately 1.5 weeks apart. Time-activity logs and dwelling characteristics data were also obtained for each subject. Daily 24-hr ambient PM₁₀ and PM_2.5 concentrations were measured at five fixed sites spaced throughout the study region. SO₄ ^2-, which is found almost exclusively in the fine particle fraction and which does not have major indoor sources, was measured in all PM_{2 5} samples as an indicator of accumulation mode particu-late matter of ambient origin.     

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   

Distribution of Light Hydrocarbons in Ambient Air

The diversity of hydrocarbons which are present in ambient polluted air provide a potentially rich source of information concerning the nature of this type of pollution. Measurements of the relative amounts of various hydrocarbons can be correlated with the various possible sources. Since hydrocarbon reactivities vary widely it is also possible to estimate the extent to which various individual hydrocarbons have reacted. Except for samples taken deliberately near sources of hydrocarbon pollution these air samples invariably resemble auto exhaust with an addition of natural gas and of C₃–C₅ paraffins which resemble gasoline vapor. Samples taken in industrial areas and near the smoke plume from a brush fire showed distinctive differences in composition. During the smog season in the fall of 1968 good data were obtained of “typical” or “representative” samples of light, medium and heavy smog. These show the expected depletion of more reactive hydrocarbons in a much more convincing way than before. By comparing these distributions with composition in unreacted samples and by making use of data from bottle irradiations, it was possible to estimate the contribution of the various hydrocarbons in terms of “amount reacted.” The amounts of higher hydrocarbons present and reacted were also estimated from gasoline composition.     

Regional Monitoring of Ambient Air Carbon Monoxide in Fairbanks,Alaska

A method employing the timed fill of Mylar bags was used to obtain average carbon monoxide concentration values for ten locations in the Fairbanks, Alaska, area. The method is shown to be accurate, reliable, and inexpensive. The correlation coefficient between the bag sampling method and a continuous carbon monoxide analyzer was 0.945; correlation of carbon monoxide data from several locations to a reference in downtown Fairbanks showed a general decrease with distance from the reference analyzer. Analysis of data from Fairbanks shows that carbon monoxide concentrations during the winter months may have to be reduced 50-75% to achieve the State and National Ambient Air Quality Standards; the high levels of carbon monoxide are the result of emissions from automobile traffic during periods of severe inversion in the Fairbanks basin.     

Characterization of Carbonaceous Species of Ambient PM2.5 in Beijing,China

Abstract

One-week integrated fine particulate matter (i.e., particles <2.5 μm in diameter; PM_2.5) samples were collected continuously with a low-flow rate sampler at a downtown site (Chegongzhuang) and a residential site (Tsinghua University) in Beijing between July 1999 and June 2000. The annual average concentrations of organic carbon (OC) and elemental carbon (EC) at the urban site were 23.9 and 8.8 μg m^?3, much higher than those in some cities with serious air pollution. Similar weekly variations of OC and EC concentrations were found for the two sampling sites with higher concentrations in the winter and autumn. The highest weekly variations of OC and EC occurred in the winter, suggesting that combustion sources for space heating were important contributors to carbonaceous particles, along with a significant impact from variable meteorological conditions. High emissions coupled with unfavorable meteorological conditions led to the max weekly carbonaceous concentration the week of November 18–25, 1999. The weekly mass ratios of OC:EC ranged between 2 and 4 for most samples and averaged 2.9, probably suggesting that secondary OC (SOC) is present most weeks. The range of contemporary carbon fraction, based on the C14 analyses of eight samples collected in 2001, is 0.330–0.479. Estimated SOC accounted for ～38% of the total OC at the two sites. Average OC and EC concentrations at Tsinghua University were 25% and 18%, respectively, higher than those at Chegongzhuang, which could be attributed to different local emissions of primary carbonaceous particles and gaseous precursors of SOC, as well as different summer photochemical intensities between the two locations.     

Impact of Toll Removal on Air Particulate Concentration in Jacksonville,Florida

The concentration of total suspended particulate (TSP) matter was determined at commercial, residential, rural and industrial sites in metropolitan Jacksonville during the summers of 1989 and 1990. These data were compared to samples taken at the Mathews Bridge Toll Plaza in 1989 and at a similar location one year later, after removal of the toll facility. All samples were analyzed by reflectance analysis and the approximate elemental carbon content used to estimate the contribution of vehicular traffic at the roadway. The results indicate a significant improvement in air quality at the location of the previous toll facility, but did not show that a widespread improvement resulted from the removal of tolls in Jacksonville, Florida.     

Contamination of the Lake Tahoe Air Basin by High Molecular Weight Petroleum Residues

The atmosphere of the Lake Tahoe air basin is contaminated with high molecular weight (> C₁₂) petroleum hydrocarbons. Aerosol samples were collected by high-volume filtration and the solvent-soluble organic matter was analyzed. The relative concentrations of petroleum residues found were as follows: winter > summer and day > night. This contamination is primarily due to the poorer combustion of diesel and home heating fuels at that altitude and during periods of colder climate.     

Evaluation of the Effects of Emission Reductions on Secondary Particulate Matter in the South Coast Air Basin of California

An Aerosol Trajectory Model (ATM) is applied to the South Coast Air Basin of California for a two-day episode in August 1982 to evaluate proposed control strategies that aim to reduce atmospheric aerosols. Model predictions Indicate that secondary organic aerosols decrease linearly with reactive hydrocarbon emissions. In addition, the model shows that If sulf ate is produced only in the gas phase by oxidation of SO₂, then reduction In SO₂ emissions yields a nearly proportional decrease In sulfate levels. Reduction in ammonia emissions, combined with reduction of NO_x emissions, gives the best results In terms of nitrate control. The order in which the emission controls are implemented Is predicted to have a major impact on the reduction of secondary atmospheric aerosols.     

Apportionment of Ambient Primary and Secondary Fine Particulate Matter during a 2001 Summer Intensive Study at the CMU Supersite and NETL Pittsburgh Site

Abstract

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 (PM_2.5) into primary and secondary contributions using PMF2. Input to the PMF2 analysis included the concentrations of PM_2.5 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 PM_2.5 were sec ondary 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 PM_2.5. 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.     

总量控制与太湖流域水污染治理——《太湖流域水环境综合治理总体方案》述评

《太湖流域水环境综合治理总体方案》是针对太湖流域的新型总量控制计划,代表中国水污染物总量控制计划的巨大进步。它与美国的每日最大总负荷(TMDL)计划比较相似。该方案的编制技术路线合理,要素比较齐全。然而该方案也存在明显缺陷。该方案的未来修订有必要考虑城市径流,提高安全余量,考虑季节性差异,提高阶段性总量控制目标和水质目标,阐明终极水质目标和总量控制目标。