The Relative Influences of Primary and Secondary Particulates to Urban Air Quality in the United Kingdom

This study uses a combination of data from U.K. monitoringstations and from modelling undertaken with the U.K.Meteorological Office's NAME Model to investigate therelative influences of primary and secondary particulateson total PM₁₀ levels at sites in the United Kingdom. Co-located PM₁₀ and sulphate aerosol measurementsindicate that sulphate has a disproportionately largeinfluence on the variation of PM₁₀ levels incomparison to its contribution to their total mass.Comparisons of measured PM₁₀ at urban centre, roadsideand rural sites suggest that local primary sources havevery little influence on daily mean levels. NAME has beenused to model both primary particles and sulphate aerosolfrom sources across the whole of Europe. The discrepanciesbetween modelled and observed PM₁₀ suggest that coarseparticles, such as windblown dust and resuspended roaddust,may comprise a very large, if not dominant, proportion ofobserved PM₁₀ levels. The apparently minor role ofprimary particles (especially locally-sourced ones) raisesa number of issues regarding the suitability of current U.K.and European legislation to addressing the particle problem.     

Characteristics of air pollution in Beijing during sand-dust storm periods

In the Beijing area, March and April have the highest frequency of sand-dust weather. Floating dust, blowing sand, and dust storms, primarily from Mongolia, account for 71%, 20%, and 9% of sand-dust weather, respectively. Ambient air monitoring and analysis of recent meteorological data from Beijing sand-dust storm periods revealed that PM₁₀ mass concentrations during dust storm events remained at 1500 μg m⁻³, which is five to ten times higher than during non-dust storm periods, for fourteen hours on both April 6 and 25, 2000. During the same period, the concentrations in urban areas were comparable to those in suburban areas, while the concentrations of gaseous pollutants, such as SO₂, NO _x , NO₂, and O₃, remained at low levels, owing to strong winds. Furthermore, during sand-dust storm periods, aerosols were created that consisted not only of many coarse particles, but also of a large quantity of fine particles. The PM_2.5 concentration was approximately 230 μg m⁻³, accounting for 28% of the total PM₁₀ mass concentration. Crustal elements accounted for 60–70% of the chemical composition of PM_2.5, and sulfate and nitrate for much less, unlike the chemical composition of PM_2.5 on pollution days, which was primarily composed of sulfates, nitrates, and organic material. Although the very large particle specific surface area provided by dust storms would normally be conducive to heterogeneous reactions, the conversion rate from SO₂ to SO₄ ²⁻ was very low, because the relative humidity, less than 30%, was not high enough.     

Formation and Transport of Atmospheric Aerosol over Athens, Greece

The effects of meteorology on ambient aerosol concentrations and aerosol transport, within the Greater Athens Area during the summer period, was investigated. Measurements of size fractionated anions and cations were made at two sites (inland at Ag. Stefanos and on the coast at Pireas) within the Greater Athens Area. The wind regime exhibited a distinctinfluence such that the sea-breeze circulation strongly enhanced the formation of secondary aerosols. For sulphate the difference in concentration between the two sites was,on average, 8 times greater on sea-breeze days compared with Etesian days (warm days with NE winds). During `normal' days,any differences in concentrations were possibly due to localemissions. Elevated concentrations in the fine mode were detectedat both sites during the sea-breeze days. The sea-breezecirculation enhances the development of secondary aerosolswhich was clearly shown at the inland site. Nitrous acid,hydrochloric acid and particulate nitrate, sulphate andammonium increase during sea-breeze days. Elevated levelsof nitrate, 4 m diameter, were particularly observedon the days with a strong sea-breeze circulation. Sulphatewas well correlated with both sulphur dioxide and ammoniumsuggesting the production of NH₄HSO₄/(NH₄)₂SO₄ aerosols, formedthrough the neutralisation of NH₃ with sulphuric acids.Ammonium sulphate was found to be the major ammoniumcomponent in Athens.     

Source Apportionment in the Town of La Spezia (Italy) by Continuous Aerosol Sampling and PIXE Analysis

We describe the results of an aerosol sampling campaign performedin 1999 in the medium-size industrial town of La Spezia, in theNorthwest of Italy. We used two-stage continuous streakersamplers in three different sites and periods of the year. This kind of samplers allows the separation of the PM₁₀ andPM_2.2 fractions of the particulate matter. Moreover, the hourly resolution in the aerosol collection is particularly useful inan urban environment where, typically, many pollution sourceswith fast variations are present. Up to 1700 samples have beenanalysed by Particle Induced X-ray Emission (PIXE) at the INFNaccelerator facility in Florence, obtaining hourly concentrationfor about 20 elements from Na to Pb, with a sensitivity rangingfrom below 1 to about 10 ng m^-3. The total hourly aerosolmass has been estimated with an optical analysis of the samesamples performed (before the PIXE analysis) by an equipment designed and mounted in Genoa. An extensive statistical analysisof the data included standard and Absolute Principal ComponentFactor Analysis (PCFA and APCFA) to deduce the compositionand the weight of the major aerosol sources in both fractions.Thorough different statistical approaches, we generally resolvedcontributions from vehicle emission, fossil fuel combustion,soil-road dust and sea salt aerosol.     

Modeling of Combined Aerosol and Photooxidant Processes in the Mediterranean Area

The combined UAM-AERO/RAMS modeling system has been applied to study the dynamics of photochemical gaseous species and particulate matter processes in the eastern Mediterranean area between the Greek mainland and the island of Crete. In particular, the modeling system is applied to simulate atmospheric conditions for two periods, i.e., 13-16 July 2000 and 26-30 July 2000. The spatial and temporal distributions of both gaseous and particulate matter pollutants have been extensively studied together with the identification of major emission sources in the area. New pre-processors were developed for the UAM-AERO model for evaluating detailed emission inventories for biogenic compounds, resuspended dust and sea salt. Comparison of the modeling results with measured data was performed and satisfactory agreement was found for a number of gaseous species. However, the model underestimates the PM₁₀ measured concentrations during summer. This is mainly due to the considerable underestimation of particulate matter emissions and in particular dust resuspension, the effect of forest fire emissions and the contribution of Saharan dust episodes.     

Identification of PM10 Sources in a Mediterranean Island

Due to the dry Mediterranean climate in Cyprus, particulate matter is resuspended from soils and other surfaces. From November 2002 to August 2003, gravimetric PM₁₀ measurements were carried out at three characteristic sites (traffic, residential and rural). A significant seasonal trend with high winter concentrations was observed at the traffic site. Special events, e.g. long-range transport of Sahara dust storms, were recorded over traffic, residential and rural areas in the order of six to eight events per year, with a major frequency in summer and spring periods. This contributes to the increase of 24-h EU limit value exceedances for PM₁₀ at the three investigated sites. The origin of the PM₁₀ load was determined by enrichment factors based on analyses of the local soil deposition at the investigated sites. Furthermore, positive matrix factorisation modelling was applied to find the sources of PM₁₀. Results indicate that the major emission sources affecting the PM₁₀ load were mineral soil, sea salt, road dust, oil combustion, secondary pollutants and gasoline vehicles. The natural contribution (local mineral soil and sea salt) at the three sites was in the range of 7–9 μg m^?3 in PM₁₀. Besides the Sahara dust storms and natural background concentrations, the vehicular pollution was found as the largest contributor (12–14 μg m^?3) to PM₁₀ load at the traffic site.     

Comparison of PM2.5 and PM10 in A Suburban Area in Korea During April, 2003

Airborne particulate matter (PM) concentrations were measured in Iksan, a suburban area in South Korea during April, 2003. PM_2.5 (particles with an aerodynamic diameter less than 2.5 μm) and PM₁₀ (particles with an aerodynamic diameter less than 10 μm) samples were collected, and the chemical characteristics of particles were examined for diurnal patterns, yellow dust/rainfall influences, and scavenging effects. Average concentrations of PM_2.5 and PM₁₀ mass measured were 37.3 ± 16.2 μg m⁻³ and 60.8 ± 29.5 μg m⁻³, respectively. The sum of ionic chemical species concentrations for PM_2.5 and PM₁₀ was 16.9 ± 7.3 and 23.1 ± 10.1 μg/m³, respectively. A significant reduction in PM mass concentrations during rainfall days was observed for coarse mode (PM_{2.5 − 10}) particles, but less reduction was found for fine (PM_2.5) mass concentration. SO₄ ²⁻, NH₄ ⁺, and K⁺ predominated in fine particulate mode, NO₃ ⁻ and Cl⁻ predominated in fine particle mode and coarse particle mode, but Na⁺, Mg²⁺, and Ca²⁺ mostly existed in coarse mode. The high concentration of ammonium due to local emissions and long-range transport neutralized sulfate and nitrate to ammonium sulfate and ammonium nitrate, which were major forms of airborne PM in Iksan. Average mass concentrations of PM₁₀ in daytime and at night were 57.6 and 70.0 μg m⁻³, and those of PM_2.5 were 35.4 and 42.5 μg m⁻³, respectively. NO₃ ⁻ and Cl⁻ in both PM_2.5 and PM₁₀ were about double at night than in the daytime, while the rest of the chemical species were equal or a little higher at night than in the daytime. The results suggest the formation of ammonium nitrate and chloride when high ammonia concentration and low air temperature are allowed. Backward air trajectory analyses showed that air masses arriving at the site during yellow dust period were transported from arid Chinese regions, which resulted in high concentrations of airborne PM mass concentrations. In the meantime, air mass trajectories during a rainfall period were mostly from the Pacific Ocean or the East China Sea, along with a relatively low PM concentration.     

The effect of dust emissions from open storage piles to particle ambient concentration and human exposure

The current study focus on the determination of dust emissions from piles in open storage yards of a municipal solid waste (MSW) composting site and the subsequent atmospheric dust dispersion. The ISC3-ST (Industrial Source Complex Version 3 – Short Term) model was used for the evaluation of the PM₁₀ ambient concentrations associated with the dispersion of MSW compost dust emissions in air. Dust emission rates were calculated using the United States Environmental Protection Agency proposed dust resuspension formulation from open storage piles using local meteorological data. The dispersion modelling results on the spatial distribution of PM₁₀ source depletion showed that the maximum concentrations were observed at a distance 25–75 m downwind of the piles in the prevailing wind direction. Sensitivity calculations were performed also to reveal the effect of the compost pile height, the friction velocity and the receptor height on the ambient PM₁₀ concentration. It was observed that PM₁₀ concentrations (downwind in the prevailing wind direction) increased with increasing the friction velocity, increasing the pile height (for distances greater than 125 m from the source) and decreasing the receptor height (for distances greater than 125 m from the source). Furthermore, the results of ISC3-ST were analysed with the ExDoM (Exposure Dose Model) human exposure model. The ExDoM is a model for calculating the human exposure and the deposition dose, clearance, and finally retention of aerosol particles in the human respiratory tract (RT). PM₁₀ concentration at the composting site was calculated as the sum of the concentration from compost pile dust resuspension and the background concentration. It was found that the exposure to PM₁₀ and deposited lung dose for an adult Caucasian male who is not working at the composting site is less by 20–74% and 29–84%, respectively, compared to those for a worker exposed to PM concentrations at the composting site.     

On East Asian Sand and Duststorms and Associated Significant Dustfall Observed from January to May 2001

Monitoring of dust pollution at the western shore of Tae-ahn Peninsula (TAP) and in the Chongju area of central Korea was carried out from January to May 2001. It was found that in Koreathere were 9 cases of sand and duststorms (DS) and 16 associatedsignificant dustfall (SD) days. Observed maximum concentrations of DS and SD coming from NW China and Mongolia were in the rangeof 300–920 for TSP, 200–690 for PM₁₀ and 100–170 g m^-3 for PM_2.5.Satellite measurements clearly showed the formation and subsequent movement of DS to the Korean Peninsula and onward to the Korea East Sea, Japan and the Gulf of Alaska. According to satellite image analysis of dust clouds there were abundant coarse particles, measuring in size of 11.0 m. Medium-sizedparticles measuring in the range of 3.5–7.0 were also prevalent,while fine particles of less than 2.0 m were less distinctive in reflectivity. Measured values of PM_2.5 were alsorelatively low with SD events.The measured average pH values of dusty precipitation associatedwith DS were 7.24. Alkaline precipitation can play a `temporary'role in the neutralization of acidified soil until the subsequentevent of acidic rain. The new selection criteria of SD days from PM_2.5 at 85 g m^-3, PM₁₀ 190 g m^-3 and TSP 250 g m^-3 are recommended on dust pollution occurring from the invasion of a DS elsewhere.     

The Spatial and Temporal Variation of Measured Urban PM10 and PM2.5 in the Helsinki Metropolitan Area

We have studied particulate matter (PM) concentrations,PM₁₀ and PM_2.5, measured in an urban air qualitymonitoring network in the Helsinki Metropolitan Area during1997–1999. The data includes PM₁₀ concentrationsmeasured at five locations (two urban traffic, one suburbantraffic, one urban background and one regional backgroundsite) and PM_2.5 concentrations measured at twolocations (urban traffic and urban background sites). Theconcentrations of PM₁₀ show a clear diurnal variation,as well as a spatial variation within the area. Bycontrast, both the spatial and temporal variation of thePM_2.5 concentrations was moderate. We have analysedthe evolution of urban PM concentrations in terms of therelevant meteorological parameters in the course of oneselected peak pollution episode during 21–31 March, 1998.The meteorological variables considered included wind speedand direction, ambient temperature, precipitation, relativehumidity, atmospheric pressure at the ground level,atmospheric stability and mixing height. The elevated PMconcentrations during the 1998 March episode were clearlyrelated to conditions of high atmospheric pressure,relatively low ambient temperatures and low wind speeds inpredominantly stable atmospheric conditions. The resultsprovide indirect evidence indicating that the PM₁₀concentrations originate mainly from local vehiculartraffic (direct emissions and resuspension), while thePM_2.5 concentrations are mostly of regionally andlong-range transported origin.     

Comparison of Surface Organic Compound Mass Spectrum Patterns by LD-TOFMS for Megalopolis Atmospheric Particles and Diesel Exhaust Particles (DEP)

PM_2.5 and PM₁₀ samples for megalopolis atmospheric particles were collected at Shinjuku, Tokyo in December 1998–January 1999 and August 1999, for two weeks both in winter and summer, with a 24 hr sampling interval. Sampling of PM_2.5 and PM₁₀ in diesel exhaust particles (DEP) was carried out using an automobile exhaust testing system, with a diesel truck placed on a chassis dynamometer. Sampling conditions included idling, constant speed of 40 km hr^-1, M-15 test pattern and 60%-revolution/40%-load of maximum power. Mass spectrums of organic compounds adhering to the surface of the PM_2.5 and PM₁₀ samples were analyzed by laser desorption time-of-flight mass spectrometry (LD-TOFMS, analytical mass range: m/z 1–m/z 380 000). LD-TOFMS analysis of those samples revealed consistently the detection of low-mass organic compounds up to m/z 800. For the megalopolis atmospheric particles, the mass spectrum pattern of wintertime samples was almost the same as that of the summertime samples for both PM_2.5 and PM₁₀. The major peak was m/z 177, and the minor peaks were m/z 84, 94, 101, 163, 189 and 235. The mass spectrum pattern of DEP was the same for all samples under all test conditions. The major peak was m/z 101, and other detected peaks were small.     

Atmospheric Loadings,Concentrations and Visibility Associated with Sandstorms: Satellite and Meteorological Analysis

This Korea-China study monitored the phenomena of sandstorms and significant dustfall (SD) from 1997 to 2000. The analysis of our data included ground measurements of dust concentration, visibility, satellite imagery, aircraft and lidar observations. In addition, an estimation of atmospheric loadings and a studyon the relationship between dust concentrations and visibilitywere carried out. The movement and invasion of dust clouds toKorea were clearly identified with meteorological and satellitedata. The increasing concentrations of TSP and PM₁₀ concurredwell with the satellite information. From case studies, weestimated that atmospheric loadings of a dust cloud were over 1million ton and that the deposition over the Korean Peninsulawas in the range from 46 000 to 86 000 tons. For SD withvisibility of 3 km, we predict TSP 659 g m^-3 and PM₁₀ 493 g m^-3. We recommend the issuance of an SD Watch(advisory) and an SD Warning for the general public.     

Controlling Air Toxics Emissions From Remediation by Monitoring of Surrogate Parameters

Particulate matter (dust) from remediation and demolition sites may pose a potential risk to the nearby public due to the presence of various contaminants. Unfortunately, there are no good options for real‐time monitoring of metals, polychlorinated biphenyls, etc. in wind‐blown dust. A three‐tiered approach involving a combination of real‐time monitoring and off‐site analysis that has proved successful is described in this article. PM₁₀ is used as a surrogate parameter for metals and other nonvolatile pollutants, and real‐time monitoring is used to guide dust control measures. If dust emissions are controlled, air emissions of metals and other nonvolatile pollutants also are controlled. © 2014 Wiley Periodicals, Inc.     

Heterogeneous Sulfate Formation on Dust Surface and Its Dependence on Mineralogy: Balloon-Borne Observations from Balloon-Borne Measurements in The Surface Atmosphere of Beijing, China

This study focuses on providing a direct insight into the process by which sulfate is formed on mineral dust surface in the actual atmosphere. Six sets of aerosol measurements were conducted in the outskirts of Beijing, China, in 2002–2003 using a tethered balloon. The mineralogy of individual dust particles, as well as its influence on the S (sulfur) loadings was investigated by SEM-EDX analysis of the directly collected particles. The mixed layer in the urban atmosphere was found to be quite low (500–600m), often appearing as a particle dense stagnant layer above the surface. It is suggested that mineral dust is a common and important fraction of the coarse particles in Beijing (35–68%), and that it is relatively enriched with Calcite (>28%). An exceptional amount of S was detected in the mineral particles, which can be explained neither by their original composition, nor by coagulation processes between the submicron sulfates and the dust. Heterogeneous uptake of gaseous SO₂, and its subsequent oxidation on dust was suggested as the main pathway that has actually taken place in the ambient environment. The mineral class found with the largest number of particles containing S was Calcite, followed by Dolomite, Clay, Amphibole etc., Feldspar, and Quartz. Among them, Calcite and Dolomite showed distinctly higher efficiency in collecting sulfate than the other types. A positive correlation was found with the number of S containing particles and the relative humidity. Calcite in particular, since almost all of its particles was found to contain S above 60% r.h. On the other hand, the active uptake of SO₂ by the carbonates was not suggested in the free troposphere downwind, and all the mineral classes exhibited similar S content. Relative humidity in the free troposphere was suggested as the key factor controlling the SO₂ uptake among the mineral types. In terms of sulfate loadings, the relationship was not linear, but rather increased exponentially as a function of relative humidity. The humidity-dependent uptake capacity of mineral types altogether showed an intermediate value of 0.07 gSO₄ ²⁻ g⁻¹ mineral at 30% r.h. and 0.40 gSO₄ ²⁻ g⁻¹ mineral at 80%, which is fairly consistent with laboratory experiments.     

Fate and behavior of selected heavy metals with mercury mass distribution in a fluidized bed sewage sludge incinerator

In this paper, emission and distribution behavior of six heavy metals (As, Cd, Cr, Ni, Pb, and Hg), particulate matter and mass distribution of mercury within the different streams of a fluidized bed sewage sludge incinerator are presented. At the inlet of air pollution control devices (APCDs); Cd, Cr, Ni and Pb were mainly enriched in coarse particles; comparatively As content was higher in fine particles (<PM_2.5). The concentration of heavy metals in total particulate matter and PM_2.5, at the inlet of APCDs, were in the order of Cr > Ni > Pb > As > Cd. Mercury was almost always distributed in flue gas. Metals, other than mercury, were efficiently removed in APCDs and their concentrations in bottom ash, with fly ash being higher, whereas for that in wastewater, then waste sand was lesser. Overall mercury removal efficiency of APCDs was 98.6 %. More than 83.3 % of mercury was speciated into oxidized form at the inlet of APCDs, attributed by higher chlorine content in sludge. Mercury was mainly distributed in wastewater (78.4 %), wastewater from a spray dry reactor (16.8 %), fly ash in a hopper (3.4 %) and flue gas (1.4 %). This result is one of the first for data to be obtained; more experiments are required to control emission from such sources.     

Measurements of particulate matter concentrations at a landfill site (Crete,Greece)

Large amounts of solid waste are disposed in landfills and the potential of particulate matter (PM) emissions into the atmosphere is significant. Particulate matter emissions in landfills are the result of resuspension from the disposed waste and other activities such as mechanical recycling and composting, waste unloading and sorting, the process of coating residues and waste transport by trucks. Measurements of ambient levels of inhalable particulate matter (PM₁₀) were performed in a landfill site located at Chania (Crete, Greece). Elevated PM₁₀ concentrations were measured in the landfill site during several landfill operations. It was observed that the meteorological conditions (mainly wind velocity and temperature) influence considerably the PM₁₀ concentrations. Comparison between the PM₁₀ concentrations at the landfill and at a PM₁₀ background site indicates the influence of the landfill activities on local concentrations at the landfill. No correlation was observed between the measurements at the landfill and the background sites. Finally, specific preventing measures are proposed to control the PM concentrations in landfills.     

Study of Asian Dust Phenomena in 2001–2003 Using A Network of Continuously Operated Polarization Lidars

We have conducted dust observations at a number of locations including Beijing, Hefei, Suwon, Fukue, Nagasaki, Tsukuba, and Sapporo using automated two-wavelength polarization lidars o study Asian dust phenomena, including generation, transport, and change during transport. We developed a method using the depolarization ratio for estimating the contributions of Asian dust and spherical air-pollution aerosols in observed aerosol mixtures. We analyzed the dust profiles statistically to derive climatological characteristics and year-on-year variations. We also studied dust source and transport path for each dust event using the regional chemical transport model CFORS. The statistical analysis clearly demonstrated the year-on-year variation of dust phenomena and the characteristics depending on the locations of the observational sites. Most major dust events in 2001 and 2002 originated in Inner Mongolia and/or Mongolia at the southern edge of a low-pressure area located in Siberia and were transported by strong westerlies. In 2003, the typical meteorological pattern for heavy dust cases accompanying a strong low in Siberia was not seen, except for one case in April. Furthermore, the lidar observation in Beijing suggests that less dust was generated in the source regions in Inner Mongolia and/or Mongolia, probably due to higher precipitation in 2003.     

On Sand and Duststorms and Associated Significant Dustfall Observed in Chongju-Chongwon,Korea during 1997–2000

Monitoring of the occurrence of sandstorms and dustfallphenomena from 1997 to 2000 was carried out. We refer tosandstorms, duststorms and blowing sand as the phenomenaoccurring in the source region, while significant dustfall is thephenomenon that occur in the sink area. It was noted that while the sandstorms in deserts and loess in NW-N China and Mongolia occurred any time during the year while severe sandstorms occurred frequently from March to May after the springthaw. The wind erosion in the source region usually occurred withwind speeds greater than 8 ms^-1. However, severe sandstorm phenomenon occurred with wind greater than 15 ms^-1 for at least 3 hr or more. In the source regions, sandstorms occurred over60–120 days per year. In Mongolia, the observation of thenumber of sandstorm days decreased due to the increase in rainy days.When a dust cloud from a desert reached the sink region,significant dustfall in the Korean Peninsula occurred due tothe lack of strong winds. We defined the episode ofsignificant dustfall (SD) with the following values: TSP250, PM₁₀ 190 g m^-3 and visibility 6.5 km or less. In Korea, 8–12 episodes of SD occurred per yearwith 12 to 22 SD days. The maximum concentrations of TSP recorded were 989–1396 g m^-3 with PM₁₀ values of 861–996 g m^-3 and with the lowestvisibility of 1.4–1.6 km.     

Deliquescence of Deposited Atmospheric Particles on Leaf Surfaces

A large fraction of deposited aerosol particles on leafsurfaces represents hygroscopic material in a high humidity environment, likely to become deliquescent within the water vapour transpired by the leaf. Microscopic observations on leaf surfaces of beech, kohlrabi and elder leaves grown in a particle-free environment and/or treated with defined particle load are presented. Spreading of deliquescent particles, formation of salt crusts, and encoating of and by waxes was observed. Deliquescence of NaNO₃ particles (deliquescence point 74% RH at 25 °C) was observed on and near the stomata at 35% relative humidity (RH) of the surrounding air, illustrating the influence of the boundary layer. Aerosols are difficult to identify on leaf surfaces, as similar patterns may be produced by deliquescent particles and processes like salt creep. These problems are especially important on leaves from the natural environment if only scanning electron microscopy (SEM) is used. These patterns could appear similar to the fused waxes described in forest decline research. Strong gradients are formed between deliquescent particles and the apoplastic solution within the leaf, promoting cuticular and stomatal uptake.