scholarly journals Chemical characterization of the inorganic fraction of aerosols and mechanisms of the neutralization of atmospheric acidity in Athens, Greece

2006 ◽  
Vol 6 (6) ◽  
pp. 12389-12431
Author(s):  
E. T. Karageorgos ◽  
S. Rapsomanikis ◽  
P. Wåhlin

Abstract. Mass concentration levels and the inorganic chemical composition of PM10 (two fractions; PM10−2.5 and PM2.5) were determined during August 2003 and March 2004, in the centre of Athens, Greece. August 2003 monthly mean PM10 mass concentration, at 5 m above ground, was 56 μg/m3 and the EU imposed daily limit of 50 μg/m3 was exceeded on 16 occasions. The corresponding monthly mean for March 2004 was 92 μg/m3 and the aforementioned daily limit was exceeded on 23 occasions. The PM10 (PM10−2.5+PM2.5) mass concentrations at 1.5 m above ground were found to be approximately 20% higher compared to the respective PM10 measured at 5 m. Consequently, for a realistic estimation of the exposure of citizens to particulate matter, PM10 sampling at a height of 1.5–3 m above ground, in the "breathing zone" is necessary. Such data are presented for the first time for the centre of Athens. In both campaigns, calcium was found to be the predominant component of the coarse fraction while crust-related aluminosilicates and iron were found to be the other major components of the same fraction. The above elements constitute the most important components of the fine fraction, together with the predominant sulphur. Toxic metals were found to be below the air quality limits and in lower concentrations compared to older studies, with the exception of Cu and V for which some increase was observed. Pb, in particular, appeared mostly in the fine fraction and in very low concentrations compared to studies dating more than a decade back. The major ions of the coarse fraction have been found to be Ca2+, NO3− and Cl−, while SO4−2, Ca2+ and NH4+ were the major ionic components of the fine fraction. The low molar ratio of NH4+/SO4−2 indicated an ammonium-poor ambient air, where atmospheric ammonia is not sufficient to neutralize all acidity and the formation of NH4NO3 does not occur to a significant extend. Calcium predominated the coarse fraction and its good correlations with NO3− and SO4−2 indicated its role as an important neutralizing agent of atmospheric acidity in this particle size range. In the fine fraction, both Ca2+ and NH4+ participate in the neutralizing processes with NH4+ being the major neutralizing agent of SO4−2. Chloride depletion from NaCl or MgCl2 was not found to occur to a significant extend. Total analyzed inorganic mass (elemental+ionic) was found to be ranging between approximately 25–33% of the total coarse particle mass and 35–42% of the total fine particle mass.

2007 ◽  
Vol 7 (11) ◽  
pp. 3015-3033 ◽  
Author(s):  
E. T. Karageorgos ◽  
S. Rapsomanikis

Abstract. The PM10 mass concentration levels and inorganic chemical composition were determined on 12-h resolution sampling during August 2003 and March 2004, in the centre of Athens, Greece. The August 2003 campaign mean PM10 mass concentration, obtained by Beta Attenuation at 5 m above ground in Athinas Street, was 56 μg m−3 while the corresponding value for March 2004 was 92 μg m−3. In both campaigns the E.U. imposed daily limit of 50 μg m−3 was exceeded on several days. During the March campaign, in Athinas Street, additionally obtained DSFU-PM10 (PM10-2.5+PM2.5) gravimetric mass concentrations (mean: 121 μg m−3) in the "breathing zone", at 1.5 m above ground were significantly higher compared to the respective mean PM10 mass concentrations obtained by the same method at 25 m above ground, in a second site (AEDA; mean: 86 μg m−3) also in the centre of the city. The above findings suggest that, for a realistic estimation of the exposure of citizens to particulate matter, PM10 sampling in the "breathing zone" (1.5–3 m above ground) is necessary. Such data are presented for the first time for the centre of Athens. In both campaigns, calcium was found to be the predominant component of the coarse fraction while crust-related aluminosilicates and iron were the other major components. The above elements constitute the most important components of the fine fraction, together with the predominant sulphur. All toxic metals were found in concentrations below the established air quality limits, and most of them in lower concentrations compared to older studies. Lead in particular, appeared mostly in the fine fraction and in very low concentrations compared to studies dating more than a decade back. The predominant ions of the coarse fraction have been found to be Ca2+, NO3−, Na+ and Cl−, while SO42−, Ca2+ and NH4+ were the major ionic components of the fine fraction. In the fine particles, a low molar ratio of NH4+/SO42− indicated an ammonium-poor ambient air, and together with inter-ionic correlations suggested that atmospheric ammonia is the major neutralizing agent of sulfate, while being insufficient to neutralize it to full extend. The formation of NH4NO3 is therefore not favored and additional contribution to the neutralization of acidity has been shown to be provided by Ca2+ and Mg2+. In the coarse particle fraction, the predominantly abundant Ca2+ has been found to correlate well with NO3− and SO42−, indicating its role as important neutralizing agent in this particle size range. The proximity of the location under study to the sea explains the important concentrations of salts with marine origin like NaCl and MgCl2 that were found in the coarse fraction, while chloride depletion in the gaseous phase was found to be limited to the fine particulate fraction. Total analyzed inorganic mass (elemental+ionic) was found to be ranging between approximately 25–33% of the total coarse particle mass and 35–42% of the total fine particle mass.


2007 ◽  
Vol 7 (6) ◽  
pp. 1657-1670 ◽  
Author(s):  
B. Guinot ◽  
H. Cachier ◽  
K. Oikonomou

Abstract. The aerosol chemical mass closure is revisited and a simple and inexpensive methodology is proposed. This methodology relies on data obtained for aerosol mass, and concentration of the major ions and the two main carbon components, the organic carbon (OC) and the black carbon (BC). Atmospheric particles are separated into coarse (AD>2 μm) and fine (AD<2 μm) fractions and are treated separately. For the coarse fraction the carbonaceous component is minor and assumption is made for the conversion factor k of OC-to-POM (Particulate Organic Matter) which is fixed to the value of 1.8 accounting for secondary species. The coarse soluble calcium is shown to display a correlation (regression coefficient f, y axis intercept b) with the missing mass. Conversely, the fine fraction is dominated by organic species and assumption is made for dust which is assumed to have the same f factor as the coarse mode dust. The fine mode mass obtained from chemical analyses is then adjusted to the actual weighed mass by tuning the k conversion factor. The k coefficient is kept different in the two modes due to the expected different origins of the organic particles. Using the f and k coefficient obtained from the data set, the mass closure is reached for each individual sample with an undetermined fraction less than 10%. The procedure has been applied to different urban and peri-urban environments in Europe and in Beijing and its efficiency and uncertainties on f and k values are discussed. The f and k coefficients are shown to offer consistent geochemical indications on aerosol origin and transformations. f allows to retrieve dust mass and its value accounting for Ca abundance in dust at the site of investigation may serve as an indicator of dust origin and aerosol interactions with anthropogenic acids. f values were found to vary in the 0.08–0.12 range in European urban areas, and a broader range in Beijing (0.01–0.16). As expected, k appears to be a relevant proxy for particle origin and ageing and varies in the 1.4–1.8 range. For Beijing, k exhibits high values of about 1.7 in winter and summer. Winter values suggest that fresh coal aerosol might be responsible for such a high k value, which was not taken into account in previous works.


2008 ◽  
Vol 42 (36) ◽  
pp. 8543-8548 ◽  
Author(s):  
A TITTARELLI ◽  
A BORGINI ◽  
M BERTOLDI ◽  
E DESAEGER ◽  
A RUPRECHT ◽  
...  

2006 ◽  
Vol 6 (6) ◽  
pp. 12021-12055 ◽  
Author(s):  
B. Guinot ◽  
H. Cachier ◽  
K. Oikonomou

Abstract. The aerosol chemical mass closure is revisited and a simple and inexpensive methodology is proposed. This methodology relies on data obtained for aerosol mass, and concentration of the major ions and the two main carbon components, the organic carbon (OC) and the black carbon (BC). Atmospheric particles are separated into coarse (AD>2µm) and fine (AD<2µm) fractions and are treated separately. For the coarse fraction the carbonaceous component is minor and assumption is made for the conversion factor k, of OC-to-POM (Particulate Organic Matter) which is fixed to the value of 1.8 accounting for secondary species. The coarse soluble calcium is shown to display a correlation (regression coefficient f, y axis intercept b) with the missing mass. Conversely, the fine fraction is dominated by organic species and assumption is made for dust which is assumed to have the same f factor as the coarse mode dust. The fine mode mass obtained from chemical analyses is then adjusted to the actual weighed mass by tuning the k conversion factor. The k coefficient is kept different in the two modes due to the expected different origins of the organic particles. Using the f and k coefficients obtained from the data set, the mass closure is reached for each individual sample with an undetermined fraction less than 10%. The procedure has been applied to different urban and peri-urban environments in Europe and in Beijing and its efficiency and uncertainties on f and k values are discussed. The f and k coefficients are shown to offer consistent geochemical indications on aerosol origin and transformations. f allows to retrieve dust mass and its value accounting for Ca abundance in dust at the site of investigation may serve as an indicator of dust origin and aerosol interactions with anthropogenic acids. f values were found to vary in the 0.08–0.12 range in European urban areas, and a broader range in Beijing (0.01–0.16). As expected, k appears to be a relevant proxy for particle origin and ageing and varies in the 1.4–1.8 range. For Beijing, k exhibits high values of about 1.7 in winter and summer. Winter values suggest that fresh coal aerosol might be responsible for such a high k value, which was not taken into account in previous works.


Author(s):  
Karen A. Katrinak ◽  
James R. Anderson ◽  
Peter R. Buseck

Aerosol samples were collected in Phoenix, Arizona on eleven dates between July 1989 and April 1990. Elemental compositions were determined for approximately 1000 particles per sample using an electron microprobe with an energy-dispersive x-ray spectrometer. Fine-fraction samples (particle cut size of 1 to 2 μm) were analyzed for each date; coarse-fraction samples were also analyzed for four of the dates.The data were reduced using multivariate statistical methods. Cluster analysis was first used to define 35 particle types. 81% of all fine-fraction particles and 84% of the coarse-fraction particles were assigned to these types, which include mineral, metal-rich, sulfur-rich, and salt categories. "Zero-count" particles, consisting entirely of elements lighter than Na, constitute an additional category and dominate the fine fraction, reflecting the importance of anthropogenic air pollutants such as those emitted by motor vehicles. Si- and Ca-rich mineral particles dominate the coarse fraction and are also numerous in the fine fraction.


2018 ◽  
Vol 141 (1) ◽  
Author(s):  
Andreas Vogel ◽  
Adam J. Durant ◽  
Massimo Cassiani ◽  
Rory J. Clarkson ◽  
Michal Slaby ◽  
...  

Volcanic ash (VA) clouds in flight corridors present a significant threat to aircraft operations as VA particles can cause damage to gas turbine engine components that lead to a reduction of engine performance and compromise flight safety. In the last decade, research has mainly focused on processes such as erosion of compressor blades and static components caused by impinging ash particles as well as clogging and/or corrosion effects of soft or molten ash particles on hot section turbine airfoils and components. However, there is a lack of information on how the fan separates ingested VA particles from the core stream flow into the bypass flow and therefore influences the mass concentration inside the engine core section, which is most vulnerable and critical for safety. In this numerical simulation study, we investigated the VA particle–fan interactions and resulting reductions in particle mass concentrations entering the engine core section as a function of particle size, fan rotation rate, and for two different flight altitudes. For this, we used a high-bypass gas-turbine engine design, with representative intake, fan, spinner, and splitter geometries for numerical computational fluid dynamics (CFD) simulations including a Lagrangian particle-tracking algorithm. Our results reveal that particle–fan interactions redirect particles from the core stream flow into the bypass stream tube, which leads to a significant particle mass concentration reduction inside the engine core section. The results also show that the particle–fan interactions increase with increasing fan rotation rates and VA particle size. Depending on ingested VA size distributions, the particle mass inside the engine core flow can be up to 30% reduced compared to the incoming particle mass flow. The presented results enable future calculations of effective core flow exposure or dosages based on simulated or observed atmospheric VA particle size distribution, which is required to quantify engine failure mechanisms after exposure to VA. As an example, we applied our methodology to a recent aircraft encounter during the Mt. Kelud 2014 eruption. Based on ambient VA concentrations simulated with an atmospheric particle dispersion model (FLEXPART), we calculated the effective particle mass concentration inside the core stream flow along the actual flight track and compared it with the whole engine exposure.


2019 ◽  
Vol 29 (2) ◽  
Author(s):  
Miroslav Josipovic ◽  
Catherine Leal-Liousse ◽  
Belinda Crobeddu ◽  
Armelle Baeza-Squiban ◽  
C. Keitumetse Segakweng ◽  
...  

This study aimed to characterise aerosols sampled in the vicinity of a major industrialised area, i.e. the Vaal Triangle. It included thedetermination of oxidative potential as a predictive indicator of particle toxicity. Aerosol samples were collated through the cascadefiltering during an eight-month period (12 h over three days in one week). Three size fractions were analysed for organic carbon(OC), black carbon (BC) and oxidative potential (OP), while ionic content was presented as monthly and seasonal concentrations. Thecontinuous measurement of black carbon by an optical attenuation instrument was collated concurrently with cascade filtering. Thecarbonaceous content was low compared to the ionic one. Within the carbonaceous concentrations, the organic carbon was higherthan concentrations of black carbon in both seasons in the ultra-fine fraction; the opposite was the case for the fine fraction, whilethe coarse fraction concentrations of organic carbon in the dry season had higher concentrations than black carbon in the wet seasonand organic carbon in the wet season. The OP tended to increase as the size was decreasing for wet season aerosols, whereas, forthe dry season, the highest OP was exerted by the fine fraction. The ultrafine fraction was the one showing the most contrasting OPbetween the two seasons. Continuous monitoring indicated that the higher BC concentrations were recorded in the dry/winter partof the year, with the daily pattern of concentrations being typically bimodal, having both the morning and evening peaks in bothseasons. Within the ionic content, the dominance of sulphate, nitrate and ammonium was evident. Multiple linear correlations wereperformed between all determined compounds. Strong correlations of carboxylic acids with other organic compounds were revealed.These acids point to emissions of VOC, both anthropogenic and biogenic. Since they were equally present in both seasons, a mixtureof sources was responsible, both present in the wider area and throughout the year.


Author(s):  
Kateryna Deineka ◽  
Yurii Naumenko

The influence of the structure of a two-fraction polygranular feed of the chamber on the value of the drum rotation speed at auto-excitation of self-excited oscillations with a maximum swing is considered. Such a pulsating mode of movement of the charge is used in the self-oscillating process of grinding in a tumbling mill. The coarse fraction simulated the grinding bodies was steel bullets with a relative size ψdb=0.026. The fine fraction, simulated the particles of the crushed material, was a cement clinker with a relative particle size ψdm=0.00013. Variable factors of experimental studies were: the degree of filling the chamber in the state of rest κbr=0.25; 0.29; 0.33 and the degree of filling the gaps between the particles of the coarse fraction with particles of the fine fraction κmbgr=0.0625; 0.375; 0.6875; 1. The method of visual analysis of transient processes of self-oscillating modes of feed behavior in the cross section of the rotating drum chamber is applied. Measurements of the speed limits of the drum rotation were carried out with auto-excitation of self-oscillations of the filling. The magnitude of the self-oscillation swing was estimated by the increase in the difference between the maximum and minimum values of the filling dilatancy for one period of pulsations. An increase in the upper limit of the speed range ψω2 with a decrease in κbr and κmbgr was established. The growth rate of ψω2 increases at low values of κbr and κmbgr. Some increase in the lower limit of the ψω1 range with a decrease in κbr and κmbgr was revealed. An increase in the range of speeds of rotation was recorded at the maximum range of self-oscillations ψω1–ψω2 with a decrease in the connected interaction of the intra-mill filling. This coherent interaction is due to an increase in κbr and κmbgr. The value of the ψω1–ψω2 range varies from 1.01–1.03 at κbr=0.33 and κmbg=1 to 1.22–1.66 at κbr=0.25 and κmbgr=0.0625. The range gets its maximum value with fine and superfine grinding


2012 ◽  
Vol 12 (4) ◽  
pp. 1681-1700 ◽  
Author(s):  
R. M. Healy ◽  
J. Sciare ◽  
L. Poulain ◽  
K. Kamili ◽  
M. Merkel ◽  
...  

Abstract. An Aerosol Time-Of-Flight Mass Spectrometer (ATOFMS) was deployed to investigate the size-resolved chemical composition of single particles at an urban background site in Paris, France, as part of the MEGAPOLI winter campaign in January/February 2010. ATOFMS particle counts were scaled to match coincident Twin Differential Mobility Particle Sizer (TDMPS) data in order to generate hourly size-resolved mass concentrations for the single particle classes observed. The total scaled ATOFMS particle mass concentration in the size range 150–1067 nm was found to agree very well with the sum of concurrent High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and Multi-Angle Absorption Photometer (MAAP) mass concentration measurements of organic carbon (OC), inorganic ions and black carbon (BC) (R2 = 0.91). Clustering analysis of the ATOFMS single particle mass spectra allowed the separation of elemental carbon (EC) particles into four classes: (i) EC attributed to biomass burning (ECbiomass), (ii) EC attributed to traffic (ECtraffic), (iii) EC internally mixed with OC and ammonium sulfate (ECOCSOx), and (iv) EC internally mixed with OC and ammonium nitrate (ECOCNOx). Average hourly mass concentrations for EC-containing particles detected by the ATOFMS were found to agree reasonably well with semi-continuous quantitative thermal/optical EC and optical BC measurements (r2 = 0.61 and 0.65–0.68 respectively, n = 552). The EC particle mass assigned to fossil fuel and biomass burning sources also agreed reasonably well with BC mass fractions assigned to the same sources using seven-wavelength aethalometer data (r2 = 0.60 and 0.48, respectively, n = 568). Agreement between the ATOFMS and other instrumentation improved noticeably when a period influenced by significantly aged, internally mixed EC particles was removed from the intercomparison. 88% and 12% of EC particle mass was apportioned to fossil fuel and biomass burning respectively using the ATOFMS data compared with 85% and 15% respectively for BC estimated from the aethalometer model. On average, the mass size distribution for EC particles is bimodal; the smaller mode is attributed to locally emitted, mostly externally mixed EC particles, while the larger mode is dominated by aged, internally mixed ECOCNOx particles associated with continental transport events. Periods of continental influence were identified using the Lagrangian Particle Dispersion Model (LPDM) "FLEXPART". A consistent minimum between the two EC mass size modes was observed at approximately 400 nm for the measurement period. EC particles below this size are attributed to local emissions using chemical mixing state information and contribute 79% of the scaled ATOFMS EC particle mass, while particles above this size are attributed to continental transport events and contribute 21% of the EC particle mass. These results clearly demonstrate the potential benefit of monitoring size-resolved mass concentrations for the separation of local and continental EC emissions. Knowledge of the relative input of these emissions is essential for assessing the effectiveness of local abatement strategies.


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