scholarly journals Lessons learnt from the first EMEP intensive measurement periods

2012 ◽  
Vol 12 (2) ◽  
pp. 3731-3780 ◽  
Author(s):  
W. Aas ◽  
S. Tsyro ◽  
E. Bieber ◽  
R. Bergström ◽  
D. Ceburnis ◽  
...  

Abstract. The first EMEP intensive measurement periods were held in June 2006 and January 2007. The measurements aimed to characterize the aerosol chemical compositions, including the gas/aerosol partitioning of inorganic compounds. The measurement program during these periods included daily or hourly measurements of the secondary inorganic components, with additional measurements of elemental- and organic carbon (EC and OC) and mineral dust in PM1, PM2.5 and PM10. These measurements have provided extended knowledge regarding the composition of particulate matter and the temporal and spatial variability of PM, as well as an extended database for the assessment of chemical transport models. This paper summarise the first experiences of making use of measurements from the first EMEP intensive measurement periods along with EMEP model results from the updated model version to characterise aerosol composition. We investigated how the PM chemical composition varies between the summer and the winter month and geographically. The observation and model data are in general agreement regarding the main features of PM10 and PM2.5 composition and the relative contribution of different components, though the EMEP model tends to slightly underestimate PM10 and PM2.5 compared to measurements. The intensive measurement data has identified areas where improvements are needed. In particular, the model description of formation of coarse nitrate on sea salt and dust particles requires further attention. Hourly concurrent measurements of gaseous and particulate components for the first time facilitated testing of modelled diurnal variability of the gas/aerosol partitioning of nitrogen species. In general, the modelled diurnal cycles of nitrate and ammonium aerosols are in good agreement with the measurements. As expected, the diurnal variability of ammonia is not very well captured, but this will probably improve if the EMEP model is coupled to a dynamic, mechanistic ammonia emission module. The largest underestimations of aerosol mass are seen in Italy during winter, which to a large extent may be explained by an underestimation of residential wood burning source. It should be noted that both primary and secondary OC has been included in the calculations for the first time, showing promising results. Mineral dust is important, especially in southern Europe, and the model seems to capture the dust episodes well. The lack of measurements of mineral dust hampers the possibility for model evaluation for this highly uncertain PM component. There are also lessons learnt regarding improved measurements for future intensive periods. There is a need for increased comparability between the measurements at different sites. For the nitrogen compounds it is clear that more measurements using artefact free methods based on continuous measurement methods and/or denuders are needed. For EC/OC, a reference methodology (both in field and laboratory) was lacking during these periods giving problems with comparability, though presently measurement protocols have been established and these should be followed by the Parties to the EMEP Protocol. For measurements with no defined protocols, it might be a good solution to use centralised laboratories to ensure comparability across the network. To cope with the introduction of these new measurements new reporting guidelines have been developed to ensure that all proper information about the methodologies and data quality is given.

2012 ◽  
Vol 12 (17) ◽  
pp. 8073-8094 ◽  
Author(s):  
W. Aas ◽  
S. Tsyro ◽  
E. Bieber ◽  
R. Bergström ◽  
D. Ceburnis ◽  
...  

Abstract. The first EMEP intensive measurement periods were held in June 2006 and January 2007. The measurements aimed to characterize the aerosol chemical compositions, including the gas/aerosol partitioning of inorganic compounds. The measurement program during these periods included daily or hourly measurements of the secondary inorganic components, with additional measurements of elemental- and organic carbon (EC and OC) and mineral dust in PM1, PM2.5 and PM10. These measurements have provided extended knowledge regarding the composition of particulate matter and the temporal and spatial variability of PM, as well as an extended database for the assessment of chemical transport models. This paper summarise the first experiences of making use of measurements from the first EMEP intensive measurement periods along with EMEP model results from the updated model version to characterise aerosol composition. We investigated how the PM chemical composition varies between the summer and the winter month and geographically. The observation and model data are in general agreement regarding the main features of PM10 and PM2.5 composition and the relative contribution of different components, though the EMEP model tends to give slightly lower estimates of PM10 and PM2.5 compared to measurements. The intensive measurement data has identified areas where improvements are needed. Hourly concurrent measurements of gaseous and particulate components for the first time facilitated testing of modelled diurnal variability of the gas/aerosol partitioning of nitrogen species. In general, the modelled diurnal cycles of nitrate and ammonium aerosols are in fair agreement with the measurements, but the diurnal variability of ammonia is not well captured. The largest differences between model and observations of aerosol mass are seen in Italy during winter, which to a large extent may be explained by an underestimation of residential wood burning sources. It should be noted that both primary and secondary OC has been included in the calculations for the first time, showing promising results. Mineral dust is important, especially in southern Europe, and the model seems to capture the dust episodes well. The lack of measurements of mineral dust hampers the possibility for model evaluation for this highly uncertain PM component. There are also lessons learnt regarding improved measurements for future intensive periods. There is a need for increased comparability between the measurements at different sites. For the nitrogen compounds it is clear that more measurements using artefact free methods based on continuous measurement methods and/or denuders are needed. For EC/OC, a reference methodology (both in field and laboratory) was lacking during these periods giving problems with comparability, though measurement protocols have recently been established and these should be followed by the Parties to the EMEP Protocol. For measurements with no defined protocols, it might be a good solution to use centralised laboratories to ensure comparability across the network. To cope with the introduction of these new measurements, new reporting guidelines have been developed to ensure that all proper information about the methodologies and data quality is given.


Minerals ◽  
2021 ◽  
Vol 11 (2) ◽  
pp. 125
Author(s):  
Mariola Jabłońska ◽  
Janusz Janeczek ◽  
Beata Smieja-Król

For the first time, it is shown that inhaled ambient air-dust particles settled in the human lower respiratory tract induce lung calcification. Chemical and mineral compositions of pulmonary calcium precipitates in the lung right lower-lobe (RLL) tissues of 12 individuals who lived in the Upper Silesia conurbation in Poland and who had died from causes not related to a lung disorder were determined by transmission and scanning electron microscopy. Whereas calcium salts in lungs are usually reported as phosphates, calcium salts precipitated in the studied RLL tissue were almost exclusively carbonates, specifically Mg-calcite and calcite. These constituted 37% of the 1652 mineral particles examined. Mg-calcite predominated in the submicrometer size range, with a MgCO3 content up to 50 mol %. Magnesium plays a significant role in lung mineralization, a fact so far overlooked. The calcium phosphate (hydroxyapatite) content in the studied RLL tissue was negligible. The predominance of carbonates is explained by the increased CO2 fugacity in the RLL. Carbonates enveloped inhaled mineral-dust particles, including uranium-bearing oxides, quartz, aluminosilicates, and metal sulfides. Three possible pathways for the carbonates precipitation on the dust particles are postulated: (1) precipitation of amorphous calcium carbonate (ACC), followed by its transformation to calcite; (2) precipitation of Mg-ACC, followed by its transformation to Mg-calcite; (3) precipitation of Mg-free ACC, causing a localized relative enrichment in Mg ions and subsequent heterogeneous nucleation and crystal growth of Mg-calcite. The actual number of inhaled dust particles may be significantly greater than was observed because of the masking effect of the carbonate coatings. There is no simple correlation between smoking habit and lung calcification.


Author(s):  
Mariola Jablonska ◽  
Janusz Janeczek ◽  
Beata Smieja-Król

For the first time, it is shown that inhaled ambient air-dust particles settled in the human lower respiratory tract induce lung calcification. Chemical- and mineral compositions of pulmonary calcium precipitates in the lung right lower-lobe (RLL) tissues of 12 individuals who lived in Upper Silesia Conurbation in Poland and who had died from causes not related to lung disorder were determined by transmission- and scanning electron microscopy. Whereas calcium salts in lungs are usually reported as phosphates, calcium salts precipitated in RLL are almost exclusively carbonates, i.e. Mg-calcite and calcite. These constitute 37% of 1652 mineral particles examined. Mg-calcite predominates in the submicron size range with the MgCO3 content up to 50 mol%. Magnesium plays a significant role in the lung mineralization, a fact so far overlooked. The calcium phosphate (hydroxyapatite) content in RLL is negligible. The predominance of carbonates is explained by increased CO2 fugacity in RLL. Carbonates enveloped inhaled mineral-dust particles, including uranium-bearing oxides, quartz, aluminosilicates, and metal sulfides. Three possible pathways for the carbonates precipitation on the dust particles are postulated: (1) precipitation of amorphous calcium carbonate (ACC) followed by its transformation to calcite; (2) precipitation of Mg-ACC followed by its transformation to Mg-calcite; (3) precipitation of Mg-free ACC causing a localized relative enrichment in Mg ions and subsequent heterogeneous nucleation and crystal growth of Mg-calcite. The actual number of inhaled dust particles may be significantly greater than observed because of the masking effect of the carbonate coatings. There is no simple correlation between smoking habit and lung calcification.


2019 ◽  
Vol 19 (1) ◽  
pp. 219-232 ◽  
Author(s):  
Xiaole Pan ◽  
Baozhu Ge ◽  
Zhe Wang ◽  
Yu Tian ◽  
Hang Liu ◽  
...  

Abstract. Depolarization ratio (δ) of backscattered light is an applicable parameter for distinguishing the sphericity of particles in real time, which has been widely adopted by ground-based lidar observation systems. In this study, δ values of particles and chemical compositions in both PM2.5 (aerodynamic diameter less than 2.5 µm) and PM10 (aerodynamic diameter less than 10 µm) were concurrently measured on the basis of a bench-top optical particle counter with a polarization detection module (POPC) and a continuous dichotomous aerosol chemical speciation analyzer (ACSA-14) from November 2016 to February 2017 at an urban site in Beijing megacity. In general, measured δ values depended on both size and sphericity of the particles. During the observation period, mass concentrations of NO3- in PM2.5 (fNO3) were about an order of magnitude higher than that in PM2.5−10 (cNO3) with a mean fNO3∕cNO3 ratio of 14±10. A relatively low fNO3∕cNO3 ratio (∼5) was also observed under higher relative humidity conditions, mostly due to heterogeneous processes and particles in the coarse mode. We found that δ values of ambient particles in both PM2.5 and PM2.5−10 obviously decreased as mass concentration of water-soluble species increased at unfavorable meteorological conditions. This indicated that the morphology of particles was changed as a result of water-absorbing processes. The particles with optical size (Dp) of Dp = 5 µm were used to represent mineral dust particles, and its δ values (δDp=5) decreased by 50 % as the mass fraction of cNO3 increased from 2 % to 8 % and ambient relative humidity increased up to 80 %, suggesting that mineral dust particles were likely to be spherical during humid pollution episodes. During the observation, relative humidity inside the POPC measuring chamber was stable at 34±2 %, lower than the ambient condition. Its influence on the morphology was estimated to be limited and did not change our major conclusion. This study highlights the evident alteration of non-sphericity of mineral dust particles during their transport owing to a synergistic effect of both pollutant coatings and hygroscopic processes, which plays an important role in the evaluation of its environmental effect.


2017 ◽  
Author(s):  
Mingjin Tang ◽  
Xin Huang ◽  
Keding Lu ◽  
Maofa Ge ◽  
Yongjie Li ◽  
...  

Abstract. Heterogeneous reactions of mineral dust aerosol with trace gases in the atmosphere could directly and indirectly affect tropospheric oxidation capacity, in addition to aerosol composition and physicochemical properties. In this article we provide a comprehensive and critical review of laboratory studies of heterogeneous uptake of OH, NO3, O3, and their directly related species as well (including HO2, H2O2, HCHO, HONO, and N2O5) by mineral dust particles. Atmospheric importance of heterogeneous uptake as sinks for these species are assessed (i) by comparing their lifetimes with respect to heterogeneous reactions with mineral dust to lifetimes with respect to other major loss processes and (ii) by discussing relevant field and modelling studies. We have also outlined major open questions and challenges in laboratory studies of heterogeneous uptake by mineral dust and discussed research strategies to address them in order to better understand the effects of heterogeneous reactions with mineral dust on tropospheric oxidation capacity.


2021 ◽  
Vol 21 (24) ◽  
pp. 18147-18174
Author(s):  
Nabil Deabji ◽  
Khanneh Wadinga Fomba ◽  
Souad El Hajjaji ◽  
Abdelwahid Mellouki ◽  
Laurent Poulain ◽  
...  

Abstract. Field measurements were conducted to determine aerosol chemical composition at a newly established remote high-altitude site in North Africa at the Atlas Mohammed V (AMV) atmospheric observatory located in the Middle Atlas Mountains. The main objectives of the present work are to investigate the variations in the aerosol composition and better assess global and regional changes in atmospheric composition in North Africa. A total of 200 particulate matter (PM10) filter samples were collected at the site using a high-volume (HV) collector in a 12 h sampling interval from August to December 2017. The chemical composition of the samples was analyzed for trace metals, water-soluble ions, organic carbon (OC/EC), aliphatic hydrocarbons, and polycyclic aromatic hydrocarbon (PAH) contents. The results indicate that high-altitude aerosol composition is influenced by both regional and transregional transport of emissions. However, local sources play an important role, especially during low wind speed periods, as observed for November and December. During background conditions characterized by low wind speeds (avg. 3 m s-1) and mass concentrations in the range from 9.8 to 12 μg m-3, the chemical composition is found to be dominated by inorganic elements, mainly suspended dust (61 %) and ionic species (7 %), followed by organic matter (7 %), water content (12 %), and unidentified mass (11 %). Despite the proximity of the site to the Sahara, its influence on the atmospheric composition at this high-altitude site was mainly seasonal and accounted for only 22 % of the sampling duration. Biogenic organics contributed up to 7 % of the organic matter with high contributions from compounds such as heneicosane, hentriacontane, and nonacosane. The AMV site is dominated by four main air mass inflows, which often leads to different aerosol chemical compositions. Mineral dust influence was seasonal and ranged between 21 % and 74 % of the PM mass, with peaks observed during the summer, and was accompanied by high concentrations of SO42- of up to 3.0 μg m-3. During winter, PM10 concentrations are low (<30 μg m-3), the influence of the desert is weaker, and the marine air masses (64 %) are more dominant with a mixture of sea salt and polluted aerosol from the coastal regions (Rabat and Casablanca). During the daytime, mineral dust contribution to PM increased by about 42 % because of road dust resuspension. In contrast, during nighttime, an increase in the concentrations of alkanes, PAHs, alkane-2-ones, and anthropogenic metals such as Pb, Ni, and Cu was found due to variations in the boundary layer height. The results provide the first detailed seasonal and diurnal variation of the aerosol chemical composition, which is valuable for long-term assessment of climate and regional influence of air pollution in North Africa.


2021 ◽  
Author(s):  
Perla Alalam ◽  
Hervé Herbin

&lt;p&gt;Large desert lands such as Sahara, Gobi or Australia present main sources of atmospheric mineral dust caused by intense dust storms. Transported dust particles undergo physical and chemical changes affecting their microphysical and optical properties. This modifies their scattering and absorption properties and alters the global atmospheric radiative budget.&lt;/p&gt;&lt;p&gt;Currently, remote sensing techniques represent a powerful tool for quantitative atmospheric measurements and the only means of analyzing its evolution from local to global scale. In order to improve the knowledge of atmospheric aerosol distributions, many efforts were made particularly in the development of hyperspectral infrared spectrometers and processing algorithms. However, to fully exploit these measurements, a perfect knowledge of Complex Refractive Index (CRI) is required.&lt;/p&gt;&lt;p&gt;In that purpose, a new methodology&amp;#160;&lt;sup&gt;&lt;/sup&gt;based on laboratory measurements of mineral dust in suspension coupled with an optimal estimation method has been developed. This approach allows getting access to CRI of several desert samples with various chemical compositions.&lt;/p&gt;&lt;p&gt;Here, we present the first results of the physical parameters (effective radius and concentration) retrievals using Infrared Atmospheric Sounding Interferometer IASI data, during dust storm events. The latter use the CRI of different desert samples obtained in laboratory and a new radiative transfer algorithm (ARAHMIS) developed at Laboratoire d&amp;#8217;Optique Atmosph&amp;#233;rique LOA.&lt;/p&gt;


2014 ◽  
Vol 14 (7) ◽  
pp. 3307-3323 ◽  
Author(s):  
H. Geng ◽  
H. Hwang ◽  
X. Liu ◽  
S. Dong ◽  
C.-U. Ro

Abstract. This is the first study of Asian dust storm (ADS) particles collected in Beijing, China, and Incheon, Korea, during a spring ADS event. Using a seven-stage May impactor and a quantitative electron probe X-ray microanalysis (ED-EPMA, also known as low-Z particle EPMA), we examined the composition and morphology of 4200 aerosol particles at stages 1–6 (with a size cut-off of 16, 8, 4, 2, 1, and 0.5 μm in equivalent aerodynamic diameter, respectively) collected during an ADS event on 28–29 April 2005. The results showed that there were large differences in the chemical compositions between particles in sample S1 collected in Beijing immediately after the peak time of the ADS and in samples S2 and S3, which were collected in Incheon approximately 5 h and 24 h later, respectively. In sample S1, mineral dust particles accounted for more than 88% in relative number abundance at stages 1–5; and organic carbon (OC) and reacted NaCl-containing particles accounted for 24% and 32%, respectively, at stage 6. On the other hand, in samples S2 and S3, in addition to approximately 60% mineral dust, many sea spray aerosol (SSA) particles reacted with airborne SO2 and NOx (accounting for 24% and 14% on average in samples S2 and S3, respectively), often mixed with mineral dust, were encountered at stages 1–5, and (C, N, O, S)-rich particles (likely a mixture of water-soluble organic carbon with (NH4)2SO4 and NH4NO3) were abundantly observed at stage 6 (accounting for 68% and 51% in samples S2 and S3, respectively). This suggests that an accumulation of sea-salt components on individual ADS particles larger than 1 μm in diameter occurred and many secondary aerosols smaller than 1 μm in diameter were formed when the ADS particles passed over the Yellow Sea. In the reacted or aged mineral dust and SSA particles, nitrate-containing and both nitrate- and sulfate-containing species vastly outnumbered the sulfate-containing species, implying that ambient NOx had a greater influence on the atmospheric particles than SO2 during this ADS episode. In addition to partially- or totally-reacted CaCO3, reacted or aged Mg-containing aluminosilicates were observed frequently in samples S2 and S3; furthermore, a student's t test showed that both their atomic concentration ratios of [Mg] / [Al] and [Mg] / [Si] were significantly elevated (P < 0.05) compared to those in samples S1 (for [Mg] / [Al], 0.34 ± 0.09 and 0.40 ± 0.03 in samples S2 and S3, respectively, vs. 0.24 ± 0.01 in sample S1; for [Mg] / [Si], 0.21 ± 0.05 and 0.22 ± 0.01 in samples S2 and S3, respectively, vs. 0.12 ± 0.02 in sample S1). The significant increase of [Mg] / [Al] and [Mg] / [Si] ratios in Mg-containing aluminosilicates indicates that a significant evolution or aging must have occurred on the ADS particles in the marine atmosphere during transport from China to Korea.


2017 ◽  
Vol 17 (19) ◽  
pp. 11727-11777 ◽  
Author(s):  
Mingjin Tang ◽  
Xin Huang ◽  
Keding Lu ◽  
Maofa Ge ◽  
Yongjie Li ◽  
...  

Abstract. Heterogeneous reactions of mineral dust aerosol with trace gases in the atmosphere could directly and indirectly affect tropospheric oxidation capacity, in addition to aerosol composition and physicochemical properties. In this article we provide a comprehensive and critical review of laboratory studies of heterogeneous uptake of OH, NO3, O3, and their directly related species as well (including HO2, H2O2, HCHO, HONO, and N2O5) by mineral dust particles. The atmospheric importance of heterogeneous uptake as sinks for these species is assessed (i) by comparing their lifetimes with respect to heterogeneous reactions with mineral dust to lifetimes with respect to other major loss processes and (ii) by discussing relevant field and modeling studies. We have also outlined major open questions and challenges in laboratory studies of heterogeneous uptake by mineral dust and discussed research strategies to address them in order to better understand the effects of heterogeneous reactions with mineral dust on tropospheric oxidation capacity.


2014 ◽  
Vol 14 (22) ◽  
pp. 12415-12428 ◽  
Author(s):  
G. Y. Jeong ◽  
E. P. Achterberg

Abstract. Mineral dust supplied to remote ocean regions stimulates phytoplankton growth through delivery of micronutrients, notably iron (Fe). Although attention is usually paid to Fe (hydr)oxides as major sources of available Fe, Fe-bearing clay minerals are typically the dominant phase in mineral dust. The mineralogy and chemistry of clay minerals in dust particles, however, are largely unknown. We conducted microscopic identification and chemical analysis of the clay minerals in Asian and Saharan dust particles. Cross-sectional slices of dust particles were prepared by focused ion beam (FIB) techniques and analyzed by transmission electron microscopy (TEM) combined with energy dispersive X-ray spectroscopy (EDXS). TEM images of FIB slices revealed that clay minerals occurred as either nano-thin platelets or relatively thick plates. Chemical compositions and lattice fringes of the nano-thin platelets suggested that they included illite, smectite, illite–smectite mixed layers, and their nanoscale mixtures (illite–smectite series clay minerals, ISCMs) which could not be resolved with an electron microbeam. EDXS chemical analysis of the clay mineral grains revealed that the average Fe content was 5.8% in nano-thin ISCM platelets assuming 14% H2O, while the Fe content of illite and chlorite was 2.8 and 14.8%, respectively. In addition, TEM and EDXS analyses were performed on clay mineral grains dispersed and loaded on micro-grids. The average Fe content of clay mineral grains was 6.7 and 5.4% in Asian and Saharan dusts, respectively. A comparative X-ray diffraction analysis of bulk dusts showed that Saharan dust was more enriched in clay minerals than Asian dust, while Asian dust was more enriched in chlorite. Clay minerals, in particular nanocrystalline ISCMs and Fe-rich chlorite, are probably important sources of Fe to remote marine ecosystems. Further detailed analyses of the mineralogy and chemistry of clay minerals in global mineral dusts are required to evaluate the inputs of Fe to surface ocean microbial communities.


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