scholarly journals Airborne measurements of the spatial distribution of aerosol chemical composition across Europe and evolution of the organic fraction

2010 ◽  
Vol 10 (8) ◽  
pp. 4065-4083 ◽  
Author(s):  
W. T. Morgan ◽  
J. D. Allan ◽  
K. N. Bower ◽  
E. J. Highwood ◽  
D. Liu ◽  
...  
Keyword(s):  
Spatial Distribution ◽  
Chemical Composition ◽  
Ammonium Nitrate ◽  
Western Europe ◽  
Volatile Component ◽  
Organic Aerosol ◽  
Chemical Components ◽  
Airborne Measurements ◽  
North Western ◽  
Aerosol Chemical Composition

Abstract. The spatial distribution of aerosol chemical composition and the evolution of the Organic Aerosol (OA) fraction is investigated based upon airborne measurements of aerosol chemical composition in the planetary boundary layer across Europe. Sub-micron aerosol chemical composition was measured using a compact Time-of-Flight Aerosol Mass Spectrometer (cToF-AMS). A range of sampling conditions were evaluated, including relatively clean background conditions, polluted conditions in North-Western Europe and the near-field to far-field outflow from such conditions. Ammonium nitrate and OA were found to be the dominant chemical components of the sub-micron aerosol burden, with mass fractions ranging from 20–50% each. Ammonium nitrate was found to dominate in North-Western Europe during episodes of high pollution, reflecting the enhanced NOx and ammonia sources in this region. OA was ubiquitous across Europe and concentrations generally exceeded sulphate by 30–160%. A factor analysis of the OA burden was performed in order to probe the evolution across this large range of spatial and temporal scales. Two separate Oxygenated Organic Aerosol (OOA) components were identified; one representing an aged-OOA, termed Low Volatility-OOA and another representing fresher-OOA, termed Semi Volatile-OOA on the basis of their mass spectral similarity to previous studies. The factors derived from different flights were not chemically the same but rather reflect the range of OA composition sampled during a particular flight. Significant chemical processing of the OA was observed downwind of major sources in North-Western Europe, with the LV-OOA component becoming increasingly dominant as the distance from source and photochemical processing increased. The measurements suggest that the aging of OA can be viewed as a continuum, with a progression from a less oxidised, semi-volatile component to a highly oxidised, less-volatile component. Substantial amounts of pollution were observed far downwind of continental Europe, with OA and ammonium nitrate being the major constituents of the sub-micron aerosol burden. Such anthropogenically perturbed air masses can significantly perturb regional climate far downwind of major source regions.

scholarly journals Airborne measurements of the spatial distribution of aerosol chemical composition across Europe and evolution of the organic fraction

2009 ◽  
Vol 9 (6) ◽  
pp. 27215-27265 ◽  
Author(s):  
W. T. Morgan ◽  
J. D. Allan ◽  
K. N. Bower ◽  
E. J. Highwood ◽  
D. Liu ◽  
...  
Keyword(s):  
Spatial Distribution ◽  
Chemical Composition ◽  
Ammonium Nitrate ◽  
Western Europe ◽  
Volatile Component ◽  
Organic Aerosol ◽  
Chemical Components ◽  
Airborne Measurements ◽  
North Western ◽  
Aerosol Chemical Composition

Abstract. The spatial distribution of aerosol chemical composition and the evolution of the Organic Aerosol (OA) fraction is investigated based upon airborne measurements of aerosol chemical composition in the planetary boundary layer across Europe. Sub-micron aerosol chemical composition was measured using a compact Time-of-Flight Aerosol Mass Spectrometer (cToF-AMS). A range of sampling conditions were evaluated, including relatively clean background conditions, polluted conditions in North-Western Europe and the near-field to far-field outflow from such conditions. Ammonium nitrate and OA were found to be the dominant chemical components of the sub-micron aerosol burden, with mass fractions ranging from 20–50% each. Ammonium nitrate was found to dominate in North-Western Europe during episodes of high pollution, reflecting the enhanced NOx and ammonia sources in this region. OA was ubiquitous across Europe and concentrations generally exceeded sulphate by 50–100%. A factor analysis of the OA burden was performed in order to probe the evolution across this large range of spatial and temporal scales. Two separate Oxygenated Organic Aerosol (OOA) components were identified; one representing an aged-OOA, termed Low Volatility-OOA and another representing fresher-OOA, termed Semi Volatile-OOA on the basis of their mass spectral similarity to previous studies. The factors derived from different flights were not chemically the same but rather reflect the range of OA composition sampled during a particular flight. Significant chemical processing of the OA was observed downwind of major sources in North-Western Europe, with the LV-OOA component becoming increasingly dominant as the distance from source and photochemical processing increased. The measurements suggest that the aging of OA can be viewed as a continuum, with a progression from a less oxidised, semi-volatile component to a highly oxidised, less-volatile component. Substantial amounts of pollution were observed far downwind of continental Europe, with OA and ammonium nitrate being the major constituents of the sub-micron aerosol burden. Such anthropogenically perturbed air masses can significantly perturb regional climate far downwind of major source regions.

scholarly journals Influence of aerosol chemical composition on N<sub>2</sub>O<sub>5</sub> uptake: airborne regional measurements in North-Western Europe

2014 ◽  
Vol 14 (13) ◽  
pp. 19673-19718 ◽  
Author(s):  
W. T. Morgan ◽  
B. Ouyang ◽  
J. D. Allan ◽  
E. Aruffo ◽  
P. Di Carlo ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Ammonium Nitrate ◽  
Water Content ◽  
Atmospheric Chemistry ◽  
Western Europe ◽  
Organic Aerosol ◽  
Atmospheric Composition ◽  
Airborne Measurements ◽  
North Western ◽  
Aerosol Chemical Composition

Abstract. Aerosol chemical composition was found to influence nighttime atmospheric chemistry during a series of airborne measurements in North-Western Europe in summer conditions, which has implications for regional air quality and climate. The uptake of dinitrogen pentoxide, γ (N2O5), to particle surfaces was found to be modulated by the amount of water content and ammonium nitrate present in the aerosol. The conditions prevalent in this study suggest that the net uptake rate of N2O5 to atmospheric aerosols was relatively efficient compared to previous studies, with γ (N2O5) values in the range 0.01–0.03. This is likely a consequence of the elevated relative humidity in the region, which promotes greater aerosol water content. Increased nitrate concentrations relative to particulate water were found to suppress N2O5 uptake. The results presented here contrast with previous ambient studies of N2O5 uptake, which have generally taken place in low-nitrate environments in the USA. Comparison of the N2O5 uptake derived from the measurements with a parameterised scheme that is based on the ratio of particulate water to nitrate yielded reasonably good agreement in terms of the magnitude and variation in uptake, provided the effect of chloride was neglected. An additional suppression of the parameterised uptake is likely required to fully capture the variation in N2O5 uptake, which could be achieved via the known suppression by organic aerosol. However, existing parameterisations representing the suppression by organic aerosol were unable to fully represent the variation in N2O5 uptake. These results provide important ambient measurement constraint on our ability to predict N2O5 uptake in regional and global aerosol models. N2O5 uptake is a potentially important source of nitrate aerosol and a sink of the nitrate radical, which is the main nocturnal oxidant in the atmosphere. The results further highlight the importance of ammonium nitrate in North-Western Europe as a key component of atmospheric composition in the region.

scholarly journals Influence of aerosol chemical composition on N<sub>2</sub>O<sub>5</sub> uptake: airborne regional measurements in northwestern Europe

2015 ◽  
Vol 15 (2) ◽  
pp. 973-990 ◽  
Author(s):  
W. T. Morgan ◽  
B. Ouyang ◽  
J. D. Allan ◽  
E. Aruffo ◽  
P. Di Carlo ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Ammonium Nitrate ◽  
Water Content ◽  
Atmospheric Aerosols ◽  
Atmospheric Chemistry ◽  
Organic Aerosol ◽  
Atmospheric Composition ◽  
Airborne Measurements ◽  
The Usa ◽  
Aerosol Chemical Composition

Abstract. Aerosol chemical composition was found to influence nighttime atmospheric chemistry during a series of airborne measurements in northwestern Europe in summer conditions, which has implications for regional air quality and climate. The uptake of dinitrogen pentoxide, γ (N2O5), to particle surfaces was found to be modulated by the amount of water content and ammonium nitrate present in the aerosol. The conditions prevalent in this study suggest that the net uptake rate of N2O5 to atmospheric aerosols was relatively efficient compared to previous studies, with γ (N2O5) values in the range 0.01–0.03. This is likely a consequence of the elevated relative humidity in the region, which promotes greater aerosol water content. Increased nitrate concentrations relative to particulate water were found to suppress N2O5 uptake. The results presented here contrast with previous ambient studies of N2O5 uptake, which have generally taken place in low-nitrate environments in the USA. Comparison of the N2O5 uptake derived from the measurements with a parameterised scheme that is based on the ratio of particulate water to nitrate yielded reasonably good agreement in terms of the magnitude and variation in uptake, provided the effect of chloride was neglected. An additional suppression of the parameterised uptake is likely required to fully capture the variation in N2O5 uptake, which could be achieved via the known suppression by organic aerosol. However, existing parameterisations representing the suppression by organic aerosol were unable to fully represent the variation in N2O5 uptake. These results provide important ambient measurement constraint on our ability to predict N2O5 uptake in regional and global aerosol models. N2O5 uptake is a potentially important source of nitrate aerosol and a sink of the nitrate radical, which is the main nocturnal oxidant in the atmosphere. The results further highlight the importance of ammonium nitrate in northwestern Europe as a key component of atmospheric composition in the region.

scholarly journals Enhancement of the aerosol direct radiative effect by semi-volatile aerosol components: airborne measurements in North-Western Europe

2010 ◽  
Vol 10 (4) ◽  
pp. 10653-10705 ◽  
Author(s):  
W. T. Morgan ◽  
J. D. Allan ◽  
K. N. Bower ◽  
M. Esselborn ◽  
B. Harris ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Chemical Composition ◽  
Vertical Distribution ◽  
Ammonium Nitrate ◽  
Sulphur Dioxide ◽  
Radiative Forcing ◽  
Western Europe ◽  
Aerosol Mass ◽  
Sulphur Dioxide Emissions ◽  
North Western

Abstract. A case study of atmospheric aerosol measurements exploring the impact of the vertical distribution of aerosol chemical composition upon the radiative budget in North-Western Europe is presented. Sub-micron aerosol chemical composition was measured by an Aerodyne Aerosol Mass Spectrometer (AMS) on both an airborne platform and a ground-based site at Cabauw in the Netherlands. The examined period in May 2008 was characterised by enhanced pollution loadings in North-Western Europe and was dominated by ammonium nitrate and Organic Matter (OM). Both ammonium nitrate and OM were observed to increase with altitude in the atmospheric boundary layer. This is primarily attributed to partitioning of semi-volatile gas phase species to the particle phase at reduced temperature and enhanced relative humidity. Increased ammonium nitrate concentrations in particular were found to strongly increase the ambient scattering potential of the aerosol burden, which was a consequence of the large amount of associated water as well as the enhanced mass. During particularly polluted conditions, increases in aerosol optical depth of 50–100% were estimated to occur due to the observed increase in secondary aerosol mass and associated water uptake. Furthermore, the single scattering albedo was also shown to increase with height in the boundary layer. These enhancements combined to increase the negative direct aerosol radiative forcing by close to a factor of two at the median percentile level. Such increases have major ramifications for regional climate predictions as semi-volatile components are often not included in aerosol models. The results presented here provide an ideal opportunity to test regional and global representations of both the aerosol vertical distribution and subsequent impacts in North-Western Europe. North-Western Europe can be viewed as an analogue for the possible future air quality over other polluted regions of the Northern Hemisphere, where substantial reductions in sulphur dioxide emissions have yet to occur. Anticipated reductions in sulphur dioxide in polluted regions will result in an increase in the availability of ammonia to form ammonium nitrate as opposed to ammonium sulphate. This will be most important where intensive agricultural practises occur. Our observations over North-Western Europe, a region where sulphur dioxide emissions have already been reduced, indicate that failure to include the semi-volatile behaviour of ammonium nitrate will result in significant errors in predicted aerosol direct radiative forcing. Such errors will be particularly significant on regional scales.

scholarly journals Enhancement of the aerosol direct radiative effect by semi-volatile aerosol components: airborne measurements in North-Western Europe

2010 ◽  
Vol 10 (17) ◽  
pp. 8151-8171 ◽  
Author(s):  
W. T. Morgan ◽  
J. D. Allan ◽  
K. N. Bower ◽  
M. Esselborn ◽  
B. Harris ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Chemical Composition ◽  
Vertical Distribution ◽  
Ammonium Nitrate ◽  
Sulphur Dioxide ◽  
Radiative Forcing ◽  
Western Europe ◽  
Aerosol Mass ◽  
Sulphur Dioxide Emissions ◽  
North Western

Abstract. A case study of atmospheric aerosol measurements exploring the impact of the vertical distribution of aerosol chemical composition upon the radiative budget in North-Western Europe is presented. Sub-micron aerosol chemical composition was measured by an Aerodyne Aerosol Mass Spectrometer (AMS) on both an airborne platform and a ground-based site at Cabauw in the Netherlands. The examined period in May 2008 was characterised by enhanced pollution loadings in North-Western Europe and was dominated by ammonium nitrate and Organic Matter (OM). Both ammonium nitrate and OM were observed to increase with altitude in the atmospheric boundary layer. This is primarily attributed to partitioning of semi-volatile gas phase species to the particle phase at reduced temperature and enhanced relative humidity. Increased ammonium nitrate concentrations in particular were found to strongly increase the ambient scattering potential of the aerosol burden, which was a consequence of the large amount of associated water as well as the enhanced mass. During particularly polluted conditions, increases in aerosol optical depth of 50–100% were estimated to occur due to the observed increase in secondary aerosol mass and associated water uptake. Furthermore, the single scattering albedo was also shown to increase with height in the boundary layer. These enhancements combined to increase the negative direct aerosol radiative forcing by close to a factor of two at the median percentile level. Such increases have major ramifications for regional climate predictions as semi-volatile components are often not included in aerosol models. The results presented here provide an ideal opportunity to test regional and global representations of both the aerosol vertical distribution and subsequent impacts in North-Western Europe. North-Western Europe can be viewed as an analogue for the possible future air quality over other polluted regions of the Northern Hemisphere, where substantial reductions in sulphur dioxide emissions have yet to occur. Anticipated reductions in sulphur dioxide in polluted regions will result in an increase in the availability of ammonia to form ammonium nitrate as opposed to ammonium sulphate. This will be most important where intensive agricultural practises occur. Our observations over North-Western Europe, a region where sulphur dioxide emissions have already been reduced, indicate that failure to include the semi-volatile behaviour of ammonium nitrate will result in significant errors in predicted aerosol direct radiative forcing. Such errors will be particularly significant on regional scales.

scholarly journals Sources and processes that control the submicron organic aerosol in an urban Mediterranean environment (Athens) using high temporal resolution chemical composition measurements

2018 ◽  
Author(s):  
Iasonas Stavroulas ◽  
Aikaterini Bougiatioti ◽  
Despina Paraskevopoulou ◽  
Georgios Grivas ◽  
Eleni Liakakou ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Biomass Burning ◽  
Volatile Component ◽  
Organic Aerosol ◽  
Urban Environments ◽  
High Temporal Resolution ◽  
Organic Fraction ◽  
Scanning Mobility Particle Sizer ◽  
Secondary Aerosol ◽  
Combustion Sources

Abstract. Submicron aerosol chemical composition has been studied during a year-long period (26/07/2016–31/07/2017) and two winter-time intensive campaigns (18/12/2013–21/02/2014 and 23/12/2015–17/02/2016), at a central site in Athens, Greece, using an Aerosol Chemical Speciation Monitor (ACSM). Concurrent measurements include a Particle-Into-Liquid Sampler (PILS-IC), a Scanning Mobility Particle Sizer (SMPS), an AE-33 Aethalometer and Ion Chromatography analysis on 24 or 12 hour filter samples. Quality of the ACSM data was assured by comparison versus the above mentioned measurements. The aim of the study was to characterize the seasonal variability of the main fine aerosol constituents and decipher the sources of organic aerosol (OA). Organics were found to contribute almost half of the submicron mass, with concentrations during wintertime reaching up to 200 μg m−3, on occasions. During this season, the primary sources contribute about 34 % of the organic fraction, comprising of biomass burning (10 %), fossil fuel combustion (16 %) and cooking (8 %), while the remaining 66 % is attributed to secondary aerosol. The semi-volatile component of the oxidized organic aerosol (SV-OOA; 31 %) was found to be clearly linked to combustion sources and in particular biomass burning, and even a part of the very oxidized, low-volatility component (LV-OOA; 35 %) could also be attributed to the oxidation of emissions from these primary combustion sources. These results highlight the rising importance of biomass burning in urban environments during wintertime, as revealed through this characteristic example of Athens, Greece, where the economic recessions led to an abrupt shift to biomass burning for heating purposes in winter. During summer, when concentrations of fine aerosols are considerably lower, more than 80 % of the organic fraction is attributed to secondary aerosol (SV-OOA 30 % and LV-OOA 53 %). In contrast to winter, SV-OOA appears to result from a well-mixed type of aerosol, linked to fast photochemical processes and the oxidation of primary traffic and biogenic emissions. Finally, LV-OOA presents a more regional character in summer, owing to the oxidation, within a few days, of organic aerosol.

scholarly journals Comparison between simulated and observed chemical composition of fine aerosols in Paris (France) during springtime: contribution of regional versus continental emissions

2010 ◽  
Vol 10 (24) ◽  
pp. 11987-12004 ◽  
Author(s):  
J. Sciare ◽  
O. d'Argouges ◽  
Q. J. Zhang ◽  
R. Sarda-Estève ◽  
C. Gaimoz ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Secondary Organic Aerosols ◽  
Transport Model ◽  
Organic Aerosols ◽  
Carbonaceous Material ◽  
Chemical Components ◽  
Carbonaceous Aerosols ◽  
Time Resolved ◽  
Air Masses ◽  
North Western

Abstract. Hourly concentrations of inorganic salts (ions) and carbonaceous material in fine aerosols (aerodynamic diameter, A.D. <2.5 μm) have been determined experimentally from fast measurements performed for a 3-week period in spring 2007 in Paris (France). The sum of these two chemical components (ions and carbonaceous aerosols) has shown to account for most of the fine aerosol mass (PM2.5). This time-resolved dataset allowed investigating the factors controlling the levels of PM2.5 in Paris and showed that polluted periods with PM2.5 > 15 μg m−3 were characterized by air masses of continental (North-Western Europe) origin and chemical composition made by 75% of ions. By contrast, periods with clean marine air masses have shown the lowest PM2.5 concentrations (typically of about 10 μg m−3); carbonaceous aerosols contributing for most of this mass (typically 75%). In order to better discriminate between local and continental contributions to the observed chemical composition and concentrations of PM2.5 over Paris, a comparative study was performed between this time-resolved dataset and the outputs of a chemistry transport model (CHIMERE), showing a relatively good capability of the model to reproduce the time-limited intense maxima observed in the field for PM2.5 and ion species. Different model scenarios were then investigated switching off local and European (North-Western and Central) emissions. Results of these scenarios have clearly shown that most of the ions observed over Paris during polluted periods, were either transported or formed in-situ from gas precursors transported from Northern Europe. On the opposite, long-range transport from Europe appeared to weakly contribute to the levels of carbonaceous aerosols observed over Paris. The model failed to properly account for the concentration levels and variability of secondary organic aerosols (SOA) determined experimentally by the EC-tracer method. The abundance of SOA (relatively to organic aerosol, OA) was as much as 75%, showing a weak dependence on air masses origin. Elevated SOA/OA ratios were also observed for air masses having residence time above ground of less than 10 h, suggesting intense emissions and/or photochemical processes leading to rapid formation of secondary organic aerosols.

scholarly journals Characterization of aerosol chemical composition with aerosol mass spectrometry in Central Europe: an overview

2010 ◽  
Vol 10 (21) ◽  
pp. 10453-10471 ◽  
Author(s):  
V. A. Lanz ◽  
A. S. H. Prévôt ◽  
M. R. Alfarra ◽  
S. Weimer ◽  
C. Mohr ◽  
...  
Keyword(s):  
Mass Spectrometry ◽  
Chemical Composition ◽  
Organic Aerosol ◽  
Volatile Fraction ◽  
Aerosol Composition ◽  
Aerosol Mass ◽  
Aerosol Mass Spectrometry ◽  
Field Campaigns ◽  
Alpine Valleys ◽  
Aerosol Chemical Composition

Abstract. Real-time measurements of non-refractory submicron aerosols (NR-PM1) were conducted within the greater Alpine region (Switzerland, Germany, Austria, France and Liechtenstein) during several week-long field campaigns in 2002–2009. This region represents one of the most important economic and recreational spaces in Europe. A large variety of sites was covered including urban backgrounds, motorways, rural, remote, and high-alpine stations, and also mobile on-road measurements were performed. Inorganic and organic aerosol (OA) fractions were determined by means of aerosol mass spectrometry (AMS). The data originating from 13 different field campaigns and the combined data have been utilized for providing an improved temporal and spatial data coverage. The average mass concentration of NR-PM1 for the different campaigns typically ranged between 10 and 30 μg m−3. Overall, the organic portion was most abundant, ranging from 36% to 81% of NR-PM1. Other main constituents comprised ammonium (5–15%), nitrate (8–36%), sulfate (3–26%), and chloride (0–5%). These latter anions were, on average, fully neutralized by ammonium. As a major result, time of the year (winter vs. summer) and location of the site (Alpine valleys vs. Plateau) could largely explain the variability in aerosol chemical composition for the different campaigns and were found to be better descriptors for aerosol composition than the type of site (urban, rural etc.). Thus, a reassessment of classifications of measurements sites might be considered in the future, possibly also for other regions of the world. The OA data was further analyzed using positive matrix factorization (PMF) and the multi-linear engine ME (factor analysis) separating the total OA into its underlying components, such as oxygenated (mostly secondary) organic aerosol (OOA), hydrocarbon-like and freshly emitted organic aerosol (HOA), as well as OA from biomass burning (BBOA). OOA was ubiquitous, ranged between 36% and 94% of OA, and could be separated into a low-volatility and a semi-volatile fraction (LV-OOA and SV-OOA) for all summer campaigns at low altitude sites. Wood combustion (BBOA) accounted for a considerable fraction during wintertime (17–49% OA), particularly in narrow Alpine valleys BBOA was often the most abundant OA component. HOA/OA ratios were comparatively low for all campaigns (6–16%) with the exception of on-road, mobile measurements (23%) in the Rhine Valley. The abundance of the aerosol components and the retrievability of SV-OOA and LV-OOA are discussed in the light of atmospheric chemistry and physics.

scholarly journals Variation in global chemical composition of PM<sub>2.5</sub>: emerging results from SPARTAN

2016 ◽  
Vol 16 (15) ◽  
pp. 9629-9653 ◽  
Author(s):  
Graydon Snider ◽  
Crystal L. Weagle ◽  
Kalaivani K. Murdymootoo ◽  
Amanda Ring ◽  
Yvonne Ritchie ◽  
...  
Keyword(s):  
Particulate Matter ◽  
Chemical Composition ◽  
Ammonium Nitrate ◽  
Black Carbon ◽  
Major Ions ◽  
Dry Season ◽  
Chemical Components ◽  
Spatial And Temporal Variability ◽  
Crustal Material ◽  
Effective Manner

Abstract. The Surface PARTiculate mAtter Network (SPARTAN) is a long-term project that includes characterization of chemical and physical attributes of aerosols from filter samples collected worldwide. This paper discusses the ongoing efforts of SPARTAN to define and quantify major ions and trace metals found in fine particulate matter (PM2.5). Our methods infer the spatial and temporal variability of PM2.5 in a cost-effective manner. Gravimetrically weighed filters represent multi-day averages of PM2.5, with a collocated nephelometer sampling air continuously. SPARTAN instruments are paired with AErosol RObotic NETwork (AERONET) sun photometers to better understand the relationship between ground-level PM2.5 and columnar aerosol optical depth (AOD).We have examined the chemical composition of PM2.5 at 12 globally dispersed, densely populated urban locations and a site at Mammoth Cave (US) National Park used as a background comparison. So far, each SPARTAN location has been active between the years 2013 and 2016 over periods of 2–26 months, with an average period of 12 months per site. These sites have collectively gathered over 10 years of quality aerosol data. The major PM2.5 constituents across all sites (relative contribution ± SD) are ammoniated sulfate (20 % ± 11 %), crustal material (13.4 % ± 9.9 %), equivalent black carbon (11.9 % ± 8.4 %), ammonium nitrate (4.7 % ± 3.0 %), sea salt (2.3 % ± 1.6 %), trace element oxides (1.0 % ± 1.1 %), water (7.2 % ± 3.3 %) at 35 % RH, and residual matter (40 % ± 24 %).Analysis of filter samples reveals that several PM2.5 chemical components varied by more than an order of magnitude between sites. Ammoniated sulfate ranges from 1.1 µg m−3 (Buenos Aires, Argentina) to 17 µg m−3 (Kanpur, India in the dry season). Ammonium nitrate ranged from 0.2 µg m−3 (Mammoth Cave, in summer) to 6.8  µg m−3 (Kanpur, dry season). Equivalent black carbon ranged from 0.7 µg m−3 (Mammoth Cave) to over 8 µg m−3 (Dhaka, Bangladesh and Kanpur, India). Comparison of SPARTAN vs. coincident measurements from the Interagency Monitoring of Protected Visual Environments (IMPROVE) network at Mammoth Cave yielded a high degree of consistency for daily PM2.5 (r2 = 0.76, slope  =  1.12), daily sulfate (r2 = 0.86, slope  =  1.03), and mean fractions of all major PM2.5 components (within 6 %). Major ions generally agree well with previous studies at the same urban locations (e.g. sulfate fractions agree within 4 % for 8 out of 11 collocation comparisons). Enhanced anthropogenic dust fractions in large urban areas (e.g. Singapore, Kanpur, Hanoi, and Dhaka) are apparent from high Zn : Al ratios.The expected water contribution to aerosols is calculated via the hygroscopicity parameter κv for each filter. Mean aggregate values ranged from 0.15 (Ilorin) to 0.28 (Rehovot). The all-site parameter mean is 0.20 ± 0.04. Chemical composition and water retention in each filter measurement allows inference of hourly PM2.5 at 35 % relative humidity by merging with nephelometer measurements. These hourly PM2.5 estimates compare favourably with a beta attenuation monitor (MetOne) at the nearby US embassy in Beijing, with a coefficient of variation r2 =  0.67 (n =  3167), compared to r2 = 0.62 when κv was not considered. SPARTAN continues to provide an open-access database of PM2.5 compositional filter information and hourly mass collected from a global federation of instruments.

scholarly journals Effect of NO<sub>x</sub> level on secondary organic aerosol (SOA) formation from the photooxidation of terpenes

2007 ◽  
Vol 7 (19) ◽  
pp. 5159-5174 ◽  
Author(s):  
N. L. Ng ◽  
P. S. Chhabra ◽  
A. W. H. Chan ◽  
J. D. Surratt ◽  
J. H. Kroll ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Secondary Organic Aerosol ◽  
Organic Aerosol ◽  
Organic Nitrates ◽  
Biogenic Hydrocarbons ◽  
Alkoxy Radicals ◽  
Volatile Products ◽  
Products Analysis ◽  
Environmental Chambers ◽  
Aerosol Chemical Composition

Abstract. Secondary organic aerosol (SOA) formation from the photooxidation of one monoterpene (α-pinene) and two sesquiterpenes (longifolene and aromadendrene) is investigated in the Caltech environmental chambers. The effect of NOx on SOA formation for these biogenic hydrocarbons is evaluated by performing photooxidation experiments under varying NOx conditions. The NOx dependence of α-pinene SOA formation follows the same trend as that observed previously for a number of SOA precursors, including isoprene, in which SOA yield (defined as the ratio of the mass of organic aerosol formed to the mass of parent hydrocarbon reacted) decreases as NOx level increases. The NOx dependence of SOA yield for the sesquiterpenes, longifolene and aromadendrene, however, differs from that determined for isoprene and α-pinene; the aerosol yield under high-NOx conditions substantially exceeds that under low-NOx conditions. The reversal of the NOx dependence of SOA formation for the sesquiterpenes is consistent with formation of relatively low-volatility organic nitrates, and/or the isomerization of large alkoxy radicals leading to less volatile products. Analysis of the aerosol chemical composition for longifolene confirms the presence of organic nitrates under high-NOx conditions. Consequently the formation of SOA from certain biogenic hydrocarbons such as sesquiterpenes (and possibly large anthropogenic hydrocarbons as well) may be more efficient in polluted air.

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