scholarly journals Receptor modelling of secondary and carbonaceous particulate matter at a southern UK site

2013 ◽  
Vol 13 (4) ◽  
pp. 1879-1894 ◽  
Author(s):  
A. Charron ◽  
C. Degrendele ◽  
B. Laongsri ◽  
R. M. Harrison
Keyword(s):  
Organic Carbon ◽  
Secondary Organic Aerosol ◽  
Concentration Field ◽  
Organic Aerosol ◽  
Careful Analysis ◽  
Rural Site ◽  
Back Trajectories ◽  
Regional Influence ◽  
Secondary Organic Carbon ◽  
The One

Abstract. Complementary approaches have been taken to better understand the sources and their spatial distribution for secondary inorganic (nitrate and sulphate) and secondary organic aerosol sampled at a rural site (Harwell) in the southern United Kingdom. A concentration field map method was applied to 1581 daily samples of chloride, nitrate and sulphate from 2006 to 2010, and 982 samples for organic carbon and elemental carbon from 2007 to 2010. This revealed a rather similar pattern of sources for nitrate, sulphate and secondary organic carbon within western/central Europe, which in the case of nitrate, sulphate, organic carbon and secondary organic carbon, correlated significantly with EMEP emissions maps of NOx, SO2, and VOC respectively. A slightly more southerly source emphasis for secondary organic carbon may reflect the contribution of biogenic sources. Trajectory clusters confirm this pattern of behaviour with a major contribution from mainland European sources. Similar behaviours of, on the one hand, sulphate and organic carbon and, on the other hand, EC and nitrate showed that the former are more subject to regional influence than the latter in agreement with the slower atmospheric formation of sulphate and secondary organic aerosol than for nitrate, and the local/mesoscale influences upon primary EC. However, careful analysis of back trajectories and Concentration Field Maps indicates a strong contribution of mainland European sites to EC concentrations at Harwell. In a separate study, measurements of sulphate, nitrate, elemental and organic carbon were made in 100 simultaneously collected samples at Harwell and at a suburban site in Birmingham (UK). This showed a significant correlation in concentrations between the two sites for all of the secondary constituents, further indicating secondary organic aerosol to be a regional pollutant behaving similarly to sulphate and nitrate.

scholarly journals Receptor modelling of secondary particulate matter at UK sites

2012 ◽  
Vol 12 (10) ◽  
pp. 27255-27295
Author(s):  
A. Charron ◽  
C. Degrendele ◽  
B. Laongsri ◽  
R. M. Harrison
Keyword(s):  
Organic Carbon ◽  
Secondary Organic Aerosol ◽  
Concentration Field ◽  
Organic Aerosol ◽  
Rural Site ◽  
Regional Influence ◽  
Secondary Organic Carbon ◽  
The One ◽  
Atmospheric Formation ◽  
Made In

Abstract. Complementary approaches have been taken to better understand the sources and their spatial distribution for secondary inorganic (nitrate and sulphate) and secondary organic aerosol sampled at a rural site (Harwell) in the southern United Kingdom. A concentration field map method was applied to 1581 daily samples of chloride, nitrate and sulphate from 2006 to 2010, and 982 samples for organic carbon and elemental carbon from 2007 to 2010. This revealed a rather similar pattern of sources for nitrate, sulphate and secondary organic carbon within western/central Europe, which in the case of nitrate and sulphate, correlated significantly with EMEP emissions maps of NOx and SO2. A slightly more southerly source emphasis for secondary organic carbon may reflect the contribution of biogenic sources. Trajectory clusters confirm this pattern of behaviour with a major contribution from mainland European sources. Similar behaviours of, on the one hand, sulphate and organic carbon and, on the other hand, EC and nitrate showed that the former are more subject to regional influence than the latter in agreement with the slower atmospheric formation of sulphate and secondary organic aerosol than for nitrate, and the local/mesoscale influences upon primary EC. In a separate study, measurements of sulphate, nitrate, elemental and organic carbon were made in 100 simultaneously collected samples at Harwell and at a suburban site in Birmingham (UK). This showed a significant correlation in concentrations between the two sites for all of the secondary constituents, further indicating secondary organic aerosol to be a regional pollutant behaving similarly to sulphate and nitrate.

scholarly journals Atmospheric oxidation of isoprene and 1,3-butadiene: influence of aerosol acidity and relative humidity on secondary organic aerosol

2015 ◽  
Vol 15 (7) ◽  
pp. 3773-3783 ◽  
Author(s):  
M. Lewandowski ◽  
M. Jaoui ◽  
J. H. Offenberg ◽  
J. D. Krug ◽  
T. E. Kleindienst
Keyword(s):  
Organic Carbon ◽  
Secondary Organic Aerosol ◽  
Absolute Humidity ◽  
Organic Aerosol ◽  
Photochemical Oxidation ◽  
Pronounced Increase ◽  
Acid Sensitivity ◽  
Aerosol Acidity ◽  
Acidic Sulfate ◽  
Secondary Organic Carbon

Abstract. The effects of acidic seed aerosols on the formation of secondary organic aerosol (SOA) have been examined in a number of previous studies, several of which have observed strong linear correlations between the aerosol acidity (measured as nmol H+ m−3 air sample volume) and the percent change in secondary organic carbon (SOC). The measurements have used several precursor compounds representative of different classes of biogenic hydrocarbons including isoprene, monoterpenes, and sesquiterpenes. To date, isoprene has displayed the most pronounced increase in SOC, although few measurements have been conducted with anthropogenic hydrocarbons. In the present study, we examine several aspects of the effect of aerosol acidity on the secondary organic carbon formation from the photooxidation of 1,3-butadiene, and extend the previous analysis of isoprene. The photooxidation products measured in the absence and presence of acidic sulfate aerosols were generated either through photochemical oxidation of SO2 or by nebulizing mixtures of ammonium sulfate and sulfuric acid into a 14.5 m3 smog chamber system. The results showed that, like isoprene and β-caryophyllene, 1,3-butadiene SOC yields linearly correlate with increasing acidic sulfate aerosol. The observed acid sensitivity of 0.11% SOC increase per nmol m−3 increase in H+ was approximately a factor of 3 less than that measured for isoprene. The results also showed that the aerosol yield decreased with increasing humidity for both isoprene and 1,3-butadiene, although to different degrees. Increasing the absolute humidity from 2 to 12 g m−3 reduced the 1,3-butadiene yield by 45% and the isoprene yield by 85%.

scholarly journals Atmospheric oxidation of isoprene and 1,3-butadiene: influence of aerosol acidity and relative humidity on secondary organic aerosol

2014 ◽  
Vol 14 (21) ◽  
pp. 29429-29458 ◽  
Author(s):  
M. Lewandowski ◽  
M. Jaoui ◽  
J. H. Offenberg ◽  
J. D. Krug ◽  
T. E. Kleindienst
Keyword(s):  
Organic Carbon ◽  
Secondary Organic Aerosol ◽  
Absolute Humidity ◽  
Organic Aerosol ◽  
Photochemical Oxidation ◽  
Pronounced Increase ◽  
Acid Sensitivity ◽  
Aerosol Acidity ◽  
Acidic Sulfate ◽  
Secondary Organic Carbon

Abstract. The effects of acidic seed aerosols on the formation of secondary organic aerosol (SOA) have been examined in a number of previous studies, several of which have observed strong linear correlations between the aerosol acidity (measured as nmol H+ per m3 air sample volume) and the percent change of secondary organic carbon (SOC). The measurements have used several precursor compounds representative of different classes of biogenic hydrocarbons including isoprene, monoterpenes, and sesquiterpenes. To date, isoprene has displayed the most pronounced increase in SOC, although few measurements have been conducted with anthropogenic hydrocarbons. In the present study, we examine several aspects of the effect of aerosol acidity on the secondary organic carbon formation from the photooxidation of 1,3-butadiene, as well as extending the previous analysis of isoprene. The photooxidation products measured in the absence and presence of acidic sulfate aerosols were generated either through photochemical oxidation of SO2 or by nebulizing mixtures of ammonium sulfate and sulfuric acid into a 14.5 m3 smog chamber system. The results showed that, like isoprene and β-caryophyllene, 1,3-butadiene SOC yields linearly correlate with increasing acidic sulfate aerosol. The observed acid sensitivity of 0.11% SOC increase per nmol m−3 increase in H+ was approximately a factor of three less than that measured for isoprene. The results also showed that the aerosol yield decreased with increasing humidity for both isoprene and 1,3-butadiene, although to different degrees. Increasing the absolute humidity from 2 to 12 g m−3 reduced the 1,3-butadiene yield by 45% and the isoprene yield by 85%.

scholarly journals Tracer-based source apportioning of atmospheric organic carbon and the influence of anthropogenic emissions on secondary organic aerosol formation in Hong Kong

2021 ◽  
Vol 21 (13) ◽  
pp. 10589-10608
Author(s):  
Yubo Cheng ◽  
Yiqiu Ma ◽  
Di Hu
Keyword(s):  
Hong Kong ◽  
Organic Carbon ◽  
Secondary Organic Aerosol ◽  
Large Fraction ◽  
Linear Regression Analysis ◽  
Temporal Trends ◽  
Organic Aerosol ◽  
Gas Chromatography Mass Spectrometry ◽  
Multivariate Linear Regression Analysis ◽  
Aerosol Formation

Abstract. Here we conducted comprehensive chemical characterization and source apportionment of 49 PM2.5 samples collected in Hong Kong. Besides the major aerosol constituents, 39 polar organic species, including 14 secondary organic aerosol (SOA) tracers of isoprene, monoterpenes, β-caryophyllene, and naphthalene, were quantified using gas chromatography–mass spectrometry (GC–MS). Six factors, i.e., SOA, secondary sulfate (SS), biomass burning (BB)/SOA, sea salt, marine vessels, and vehicle emissions, were apportioned by positive matrix factorization (PMF) as the major sources of ambient organic carbon (OC) in Hong Kong. The secondary formation, including OC from SOA, SS, and aging of BB plume, was the leading contributor to OC (51.4 %, 2.15 ± 1.37 µg C m−3) throughout the year. We then applied a tracer-based method (TBM) to estimate the SOA formation from the photo-oxidation of four selected precursors, and monoterpene SOA was the most abundant. A Kintecus kinetic model was used to examine the formation channels of isoprene SOA, and the aerosol-phase ring-opening reaction of isoprene epoxydiols (IEPOXs) was found to be the dominant formation pathway. Consistently, IEPOX tracers contributed 94 % to total GC–MS-quantified isoprene SOA tracers. The TBM-estimated secondary organic carbon (SOCTBM) and PMF-apportioned SOC (SOCPMF) showed similar temporal trends; however, SOCTBM only accounted for 26.5 % of SOCPMF, indicating a large fraction of ambient SOA was from other reaction pathways or precursors. Results of Pearson's R and multivariate linear regression analysis showed that NOx processing played a key role in both daytime and nighttime SOA production in the region. Moreover, sulfate had a significant positive linear relationship with SOCPMF and SS-related SOC, and particle acidity was significantly correlated with SOC from the aging of BB.

scholarly journals Chemical Characterization of Secondary Organic Aerosol at a Rural Site in the Southeastern U.S.: Insights from Simultaneous HR-ToF-AMS and FIGAERO-CIMS Measurements

2020 ◽  
Author(s):  
Yunle Chen ◽  
Masayuki Takeuchi ◽  
Theodora Nah ◽  
Lu Xu ◽  
Manjula R. Canagaratna ◽  
...  
Keyword(s):  
High Resolution ◽  
Mass Spectrometer ◽  
Secondary Organic Aerosol ◽  
Time Of Flight ◽  
Organic Aerosol ◽  
Rural Site ◽  
Organic Nitrate ◽  
Ionization Mass ◽  
Resolution Time ◽  
Radical Oxidation

Abstract. The formation and evolution of secondary organic aerosol (SOA) was investigated at Yorkville, GA, in late summer (mid-August ~ mid-October, 2016). Organic aerosol (OA) composition was measured using two on-line mass spectrometry instruments, the high-resolution time-of-flight aerosol mass spectrometer (AMS) and the Filter Inlet for Gases and AEROsols coupled to a high-resolution time-of-flight iodide-adduct chemical ionization mass spectrometer (FIGAERO-CIMS). Through analysis of speciated organics data from FIGAERO-CIMS and factorization analysis of data obtained from both instruments, we observed notable SOA formation from isoprene and monoterpenes during both day and night. Specifically, in addition to isoprene epoxydiols (IEPOX) uptake, we identified isoprene SOA formation via hydroxyl hydroperoxide oxidation (ISOPOOH oxidation via non-IEPOX pathways) and isoprene organic nitrate formation via photooxidation in the presence of NOx and nitrate radical oxidation. Monoterpenes were found to be the most important SOA precursors at night. We observed significant contributions from highly-oxidized acid-like compounds to the aged OA factor from FIGAERO-CIMS. Taken together, our results showed that FIGAERO-CIMS measurements are highly complementary to the extensively used AMS factorization analysis, and together they provide more comprehensive insights into OA sources and composition.

scholarly journals Diurnal variations of organic molecular tracers and stable carbon isotopic compositions in atmospheric aerosols over Mt. Tai in North China Plain: an influence of biomass burning

2012 ◽  
Vol 12 (4) ◽  
pp. 9079-9124
Author(s):  
P. Q. Fu ◽  
K. Kawamura ◽  
J. Chen ◽  
J. Li ◽  
Y. L. Sun ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Biomass Burning ◽  
North China Plain ◽  
North China ◽  
Secondary Organic Aerosol ◽  
Organic Aerosol ◽  
Total Carbon ◽  
Stable Carbon ◽  
Isotopic Compositions ◽  
Carbon Isotopic

Abstract. Organic tracer compounds of tropospheric aerosols, as well as organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC), and stable carbon isotope ratios (δ13C) of total carbon (TC) have been investigated for aerosol samples collected during early and late periods of Mount Tai eXperiment 2006 (MTX2006) field campaign in North China Plain. Total solvent extracts were investigated by gas chromatography/mass spectrometry. More than 130 organic compounds were detected in the aerosol samples. They were grouped into twelve organic compound classes, including biomass burning tracers, biogenic primary sugars, biogenic secondary organic aerosol (SOA) tracers, and anthropogenic tracers such as phthalates, hopanes and polycyclic aromatic hydrocarbons (PAHs). In early June when the field burning activities of wheat straws in North China Plain were very active, the total identified organics (2090 ± 1170 ng m−3) were double those in late June (926 ± 574 ng m−3). All the compound classes were more abundant in early June than in late June, except phthalate esters, which were higher in late June. Levoglucosan (88–1210 ng m−3, 403 ng m−3) was found as the most abundant single compound in early June, while diisobutyl phthalate was the predominant species in late June. During the biomass-burning period in early June, the diurnal trends of most of the primary and secondary organic aerosol tracers were characterized by the concentration peaks observed at mid-night or in early morning, while in late June most of the organic species peaked in late afternoon. This suggests that smoke plumes from biomass burning can uplift the aerosol particulate matter to a certain altitude and then transported to and encountered the summit of Mt. Tai during nighttime. On the basis of the tracer-based method for the estimation of biomass-burning OC, fungal-spore OC and biogenic secondary organic carbon (SOC), we estimate that an average of 24% (up to 64%) of the OC in the Mt. Tai aerosols was due to biomass burning in early June, followed by the contribution of isoprene SOC (mean 4.3%). In contrast, isoprene SOC was the main contributor (6.6%) to OC, and only 3.0% of the OC was due to biomass burning in late June. In early June, δ13C of TC (−26.6‰ to −23.2‰, mean −25.0‰) were lower than those (−23.9‰ to −21.9‰, mean −22.9‰) in late June. In addition, a strong anti-correlation was found between levoglucosan and δ13C values. This study demonstrates that crop-residue burning activities can significantly enhance the organic aerosol loading and alter the organic molecular compositions and stable carbon isotopic compositions of aerosol particles in the troposphere over North China Plain.

scholarly journals Fossil and non-fossil sources of organic carbon (OC) and elemental carbon (EC) in Göteborg, Sweden

2009 ◽  
Vol 9 (5) ◽  
pp. 1521-1535 ◽  
Author(s):  
S. Szidat ◽  
M. Ruff ◽  
N. Perron ◽  
L. Wacker ◽  
H.-A. Synal ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Elemental Carbon ◽  
Latin Hypercube Sampling ◽  
Water Soluble ◽  
Total Carbon ◽  
Rural Site ◽  
Urban Site ◽  
Winter Period ◽  
Back Trajectories ◽  
Wood Burning

Abstract. Particulate matter was collected at an urban site in Göteborg (Sweden) in February/March 2005 and in June/July 2006. Additional samples were collected at a rural site for the winter period. Total carbon (TC) concentrations were 2.1–3.6 μg m−3, 1.8–1.9 μg m−3, and 2.2–3.0 μg m−3 for urban/winter, rural/winter, and urban/summer conditions, respectively. Elemental carbon (EC), organic carbon (OC), water-insoluble OC (WINSOC), and water-soluble OC (WSOC) were analyzed for 14C in order to distinguish fossil from non-fossil emissions. As wood burning is the single major source of non-fossil EC, its contribution can be quantified directly. For non-fossil OC, the wood-burning fraction was determined independently by levoglucosan and 14C analysis and combined using Latin-hypercube sampling (LHS). For the winter period, the relative contribution of EC from wood burning to the total EC was >3 times higher at the rural site compared to the urban site, whereas the absolute concentrations of EC from wood burning were elevated only moderately at the rural compared to the urban site. Thus, the urban site is substantially more influenced by fossil EC emissions. For summer, biogenic emissions dominated OC concentrations most likely due to secondary organic aerosol (SOA) formation. During both seasons, a more pronounced fossil signal was observed for Göteborg than has previously been reported for Zurich, Switzerland. Analysis of air mass origin using back trajectories suggests that the fossil impact was larger when local sources dominated, whereas long-range transport caused an enhanced non-fossil signal. In comparison to other European locations, concentrations of levoglucosan and other monosaccharide anhydrides were low for the urban and the rural site in the area of Göteborg during winter.

CMAQ Model Performance Enhanced When In-Cloud Secondary Organic Aerosol is Included: Comparisons of Organic Carbon Predictions with Measurements

2008 ◽  
Vol 42 (23) ◽  
pp. 8798-8802 ◽  
Author(s):  
Annmarie G. Carlton ◽  
Barbara J. Turpin ◽  
Katye E. Altieri ◽  
Sybil P. Seitzinger ◽  
Rohit Mathur ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Secondary Organic Aerosol ◽  
Model Performance ◽  
Organic Aerosol

scholarly journals Fossil and non-fossil sources of organic carbon (OC) and elemental carbon (EC) in Göteborg, Sweden

2008 ◽  
Vol 8 (4) ◽  
pp. 16255-16289 ◽  
Author(s):  
S. Szidat ◽  
M. Ruff ◽  
L. Wacker ◽  
H.-A. Synal ◽  
M. Hallquist ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Elemental Carbon ◽  
Latin Hypercube Sampling ◽  
Water Soluble ◽  
Rural Site ◽  
Urban Site ◽  
Winter Period ◽  
Back Trajectories ◽  
Relative Contribution ◽  
Wood Burning

Abstract. Particulate matter was collected at an urban site in Göteborg (Sweden) in February/March 2005 and in June/July 2006. Additional samples were collected at a rural site for the winter period. Elemental carbon (EC), organic carbon (OC), water-insoluble OC (WINSOC), and water-soluble OC (WSOC) were analyzed for 14C in order to distinguish fossil from non-fossil emissions. As wood burning is the single major source of non-fossil EC, its contribution can be quantified directly. For non-fossil OC, the wood burning fraction was determined independently by levoglucosan and 14C analysis and combined using Latin-hypercube sampling (LHS). For the winter period, the relative contribution of EC from wood burning to the total EC was >3 times higher at the rural site compared to the urban site, whereas the absolute concentrations of EC from wood burning were comparable at both sites. Thus, the urban site is substantially more influenced by fossil EC emissions. For summer, biogenic emissions dominated OC concentrations most likely due to secondary organic aerosol (SOA) formation. During both seasons, a more pronounced fossil signal was observed for Göteborg than has previously been reported for Zurich, Switzerland. Analysis of air mass origin using back trajectories suggests that the fossil impact was larger when local sources dominated, whereas long-range transport caused an enhanced non-fossil signal. In comparison to other European locations, concentrations of levoglucosan and other monosaccharide anhydrides were low for the urban and the rural site in the area of Göteborg during winter. The comparison of summer and winter results provides insight into the annual cycle of anthropogenic vs. biogenic contributions to the atmospheric aerosol.

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