scholarly journals Characteristics and the origins of the carbonaceous aerosol at a rural site of PRD in summer 2006

2011 ◽  
Vol 11 (7) ◽  
pp. 21601-21629
Author(s):  
W. W. Hu ◽  
M. Hu ◽  
Z. Q. Deng ◽  
R. Xiao ◽  
Y. Kondo ◽  
...  

Abstract. Both organic carbon (OC) and elemental carbon (EC) were measured at a rural site, Back Garden (BG), 50km northwest of the Guangzhou City, by using a semi-continuous thermal-optical analyzer during PRIDE-PRD 2006 summer intensive campaign. Together with the online EC/OC instrument, multiple instruments were also employed here which provided a good opportunity to check data quality. The regressions between the mass of organic aerosol (OM) and OC, as well as OC and water soluble organic carbon (WSOC) imply reliability of the data measured in this campaign. The average OC concentrations in fine particle for three typical periods during the campaign (local emission influence, typhoon and participation, normal days) were 28.1 μg C m−3, 4.0 μg C m−3 and 5.7 μg C m−3, respectively, and EC were 11.6 μg C m−3, 1.8 μg C m−3, and 3.3 μg C m−3 orderly. Diurnal variations of EC and OC showed that there were two peaks for EC and OC concentrations, i.e. at night and early morning, which were probably caused by the primary emission accumulation when the boundary layer was shallow. Compare to the constant diurnal enhancement ratios of primary EC, the enhancement ratio of OC (OC versus (CO-CObackground)) remained in a relative high level in the afternoon with a similar diurnal variation to oxygenated organic aerosol (OOA), indicating the strong photochemical formation of OC. The traditional EC tracer method was modified to estimate the secondary organic carbon (SOC) formation, which shows that the average SOC concentration in BG site was about 2.0 ± 2.3 μg C m−3.The SOC fraction in OC reached up to 80 % with the average of 47 %. Good correlations between estimated SOC versus measured OOA or WSOC, and estimated POC versus measured hydrocarbon-like organic aerosol (HOA) also proved the reliable results by the modified EC tracer method in this paper.

2012 ◽  
Vol 12 (4) ◽  
pp. 1811-1822 ◽  
Author(s):  
W. W. Hu ◽  
M. Hu ◽  
Z. Q. Deng ◽  
R. Xiao ◽  
Y. Kondo ◽  
...  

Abstract. Both organic carbon (OC) and elemental carbon (EC) were measured during PRIDE-PRD 2006 summer campaign by using a semi-continuous thermal-optical carbon analyzer at a rural site, Back Garden (BG), which is located 50 km to the northwest of Guangzhou City. Together with the online EC/OC analyzer, various kinds of instruments related to aerosol chemical properties were employed here, which provided a good opportunity to check data quality. The concentrations of OC correlated well with the mass of organic matter (OM) and water soluble organic carbon (WSOC), implying the reliability of the data measured in this campaign. The average OC concentrations in fine particle for three typical periods during the campaign (local emission influence, typhoon and precipitation and normal days) were 28.1 μgC m−3, 4.0 μgC m−3 and 5.7 μgC m−3, respectively; and EC were 11.6 μgC m−3, 1.8 μgC m−3, and 3.3 μgC m−3, respectively. The diurnal patterns of EC and OC during the campaign were higher at night and in early morning than daytime, which was probably caused by the primary emission and accumulation in the occurrence of low boundary layer. Compared with the constant diurnal enhancement ratios of EC, the enhancement ratio of OC (OC versus (CO-CObackground)) kept in a relative high level in the afternoon, with a similar diurnal profile to oxygenated organic aerosol (OOA), due to the strong photochemical formation of OC. Here, a modified EC tracer method was used to estimate the formation of secondary organic carbon (SOC). These results showed that the average SOC concentration (normal days) at BG site was about 2.0 ± 2.3 μgC m−3, and the SOC fraction in OC could reach up to 80% with the average of 47%. The modified approach in this study proved to be effective and reliable for SOC estimation based on good correlations between estimated SOC versus OOA or WSOC, and estimated POC versus hydrocarbon-like organic aerosol (HOA).


2013 ◽  
Vol 9 (4) ◽  
pp. 1403-1416 ◽  
Author(s):  
S. Preunkert ◽  
M. Legrand

Abstract. Seasonally resolved chemical ice core records available from the Col du Dôme glacier (4250 m elevation, French Alps), are here used to reconstruct past aerosol load and composition of the free European troposphere from before World War II to present. Available ice core records include inorganic (Na+, Ca2+, NH4+, Cl−, NO3−, and SO42−) and organic (carboxylates, HCHO, humic-like substances, dissolved organic carbon, water-insoluble organic carbon, and black carbon) compounds and fractions that permit reconstructing the key aerosol components and their changes over the past. It is shown that the atmospheric load of submicron aerosol has been increased by a factor of 3 from the 1921–1951 to 1971–1988 years, mainly as a result of a large increase of sulfate (a factor of 5), ammonium and water-soluble organic aerosol (a factor of 3). Thus, not only growing anthropogenic emissions of sulfur dioxide and ammonia have caused the enhancement of the atmospheric aerosol load but also biogenic emissions producing water-soluble organic aerosol. This unexpected change of biospheric source of organic aerosol after 1950 needs to be considered and further investigated in scenarios dealing with climate forcing by atmospheric aerosol.


2021 ◽  
Vol 21 (10) ◽  
pp. 8067-8088
Author(s):  
Vincent Michoud ◽  
Elise Hallemans ◽  
Laura Chiappini ◽  
Eva Leoz-Garziandia ◽  
Aurélie Colomb ◽  
...  

Abstract. The characterization of the molecular composition of organic carbon in both gaseous and aerosol is key to understanding the processes involved in the formation and aging of secondary organic aerosol. Therefore a technique using active sampling on cartridges and filters and derivatization followed by analysis using a thermal desorption–gas chromatography–mass spectrometer (TD–GC–MS) has been used. It is aimed at studying the molecular composition of organic carbon in both gaseous and aerosol phases (PM2.5) during an intensive field campaign which took place in Corsica (France) during the summer of 2013: the ChArMEx (Chemistry and Aerosol Mediterranean Experiment) SOP1b (Special Observation Period 1B) campaign. These measurements led to the identification of 51 oxygenated (carbonyl and or hydroxyl) compounds in the gaseous phase with concentrations between 21 and 3900 ng m−3 and of 85 compounds in the particulate phase with concentrations between 0.3 and 277 ng m−3. Comparisons of these measurements with collocated data using other techniques have been conducted, showing fair agreement in general for most species except for glyoxal in the gas phase and malonic, tartaric, malic and succinic acids in the particle phase, with disagreements that can reach up to a factor of 8 and 20 on average, respectively, for the latter two acids. Comparison between the sum of all compounds identified by TD–GC–MS in the particle phase and the total organic matter (OM) mass reveals that on average 18 % of the total OM mass can be explained by the compounds measured by TD–GC–MS. This number increases to 24 % of the total water-soluble OM (WSOM) measured by coupling the Particle Into Liquid Sampler (PILS)-TOC (total organic carbon) if we consider only the sum of the soluble compounds measured by TD–GC–MS. This highlights the important fraction of the OM mass identified by these measurements but also the relative important fraction of OM mass remaining unidentified during the campaign and therefore the complexity of characterizing exhaustively the organic aerosol (OA) molecular chemical composition. The fraction of OM measured by TD–GC–MS is largely dominated by di-carboxylic acids, which represent 49 % of the PM2.5 content detected and quantified by this technique. Other contributions to PM2.5 composition measured by TD–GC–MS are then represented by tri-carboxylic acids (15 %), alcohols (13 %), aldehydes (10 %), di-hydroxy-carboxylic acids (5 %), monocarboxylic acids and ketones (3 % each), and hydroxyl-carboxylic acids (2 %). These results highlight the importance of polyfunctionalized carboxylic acids for OM, while the chemical processes responsible for their formation in both phases remain uncertain. While not measured by the TD–GC–MS technique, humic-like substances (HULISs) represent the most abundant identified species in the aerosol, contributing for 59 % of the total OM mass on average during the campaign. A total of 14 compounds were detected and quantified in both phases, allowing the calculation of experimental partitioning coefficients for these species. The comparison of these experimental partitioning coefficients with theoretical ones, estimated by three different models, reveals large discrepancies varying from 2 to 7 orders of magnitude. These results suggest that the supposed instantaneous equilibrium being established between gaseous and particulate phases assuming a homogeneous non-viscous particle phase is questionable.


2014 ◽  
Vol 14 (4) ◽  
pp. 4787-4826 ◽  
Author(s):  
S. Gilardoni ◽  
P. Massoli ◽  
L. Giulianelli ◽  
M. Rinaldi ◽  
M. Paglione ◽  
...  

Abstract. The interaction of aerosol with atmospheric water affects the processing and wet removal of atmospheric particles. Understanding such interaction is mandatory to improve model description of aerosol lifetime and ageing. We analyzed the aerosol-water interaction at high relative humidity during fog events in the Po Valley, in the framework of the ARPA-ER Supersite project. For the first time in this area, the changes in particle chemical composition caused by fog are discussed along with changes in particle microphysics. During the experiment, 14 fog events were observed. The average mass scavenging efficiency was 70% for nitrate, 68% for ammonium, 61% for sulfate, 50% for organics, and 39% for black carbon. After fog formation, the interstitial aerosol was dominated by particles smaller than 200 nm Dva (vacuum aerodynamic diameter) and enriched in carbonaceous aerosol, mainly black carbon and water insoluble organic aerosol (WIOA). For each fog event, the size segregated scavenging efficiency of nitrate and organic aerosol (OA) was calculated by comparing chemical species size distribution before and after fog formation. For both nitrate and OA, the size segregated scavenging efficiency followed a sigmoidal curve, with values close to zero below 100 nm Dva and close to 1 above 700 nm Dva. OA was able to affect scavenging efficiency of nitrate in particles smaller than 300 nm Dva. A linear correlation between nitrate scavenging and particle hygroscopicity (κ) was observed, indicating that 44–51% of the variability of nitrate scavenging in smaller particles (below 300 nm Dva) was explained by changes in particle chemical composition. The size segregated scavenging curves of OA followed those of nitrate, suggesting that organic scavenging was controlled by mixing with water-soluble species. In particular, functional group composition and OA elemental analysis indicated that more oxidized OA was scavenged more efficiently than less oxidized OA. Nevertheless, the small variability of organic functional group composition during the experiment did not allow us to discriminate the effect of different organic functionalities on OA scavenging.


2020 ◽  
Vol 13 (6) ◽  
pp. 3205-3219 ◽  
Author(s):  
Weiqi Xu ◽  
Yao He ◽  
Yanmei Qiu ◽  
Chun Chen ◽  
Conghui Xie ◽  
...  

Abstract. Source apportionment of organic aerosol (OA) from aerosol mass spectrometer (AMS) or aerosol chemical speciation monitor (ACSM) measurements relies largely upon mass spectral profiles from different source emissions. However, the changes in mass spectra of primary emissions from AMS–ACSM with the newly developed capture vaporizer (CV) are poorly understood. Here we conducted 21 cooking, crop straw, wood, and coal burning experiments to characterize the mass spectral features of OA and water-soluble OA (WSOA) using SV-AMS and CV-ACSM. Our results show overall similar spectral characteristics between SV-AMS and CV-ACSM for different primary emissions despite additional thermal decomposition in CV, and the previous spectral features for diagnostics of primary OA factors are generally well retained. However, the mass spectral differences between OA and WSOA can be substantial for both SV-AMS and CV-ACSM. The changes in f55 (fraction of m∕z 55 in OA) vs. f57, f44 vs. f60, and f44 vs. f43 in CV-ACSM are also observed, yet the evolving trends are similar to those of SV-AMS. By applying the source spectral profiles to a winter CV-ACSM study at a highly polluted rural site in the North China Plain, the source apportionment of primary OA was much improved, highlighting the two most important primary sources of biomass burning and coal combustion (32 % and 21 %). Considering the rapidly increasing deployments of CV-ACSM and WSOA studies worldwide, the mass spectral characterization has significant implications by providing essential constraints for more accurate source apportionment and making better strategies for air pollution control in regions with diverse primary emissions.


2017 ◽  
Vol 17 (1) ◽  
pp. 343-369 ◽  
Author(s):  
Havala O. T. Pye ◽  
Benjamin N. Murphy ◽  
Lu Xu ◽  
Nga L. Ng ◽  
Annmarie G. Carlton ◽  
...  

Abstract. Organic compounds and liquid water are major aerosol constituents in the southeast United States (SE US). Water associated with inorganic constituents (inorganic water) can contribute to the partitioning medium for organic aerosol when relative humidities or organic matter to organic carbon (OM ∕ OC) ratios are high such that separation relative humidities (SRH) are below the ambient relative humidity (RH). As OM ∕ OC ratios in the SE US are often between 1.8 and 2.2, organic aerosol experiences both mixing with inorganic water and separation from it. Regional chemical transport model simulations including inorganic water (but excluding water uptake by organic compounds) in the partitioning medium for secondary organic aerosol (SOA) when RH  >  SRH led to increased SOA concentrations, particularly at night. Water uptake to the organic phase resulted in even greater SOA concentrations as a result of a positive feedback in which water uptake increased SOA, which further increased aerosol water and organic aerosol. Aerosol properties, such as the OM ∕ OC and hygroscopicity parameter (κorg), were captured well by the model compared with measurements during the Southern Oxidant and Aerosol Study (SOAS) 2013. Organic nitrates from monoterpene oxidation were predicted to be the least water-soluble semivolatile species in the model, but most biogenically derived semivolatile species in the Community Multiscale Air Quality (CMAQ) model were highly water soluble and expected to contribute to water-soluble organic carbon (WSOC). Organic aerosol and SOA precursors were abundant at night, but additional improvements in daytime organic aerosol are needed to close the model–measurement gap. When taking into account deviations from ideality, including both inorganic (when RH  >  SRH) and organic water in the organic partitioning medium reduced the mean bias in SOA for routine monitoring networks and improved model performance compared to observations from SOAS. Property updates from this work will be released in CMAQ v5.2.


2018 ◽  
Vol 18 (6) ◽  
pp. 3969-3985 ◽  
Author(s):  
Qijing Bian ◽  
Badr Alharbi ◽  
Mohammed M. Shareef ◽  
Tahir Husain ◽  
Mohammad J. Pasha ◽  
...  

Abstract. Knowledge of the sources of carbonaceous aerosol affecting air quality in Riyadh, Saudi Arabia, is limited but needed for the development of pollution control strategies. We conducted sampling of PM2.5 from April to September 2012 at various sites in the city and used a thermo-optical semi-continuous method to quantify the organic carbon (OC) and elemental carbon (EC) concentrations. The average OC and EC concentrations were 4.7 ± 4.4 and 2.1 ± 2.5 µg m−3, respectively, during this period. Both OC and EC concentrations had strong diurnal variations, with peaks at 06:00–08:00 LT and 20:00–22:00 LT, attributed to the combined effect of increased vehicle emissions during rush hour and the shallow boundary layer in the early morning and at night. This finding suggested a significant influence of local vehicular emissions on OC and EC. The OC ∕ EC ratio in primary emissions was estimated to be 1.01, close to documented values for diesel emissions. Estimated primary organic carbon (POC) and secondary organic carbon (SOC) concentrations were comparable, with average concentrations of 2.0 ± 2.4 and 2.8 ± 3.4 µg m−3, respectively. We also collected 24 h samples of PM10 onto quartz microfiber filters and analyzed these for an array of metals by inductively coupled plasma atomic emission spectroscopy (ICP-AES). Total OC was correlated with Ca (R2 of 0.63), suggesting that OC precursors and Ca may have similar sources, and the possibility that they underwent similar atmospheric processing. In addition to a ubiquitous dust source, Ca is emitted during desalting processes in the numerous refineries in the region and from cement kilns, suggesting these sources may also contribute to observed OC concentrations in Riyadh. Concentration weighted trajectory (CWT) analysis showed that high OC and EC concentrations were associated with air masses arriving from the Persian Gulf and the region around Baghdad, locations with high densities of oil fields and refineries as well as a large Saudi Arabian cement plant. We further applied positive matrix factorization to the aligned dataset of EC, OC, and metal concentrations (Al, Ca, Cu, Fe, K, Mg, Mn, Na, Ni, Pb, and V). Three factors were derived and were proposed to be associated with oil combustion, industrial emissions (Pb based), and a combined source from oil fields, cement production, and local vehicular emissions. The dominant OC and EC source was the combined source, contributing 3.9 µg m−3 (80 %) to observed OC and 1.9 µg m−3 (92 %) to observed EC.


2009 ◽  
Vol 9 (5) ◽  
pp. 1521-1535 ◽  
Author(s):  
S. Szidat ◽  
M. Ruff ◽  
N. Perron ◽  
L. Wacker ◽  
H.-A. Synal ◽  
...  

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.


2011 ◽  
Vol 11 (22) ◽  
pp. 11497-11510 ◽  
Author(s):  
Y. Cheng ◽  
K.-B. He ◽  
M. Zheng ◽  
F.-K. Duan ◽  
Z.-Y. Du ◽  
...  

Abstract. The mass absorption efficiency (MAE) of elemental carbon (EC) in Beijing was quantified using a thermal-optical carbon analyzer. The MAE measured at 632 nm was 8.45±1.71 and 9.41±1.92 m2 g−1 during winter and summer respectively. The daily variation of MAE was found to coincide with the abundance of organic carbon (OC), especially the OC to EC ratio, perhaps due to the enhancement by coating with organic aerosol (especially secondary organic aerosol, SOA) or the artifacts resulting from the redistribution of liquid-like organic particles during the filter-based absorption measurements. Using a converting approach that accounts for the discrepancy caused by measurements methods of both light absorption and EC concentration, previously published MAE values were converted to the equivalent-MAE, which is the estimated value if using the same measurement methods as used in this study. The equivalent-MAE was found to be much lower in the regions heavily impacted by biomass burning (e.g., below 2.7 m2 g−1 for two Indian cities). Results from source samples (including diesel exhaust samples and biomass smoke samples) also demonstrated that emissions from biomass burning would decrease the MAE of EC. Moreover, optical properties of water-soluble organic carbon (WSOC) in Beijing were presented. Light absorption by WSOC exhibited strong wavelength (λ) dependence such that absorption varied approximately as λ−7, which was characteristic of the brown carbon spectra. The MAE of WSOC (measured at 365 nm) was 1.79±0.24 and 0.71±0.20 m2 g−1 during winter and summer respectively. The large discrepancy between the MAE of WSOC during winter and summer was attributed to the difference in the precursors of SOA such that anthropogenic volatile organic compounds (AVOCs) should be more important as the precursors of SOA in winter. The MAE of WSOC in Beijing was much higher than results from the southeastern United States which were obtained using the same method as used in this study, perhaps due to the stronger emissions of biomass burning in China.


2012 ◽  
Vol 12 (11) ◽  
pp. 28661-28703 ◽  
Author(s):  
S. L. Mkoma ◽  
K. Kawamura ◽  
P. Fu

Abstract. Atmospheric aerosol samples of PM2.5 and PM10 were collected at a rural site in Tanzania in 2011 during wet and dry seasons and they were analysed for carbonaceous components, levoglucosan and water-soluble inorganic ions. The mean mass concentrations of PM2.5 and PM10 were 28.2±6.4 μg m−3 and 47±8.2 μg m−3 in wet season, and 39.1±9.8 μg m−3 and 61.4±19.2 μg m−3 in dry season, respectively. Total carbon (TC) accounted for 16–19% of the PM2.5 mass and 13–15% of the PM10 mass. On average, 85.9 to 88.7% of TC in PM2.5 and 87.2 to 90.1% in PM10 was organic carbon (OC), of which 67–72% and 63% was found to be water-soluble organic carbon (WSOC) in PM2.5 and PM10, respectively. Water-soluble potassium (K+) and sulphate (SO42−) in PM2.5 and, sodium (Na+) and SO42− in PM10 were the dominant ionic species. We found, that concentrations of biomass burning tracers (levoglucosan and mannosan) well correlated with non-sea-salt-K+, WSOC and OC in the aerosols from Tanzania, East Africa. Mean contributions of levoglucosan to OC ranged between 3.9–4.2% for PM2.5 and 3.5–3.8% for PM10. This study demonstrates that emissions from biomass- and biofuel-burning activities followed by atmospheric photochemical processes mainly control the air quality in Tanzania.


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