scholarly journals Six-year source apportionment of submicron organic aerosols from near-continuous measurements at SIRTA (Paris area, France)

2019 ◽  
Author(s):  
Yunjiang Zhang ◽  
Olivier Favez ◽  
Jean-Eudes Petit ◽  
Francesco Canonaco ◽  
Francois Truong ◽  
...  

Abstract. Organic aerosol (OA) particles are recognized as key factors influencing air quality and climate change. However, highly-time resolved year-round characterizations of their composition and sources in ambient air are still very limited due to challenging continuous observations. Here, we present an analysis of long-term variability of submicron OA using the combination of Aerosol Chemical Speciation Monitor (ACSM) and multi-wavelength aethalometer from November 2011 to March 2018 at a background site of the Paris region (France). Source apportionment of OA was achieved via partially constrained positive matrix factorization (PMF) using the multilinear engine (ME-2). Two primary OA (POA) and two oxygenated OA (OOA) factors were identified and quantified over the entire studied period. POA factors were designated as hydrocarbon-like OA (HOA) and biomass burning OA (BBOA). The latter factor presented a significant seasonality with higher concentrations in winter with significant monthly contributions to OA (18–33 %) due to enhanced residential wood burning emissions. HOA mainly originated from traffic emissions but was also influenced by biomass burning in cold periods. OOA factors were distinguished between their less- and more-oxidized fractions (LO-OOA and MO-OOA, respectively). These factors presented distinct seasonal patterns, associated with different atmospheric formation pathways. A pronounced increase of LO-OOA concentrations and contributions (50–66 %) was observed in summer, which may be mainly explained by secondary OA (SOA) formation processes involving biogenic gaseous precursors. Conversely high concentrations and OA contributions (32–62 %) of MO-OOA during winter and spring seasons were partly associated with anthropogenic emissions and/or long-range transport from northeastern Europe. The contribution of the different OA factors as a function of OA mass loading highlighted the dominant roles of POA during pollution episodes in fall and winter, and of SOA for highest springtime and summertime OA concentrations. Finally, long-term trend analyses indicated a decreasing feature (of about 200 ng m−3 yr−1) for MO-OOA, very limited or insignificant decreasing trends for primary anthropogenic carbonaceous aerosols (BBOA and HOA, along with the fossil fuel and biomass burning black carbon components), and no trend for LO-OOA over the 6+-year investigated period.

2019 ◽  
Vol 19 (23) ◽  
pp. 14755-14776 ◽  
Author(s):  
Yunjiang Zhang ◽  
Olivier Favez ◽  
Jean-Eudes Petit ◽  
Francesco Canonaco ◽  
Francois Truong ◽  
...  

Abstract. Organic aerosol (OA) particles are recognized as key factors influencing air quality and climate change. However, highly time-resolved long-term characterizations of their composition and sources in ambient air are still very limited due to challenging continuous observations. Here, we present an analysis of long-term variability of submicron OA using the combination of an aerosol chemical speciation monitor (ACSM) and a multiwavelength Aethalometer from November 2011 to March 2018 at a peri-urban background site of the Paris region (France). Source apportionment of OA was achieved via partially constrained positive matrix factorization (PMF) using the multilinear engine (ME-2). Two primary OA (POA) and two oxygenated OA (OOA) factors were identified and quantified over the entire studied period. POA factors were designated as hydrocarbon-like OA (HOA) and biomass burning OA (BBOA). The latter factor presented a significant seasonality with higher concentrations in winter with significant monthly contributions to OA (18 %–33 %) due to enhanced residential wood burning emissions. HOA mainly originated from traffic emissions but was also influenced by biomass burning in cold periods. OOA factors were distinguished between their less- and more-oxidized fractions (LO-OOA and MO-OOA, respectively). These factors presented distinct seasonal patterns, associated with different atmospheric formation pathways. A pronounced increase in LO-OOA concentrations and contributions (50 %–66 %) was observed in summer, which may be mainly explained by secondary OA (SOA) formation processes involving biogenic gaseous precursors. Conversely, high concentrations and OA contributions (32 %–62 %) of MO-OOA during winter and spring seasons were partly associated with anthropogenic emissions and/or long-range transport from northeastern Europe. The contribution of the different OA factors as a function of OA mass loading highlighted the dominant roles of POA during pollution episodes in fall and winter and of SOA for highest springtime and summertime OA concentrations. Finally, long-term trend analyses indicated a decreasing feature (of about −175 ng m−3 yr−1) for MO-OOA, very limited or insignificant decreasing trends for primary anthropogenic carbonaceous aerosols (BBOA and HOA, along with the fossil-fuel and biomass-burning black carbon components) and no statistically significant trend for LO-OOA over the 6-year investigated period.


2020 ◽  
Author(s):  
Mengying Bao ◽  
Yan-Lin Zhang ◽  
Fang Cao ◽  
Yu-Chi Lin ◽  
Yuhang Wang ◽  
...  

Abstract. Carbonaceous aerosols have great influence on the air quality, human health and climate change. Except for organic carbon (OC) and elemental carbon (EC), brown carbon (BrC), mainly originates from biomass burning, as a group of OC with strong absorption from the visible to near-ultraviolet wavelengths, makes a considerable contribution to global warming. Large amounts of studies have reported long-term observation of OC and EC concentrations throughout the word, but studies of BrC based on long-term observations are rather limited. In this study, we established a two-wavelength method (658 nm and 405 nm) applied in the Sunset thermo/optical carbon analyzer. Based on one-year observation, we firstly investigated the characteristics, meteorological impact and transport process of OC and EC. Due to BrC absorbs light at 405 nm more effectively than 658 nm, we defined the enhanced concentrations (dEC = EC405 nm−EC658 nm) and gave the possibility to provide an indicator of BrC. The receptor model and MODIS fire information were used to identify the presence of BrC aerosols. Our results showed that the carbonaceous aerosols concentrations were highest in winter and lowest in summer. Traffic emission was an important source of carbonaceous aerosols in Nanjing. Receptor model results showed that strong local emissions were found in OC and EC aerosols, however dEC aerosols were significantly affected by regional or long-range transport. The dEC / OC and OC / EC ratios showed similar diurnal patterns and the dEC / OC increased when the OC / EC ratios increased, indicating strong secondary sources or biomass burning contributions to dEC. Two biomass burning events both in summer and winter were analyzed and the results showed that the dEC concentrations were obvious higher in biomass burning days, however, no similar levels of the OC and EC concentrations were found both in biomass burning days and normal days in summer, suggesting that biomass burning emission made a great contribution to dEC and the sources of OC and EC were more complicated. Large number of open fire counts from the northwest and southwest areas of the study site were monitored in winter, significantly contributed to OC, EC and dEC. In addition, the near-by YRD area was one of the main potential source areas of dEC, suggesting that anthropogenic emissions could also be important sources of dEC. The results proved that dEC can be an indicator of BrC in biomass burning days. Our modified two-wavelength instrument provided more information than traditional single-wavelength thermo/optical carbon analyzer and gave a new idea about the measurement of BrC, the application of dEC data need to be further investigated.


2019 ◽  
Vol 19 (24) ◽  
pp. 15247-15270 ◽  
Author(s):  
Jianhui Jiang ◽  
Sebnem Aksoyoglu ◽  
Imad El-Haddad ◽  
Giancarlo Ciarelli ◽  
Hugo A. C. Denier van der Gon ◽  
...  

Abstract. Source apportionment of organic aerosols (OAs) is of great importance to better understand the health impact and climate effects of particulate matter air pollution. Air quality models are used as potential tools to identify OA components and sources at high spatial and temporal resolution; however, they generally underestimate OA concentrations, and comparisons of their outputs with an extended set of measurements are still rare due to the lack of long-term experimental data. In this study, we addressed such challenges at the European level. Using the regional Comprehensive Air Quality Model with Extensions (CAMx) and a volatility basis set (VBS) scheme which was optimized based on recent chamber experiments with wood burning and diesel vehicle emissions, and which contains more source-specific sets compared to previous studies, we calculated the contribution of OA components and defined their sources over a whole-year period (2011). We modeled separately the primary and secondary OA contributions from old and new diesel and gasoline vehicles, biomass burning (mostly residential wood burning and agricultural waste burning excluding wildfires), other anthropogenic sources (mainly shipping, industry and energy production) and biogenic sources. An important feature of this study is that we evaluated the model results with measurements over a longer period than in previous studies, which strengthens our confidence in our modeled source apportionment results. Comparison against positive matrix factorization (PMF) analyses of aerosol mass spectrometric measurements at nine European sites suggested that the modified VBS scheme improved the model performance for total OA as well as the OA components, including hydrocarbon-like (HOA), biomass burning (BBOA) and oxygenated components (OOA). By using the modified VBS scheme, the mean bias of OOA was reduced from −1.3 to −0.4 µg m−3 corresponding to a reduction of mean fractional bias from −45 % to −20 %. The winter OOA simulation, which was largely underestimated in previous studies, was improved by 29 % to 42 % among the evaluated sites compared to the default parameterization. Wood burning was the dominant OA source in winter (61 %), while biogenic emissions contributed ∼ 55 % to OA during summer in Europe on average. In both seasons, other anthropogenic sources comprised the second largest component (9 % in winter and 19 % in summer as domain average), while the average contributions of diesel and gasoline vehicles were rather small (∼ 5 %) except for the metropolitan areas where the highest contribution reached 31 %. The results indicate the need to improve the emission inventory to include currently missing and highly uncertain local emissions, as well as further improvement of VBS parameterization for winter biomass burning. Although this study focused on Europe, it can be applied in any other part of the globe. This study highlights the ability of long-term measurements and source apportionment modeling to validate and improve emission inventories, and identify sources not yet properly included in existing inventories.


2007 ◽  
Vol 7 (17) ◽  
pp. 4527-4536 ◽  
Author(s):  
S. Eckhardt ◽  
K. Breivik ◽  
S. Manø ◽  
A. Stohl

Abstract. Soils and forests in the boreal region of the Northern Hemisphere are recognised as having a large capacity for storing air-borne Persistent Organic Pollutants (POPs), such as the polychlorinated biphenyls (PCBs). Following reductions of primary emissions of various legacy POPs, there is an increasing interest and debate about the relative importance of secondary re-emissions on the atmospheric levels of POPs. In spring of 2006, biomass burning emissions from agricultural fires in Eastern Europe were transported to the Zeppelin station on Svalbard, where record-high levels of many air pollutants were recorded (Stohl et al., 2007). Here we report on the extremely high concentrations of PCBs that were also measured during this period. 21 out of 32 PCB congeners were enhanced by more than two standard deviations above the long-term mean concentrations. In July 2004, about 5.8 million hectare of boreal forest burned in North America, emitting a pollution plume which reached the Zeppelin station after a travel time of 3–4 weeks (Stohl et al., 2006). Again, 12 PCB congeners were elevated above the long-term mean by more than two standard deviations, with the less chlorinated congeners being most strongly affected. We propose that these abnormally high concentrations were caused by biomass burning emissions. Based on enhancement ratios with carbon monoxide and known emissions factors for this species, we estimate that 130 and 66 μg PCBs were released per kilogram dry matter burned, respectively. To our knowledge, this is the first study relating atmospheric PCB enhancements with biomass burning. The strong effects on observed concentrations far away from the sources, suggest that biomass burning is an important source of PCBs for the atmosphere.


2007 ◽  
Vol 7 (3) ◽  
pp. 6229-6254 ◽  
Author(s):  
S. Eckhardt ◽  
K. Breivik ◽  
S. Man\\o ◽  
A. Stohl

Abstract. Soils and forests in the boreal region of the northern hemisphere are recognised as having a large capacity for storing air-borne Persistent Organic Pollutants (POPs), such as the polychlorinated biphenyls (PCBs). Following reductions of primary emissions of various legacy POPs, there is an increasing interest and debate about the relative importance of secondary re-emissions on the atmospheric levels of POPs. In spring of 2006, biomass burning emissions from agricultural fires in Eastern Europe were transported to the Zeppelin station on Svalbard, where record-high levels of many air pollutants were recorded (Stohl et al., 2007). Here we report on the extremely high concentrations of PCBs that were also measured during this period. 21 out of 32 PCB congeners were enhanced by more than two standard deviations above the long-term mean concentrations. In July 2004, about 5.8 million hectare of boreal forest burned in North America, emitting a pollution plume which reached the Zeppelin station after a travel time of 3–4 weeks (Stohl et al., 2006). Again, 12 PCB congeners were elevated above the long-term mean by more than two standard deviations, with the less chlorinated congeners being most strongly affected. We propose that these abnormally high concentrations were caused by biomass burning emissions. Based on enhancement ratios with carbon monoxide and known emissions factors for this species, we estimate that 130 and 66 μg PCBs were released per kilogram dry matter burned, respectively. To our knowledge, this is the first study relating atmospheric PCB enhancements with biomass burning. The strong effects on observed concentrations far away from the sources, suggest that biomass burning is an important source of PCBs for the atmosphere.


2021 ◽  
Vol 21 (10) ◽  
pp. 8273-8292
Author(s):  
Siqi Hou ◽  
Di Liu ◽  
Jingsha Xu ◽  
Tuan V. Vu ◽  
Xuefang Wu ◽  
...  

Abstract. Carbonaceous aerosol is a dominant component of fine particles in Beijing. However, it is challenging to apportion its sources. Here, we applied a newly developed method which combined radiocarbon (14C) with organic tracers to apportion the sources of fine carbonaceous particles at an urban (IAP) and a rural (PG) site of Beijing. PM2.5 filter samples (24 h) were collected at both sites from 10 November to 11 December 2016 and from 22 May to 24 June 2017. 14C was determined in 25 aerosol samples (13 at IAP and 12 at PG) representing low pollution to haze conditions. Biomass burning tracers (levoglucosan, mannosan, and galactosan) in the samples were also determined using gas chromatography–mass spectrometry (GC-MS). Higher contributions of fossil-derived OC (OCf) were found at the urban site. The OCf / OC ratio decreased in the summer samples (IAP: 67.8 ± 4.0 % in winter and 54.2 ± 11.7 % in summer; PG: 59.3 ± 5.7 % in winter and 50.0 ± 9.0 % in summer) due to less consumption of coal in the warm season. A novel extended Gelencsér (EG) method incorporating the 14C and organic tracer data was developed to estimate the fossil and non-fossil sources of primary and secondary OC (POC and SOC). It showed that fossil-derived POC was the largest contributor to OC (35.8 ± 10.5 % and 34.1 ± 8.7 % in wintertime for IAP and PG, 28.9 ± 7.4 % and 29.1 ± 9.4 % in summer), regardless of season. SOC contributed 50.0 ± 12.3 % and 47.2 ± 15.5 % at IAP and 42.0 ± 11.7 % and 43.0 ± 13.4 % at PG in the winter and summer sampling periods, respectively, within which the fossil-derived SOC was predominant and contributed more in winter. The non-fossil fractions of SOC increased in summer due to a larger biogenic component. Concentrations of biomass burning OC (OCbb) are resolved by the extended Gelencsér method, with average contributions (to total OC) of 10.6 ± 1.7 % and 10.4 ± 1.5 % in winter at IAP and PG and 6.5 ± 5.2 % and 17.9 ± 3.5 % in summer, respectively. Correlations of water-insoluble OC (WINSOC) and water-soluble OC (WSOC) with POC and SOC showed that although WINSOC was the major contributor to POC, a non-negligible fraction of WINSOC was found in SOC for both fossil and non-fossil sources, especially during winter. In summer, a greater proportion of WSOC from non-fossil sources was found in SOC. Comparisons of the source apportionment results with those obtained from a chemical mass balance model were generally good, except for the cooking aerosol.


2021 ◽  
Vol 21 (19) ◽  
pp. 15337-15349
Author(s):  
Spiro D. Jorga ◽  
Kalliopi Florou ◽  
Christos Kaltsonoudis ◽  
John K. Kodros ◽  
Christina Vasilakopoulou ◽  
...  

Abstract. Residential biomass burning for heating purposes is an important source of air pollutants during winter. Here we test the hypothesis that significant secondary organic aerosol production can take place even during winter nights through oxidation of the emitted organic vapors by the nitrate (NO3) radical produced during the reaction of ozone and nitrogen oxides. We use a mobile dual smog chamber system which allows the study of chemical aging of ambient air against a control reference. Ambient urban air sampled during a wintertime campaign during nighttime periods with high concentrations of biomass burning emissions was used as the starting point for the aging experiments. Biomass burning organic aerosol (OA) was, on average, 70 % of the total OA at the beginning of our experiments. Ozone was added in the perturbed chamber to simulate mixing with background air (and subsequent NO3 radical production and aging), while the second chamber was used as a reference. Following the injection of ozone, rapid OA formation was observed in all experiments, leading to increases in the OA concentration by 20 %–70 %. The oxygen-to-carbon ratio of the OA increased on average by 50 %, and the mass spectra of the produced OA was quite similar to the oxidized OA mass spectra reported during winter in urban areas. Furthermore, good correlation was found for the OA mass spectra between the ambient-derived emissions in this study and the nocturnal aged laboratory-derived biomass burning emissions from previous work. Concentrations of NO3 radicals as high as 25 ppt (parts per trillion) were measured in the perturbed chamber, with an accompanying production of 0.1–3.2 µg m−3 of organic nitrate in the aerosol phase. Organic nitrate represented approximately 10 % of the mass of the secondary OA formed. These results strongly indicate that the OA in biomass burning plumes can chemically evolve rapidly even during wintertime periods with low photochemical activity.


2011 ◽  
Vol 11 (8) ◽  
pp. 23573-23618 ◽  
Author(s):  
M. C. Minguillón ◽  
N. Perron ◽  
X. Querol ◽  
S. Szidat ◽  
S. M. Fahrni ◽  
...  

Abstract. We present results from the international field campaign DAURE (Determination of the sources of atmospheric Aerosols in Urban and Rural Environments in the western Mediterranean), with the objective of apportioning the sources of fine carbonaceous aerosols. Submicron fine particulate matter (PM1) samples were collected during February-March 2009 and July 2009 at an urban background site in Barcelona (BCN) and at a forested regional background site in Montseny (MSY). We present radiocarbon (14C) analysis for elemental and organic carbon (EC and OC) and source apportionment for these data. We combine the results with those from component analysis of aerosol mass spectrometer (AMS) measurements, and compare to levoglucosan-based estimates of biomass burning OC, source apportionment of filter data with inorganic+EC+OC speciation, submicron bulk potassium (K) concentrations, and gaseous acetonitrile concentrations. At BCN, 87 % and 91 % of the EC on average, in winter and summer, respectively, had a fossil origin, whereas at MSY these fractions were 66 % and 79 %. The contribution of fossil sources to organic carbon (OC) at BCN was 40 % and 48 %, in winter and summer, respectively, and 31 % and 25 % at MSY. The combination of results obtained using the 14C technique, AMS data, and the correlations between fossil OC and fossil EC imply that the fossil OC at Barcelona is ~65 % primary whereas at MSY the fossil OC is mainly secondary (~85 %). Day-to-day variation in total carbonaceous aerosol loading and the relative contributions of different sources predominantly depended on the meteorological transport conditions. The estimated biogenic secondary OC at MSY only increased by ~40 % compared to the order-of-magnitude increase observed for biogenic volatile organic compounds (VOCs) between winter and summer, which highlights the uncertainties in the estimation of that component. Biomass burning contributions estimated using the 14C technique ranged from similar to higher than when estimated using other techniques, and the different estimations were highly or moderately correlated. Differences can be explained by the contribution of secondary organic matter (not included in the primary biomass burning source estimates), and/or by an overestimation of the biomass burning OC contribution by the 14C technique if the estimated biomass burning EC/OC ratio used for the calculations is too high for this region. Acetonitrile concentrations correlate well with the biomass burning EC determined by 14C. K is a noisy tracer for biomass burning.


2018 ◽  
Author(s):  
Jiaping Wang ◽  
Wei Nie ◽  
Yafang Cheng ◽  
Yicheng Shen ◽  
Xuguang Chi ◽  
...  

Abstract. Brown carbon (BrC), a certain group of organic carbon (OC) with strong absorption from the visible to ultraviolet (UV) wavelengths, makes considerable contribution to light absorption on both global and regional scales. High concentration and proportion of OC has been reported in China, but studies of BrC absorption based on long-term observations are rather limited in this region. In this study, we reported 3-year results of light absorption of BrC based on continuous measurement at the Station for Observation Regional Processes of the Earth System (SORPES) in the Yangtze River Delta, China combined with Mie-theory calculation. Light absorption of BrC was obtained using an improved Absorption Ångstrom exponent (AAE) segregation method to calculate AAE of pure and non-absorbing coated black carbon (BC) at each time step based on Mie-theory simulation and measurement of multi-wavelength aerosol light absorption. By using this improved method, the variation of AAE over time is taken into consideration, making it applicable for long-term analysis. The yearly average light absorption of BrC (babs_BrC) at 370 nm was 4.3 Mm−1 at the SORPES station. The contribution of BrC to total aerosol absorption (PBrC) at 370 nm ranged from 6 % to 18 % (10th and 90th percentiles, respectively), and reached up to ~ 28 % in biomass burning-dominant season and winter. Both babs_BrC and PBrC exhibited clear seasonal cycles with two peaks in later spring/early summer (May–June, babs_BrC ~ 4 Mm−1, PBrC ~ 11 %) and winter (December, babs_BrC ~ 12 Mm−1, PBrC ~ 17 %), respectively. Lagrangian modeling and chemical signature observed at the site suggested that open biomass burning and residential emissions were the dominate sources influencing BrC in the two seasons.


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