scholarly journals Chemical Composition and Source Apportionment of Total Suspended Particulate in the Central Himalayan Region

Atmosphere ◽  
2021 ◽  
Vol 12 (9) ◽  
pp. 1228
Author(s):  
Rahul Sheoran ◽  
Umesh Chandra Dumka ◽  
Dimitris Kaskaoutis ◽  
Georgios Grivas ◽  
Kirpa Ram ◽  
...  

The present study analyzes data from total suspended particulate (TSP) samples collected during 3 years (2005–2008) at Nainital, central Himalayas, India and analyzed for carbonaceous aerosols (organic carbon (OC) and elemental carbon (EC)) and inorganic species, focusing on the assessment of primary and secondary organic carbon contributions (POC, SOC, respectively) and on source apportionment by positive matrix factorization (PMF). An average TSP concentration of 69.6 ± 51.8 µg m−3 was found, exhibiting a pre-monsoon (March–May) maximum (92.9 ± 48.5 µg m−3) due to dust transport and forest fires and a monsoon (June–August) minimum due to atmospheric washout, while carbonaceous aerosols and inorganic species expressed a similar seasonality. The mean OC/EC ratio (8.0 ± 3.3) and the good correlations between OC, EC, and nss-K+ suggested that biomass burning (BB) was one of the major contributing factors to aerosols in Nainital. Using the EC tracer method, along with several approaches for the determination of the (OC/EC)pri ratio, the estimated SOC component accounted for ~25% (19.3–29.7%). Furthermore, TSP source apportionment via PMF allowed for a better understanding of the aerosol sources in the Central Himalayan region. The key aerosol sources over Nainital were BB (27%), secondary sulfate (20%), secondary nitrate (9%), mineral dust (34%), and long-range transported mixed marine aerosol (10%). The potential source contribution function (PSCF) and concentration weighted trajectory (CWT) analyses were also used to identify the probable regional source areas of resolved aerosol sources. The main source regions for aerosols in Nainital were the plains in northwest India and Pakistan, polluted cities like Delhi, the Thar Desert, and the Arabian Sea area. The outcomes of the present study are expected to elucidate the atmospheric chemistry, emission source origins, and transport pathways of aerosols over the central Himalayan region.

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.


2021 ◽  
Author(s):  
Peng Yao ◽  
Haiyan Ni ◽  
Norbertas Kairys ◽  
Lu Yang ◽  
Ru-Jin Huang ◽  
...  

<p>Isotopic source apportionment is commonly used to gain insight into sources and atmospheric processing of carbonaceous aerosols. Since elemental carbon (EC) is chemically stable, it is possible to apportion the main sources of EC (coal/biomass burning and traffic emissions) using a dual <sup>14</sup>C-<sup>13</sup>C isotope approach. However, dual-isotope source apportionment crucially relies on accurate knowledge of the <sup>13</sup>C source signatures, which are seldom measured directly for EC. In this work, we present extensive measurements of organic carbon (OC) and EC <sup>13</sup>C signatures for relevant sources in China. The EC <sup>13</sup>C source signatures are provided first time using the optical split point in a thermal-optical analyzer to isolate EC, which can greatly reduce the influence of pyrolyzed organic carbon (pOC). A series of sensitivity studies (pOC/EC separation) were conducted to investigate the reliability of our method and its relation to other EC isolation methods. Meanwhile, we summarized and compared the literature <sup>13</sup>C signatures in detail of raw source materials, total carbon (TC) and EC using a variety of thermal methods. Finally, we recommend composite EC <sup>13</sup>C source signatures with uncertainties and detailed application conditions. There are two points worth noting. First, the traffic <sup>13</sup>C signatures of raw materials and EC are separated into three groups according to geographical distribution. Second, the EC <sup>13</sup>C signature of C4 plant combustion can be influenced greatly if pOC and EC are not well separated, so the thermal-optical method is necessary. Using these EC <sup>13</sup>C source signatures in an exemplary dual-isotope source apportionment study shows improvement in precision. In addition, some interesting distinct and repeatable patterns were discovered in <sup>13</sup>C source signatures of semi-volatile, low-volatile, and non-volatile primary OC fractions.</p>


2011 ◽  
Vol 11 (23) ◽  
pp. 12067-12084 ◽  
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 composition + EC + OC, 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 ∼47 % 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 slightly 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 ◽  
Vol 18 (9) ◽  
pp. 6187-6206 ◽  
Author(s):  
Athanasia Vlachou ◽  
Kaspar R. Daellenbach ◽  
Carlo Bozzetti ◽  
Benjamin Chazeau ◽  
Gary A. Salazar ◽  
...  

Abstract. Carbonaceous aerosols are related to adverse human health effects. Therefore, identification of their sources and analysis of their chemical composition is important. The offline AMS (aerosol mass spectrometer) technique offers quantitative separation of organic aerosol (OA) factors which can be related to major OA sources, either primary or secondary. While primary OA can be more clearly separated into sources, secondary (SOA) source apportionment is more challenging because different sources – anthropogenic or natural, fossil or non-fossil – can yield similar highly oxygenated mass spectra. Radiocarbon measurements provide unequivocal separation between fossil and non-fossil sources of carbon. Here we coupled these two offline methods and analysed the OA and organic carbon (OC) of different size fractions (particulate matter below 10 and 2.5 µm – PM10 and PM2.5, respectively) from the Alpine valley of Magadino (Switzerland) during the years 2013 and 2014 (219 samples). The combination of the techniques gave further insight into the characteristics of secondary OC (SOC) which was rather based on the type of SOC precursor and not on the volatility or the oxidation state of OC, as typically considered. Out of the primary sources separated in this study, biomass burning OC was the dominant one in winter, with average concentrations of 5.36 ± 2.64 µg m−3 for PM10 and 3.83 ± 1.81 µg m−3 for PM2.5, indicating that wood combustion particles were predominantly generated in the fine mode. The additional information from the size-segregated measurements revealed a primary sulfur-containing factor, mainly fossil, detected in the coarse size fraction and related to non-exhaust traffic emissions with a yearly average PM10 (PM2.5) concentration of 0.20 ± 0.24 µg m−3 (0.05 ± 0.04 µg m−3). A primary biological OC (PBOC) was also detected in the coarse mode peaking in spring and summer with a yearly average PM10 (PM2.5) concentration of 0.79 ± 0.31 µg m−3 (0.24 ± 0.20 µg m−3). The secondary OC was separated into two oxygenated, non-fossil OC factors which were identified based on their seasonal variability (i.e. summer and winter oxygenated organic carbon, OOC) and a third anthropogenic OOC factor which correlated with fossil OC mainly peaking in winter and spring, contributing on average 13 % ± 7 % (10 % ± 9 %) to the total OC in PM10 (PM2.5). The winter OOC was also connected to anthropogenic sources, contributing on average 13 % ± 13 % (6 % ± 6 %) to the total OC in PM10 (PM2.5). The summer OOC (SOOC), stemming from oxidation of biogenic emissions, was more pronounced in the fine mode, contributing on average 43 % ± 12 % (75 % ± 44 %) to the total OC in PM10 (PM2.5). In total the non-fossil OC significantly dominated the fossil OC throughout all seasons, by contributing on average 75 % ± 24 % to the total OC. The results also suggested that during the cold period the prevailing source was residential biomass burning while during the warm period primary biological sources and secondary organic aerosol from the oxidation of biogenic emissions became important. However, SOC was also formed by aged fossil fuel combustion emissions not only in summer but also during the rest of the year.


2021 ◽  
Author(s):  
Ritu Jangirh ◽  
Sakshi Ahlawat ◽  
Rahul Arya ◽  
Arnab Mondal ◽  
Lokesh Yadav ◽  
...  

Abstract In the present study, total suspended particulate matter (TSP) samples were collected at 47 different sites (47 grids of 5 × 5 km2 area) of Delhi during winter (January-February 2019) in campaign mode. To understand the spatial variation of sources, TSP samples were analyzed for chemical compositions including carbonaceous species [organic carbon (OC), elemental carbon (EC) and water-soluble organic carbon (WSOC)], water-soluble total nitrogen (WSTN), water-soluble inorganic nitrogen (WSIN), polycyclic aromatic hydrocarbons (16 PAHs), water-soluble inorganic species (WSIS) (F−, Cl−, SO42−, NO2−, NO3−, PO43−, NH4+, Ca2+, Mg2+, Na+, and K+), and major & minor trace elements (B, Na, Mg, Al, P, S, Cl, K, Ca, Ti, Fe, Zn, Cr, Mn, Cu, As, Pd, F, and Ag). During the campaign, the maximum concentration of several components of TSP (996 µg/m3) was recorded at the Rana Pratap Bagh area representing a pollution hotspot of Delhi. The maximum concentrations of PAHs were recorded at Udhyog Nagar, a region close to heavily loaded diesel vehicles, small rubber factories, and waste burning areas. Higher content of Cl− and Cl−/Na+ ratio (> 1.7) suggests the presence of nonmarine anthropogenic sources of Cl− over Delhi. Minimum concentrations of OC, EC, WSOC, PAHs, and WSIS in TSP were observed at Kalkaji representing the least polluted area in Delhi. Enrichment factor < 5.0 at several locations and a significant correlation of Al with Mg, Fe, Ti, and Ca and C/N ratio indicated the abundance of mineral/crustal dust in TSP over Delhi. Principal component analysis (PCA) was also performed for the source apportionment of TSP and extracted soil dust was found to be the major contributor to TSP followed by biomass burning, open waste burning, secondary aerosol, and vehicular emissions.


2017 ◽  
Author(s):  
Yan-Lin Zhang ◽  
Imad El-Haddad ◽  
Ru-Jin Huang ◽  
Kin-Fai Ho ◽  
Jun-Ji Cao ◽  
...  

Abstract. Water-soluble organic carbon (WSOC) is a large fraction of organic aerosols (OA) globally and has significant impacts on climate and human health. The sources of WSOC remain very uncertain in polluted regions. Here we present a quantitative source apportionment of WSOC isolated from aerosols in China using radiocarbon (14C) and offline high-resolution time-of-flight aerosol mass spectrometer measurements. Fossil emissions on average accounted for 32–47 % of WSOC. Secondary organic carbon (SOC) dominated both the non-fossil and fossil derived WSOC, highlighting the importance of secondary formation to WSOC in severe winter haze episodes. Contributions from fossil emissions to SOC were 61 ± 4 % and 50 ± 9 % in Shanghai and Beijing, respectively, significantly larger than those in Guangzhou (36 ± 9 %) and Xi'an (26 ± 9 %). The most important primary sources were biomass burning emissions, contributing 17–26 % of WSOC. The remaining primary sources such as coal combustion, cooking and traffic were generally very small but not negligible contributors, as coal combustion contribution could exceed 10 %. Taken together with earlier 14C source apportionment studies in urban, rural, semi-urban, and background regions in Asia, Europe and USA, we demonstrated a dominant contribution of non-fossil emissions (i.e., 75 ± 11 %) to WSOC aerosols in the North Hemisphere; however, the fossil fraction is substantially larger in aerosols from East Asia and the East Asian pollution outflow especially during winter due to increasing coal combustion. Inclusion of our findings can improve a modelling of effects of WSOC aerosols on climate, atmospheric chemistry and public health.


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