scholarly journals PM<sub>1</sub> composition and source apportionment at two sites in Delhi, India, across multiple seasons

2021 ◽  
Vol 21 (15) ◽  
pp. 11655-11667
Author(s):  
Ernesto Reyes-Villegas ◽  
Upasana Panda ◽  
Eoghan Darbyshire ◽  
James M. Cash ◽  
Rutambhara Joshi ◽  
...  

Abstract. Air pollution in urban environments has been shown to have a negative impact on air quality and human health, particularly in megacities. Over recent decades, Delhi, India, has suffered high atmospheric pollution, with significant particulate matter (PM) concentrations as a result of anthropogenic activities. Organic aerosols (OAs) are composed of thousands of different chemical species and are one of the main constituents of submicron particles. However, quantitative knowledge of OA composition, their sources and their processes in urban environments is still limited. This is important particularly in India, as Delhi is a massive, inhomogeneous conurbation, where we would expect the apportionment and concentrations to vary depending on where in Delhi the measurements/source apportionment is performed, indicating the need for multisite measurements. This study presents the first multisite analysis carried out in India over different seasons, with a focus on identifying OA sources. The measurements were taken during 2018 at two sites in Delhi, India. One site was located at the India Meteorological Department, New Delhi (ND). The other site was located at the Indira Gandhi Delhi Technical University for Women, Old Delhi (OD). Non-refractory submicron aerosol (NR-PM1) concentrations (ammonium, nitrate, sulfate, chloride and organic aerosols) of four aerosol mass spectrometers were analysed. Collocated measurements of volatile organic compounds, black carbon, NOx and CO were performed. Positive matrix factorisation (PMF) analysis was performed to separate the organic fraction, identifying a number of conventional factors: hydrocarbon-like OAs (HOAs) related to traffic emissions, biomass burning OAs (BBOAs), cooking OAs (COAs) and secondary OAs (SOAs). A composition-based estimate of PM1 is defined by combining black carbon (BC) and NR-PM1 (C-PM1= BC + NR-PM1). No significant difference was observed in C-PM1 concentrations between sites, OD (142 ± 117 µg m−3) compared to ND (123 ± 71 µg m3), from post-monsoon measurements. A wider variability was observed between seasons, where pre-monsoon and monsoon showed C-PM1 concentrations lower than 60 µg m−3. A seasonal variation in C-PM1 composition was observed; SO42- showed a high contribution over pre-monsoon and monsoon seasons, while NO3- and Cl− had a higher contribution in winter and post-monsoon. The main primary aerosol source was from traffic, which is consistent with the PMF analysis and Aethalometer model analysis. Thus, in order to reduce PM1 concentrations in Delhi through local emission controls, traffic emission control offers the greatest opportunity. PMF–aerosol mass spectrometer (AMS) mass spectra will help to improve future aerosol source apportionment studies. The information generated in this study increases our understanding of PM1 composition and OA sources in Delhi, India. Furthermore, the scientific findings provide significant information to strengthen legislation that aims to improve air quality in India.

2020 ◽  
Author(s):  
Ernesto Reyes-Villegas ◽  
Upasana Panda ◽  
Eoghan Darbyshire ◽  
James M. Cash ◽  
Rutambhara Joshi ◽  
...  

Abstract. Air pollution in urban environments has been shown to have a negative impact on air quality and human health, particularly in megacities. Over recent decades, Delhi, India has suffered high atmospheric pollution, with significant particulate matter (PM) concentrations as result of anthropogenic activities. Organic aerosols (OA) are composed of thousands of different chemical species and are one of the main constituents of submicron particles. However, quantitative knowledge of OA composition, their sources and processes in urban environments is still limited. This is important particularly in India, as Delhi is a massive, inhomogeneous conurbation, which we would expect that the apportionment and concentrations will vary depending on where in Delhi the measurements/source apportionment is performed, indicating the need of multi-site measurements. This study presents the first multisite analysis carried out in India over different seasons, with a focus on identifying OA sources. The measurements were taken during 2018 at two sites in Delhi, India. One site was located at the India Meteorological Department, New Delhi (ND). The other site was located at the Indira Gandhi Delhi Technical University for Women, Old Delhi (OD). Non-refractory submicron aerosol (NR-PM1) concentrations (ammonium, nitrate, sulphate, chloride and organic aerosols) of four aerosol mass spectrometers were analysed. Collocated measurements of VOC, black carbon, NOx and CO were performed. Positive matrix factorization (PMF) analysis was performed to separate the organic fraction, identifying a number of conventional factors: hydrocarbon-like OA (HOA) related to traffic emissions, biomass burning OA (BBOA), cooking OA (COA) and secondary OA (SOA). A composition-based estimate of PM1 is defined by combining BC and NR-PM1 (C-PM1 = BC + NR-PM1). No significant difference was observed on C-PM1 concentrations between sites; OD (142 ± 117 µg m−3) compared to ND (123 ± 71 µg m−3), from post-monsoon measurements. A wider variability was observed between seasons, where pre-monsoon and monsoon showed C-PM1 concentrations lower than 60 µg m−3. A seasonal variation in C-PM1 composition was observed; SO42− showed a high contribution over pre-monsoon and monsoon seasons while NO3− and Cl− had a higher contribution in winter and post-monsoon. The main primary aerosol source was from traffic, which is consistent with the PMF analysis and aethalometer model analysis. Thus, in order to reduce PM1 concentrations in Delhi through local emission controls traffic emissions control offers the greatest opportunity. PMF-AMS mass spectra will help to improve future aerosol source apportionment studies. The information generated in this study increases our understanding of PM1 composition and OA sources in Delhi, India. Furthermore, the scientific findings provide significant information to strengthen legislation that aims to improve air quality in India.


2017 ◽  
Author(s):  
Carlo Bozzetti ◽  
Imad El Haddad ◽  
Dalia Salameh ◽  
Kaspar Rudolf Daellenbach ◽  
Paola Fermo ◽  
...  

Abstract. We investigated the seasonal trends of OA sources affecting the air quality of Marseille (France) which is the largest harbor of the Mediterranean Sea. This was achieved by measurements of nebulized filter extracts using an aerosol mass spectrometer (offline-AMS). PM2.5 (particulate matter with an aerodynamic diameter


2021 ◽  
Author(s):  
Sanna Saarikoski ◽  
Jarkko V. Niemi ◽  
Minna Aurela ◽  
Liisa Pirjola ◽  
Anu Kousa ◽  
...  

Abstract. This study investigated the sources of black carbon (BC) at two contrasting urban environments in Helsinki, Finland; residential area and street canyon. The sources of BC were explored by using positive matrix factorization (PMF) for the organic and refractory black carbon (rBC) mass spectra collected with a soot particle aerosol mass spectrometer (SP-AMS). Two sites had different local BC sources; the largest fraction of BC originated from biomass burning at the residential site (38 %) and from the vehicular emissions at the street canyon (57 %). Also, the mass size distribution of BC diverged at the sites as BC from traffic was found at the particle size of ~100–150 nm whereas BC from biomass combustion was detected at ~300 nm. At both sites, a large fraction of BC was associated with urban background or long-range transported BC indicated by the high oxidation state of organics related to those PMF factors. The results from the PMF analysis were compared with the source apportionment from the aethalometer model calculated with two pair of absorption Ångström values. It was found that several PMF factors can be attributed to wood combustion and fossil fuel fraction of BC provided by the aethalometer model. In general, the aethalometer model showed less variation between the sources within a day than PMF being less responsive to the fast changes in the BC sources at the site. The results of this study increase understanding of the limitations and validity of the BC source apportionment methods in different environments. Moreover, this study advances the current knowledge of BC sources and especially the contribution of residential combustion in urban areas.


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.


Atmosphere ◽  
2020 ◽  
Vol 11 (4) ◽  
pp. 330 ◽  
Author(s):  
Manousos Ioannis Manousakas ◽  
Kalliopi Florou ◽  
Spyros N. Pandis

Fine particulate matter (PM) originates from various emission sources and physicochemical processes. Quantification of the sources of PM is an important step during the planning of efficient mitigation strategies and the investigation of the potential risks to human health. Usually, source apportionment studies focus either on the organic or on the inorganic fraction of PM. In this study that took place in Patras, Greece, we address both PM fractions by combining measurements from a range of on- and off-line techniques, including elemental composition, organic and elemental carbon (OC and EC) measurements, and high-resolution Aerosol Mass Spectrometry (AMS) from different techniques. Six fine PM2.5 sources were identified based on the off-line measurements: secondary sulfate (34%), biomass burning (15%), exhaust traffic emissions (13%), nonexhaust traffic emissions (12%), mineral dust (10%), and sea salt (5%). The analysis of the AMS spectra quantified five factors: two oxygenated organic aerosols (OOA) factors (an OOA and a marine-related OOA, 52% of the total organic aerosols (OA)), cooking OA (COA, 11%) and two biomass burning OA (BBOA-I and BBOA-II, 37% in total) factors. The results of the two methods were synthesized, showcasing the complementarity of the two methodologies for fine PM source identification. The synthesis suggests that the contribution of biomass burning is quite robust, but that the exhaust traffic emissions are not due to local sources and may also include secondary OA from other sources.


2017 ◽  
Author(s):  
Ernesto Reyes-Villegas ◽  
Michael Priestley ◽  
Yu-Chieh Ting ◽  
Sophie Haslett ◽  
Thomas Bannan ◽  
...  

Abstract. Over the past decade, there has been an increasing interest in short-term events that negatively affect air quality such as bonfires and fireworks. High aerosol and gas concentrations generated from public bonfires/fireworks were measured in order to understand the night-time chemical processes and their atmospheric implications. Nitrate chemistry was observed during the bonfire night with nitrogen containing compounds in both gas and aerosol phase and further N2O5 and ClNO2 concentrations, which depleted early next morning due to photolysis of NO3 radicals, ceasing production. Particulate organic nitrate (PON) concentrations of 2.8 μg.m−3 were estimated using the m/z 46:30 ratios from AMS measurements, according to previously published methods. ME-2 source apportionment was performed to determine organic aerosol concentrations from different sources after modifying the fragmentation table and it was possible to identify two PON factors representing primary (pPON_ME2) and secondary (sPON_ME2) contributions. A slight improvement in the agreement between the source apportionment of the AMS and a collocated AE-31 Aethalometer was observed after modifying the prescribed fragmentation in the AMS organic spectrum (the fragmentation table) to determine PON sources, which resulted in an r2 = 0.865 between BBOA and babs_470wb compared to an r2 = 0.819 obtained without the modification. Correlations between OA sources and measurements made using Time of Flight Chemical Ionization Mass Spectrometry with an iodide adduct ion were performed in order to determine possible gas tracers to be used in future ME-2 analyses to constrain solutions. During bonfire night, high correlations (r2) were observed between BBOA and methacrylic acid (0.915), Acrylic acid (0.901), nitrous acid (0.864), propionic acid, (0.851) and Hydrogen cyanide (0.755). A series of oxygenated species, chlorine compounds as well as cresol showed good correlations with sPON_ME2 and the low volatility oxygenated organic aerosol (LVOOA) factor during an episode with low pollutant concentrations. Further analysis of pPON_ME2 and sPON_ME2 was performed in order to determine whether these PON sources absorb light near the UV region using an Aethalometer. This hypothesis was tested by doing multilinear regressions between babs_470wb and BBOA, sPON_ME2 and pPON_ME2. Our results suggest that sPON_ME2 does not absorb light at 470 nm while pPON_ME2 and LVOOA absorb light at 470 nm over that of black carbon. This may inform black carbon (BC) source apportionment studies from Aethalometer measurements, through investigation of the brown carbon contribution to babs_470wb.


2013 ◽  
Vol 13 (2) ◽  
pp. 961-981 ◽  
Author(s):  
M. Crippa ◽  
P. F. DeCarlo ◽  
J. G. Slowik ◽  
C. Mohr ◽  
M. F. Heringa ◽  
...  

Abstract. The effect of a post-industrial megacity on local and regional air quality was assessed via a month-long field measurement campaign in the Paris metropolitan area during winter 2010. Here we present source apportionment results from three aerosol mass spectrometers and two aethalometers deployed at three measurement stations within the Paris region. Submicron aerosol composition is dominated by the organic fraction (30–36%) and nitrate (28–29%), with lower contributions from sulfate (14–16%), ammonium (12–14%) and black carbon (7–13%). Organic source apportionment was performed using positive matrix factorization, resulting in a set of organic factors corresponding both to primary emission sources and secondary production. The dominant primary sources are traffic (11–15% of organic mass), biomass burning (13–15%) and cooking (up to 35% during meal hours). Secondary organic aerosol contributes more than 50% to the total organic mass and includes a highly oxidized factor from indeterminate and/or diverse sources and a less oxidized factor related to wood burning emissions. Black carbon was apportioned to traffic and wood burning sources using a model based on wavelength-dependent light absorption of these two combustion sources. The time series of organic and black carbon factors from related sources were strongly correlated. The similarities in aerosol composition, total mass and temporal variation between the three sites suggest that particulate pollution in Paris is dominated by regional factors, and that the emissions from Paris itself have a relatively low impact on its surroundings.


2021 ◽  
Vol 21 (13) ◽  
pp. 10763-10777
Author(s):  
Zainab Bibi ◽  
Hugh Coe ◽  
James Brooks ◽  
Paul I. Williams ◽  
Ernesto Reyes-Villegas ◽  
...  

Abstract. Atmospheric aerosol particles are known to have detrimental effects on human health and climate. Black carbon is an important constituent of atmospheric aerosol particulate matter (PM), emitted from incomplete combustion. Source apportionment of BC is very important, to evaluate the influence of different sources. The high-resolution soot particle aerosol mass spectrometer (HR-SP-AMS) instrument uses a laser vaporiser, which allows the real-time detection and characterisation of refractory black carbon (rBC) and its internally mixed particles such as metals, coating species, and rBC subcomponents in the form of HOA + fullerene. In this case study, the soot data were collected by using HR-SP-AMS during Guy Fawkes Night on 5 November 2014. Positive matrix factorisation was applied to positively discriminate between different wood-burning and bonfire sources for the first time, which no existing black carbon source apportionment technique is currently able to do. Along with this, the use of the fullerene signals in differentiating between soot sources and the use of metals as a tracer for fireworks has also been investigated, which did not significantly contribute to the rBC concentrations. The addition of fullerene signals and successful positive matrix factorisation (PMF) application to HR-SP-AMS data apportioned rBC into more than two sources. These bonfire sources are HOA + fullerene, biomass burning organic aerosol, more oxidised oxygenated organic aerosol (MO-OOA), and non-bonfire sources such as hydrocarbon-like OA and domestic burning. The result of correlation analysis between HR-SP-AMS data and previously published Aethalometer, MAAP, and CIMS data provides an effective way of gaining insights into the relationships between the variables and provide a quantitative estimate of the source contributions to the BC budget during this period. This research study is an important demonstration of using HR-SP-AMS for the purpose of BC source apportionment.


2017 ◽  
Vol 17 (6) ◽  
pp. 4265-4281 ◽  
Author(s):  
Johan Martinsson ◽  
Hafiz Abdul Azeem ◽  
Moa K. Sporre ◽  
Robert Bergström ◽  
Erik Ahlberg ◽  
...  

Abstract. With the present demand on fast and inexpensive aerosol source apportionment methods, the Aethalometer model was evaluated for a full seasonal cycle (June 2014–June 2015) at a rural atmospheric measurement station in southern Sweden by using radiocarbon and levoglucosan measurements. By utilizing differences in absorption of UV and IR, the Aethalometer model apportions carbon mass into wood burning (WB) and fossil fuel combustion (FF) aerosol. In this study, a small modification in the model in conjunction with carbon measurements from thermal–optical analysis allowed apportioned non-light-absorbing biogenic aerosol to vary in time. The absorption differences between WB and FF can be quantified by the absorption Ångström exponent (AAE). In this study AAEWB was set to 1.81 and AAEFF to 1.0. Our observations show that the AAE was elevated during winter (1.36 ± 0.07) compared to summer (1.12 ± 0.07). Quantified WB aerosol showed good agreement with levoglucosan concentrations, both in terms of correlation (R2 = 0.70) and in comparison to reference emission inventories. WB aerosol showed strong seasonal variation with high concentrations during winter (0.65 µg m−3, 56 % of total carbon) and low concentrations during summer (0.07 µg m−3, 6 % of total carbon). FF aerosol showed less seasonal dependence; however, black carbon (BC) FF showed clear diurnal patterns corresponding to traffic rush hour peaks. The presumed non-light-absorbing biogenic carbonaceous aerosol concentration was high during summer (1.04 µg m−3, 72 % of total carbon) and low during winter (0.13 µg m−3, 8 % of total carbon). Aethalometer model results were further compared to radiocarbon and levoglucosan source apportionment results. The comparison showed good agreement for apportioned mass of WB and biogenic carbonaceous aerosol, but discrepancies were found for FF aerosol mass. The Aethalometer model overestimated FF aerosol mass by a factor of 1.3 compared to radiocarbon and levoglucosan source apportionment. A performed sensitivity analysis suggests that this discrepancy can be explained by interference of non-light-absorbing biogenic carbon during winter. In summary, the Aethalometer model offers a cost-effective yet robust high-time-resolution source apportionment at rural background stations compared to a radiocarbon and levoglucosan alternative.


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