Source apportionment and dynamic changes of carbonaceous aerosols during the  haze bloom-decay process in China based on radiocarbon and organic molecular  tracers

Abstract. Fine carbonaceous aerosols (CAs) is the key factor influencing the currently filthy air in megacities in China, yet few studies simultaneously focus on the origins of different CAs species using specific and powerful source tracers. Here, we present a detailed source apportionment for various CAs fractions, including organic carbon (OC), water-soluble OC (WSOC), water-insoluble OC (WIOC), elemental carbon (EC) and secondary OC (SOC) in the largest cities of North (Beijing, BJ) and South China (Guangzhou, GZ), using the measurements of radiocarbon and anhydrosugars. Results show that non-fossil fuel sources such as biomass burning and biogenic emission make a significant contribution to the total CAs in Chinese megacities: 56 ± 4 in BJ and 46 ± 5 % in GZ, respectively. The relative contributions of primary fossil carbon from coal and liquid petroleum combustions, primary non-fossil carbon and secondary organic carbon (SOC) to total carbon are 19, 28 and 54 % in BJ, and 40, 15 and 46 % in GZ, respectively. Non-fossil fuel sources account for 52 in BJ and 71 % in GZ of SOC, respectively. These results suggest that biomass burning has a greater influence on regional particulate air pollution in North China than in South China. We observed an unabridged haze bloom-decay process in South China, which illustrates that both primary and secondary matter from fossil sources played a key role in the blooming phase of the pollution episode, while haze phase is predominantly driven by fossil-derived secondary organic matter and nitrate.

Download Full-text

Source apportionment and dynamic changes of carbonaceous aerosols during the haze bloom–decay process in China based on radiocarbon and organic molecular tracers

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-15-34949-2015 ◽

2015 ◽

Vol 15 (23) ◽

pp. 34949-34979 ◽

Cited By ~ 1

Author(s):

J. Liu ◽

J. Li ◽

D. Liu ◽

P. Ding ◽

C. Shen ◽

...

Keyword(s):

Organic Carbon ◽

Source Apportionment ◽

Biomass Burning ◽

South China ◽

Fossil Fuel ◽

Decay Process ◽

Water Soluble ◽

Total Carbon ◽

Carbonaceous Aerosols ◽

Fossil Carbon

Abstract. Fine carbonaceous aerosols (CAs) is the key factor influencing the currently filthy air in megacities of China, yet seldom study simultaneously focuses on the origins of different CAs species using specific and powerful source tracers. Here, we present a detailed source apportionment for various CAs fractions, including organic carbon (OC), water-soluble OC (WSOC), water-insoluble OC (WIOC), elemental carbon (EC) and secondary OC (SOC) in the largest cities of North (Beijing, BJ) and South China (Guangzhou, GZ), respectively, using the measurements of radiocarbon and anhydrosugars. Results show that non-fossil fuel sources such as biomass burning and biogenic emission make a significant contribution to the total CAs in Chinese megacities: 56 ± 4 % in BJ and 46 ± 5 % in GZ, respectively. The relative contributions of primary fossil carbon from coal and liquid petroleum combustions, primary non-fossil carbon and secondary organic carbon (SOC) to total carbon are 19, 28 and 54 % in BJ, and 40, 15 and 46 % in GZ, respectively. Non-fossil fuel sources account for 52 % in BJ and 71 % in GZ of SOC, respectively. These results suggest that biomass burning has a greater influence on regional particulate air pollution in North China than in South China. We observed an unabridged haze bloom–decay process in South China, which illustrates that both primary and secondary matter from fossil sources played a key role in the blooming phase of the pollution episode, while haze phase is predominantly driven by fossil-derived secondary organic matter and nitrate.

Download Full-text

Fossil vs. non-fossil sources of fine carbonaceous aerosols in four Chinese cities during the extreme winter haze episode of 2013

Atmospheric Chemistry and Physics ◽

10.5194/acp-15-1299-2015 ◽

2015 ◽

Vol 15 (3) ◽

pp. 1299-1312 ◽

Cited By ~ 113

Author(s):

Y.-L. Zhang ◽

R.-J. Huang ◽

I. El Haddad ◽

K.-F. Ho ◽

J.-J. Cao ◽

...

Keyword(s):

Particulate Matter ◽

Organic Carbon ◽

Biomass Burning ◽

Water Soluble ◽

Total Carbon ◽

World Health ◽

Biomass Combustion ◽

Carbonaceous Aerosols ◽

Haze Episode ◽

Mass Concentrations

Abstract. During winter 2013, extremely high concentrations (i.e., 4–20 times higher than the World Health Organization guideline) of PM2.5 (particulate matter with an aerodynamic diameter < 2.5 μm) mass concentrations (24 h samples) were found in four major cities in China including Xi'an, Beijing, Shanghai and Guangzhou. Statistical analysis of a combined data set from elemental carbon (EC), organic carbon (OC), 14C and biomass-burning marker measurements using Latin hypercube sampling allowed a quantitative source apportionment of carbonaceous aerosols. Based on 14C measurements of EC fractions (six samples each city), we found that fossil emissions from coal combustion and vehicle exhaust dominated EC with a mean contribution of 75 ± 8% across all sites. The remaining 25 ± 8% was exclusively attributed to biomass combustion, consistent with the measurements of biomass-burning markers such as anhydrosugars (levoglucosan and mannosan) and water-soluble potassium (K+). With a combination of the levoglucosan-to-mannosan and levoglucosan-to-K+ ratios, the major source of biomass burning in winter in China is suggested to be combustion of crop residues. The contribution of fossil sources to OC was highest in Beijing (58 ± 5%) and decreased from Shanghai (49 ± 2%) to Xi'an (38 ± 3%) and Guangzhou (35 ± 7%). Generally, a larger fraction of fossil OC was from secondary origins than primary sources for all sites. Non-fossil sources accounted on average for 55 ± 10 and 48 ± 9% of OC and total carbon (TC), respectively, which suggests that non-fossil emissions were very important contributors of urban carbonaceous aerosols in China. The primary biomass-burning emissions accounted for 40 ± 8, 48 ± 18, 53 ± 4 and 65 ± 26% of non-fossil OC for Xi'an, Beijing, Shanghai and Guangzhou, respectively. Other non-fossil sources excluding primary biomass burning were mainly attributed to formation of secondary organic carbon (SOC) from non-fossil precursors such as biomass-burning emissions. For each site, we also compared samples from moderately to heavily polluted days according to particulate matter mass. Despite a significant increase of the absolute mass concentrations of primary emissions from both fossil and non-fossil sources during the heavily polluted events, their relative contribution to TC was even decreased, whereas the portion of SOC was consistently increased at all sites. This observation indicates that SOC was an important fraction in the increment of carbonaceous aerosols during the haze episode in China.

Download Full-text

Source Apportionment of Aerosols by 14C Measurements in Different Carbonaceous Particle Fractions

Radiocarbon ◽

10.1017/s0033822200039783 ◽

2004 ◽

Vol 46 (1) ◽

pp. 475-484 ◽

Cited By ~ 100

Author(s):

S Szidat ◽

T M Jenk ◽

H W Gäggeler ◽

H-A Synal ◽

R Fisseha ◽

...

Keyword(s):

Organic Carbon ◽

Source Apportionment ◽

Atmospheric Aerosols ◽

Elemental Carbon ◽

Water Soluble ◽

Total Carbon ◽

Anthropogenic Sources ◽

Ambient Aerosols ◽

Carbonaceous Particle ◽

Fossil Carbon

Radiocarbon enables a distinction between contemporary and fossil carbon, which can be used for the apportionment of biogenic and anthropogenic sources in environmental studies. In order to apply this approach to carbonaceous atmospheric aerosols, it is necessary to adapt pretreatment procedures to the requirements of 14C measurements. In this work, we followed an approach in which total carbon (TC) is subdivided into fractions of different chemical and physical properties. 14C data of ambient aerosols from Zürich (Switzerland) are presented for the 2 sub-fractions of TC, organic carbon (OC) and elemental carbon (EC). Furthermore, OC is separated into water-insoluble OC (WINSOC) and water-soluble OC (WSOC). Results demonstrate the importance to differentiate between these fractions for 14C-deduced source apportionment, as the contributions can range between both extremes, nearly exclusively biogenic and anthropogenic.

Download Full-text

On the isolation of OC and EC and the optimal strategy of radiocarbon-based source apportionment of carbonaceous aerosols

Atmospheric Chemistry and Physics ◽

10.5194/acp-12-10841-2012 ◽

2012 ◽

Vol 12 (22) ◽

pp. 10841-10856 ◽

Cited By ~ 84

Author(s):

Y. L. Zhang ◽

N. Perron ◽

V. G. Ciobanu ◽

P. Zotter ◽

M. C. Minguillón ◽

...

Keyword(s):

Organic Carbon ◽

Source Apportionment ◽

Optimal Strategy ◽

Complete Removal ◽

Water Soluble ◽

Total Carbon ◽

Carbonaceous Aerosol ◽

Pure Oxygen ◽

Carbonaceous Aerosols ◽

Set Up

Abstract. Radiocarbon (14C) measurements of elemental carbon (EC) and organic carbon (OC) separately (as opposed to only total carbon, TC) allow an unambiguous quantification of their non-fossil and fossil sources and represent an improvement in carbonaceous aerosol source apportionment. Isolation of OC and EC for accurate 14C determination requires complete removal of interfering fractions with maximum recovery. The optimal strategy for 14C-based source apportionment of carbonaceous aerosols should follow an approach to subdivide TC into different carbonaceous aerosol fractions for individual 14C analyses, as these fractions may differ in their origins. To evaluate the extent of positive and negative artefacts during OC and EC separation, we performed sample preparation with a commercial Thermo-Optical OC/EC Analyser (TOA) by monitoring the optical properties of the sample during the thermal treatments. Extensive attention has been devoted to the set-up of TOA conditions, in particular, heating program and choice of carrier gas. Based on different types of carbonaceous aerosols samples, an optimised TOA protocol (Swiss_4S) with four steps is developed to minimise the charring of OC, the premature combustion of EC and thus artefacts of 14C-based source apportionment of EC. For the isolation of EC for 14C analysis, the water-extraction treatment on the filter prior to any thermal treatment is an essential prerequisite for subsequent radiocarbon measurements; otherwise the non-fossil contribution may be overestimated due to the positive bias from charring. The Swiss_4S protocol involves the following consecutive four steps (S1, S2, S3 and S4): (1) S1 in pure oxygen (O2) at 375 °C for separation of OC for untreated filters and water-insoluble organic carbon (WINSOC) for water-extracted filters; (2) S2 in O2 at 475 °C followed by (3) S3 in helium (He) at 650 °C, aiming at complete OC removal before EC isolation and leading to better consistency with thermal-optical protocols like EUSAAR_2, compared to pure oxygen methods; and (4) S4 in O2 at 760 °C for recovery of the remaining EC. WINSOC was found to have a significantly higher fossil contribution than the water-soluble OC (WSOC). Moreover, the experimental results demonstrate the lower refractivity of wood-burning EC compared to fossil EC and the difficulty of clearly isolating EC without premature evolution. Hence, simplified techniques of EC isolation for 14C analysis are prone to a substantial bias and generally tend towards an overestimation of fossil sources. To obtain the comprehensive picture of the sources of carbonaceous aerosols, the Swiss_4S protocol is not only implemented to measure OC and EC fractions, but also WINSOC as well as a continuum of refractory OC and non-refractory EC for 14C source apportionment. In addition, WSOC can be determined by subtraction of the water-soluble fraction of TC from untreated TC. Last, we recommend that 14C results of EC should in general be reported together with the EC recovery.

Download Full-text

Fossil vs. non-fossil sources of fine carbonaceous aerosols in four Chinese cities during the extreme winter haze episode in 2013

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-14-26257-2014 ◽

2014 ◽

Vol 14 (19) ◽

pp. 26257-26296 ◽

Cited By ~ 2

Author(s):

Y.-L. Zhang ◽

R.-J. Huang ◽

I. El Haddad ◽

K.-F. Ho ◽

J.-J. Cao ◽

...

Keyword(s):

Particulate Matter ◽

Organic Carbon ◽

Source Apportionment ◽

Biomass Burning ◽

Crop Residues ◽

Water Soluble ◽

World Health ◽

Biomass Combustion ◽

Carbonaceous Aerosols ◽

Haze Episode

Abstract. During winter 2013, extremely high concentrations (i.e. 4–20 times higher than the World Health Organization guideline) of PM2.5 (particulate matter with an aerodynamic diameter <2.5 μm) were reported in several large cities in China. In this work, source apportionment of fine carbonaceous aerosols during this haze episode was conducted at four major cities in China including Xian, Beijing, Shanghai and Guangzhou. An effective statistical analysis of a combined dataset from elemental carbon (EC) and organic carbon (OC), radiocarbon (14C) and biomass-burning marker measurements using Latin-hypercube sampling allowed a quantitative source apportionment of carbonaceous aerosols. We found that fossil emissions from coal combustion and vehicle exhaust dominated EC with a mean contribution of 75 ± 8% at all sites. The remaining 25 ± 8% was exclusively attributed to biomass combustion, consistent with the measurements of biomass-burning markers such as anhydrosugars (levoglucosan and mannosan) and water-soluble potassium (K+). With a combination of the levoglucosan-to-mannosan and levoglucosan-to-K+ ratios, the major source of biomass burning in winter in China is suggested to be combustion of crop residues. The contribution of fossil sources to OC was highest in Beijing (58 ± 5%) and decreased from Shanghai (49 ± 2%) to Xian (38 ± 3%) and Guangzhou (35 ± 7%). Generally, a larger fraction of fossil OC was rather from secondary origins than primary sources for all sites. Non-fossil sources accounted on average for 55 ± 10% and 48 ± 9% of OC and TC, respectively, which suggests that non-fossil emissions were very important contributors of urban carbonaceous aerosols in China. The primary biomass-burning emissions accounted for 40 ± 8%, 48 ± 18%, 53 ± 4% and 65 ± 26% of non-fossil OC for Xian, Beijing, Shanghai and Guangzhou, respectively. Other non-fossil sources excluding primary biomass-burning were mainly attributed to formation of secondary organic carbon (SOC) from non-fossil precursors such as biomass-burning emissions. For each site, we also compared samples from moderately with heavily polluted days according to particulate matter mass. Despite a significant increase of absolute mass concentrations of primary emissions from both, fossil and non-fossil sources, during the heavily polluted events, their relative contribution to TC was even decreased, whereas the portion of SOC was consistently increased at all sites. This observation indicates that SOC was an important fraction in the increment of carbonaceous aerosols during the haze episode in China.

Download Full-text

On the isolation of OC and EC and the optimal strategy of radiocarbon-based source apportionment of carbonaceous aerosols

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-12-17657-2012 ◽

2012 ◽

Vol 12 (7) ◽

pp. 17657-17702 ◽

Cited By ~ 1

Author(s):

Y. L. Zhang ◽

N. Perron ◽

V. G. Ciobanu ◽

P. Zotter ◽

M. C. Minguillón ◽

...

Keyword(s):

Organic Carbon ◽

Source Apportionment ◽

Optimal Strategy ◽

Complete Removal ◽

Water Soluble ◽

Total Carbon ◽

Carbonaceous Aerosol ◽

Pure Oxygen ◽

Carbonaceous Aerosols ◽

Set Up

Abstract. Radiocarbon (14C) measurements of elemental carbon (EC) and organic carbon (OC) separately (as opposed to only total carbon, TC) allow an unambiguous quantification of their non-fossil and fossil sources and represent an improvement in carbonaceous aerosol source apportionment. Isolation of OC and EC for accurate 14C determination requires complete removal of interfering fractions with maximum recovery. To evaluate the extent of positive and negative artefacts during OC and EC separation, we performed sample preparation with a commercial Thermo-Optical OC/EC Analyser (TOA) by monitoring the optical properties of the sample during the thermal treatments. Extensive attention has been devoted to the set-up of TOA conditions, in particular, heating program and choice of carrier gas. Based on different types of carbonaceous aerosols samples, an optimised TOA protocol (Swiss_4S) with four steps is developed to minimise the charring of OC, the premature combustion of EC and thus artefacts of 14C-based source apportionment of EC. For the isolation of EC for 14C analysis, the water-extraction treatment on the filter prior to any thermal treatment is an essential prerequisite for subsequent radiocarbon; otherwise the non-fossil contribution may be overestimated due to the positive bias from charring. The Swiss_4S protocol involves the following consecutive four steps (S1, S2, S3 and S4): (1) S1 in pure oxygen (O2) at 375 °C for separation of OC for untreated filters, and water-insoluble organic carbon (WINSOC) for water-extracted filters; (2) S2 in O2 at 475 °C, followed by (3) S3 in helium (He) at 650 °C, aiming at complete OC removal before EC isolation and leading to better consistency with thermal-optical protocols like EUSAAR_2, compared to pure oxygen methods; and (4) S4 in O2 at 760 °C for recovery of the remaining EC. WINSOC was found to have a significantly higher fossil contribution than the water-soluble OC (WSOC). Moreover, the experimental results demonstrate the lower refractivity of wood-burning EC compared to fossil EC and the difficulty of clearly isolating EC without premature evolution. Hence, simplified techniques of EC isolation for 14C analysis are prone to a substantial bias and generally tend towards an underestimation of the non-fossil sources. Consequently, the optimal strategy for 14C-based source apportionment of carbonaceous aerosols should follow an approach to subdivide TC into different carbonaceous aerosol fractions for individual 14C analyses, as these fractions differ in their origins. To obtain the comprehensive picture of the sources of carbonaceous aerosols, the Swiss_4S protocol is not only implemented to measure OC and EC fractions, but also WINSOC as well as a continuum of refractory OC and non-refractory EC for 14C source apportionment. In addition, WSOC can be determined by subtraction of the water-soluble fraction of TC from untreated TC. Last, we recommend that 14C results of EC should in general be reported together with the EC recovery.

Download Full-text

Fossil and non-fossil source contributions to atmospheric carbonaceous aerosols during extreme spring grassland fires in Eastern Europe

Atmospheric Chemistry and Physics ◽

10.5194/acp-16-5513-2016 ◽

2016 ◽

Vol 16 (9) ◽

pp. 5513-5529 ◽

Cited By ~ 21

Author(s):

Vidmantas Ulevicius ◽

Steigvilė Byčenkienė ◽

Carlo Bozzetti ◽

Athanasia Vlachou ◽

Kristina Plauškaitė ◽

...

Keyword(s):

Organic Carbon ◽

Biomass Burning ◽

Nitrogen Isotopes ◽

Early Spring ◽

Total Carbon ◽

Carbonaceous Aerosols ◽

Pmf Model ◽

Source Contributions ◽

The Baltic ◽

The Impact

Abstract. In early spring the Baltic region is frequently affected by high-pollution events due to biomass burning in that area. Here we present a comprehensive study to investigate the impact of biomass/grass burning (BB) on the evolution and composition of aerosol in Preila, Lithuania, during springtime open fires. Non-refractory submicron particulate matter (NR-PM1) was measured by an Aerodyne aerosol chemical speciation monitor (ACSM) and a source apportionment with the multilinear engine (ME-2) running the positive matrix factorization (PMF) model was applied to the organic aerosol fraction to investigate the impact of biomass/grass burning. Satellite observations over regions of biomass burning activity supported the results and identification of air mass transport to the area of investigation. Sharp increases in biomass burning tracers, such as levoglucosan up to 683 ng m−3 and black carbon (BC) up to 17 µg m−3 were observed during this period. A further separation between fossil and non-fossil primary and secondary contributions was obtained by coupling ACSM PMF results and radiocarbon (14C) measurements of the elemental (EC) and organic (OC) carbon fractions. Non-fossil organic carbon (OCnf) was the dominant fraction of PM1, with the primary (POCnf) and secondary (SOCnf) fractions contributing 26–44 % and 13–23 % to the total carbon (TC), respectively. 5–8 % of the TC had a primary fossil origin (POCf), whereas the contribution of fossil secondary organic carbon (SOCf) was 4–13 %. Non-fossil EC (ECnf) and fossil EC (ECf) ranged from 13–24 and 7–13 %, respectively. Isotope ratios of stable carbon and nitrogen isotopes were used to distinguish aerosol particles associated with solid and liquid fossil fuel burning.

Download Full-text

Sources and formation of carbonaceous aerosols in Xi'an, China: primary emissions and secondary formation constrained by radiocarbon

10.5194/egusphere-egu2020-12245 ◽

2020 ◽

Author(s):

Haiyan Ni ◽

Ru-Jin Huang ◽

Ulrike Dusek

Keyword(s):

Biomass Burning ◽

Coal Combustion ◽

Vehicle Emissions ◽

Fossil Fuel ◽

Fuel Combustion ◽

Warm Period ◽

Water Soluble ◽

Formation Mechanisms ◽

Carbonaceous Aerosols ◽

Fossil Fuel Combustion

To investigate the sources and formation mechanisms of carbonaceous aerosols, a major contributor to severe particulate air pollution, radiocarbon&#160;(14C) measurements were conducted on aerosols sampled from November&#160;2015 to November&#160;2016 in Xi'an, China. Based on the&#160;14C&#160;content in elemental carbon&#160;(EC), organic carbon&#160;(OC) and water-insoluble OC&#160;(WIOC), contributions of major sources to carbonaceous aerosols are estimated over a whole seasonal cycle: primary and secondary fossil sources, primary biomass burning, and other non-fossil carbon formed mainly from secondary processes. Primary fossil sources of&#160;EC were further sub-divided into coal and liquid fossil fuel combustion by complementing&#160;14C&#160;data with stable carbon isotopic signatures.The dominant EC&#160;source was liquid fossil fuel combustion (i.e., vehicle emissions), accounting for 64&#8201;% (median; 45&#8201;%&#8211;74&#8201;%, interquartile range) of&#160;EC in autumn, 60&#8201;% (41&#8201;%&#8211;72&#8201;%) in summer, 53&#8201;% (33&#8201;%&#8211;69&#8201;%) in spring and 46&#8201;% (29&#8201;%&#8211;59&#8201;%) in winter. An increased contribution from biomass burning to&#160;EC was observed in winter (&#8764;28&#8201;%) compared to other seasons (warm period;&#160;&#8764;15&#8201;%). In winter, coal combustion (&#8764;25&#8201;%) and biomass burning equally contributed to&#160;EC, whereas in the warm period, coal combustion accounted for a larger fraction of&#160;EC than biomass burning. The relative contribution of fossil sources to&#160;OC was consistently lower than that to&#160;EC, with an annual average of&#160;47&#177;4&#8201;%. Non-fossil OC&#160;of secondary origin was an important contributor to total&#160;OC (35&#177;4&#8201;%) and accounted for more than half of non-fossil&#160;OC (67&#177;6&#8201;%) throughout the year. Secondary fossil&#160;OC&#160;(SOCfossil) concentrations were higher than primary fossil&#160;OC&#160;(POCfossil) concentrations in winter but lower than POCfossil&#160;in the warm period.Fossil WIOC and water-soluble&#160;OC&#160;(WSOC) have been widely used as proxies for POCfossil&#160;and SOCfossil, respectively. This assumption was evaluated by (1)&#160;comparing their mass concentrations with POCfossil&#160;and SOCfossil&#160;and (2)&#160;comparing ratios of fossil WIOC to fossil&#160;EC to typical primary&#160;OC-to-EC ratios from fossil sources including both coal combustion and vehicle emissions. The results suggest that fossil WIOC and fossil WSOC are probably a better approximation for primary and secondary fossil&#160;OC, respectively, than POCfossil&#160;and SOCfossil&#160;estimated using the EC&#160;tracer method.

Download Full-text

Investigation of atmospheric aerosols over semi-urban and urban areas in Eastern Indo-Gangetic Plain: seasonal variability and source apportionment using PMF

10.5194/egusphere-egu21-14205 ◽

2021 ◽

Author(s):

Kanishtha Dubey ◽

Shubha Verma

Keyword(s):

Organic Carbon ◽

Biomass Burning ◽

Atmospheric Aerosols ◽

Urban Areas ◽

Relative Concentration ◽

Road Dust ◽

Water Soluble ◽

Carbonaceous Aerosols ◽

Gangetic Plain ◽

Brick Kilns

The study investigates the chemical composition and source of aerosol origin at a semi-urban (Kharagpur&#8211;Kgp) and urban (Kolkata&#8211;Kol) region during the period February 2015 to January 2016 and September 2010 to August 2011 respectively. Major water-soluble inorganic aerosols (WSII) were determined using Ion chromatography and carbonaceous aerosols (CA) using OC&#8211;EC analyser. A multivariate factor analysis Positive Matrix Factorization (PMF) was used in resolving source of aerosols at the study locations. Seasonal analysis of WSII at Kgp and Kol indicated relative dominance of calcium at both the places followed by sodium, chloride, and magnesium ions. Non-sea salt potassium (nss&#8211;K+), a biomass burning tracer was found higher at Kol than at Kgp. Sum of secondary aerosols sulphate (SO42-), nitrate (NO3-) and ammonium (NH4+) was higher at Kol than Kgp with relative concentration of SO42- being higher than NO3- at Kgp which was vice-versa at Kol. Examination of carbonaceous aerosols showed three times higher concentration of organic carbon (OC) than elemental carbon (EC) with monthly mean of OC/EC ratio > 2, indicating likely formation of secondary organic carbon formation. Seasonal influence of biomass burning inferred from nss&#8211;K+ (OC/EC) ratio relationship indicated dissimilarity in seasonality of biomass burning at Kgp (Kol). PMF resolved sources for Kgp constituted of secondary aerosol emissions, biomass burning, fugitive dust, marine aerosols, crustal dust and emissions from brick kilns while for Kol factors constituted of burning of waste, resuspended paved road dust, coal combustion, sea spray aerosols, vehicular emissions and biomass burning.

Download Full-text

Fossil fuel combustion, biomass burning and biogenic sources of fine carbonaceous aerosol in the Carpathian Basin

10.5194/acp-2019-792 ◽

2019 ◽

Author(s):

Imre Salma ◽

Anikó Vasanits-Zsigrai ◽

Attila Machon ◽

Tamás Varga ◽

István Major ◽

...

Keyword(s):

Biomass Burning ◽

Fossil Fuel ◽

Fuel Combustion ◽

Carpathian Basin ◽

Water Soluble ◽

Total Carbon ◽

Carbonaceous Aerosol ◽

City Centre ◽

Fossil Fuel Combustion ◽

Regional Background

Abstract. Fine-fraction aerosol samples were collected, air pollutants and meteorological properties were measured in-situ in regional background environment of the Carpathian Basin, a suburban area and central part of its largest city, Budapest in each season for 1 year-long time interval. The samples were analysed for PM2.5 mass, organic carbon (OC), elemental carbon (EC), water-soluble OC (WSOC), radiocarbon, levoglucosan (LVG) and its stereoisomers, and some chemical elements. Carbonaceous aerosol species made up 36 % of the PM2.5 mass with a modest seasonal variation and with a slightly increasing tendency from the regional background to the city centre (from 32 to 39 %). Coupled radiocarbon-LVG marker method was applied to apportion the total carbon (TC = OC + EC) into contributions of EC and OC from fossil fuel (FF) combustion (ECFF and OCFF, respectively), EC and OC from biomass burning (BB) (ECBB and OCBB, respectively) and OC from biogenic sources (OCBIO). Fossil fuel combustion showed rather constant daily or seasonal mean contributions (of 35 %) to the TC in the whole year in all atmospheric environments, while the daily contributions of BB and biogenic sources changed radically (from

Download Full-text