scholarly journals Source apportionment of fine organic carbon at an urban site of Beijing using a chemical mass balance model

2021 ◽  
Vol 21 (9) ◽  
pp. 7321-7341
Author(s):  
Jingsha Xu ◽  
Di Liu ◽  
Xuefang Wu ◽  
Tuan V. Vu ◽  
Yanli Zhang ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Mass Balance ◽  
Source Apportionment ◽  
Biomass Burning ◽  
Coal Combustion ◽  
Fine Particles ◽  
Inorganic Ions ◽  
Balance Model ◽  
Urban Site ◽  
Chemical Mass Balance

Abstract. Fine particles were sampled from 9 November to 11 December 2016 and 22 May to 24 June 2017 as part of the Atmospheric Pollution and Human Health in a Chinese Megacity (APHH-China) field campaigns in urban Beijing, China. Inorganic ions, trace elements, organic carbon (OC), elemental carbon (EC), and organic compounds, including biomarkers, hopanes, polycyclic aromatic hydrocarbons (PAHs), n-alkanes, and fatty acids, were determined for source apportionment in this study. Carbonaceous components contributed on average 47.2 % and 35.2 % of total reconstructed PM2.5 during the winter and summer campaigns, respectively. Secondary inorganic ions (sulfate, nitrate, ammonium; SNA) accounted for 35.0 % and 45.2 % of total PM2.5 in winter and summer. Other components including inorganic ions (K+, Na+, Cl−), geological minerals, and trace metals only contributed 13.2 % and 12.4 % of PM2.5 during the winter and summer campaigns. Fine OC was explained by seven primary sources (industrial and residential coal burning, biomass burning, gasoline and diesel vehicles, cooking, and vegetative detritus) based on a chemical mass balance (CMB) receptor model. It explained an average of 75.7 % and 56.1 % of fine OC in winter and summer, respectively. Other (unexplained) OC was compared with the secondary OC (SOC) estimated by the EC-tracer method, with correlation coefficients (R2) of 0.58 and 0.73 and slopes of 1.16 and 0.80 in winter and summer, respectively. This suggests that the unexplained OC by the CMB model was mostly associated with SOC. PM2.5 apportioned by the CMB model showed that the SNA and secondary organic matter were the two highest contributors to PM2.5. After these, coal combustion and biomass burning were also significant sources of PM2.5 in winter. The CMB results were also compared with results from the positive matrix factorization (PMF) analysis of co-located aerosol mass spectrometer (AMS) data. The CMB model was found to resolve more primary organic aerosol (OA) sources than AMS-PMF, but the latter could apportion secondary OA sources. The AMS-PMF results for major components, such as coal combustion OC and oxidized OC, correlated well with the results from the CMB model. However, discrepancies and poor agreements were found for other OC sources, such as biomass burning and cooking, some of which were not identified in AMS-PMF factors.

scholarly journals Source Apportionment of Fine Aerosol at an Urban Site of Beijing using a Chemical Mass Balance Model

2020 ◽  
Author(s):  
Jingsha Xu ◽  
Di Liu ◽  
Xuefang Wu ◽  
Tuan V. Vu ◽  
Yanli Zhang ◽  
...  
Keyword(s):  
Mass Balance ◽  
Source Apportionment ◽  
Biomass Burning ◽  
Coal Combustion ◽  
Fine Particles ◽  
Correlation Coefficients ◽  
Inorganic Ions ◽  
Balance Model ◽  
Urban Site ◽  
Chemical Mass Balance

Abstract. Fine particles were sampled from 9th November to 11th December 2016 and 22nd May to 24th June 2017 as part of the Atmospheric Pollution and Human Health in a Chinese megacity (APHH-China) field campaigns in urban Beijing, China. Inorganic ions, trace elements, OC, EC, and organic compounds including biomarkers, hopanes, PAHs, n-alkanes and fatty acids, were determined for source apportionment in this study. Carbonaceous components contributed on average 47.2 % and 35.2 % of total reconstructed PM2.5 during the winter and summer campaigns, respectively. Secondary inorganic ions (sulfate, nitrate, ammonium; SNA) accounted for 35.0 % and 45.2 % of total PM2.5 in winter and summer. Other components including inorganic ions (K+, Na+, Cl−), geological minerals, and trace metals only contributed 13.2 % and 12.4 % of PM2.5 during the winter and summer campaigns. Fine OC was explained by seven primary sources (industrial/residential coal burning, biomass burning, gasoline/diesel vehicles, cooking and vegetative detritus) based on a chemical mass balance (CMB) receptor model. It explained an average of 75.7 % and 56.1 % of fine OC in winter and summer, respectively. Other (unexplained) OC was compared with the secondary OC (SOC) estimated by the EC-tracer method, with correlation coefficients (R2) of 0.58 and 0.73, and slopes of 1.16 and 0.80 in winter and summer, respectively. This suggests that the unexplained OC by CMB was mostly associated with SOC. PM2.5 apportioned by CMB showed that the SNA and secondary organic matter were the highest two contributors to PM2.5. After these, coal combustion and biomass burning were also significant sources of PM2.5 in winter. The CMB results were also compared with results from Positive Matrix Factorization (PMF) analysis of co-located Aerosol Mass Spectrometer (AMS) data. The CMB was found to resolve more primary OA sources than AMS-PMF but the latter apportioned more secondary OA sources. The AMS-PMF results for major components, such as coal combustion OC and oxidized OC correlated well with the results from CMB. However, discrepancies and poor agreements were found for other OC sources, such as biomass burning and cooking, some of which were not identified in AMS-PMF factors.

scholarly journals Source apportionment of carbonaceous aerosols in Beijing with radiocarbon and organic tracers: insight into the differences between urban and rural sites

2021 ◽  
Vol 21 (10) ◽  
pp. 8273-8292
Author(s):  
Siqi Hou ◽  
Di Liu ◽  
Jingsha Xu ◽  
Tuan V. Vu ◽  
Xuefang Wu ◽  
...  
Keyword(s):  
Source Apportionment ◽  
Biomass Burning ◽  
Fine Particles ◽  
Water Soluble ◽  
Carbonaceous Aerosol ◽  
Balance Model ◽  
Gas Chromatography Mass Spectrometry ◽  
Urban Site ◽  
Carbonaceous Aerosols ◽  
Carbonaceous Particles

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.

scholarly journals Source Apportionment of Carbonaceous Aerosols in Beijing with Radiocarbon and Organic Tracers: Insight into the Differences between Urban and Rural Sites

2020 ◽  
Author(s):  
Siqi Hou ◽  
Di Liu ◽  
Jingsha Xu ◽  
Tuan V. Vu ◽  
Xuefang Wu ◽  
...  
Keyword(s):  
Source Apportionment ◽  
Biomass Burning ◽  
Fine Particles ◽  
Warm Season ◽  
Water Soluble ◽  
Carbonaceous Aerosol ◽  
Balance Model ◽  
Urban Site ◽  
Carbonaceous Aerosols ◽  
Carbonaceous Particles

Abstract. Carbonaceous aerosol is the 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 GC-MS. Higher contributions of fossil-derived OC (OCf) were found at the urban site. OCf to 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 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 winter time for IAP and PG, 28.9 ± 7.4 % and 28.9 ± 9.6 % 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), 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.

Source apportionment of fine particulate matter organic carbon in Shenzhen, China by chemical mass balance and radiocarbon methods

2018 ◽  
Vol 240 ◽  
pp. 34-43 ◽  
Author(s):  
Ibrahim M. Al-Naiema ◽  
Subin Yoon ◽  
Yu-Qin Wang ◽  
Yuan-Xun Zhang ◽  
Rebecca J. Sheesley ◽  
...  
Keyword(s):  
Particulate Matter ◽  
Organic Carbon ◽  
Mass Balance ◽  
Source Apportionment ◽  
Fine Particulate Matter ◽  
Chemical Mass Balance ◽  
Fine Particulate

scholarly journals Source apportionment of PM<sub>2.5</sub> at a regional background site in North China using PMF linked with radiocarbon analysis: insight into the contribution of biomass burning

2016 ◽  
Vol 16 (17) ◽  
pp. 11249-11265 ◽  
Author(s):  
Zheng Zong ◽  
Xiaoping Wang ◽  
Chongguo Tian ◽  
Yingjun Chen ◽  
Lin Qu ◽  
...  
Keyword(s):  
Source Apportionment ◽  
Biomass Burning ◽  
Coal Combustion ◽  
North China ◽  
Fine Particles ◽  
Vehicle Emission ◽  
Shandong Peninsula ◽  
Air Masses ◽  
Background Site ◽  
Bth Region

Abstract. Source apportionment of fine particles (PM2.5) at a background site in North China in the winter of 2014 was done using statistical analysis, radiocarbon (14C) measurement and positive matrix factorization (PMF) modeling. Results showed that the concentration of PM2.5 was 77.6 ± 59.3 µg m−3, of which sulfate (SO42−) concentration was the highest, followed by nitrate (NO3−), organic carbon (OC), elemental carbon (EC) and ammonium (NH4+). As demonstrated by backward trajectory, more than half of the air masses during the sampling period were from the Beijing–Tianjin–Hebei (BTH) region, followed by Mongolia and the Shandong Peninsula. Cluster analysis of chemical species suggested an obvious signal of biomass burning in the PM2.5 from the Shandong Peninsula, while the PM2.5 from the BTH region showed a vehicle emission pattern. This finding was further confirmed by the 14C measurement of OC and EC in two merged samples. The 14C result indicated that biogenic and biomass burning emission contributed 59 ± 4 and 52 ± 2 % to OC and EC concentrations, respectively, when air masses originated from the Shandong Peninsula, while the contributions fell to 46 ± 4 and 38 ± 1 %, respectively, when the prevailing wind changed and came from the BTH region. The minimum deviation between source apportionment results from PMF and 14C measurement was adopted as the optimal choice of the model exercises. Here, two minor overestimates with the same range (3 %) implied that the PMF result provided a reasonable source apportionment of the regional PM2.5 in this study. Based on the PMF modeling, eight sources were identified; of these, coal combustion, biomass burning and vehicle emission were the main contributors of PM2.5, accounting for 29.6, 19.3 and 15.9 %, respectively. Compared with overall source apportionment, the contributions of vehicle emission, mineral dust, coal combustion and biomass burning increased when air masses came from the BTH region, Mongolia and the Shandong Peninsula, respectively. Since coal combustion and vehicle emission have been considered as the leading emission sources to be controlled for improving air quality, biomass burning was highlighted in the present study.

scholarly journals Seasonal variations in high time-resolved chemical compositions, sources, and evolution of atmospheric submicron aerosols in the megacity Beijing

2017 ◽  
Vol 17 (16) ◽  
pp. 9979-10000 ◽  
Author(s):  
Wei Hu ◽  
Min Hu ◽  
Wei-Wei Hu ◽  
Jing Zheng ◽  
Chen Chen ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Coal Combustion ◽  
Fine Particles ◽  
Liquid Water Content ◽  
Urban Site ◽  
Chemical Components ◽  
Chemical Compositions ◽  
Average Mass ◽  
Four Seasons ◽  
Secondary Formation

Abstract. A severe regional haze problem in the megacity Beijing and surrounding areas, caused by fast formation and growth of fine particles, has attracted much attention in recent years. In order to investigate the secondary formation and aging process of urban aerosols, four intensive campaigns were conducted in four seasons between March 2012 and March 2013 at an urban site in Beijing (116.31° E, 37.99° N). An Aerodyne high-resolution time-of-flight aerosol mass spectrometry (HR-ToF-AMS) was deployed to measure non-refractory chemical components of submicron particulate matter (NR-PM1). The average mass concentrations of PM1 (NR-PM1+black carbon) were 45.1 ± 45.8, 37.5 ± 31.0, 41.3 ± 42.7, and 81.7 ± 72.4 µg m−3 in spring, summer, autumn, and winter, respectively. Organic aerosol (OA) was the most abundant component in PM1, accounting for 31, 33, 44, and 36 % seasonally, and secondary inorganic aerosol (SNA, sum of sulfate, nitrate, and ammonium) accounted for 59, 57, 43, and 55 % of PM1 correspondingly. Based on the application of positive matrix factorization (PMF), the sources of OA were obtained, including the primary ones of hydrocarbon-like (HOA), cooking (COA), biomass burning OA (BBOA) and coal combustion OA (CCOA), and secondary component oxygenated OA (OOA). OOA, which can be split into more-oxidized (MO-OOA) and less-oxidized OOA (LO-OOA), accounted for 49, 69, 47, and 50 % in four seasons, respectively. Totally, the fraction of secondary components (OOA+SNA) contributed about 60–80 % to PM1, suggesting that secondary formation played an important role in the PM pollution in Beijing, and primary sources were also non-negligible. The evolution process of OA in different seasons was investigated with multiple metrics and tools. The average carbon oxidation states and other metrics show that the oxidation state of OA was the highest in summer, probably due to both strong photochemical and aqueous-phase oxidations. It was indicated by the good correlations (r = 0.53–0.75, p < 0.01) between LO-OOA and odd oxygen (Ox =  O3 + NO2), and between MO-OOA and liquid water content in aerosols. BBOA was resolved in spring and autumn, influenced by agricultural biomass burning (e.g., field preparation burnings, straw burning after the harvest). CCOA was only identified in winter due to domestic heating. These results signified that the comprehensive management for biomass burning and coal combustion emissions is needed. High concentrations of chemical components in PM1 in Beijing, especially in winter or in adverse meteorological conditions, suggest that further strengthening the regional emission control of primary particulate and precursors of secondary species is expected.

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