scholarly journals Direct observations of organic aerosols in common wintertime hazes in North China: insights into their size, shape, mixing state, and source

2016 ◽  
Author(s):  
S. R. Chen ◽  
L. Xu ◽  
Y. X. Zhang ◽  
B. Chen ◽  
X. F. Wang ◽  
...  
Keyword(s):  
Rural Areas ◽  
Coal Combustion ◽  
North China ◽  
Fine Particles ◽  
Organic Aerosols ◽  
Urban Site ◽  
Mixing State ◽  
Spherical Type ◽  
Coating Type

Abstract. Many studies have focused on the physicochemical properties of aerosol particles in unusually severe haze episodes instead of the more freqent and less severe hazes. Consistent with this lack of attention, the morphology and mixing state of organic matter (OM) particles in the frequent light and moderate (L&M) hazes in winter in North China Plain (NCP) have not been examined, even though OM dominates these fine particles. In the present work, morphology, mixing state, and size of organic aerosols in the L&M hazes were systematically characterized using transmission electron microscopy coupled with energy-dispersive X-ray spectroscopy, atomic force microscopy, and nanoscale secondary ion mass spectrometer, with the comparisons among an urban site (Jinan, S1), a mountain site (Tai, S2), and a background island site (Changdao, S3) in the same hazes. Based on their morphology, the OM particles were divided into six different types: spherical (type 1), near-spherical (type 2), irregular (type 3), domelike (type 4), dispersed-OM (type 5), and OM-coating (type 6). In the three sampling sites, type 1–3 of OM particles were most abundant in the L&M hazes and most of them were internally mixed with non-OM particles. The abundant near-spherical OM particles with higher sphericity and lower aspect ratio indicate that these primary OM particles formed in cooling, polluted plumes from coal combustion and biomass burning. Based on the Si-O-C ratio in OM particles, we estimated that 71 % of type 1–3 OM particles were associated with coal combustion. Our result suggests that coal combustion in residential stoves was a widespread source from urban to rural areas in the NCP. Average OM thickness which correlates with the age of the air masses in type 6 particles only slightly increased from S3 to S2 to S1, suggesting that the L&M hazes were usually dry (relative humidity 

scholarly journals Direct observations of organic aerosols in common wintertime hazes in North China: insights into direct emissions from Chinese residential stoves

2017 ◽  
Vol 17 (2) ◽  
pp. 1259-1270 ◽  
Author(s):  
Shurui Chen ◽  
Liang Xu ◽  
Yinxiao Zhang ◽  
Bing Chen ◽  
Xinfeng Wang ◽  
...  
Keyword(s):  
Rural Areas ◽  
Coal Combustion ◽  
North China ◽  
Fine Particles ◽  
Organic Aerosols ◽  
Heterogeneous Reactions ◽  
Urban Site ◽  
Mixing State ◽  
Spherical Type

Abstract. Many studies have focused on the physicochemical properties of aerosol particles in unusually severe haze episodes in North China instead of the more frequent and less severe hazes. Consistent with this lack of attention, the morphology and mixing state of organic matter (OM) particles in the frequent light and moderate (L &amp; M) hazes in winter in the North China Plain (NCP) have not been examined, even though OM dominates these fine particles. In the present work, morphology, mixing state, and size of organic aerosols in the L &amp; M hazes were systematically characterized using transmission electron microscopy coupled with energy-dispersive X-ray spectroscopy, atomic force microscopy, and nanoscale secondary ion mass spectrometer, with the comparisons among an urban site (Jinan, S1), a mountain site (Mt. Tai, S2), and a background island site (Changdao, S3) in the same hazes. Based on their morphologies, the OM particles were divided into six different types: spherical (type 1), near-spherical (type 2), irregular (type 3), domelike (type 4), dispersed-OM (type 5), and OM-coating (type 6). In the three sampling sites, types 1–3 of OM particles were most abundant in the L &amp; M hazes and most of them were internally mixed with non-OM particles. The abundant near-spherical OM particles with higher sphericity and lower aspect ratio indicate that these primary OM particles formed in the cooling process after polluted plumes were emitted from coal combustion and biomass burning. Based on the Si-O-C ratio in OM particles, we estimated that 71 % of type 1–3 OM particles were associated with coal combustion. Our result suggests that coal combustion in residential stoves was a widespread source from urban to rural areas in NCP. Average OM thickness which correlates with the age of the air masses in type 6 particles only slightly increased from S1 to S2 to S3, suggesting that the L &amp; M hazes were usually dry (relative humidity < 60 %) with weak photochemistry and heterogeneous reactions between particles and gases. We conclude that the direct emissions from these coal stoves without any pollution controls in rural areas and in urban outskirts contribute large amounts of primary OM particles to the regional L &amp; M hazes in North China.

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 Mixing state, composition, and sources of fine aerosol particles in the Qinghai-Tibetan Plateau and the influence of agricultural biomass burning

2015 ◽  
Vol 15 (17) ◽  
pp. 24369-24401 ◽  
Author(s):  
W. J. Li ◽  
S. R. Chen ◽  
Y. S. Xu ◽  
X. C. Guo ◽  
Y. L. Sun ◽  
...  
Keyword(s):  
Fly Ash ◽  
Tibetan Plateau ◽  
Biomass Burning ◽  
Coal Combustion ◽  
Fine Particles ◽  
Aerosol Particles ◽  
Microscopic Analysis ◽  
Organic Coating ◽  
Pollution Level ◽  
Mixing State

Abstract. Transmission electron microscopy (TEM) was employed to obtain morphology, size, composition, and mixing state of background fine particles with diameter less than 1 μm in the Qinghai-Tibetan Plateau (QTP) during 15 September to 15 October 2013. Individual aerosol particles mainly contained secondary inorganic aerosols (SIA-sulfate and nitrate) and organics during clean periods (PM2.5: particles less than 2.5 μg m−3). The presence of KCl-NaCl associated with organics and an increase of soot particles suggest that an intense biomass burning event caused the highest PM2.5 concentrations (> 30 μg m−3) during the study. A large number fraction of the fly ash-containing particles (21.73 %) suggests that coal combustion emissions in the QTP significantly contributed to air pollutants at the median pollution level (PM2.5: 10–30 μg m−3). We concluded that emissions from biomass burning and from coal combustion both constantly contribute to anthropogenic particles in the QTP atmosphere. Based on size distributions of individual particles in different pollution levels, we found that gas condensation on existing particles is an important chemical process for the formation of SIA with organic coating. TEM observations show that refractory aerosols (e.g., soot, fly ash, and visible organic particles) likely adhere to the surface of SIA particles larger than 200 nm due to coagulation. Organic coating and soot on surface of the aged particles likely influence their hygroscopic and optical properties in the QTP, respectively. To our knowledge, this study reports the first microscopic analysis of fine particles in the background QTP air.

scholarly journals Organic aerosol volatility and viscosity in North China Plain: Contrast between summer and winter

2020 ◽  
Author(s):  
Weiqi Xu ◽  
Chun Chen ◽  
Yanmei Qiu ◽  
Ying Li ◽  
Zhiqiang Zhang ◽  
...  
Keyword(s):  
Coal Combustion ◽  
North China Plain ◽  
North China ◽  
Organic Aerosol ◽  
Rural Site ◽  
Urban Site ◽  
Aerosol Mass ◽  
Effective Saturation ◽  
Formation And Evolution ◽  
Primary Emissions

Abstract. Volatility and viscosity have substantial impacts on gas-particle partitioning, formation and evolution of aerosol, and hence the predictions of aerosol related air quality and climate effects. Here aerosol volatility and viscosity at a rural site (Gucheng) and an urban site (Beijing) in North China Plain (NCP) in summer and winter were investigated by using a thermodenuder coupled with high resolution aerosol mass spectrometer. The effective saturation concentration (C*) of organic aerosol (OA) in summer was smaller than that in winter (0.55 μg m−3 vs. 0.71–0.75 μg m−3), indicating that OA in winter in NCP is more volatile due to enhanced primary emissions from coal combustion and biomass burning. The volatility distributions varied largely different among different OA factors. In particular, we found that hydrocarbon-like OA (HOA) contained more non-volatile compounds compared to coal combustion related OA. The more oxidized oxygenated OA (MO-OOA) showed overall lower volatility than less oxidized OOA (LO-OOA) in both summer and winter, yet the volatility of MO-OOA was found to be relative humidity (RH) dependent showing more volatile properties at higher RH. Our results demonstrated the different composition and chemical formation pathways of MO-OOA under different RH levels. The glass transition temperature (Tg) and viscosity of OA in summer and winter are estimated using the recently developed parameterization formula. Our results showed that the Tg of OA in summer in Beijing (291.5 K) was higher than that in winter (289.7–290.0 K), while it varied greatly among different OA factors. The viscosity suggested that OA existed mainly as solid in winter in Beijing, but as semi-solids in Beijing in summer and Gucheng in winter. These results have important implications that kinetically limited gas-particle partitioning may need to be considered when simulating secondary OA formation in NCP.

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 Organic aerosol volatility and viscosity in the North China Plain: contrast between summer and winter

2021 ◽  
Vol 21 (7) ◽  
pp. 5463-5476
Author(s):  
Weiqi Xu ◽  
Chun Chen ◽  
Yanmei Qiu ◽  
Ying Li ◽  
Zhiqiang Zhang ◽  
...  
Keyword(s):  
Coal Combustion ◽  
North China Plain ◽  
North China ◽  
Organic Aerosol ◽  
Rural Site ◽  
Urban Site ◽  
The North ◽  
Aerosol Mass ◽  
The North China Plain ◽  
Primary Emissions

Abstract. Volatility and viscosity have substantial impacts on gas–particle partitioning, formation and evolution of aerosol and hence the predictions of aerosol-related air quality and climate effects. Here aerosol volatility and viscosity at a rural site (Gucheng) and an urban site (Beijing) in the North China Plain (NCP) in summer and winter were investigated by using a thermodenuder coupled with a high-resolution aerosol mass spectrometer. The effective saturation concentration (C*) of organic aerosol (OA) in summer was smaller than that in winter (0.55 µg m−3 vs. 0.71–0.75 µg m−3), indicating that OA in winter in the NCP is more volatile due to enhanced primary emissions from coal combustion and biomass burning. The volatility distributions varied and were largely different among different OA factors. In particular, we found that hydrocarbon-like OA (HOA) contained more nonvolatile compounds compared to coal-combustion-related OA. The more oxidized oxygenated OA (MO-OOA) showed overall lower volatility than less oxidized OOA (LO-OOA) in both summer and winter, yet the volatility of MO-OOA was found to be relative humidity (RH) dependent showing more volatile properties at higher RH. Our results demonstrated the different composition and chemical formation pathways of MO-OOA under different RH levels. The glass transition temperature (Tg) and viscosity of OA in summer and winter are estimated using the recently developed parameterization formula. Our results showed that the Tg of OA in summer in Beijing (291.5 K) was higher than that in winter (289.7–290.0 K), while it varied greatly among different OA factors. The viscosity suggested that OA existed mainly as solid in winter in Beijing (RH = 29 ± 17 %), but as semisolids in Beijing in summer (RH = 48 ± 25 %) and Gucheng in winter (RH = 68 ± 24 %). These results have the important implication that kinetically limited gas–particle partitioning may need to be considered when simulating secondary OA formation in the NCP.

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.

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

2017 ◽  
Author(s):  
Wei Hu ◽  
Min Hu ◽  
Wei-Wei Hu ◽  
Jing Zheng ◽  
Chen Chen ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Coal Combustion ◽  
Fine Particles ◽  
Urban Site ◽  
Chemical Components ◽  
Chemical Compositions ◽  
Average Mass ◽  
Four Seasons ◽  
Secondary Formation ◽  
Autumn And Winter

Abstract. 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) and other relevant instrumentations for gaseous and particulate pollutants were deployed. The average mass concentrations of submicron particulate matter (PM1) 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, usually composed of more-oxidized (MO-OOA) and less-oxidized OOA (LO-OOA), accounted for 63, 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. BBOA and CCOA were only resolved in autumn and winter, respectively, consistent with the agricultural activities (e.g., straw burning after the harvest in suburban areas) in autumn and domestic heating in winter, signifying that the comprehensive management for the emissions from biomass burning and coal combustion are 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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