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 ◽  
...  

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.

2017 ◽  
Author(s):  
Wei Hu ◽  
Min Hu ◽  
Wei-Wei Hu ◽  
Jing Zheng ◽  
Chen Chen ◽  
...  

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.


Atmosphere ◽  
2020 ◽  
Vol 11 (3) ◽  
pp. 292 ◽  
Author(s):  
Minhan Park ◽  
Yujue Wang ◽  
Jihyo Chong ◽  
Haebum Lee ◽  
Jiho Jang ◽  
...  

We performed simultaneous measurements of chemical compositions of fine particles in Beijing, China and Gwangju, Korea to better understand their sources during winter haze period. We identified PM2.5 events in Beijing, possibly caused by a combination of multiple primary combustion sources (biomass burning, coal burning, and vehicle emissions) and secondary aerosol formation under stagnant conditions and/or dust sources under high wind speeds. During the PM2.5 events in Gwangju, the contribution of biomass burning and secondary formation of nitrate and organics to the fine particles content significantly increased under stagnant conditions. We commonly observed the increases of nitrogen-containing organic compounds and biomass burning inorganic (K+) and organic (levoglucosan) markers, suggesting the importance of biomass burning sources during the winter haze events (except dust event cases) at both sites. Pb isotope ratios indicated that the fraction of Pb originated from possibly industry and coal combustion sources increased during the PM2.5 events in Gwangju, relative to nonevent days.


2021 ◽  
Vol 21 (9) ◽  
pp. 7321-7341
Author(s):  
Jingsha Xu ◽  
Di Liu ◽  
Xuefang Wu ◽  
Tuan V. Vu ◽  
Yanli Zhang ◽  
...  

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.


2020 ◽  
Author(s):  
Jingsha Xu ◽  
Di Liu ◽  
Xuefang Wu ◽  
Tuan V. Vu ◽  
Yanli Zhang ◽  
...  

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.


Author(s):  
Xing Li ◽  
Shanshan Li ◽  
Qiulin Xiong ◽  
Xingchuan Yang ◽  
Mengxi Qi ◽  
...  

Beijing, which is the capital of China, suffers from severe Fine Particles (PM2.5) pollution during the heating season. In order to take measures to control the PM2.5 pollution and improve the atmospheric environmental quality, daily PM2.5 samples were collected at an urban site from 15 November to 31 December 2016, characteristics of PM2.5 chemical compositions and their effect on atmospheric visibility were analyzed. It was found that the daily average mass concentrations of PM2.5 ranged from 7.64 to 383.00 μg m−3, with an average concentration of 114.17 μg m−3. On average, the Organic Carbon (OC) and Elemental Carbon (EC) contributed 21.39% and 5.21% to PM2.5, respectively. Secondary inorganic ions (SNA: SO42− + NO3− + NH4+) dominated the Water-Soluble Inorganic Ions (WSIIs) and they accounted for 47.09% of PM2.5. The mass concentrations of NH4+, NO3− and SO42− during the highly polluted period were 8.08, 8.88 and 6.85 times greater, respectively, than during the clean period, which contributed most to the serious PM2.5 pollution through the secondary transformation of NO2, SO2 and NH3. During the highly polluted period, NH4NO3 contributed most to the reconstruction extinction coefficient (b′ext), accounting for 35.7%, followed by (NH4)2SO4 (34.44%) and Organic Matter (OM: 15.24%). The acidity of PM2.5 in Beijing was weakly acid. Acidity of PM2.5 and relatively high humidity could aggravate PM2.5 pollution and visibility impairment by promoting the generation of secondary aerosol. Local motor vehicles contributed the most to NO3−, OC, and visibility impairment in urban Beijing. Other sources of pollution in the area surrounding urban Beijing, including coal burning, agricultural sources, and industrial sources in the Hebei, Shandong, and Henan provinces, released large amounts of SO2, NH3, and NO2. These, which were transformed into SO42−, NH4+, and NO3− during the transmission process, respectively, and had a great impact on atmospheric visibility impairment.


2009 ◽  
Vol 9 (21) ◽  
pp. 8573-8585 ◽  
Author(s):  
Q. Wang ◽  
M. Shao ◽  
Y. Zhang ◽  
Y. Wei ◽  
M. Hu ◽  
...  

Abstract. Fine particles (PM2.5, i.e., particles with an aerodynamic diameter of ≤2.5 μm) were collected from the air in August 2005, August–September 2006, and January–February 2007, in Beijing, China. The chemical compositions of particulate organic matter in the ambient samples were quantified by gas chromatography/mass spectrometry. The dominant compounds identified in summertime were n-alkanoic acids, followed by dicarboxylic acids and sugars, while sugars became the most abundant species in winter, followed by polycyclic aromatic hydrocarbons, n-alkanes, and n-alkanoic acids. The contributions of seven emission sources (i.e., gasoline/diesel vehicles, coal burning, wood/straw burning, cooking, and vegetative detritus) to particulate organic matter in PM2.5 were estimated using a chemical mass balance receptor model. The model results present the seasonal trends of source contributions to organic aerosols. Biomass burning (straw and wood) had the highest contribution in winter, followed by coal burning, vehicle exhaust, and cooking. The contribution of cooking was the highest in summer, followed by vehicle exhaust and biomass burning, while coal smoke showed only a minor contribution to ambient organic carbon.


2016 ◽  
Vol 16 (16) ◽  
pp. 10671-10687 ◽  
Author(s):  
Xiaopu Lyu ◽  
Nan Chen ◽  
Hai Guo ◽  
Lewei Zeng ◽  
Weihao Zhang ◽  
...  

Abstract. Continuous measurements of airborne particles and their chemical compositions were conducted in May, June, October, and November 2014 at an urban site in Wuhan, central China. The results indicate that particle concentrations remained at a relatively high level in Wuhan, with averages of 135.1 ± 4.4 (mean ± 95 % confidence interval) and 118.9 ± 3.7 µg m−3 for PM10 and 81.2 ± 2.6 and 85.3 ± 2.6 µg m−3 for PM2.5 in summer and autumn, respectively. Moreover, PM2.5 levels frequently exceeded the National Standard Level II (i.e., daily average of 75 µg m−3), and six PM2.5 episodes (i.e., daily PM2.5 averages above 75 µg m−3 for 3 or more consecutive days) were captured during the sampling campaign. Potassium was the most abundant element in PM2.5, with an average concentration of 2060.7 ± 82.3 ng m−3; this finding indicates intensive biomass burning in and around Wuhan during the study period, because almost no correlation was found between potassium and mineral elements (iron and calcium). The source apportionment results confirm that biomass burning was the main cause of episodes 1, 3, and 4, with contributions to PM2.5 of 46.6 % ± 3.0 %, 50.8 % ± 1.2 %, and 44.8 % ± 2.6%, respectively, whereas fugitive dust was the leading factor in episode 2. Episodes 5 and 6 resulted mainly from increases in vehicular emissions and secondary inorganic aerosols, and the mass and proportion of NO3− both peaked during episode 6. The high levels of NOx and NH3 and the low temperature during episode 6 were responsible for the increase of NO3−. Moreover, the formation of secondary organic carbon was found to be dominated by aromatics and isoprene in autumn, and the contribution of aromatics to secondary organic carbon increased during the episodes.


2020 ◽  
Author(s):  
Ting Wang ◽  
Rujin Huang ◽  
Lu Yang ◽  
Wei Yuan ◽  
Yuquan Gong

&lt;p&gt;Atmospheric brown carbon (BrC) has significant impact on Earth&amp;#8217;s radiative budget. However, due to our very limited knowledge about the relationship between BrC light absorption and the associated sources, the estimation for radiative effects of BrC is still largely constrained. In this study, we combine ultraviolet&amp;#8722;visible (UV&amp;#8722;vis) spectroscopy measurements and chemical analyses of BrC samples collected from January to December 2015 in urban Beijing, to investigated the sources of atmospheric BrC. The multiple liner regression model was applied to apportion the contributions of individual primary and secondary organic aerosol (OA) source components to light absorption of BrC. Our results indicated that biomass burning emission and secondary formation are highly absorbing up to 500 nm, and their contributions increased with the wavelengths. In contrast, the contribution of traffic emission and coal combustion to total absorption decreased with the wavelength and the large contributions were mostly found at shorter wavelengths. Then the mass absorption efficiency (MAE) of major light-absorbing components were estimated, which can provide a support to estimate the impact of BrC from these sources on the climate. The positive matrix factorization model were also used to verify the contributions of different source components of BrC absorption at 365 nm. The results consistently demonstrate that the biomass burning and secondary formation contributes significantly to the overall absorption, followed by coal combustion and traffic emission.&lt;/p&gt;


2016 ◽  
Vol 16 (17) ◽  
pp. 11249-11265 ◽  
Author(s):  
Zheng Zong ◽  
Xiaoping Wang ◽  
Chongguo Tian ◽  
Yingjun Chen ◽  
Lin Qu ◽  
...  

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.


2016 ◽  
Vol 16 (13) ◽  
pp. 8309-8329 ◽  
Author(s):  
Yele Sun ◽  
Wei Du ◽  
Pingqing Fu ◽  
Qingqing Wang ◽  
Jie Li ◽  
...  

Abstract. Winter has the worst air pollution of the year in the megacity of Beijing. Despite extensive winter studies in recent years, our knowledge of the sources, formation mechanisms and evolution of aerosol particles is not complete. Here we have a comprehensive characterization of the sources, variations and processes of submicron aerosols that were measured by an Aerodyne high-resolution aerosol mass spectrometer from 17 December 2013 to 17 January 2014 along with offline filter analysis by gas chromatography/mass spectrometry. Our results suggest that submicron aerosols composition was generally similar across the winter of different years and was mainly composed of organics (60 %), sulfate (15 %) and nitrate (11 %). Positive matrix factorization of high- and unit-mass resolution spectra identified four primary organic aerosol (POA) factors from traffic, cooking, biomass burning (BBOA) and coal combustion (CCOA) emissions as well as two secondary OA (SOA) factors. POA dominated OA, on average accounting for 56 %, with CCOA being the largest contributor (20 %). Both CCOA and BBOA showed distinct polycyclic aromatic hydrocarbons (PAHs) spectral signatures, indicating that PAHs in winter were mainly from coal combustion (66 %) and biomass burning emissions (18 %). BBOA was highly correlated with levoglucosan, a tracer compound for biomass burning (r2 = 0.93), and made a considerable contribution to OA in winter (9 %). An aqueous-phase-processed SOA (aq-OOA) that was strongly correlated with particle liquid water content, sulfate and S-containing ions (e.g. CH2SO2+) was identified. On average aq-OOA contributed 12 % to the total OA and played a dominant role in increasing oxidation degrees of OA at high RH levels (> 50 %). Our results illustrate that aqueous-phase processing can enhance SOA production and oxidation states of OA as well in winter. Further episode analyses highlighted the significant impacts of meteorological parameters on aerosol composition, size distributions, oxidation states of OA and evolutionary processes of secondary aerosols.


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