scholarly journals Persistent residential burning-related primary organic particles during wintertime hazes in North China: insights into their aging and optical changes

Author(s):  
Lei Liu ◽  
Jian Zhang ◽  
Weijun Li

<p>Primary organic aerosol (POA) is a major component of PM<sub>2.5</sub> in winter polluted air in the North China Plain (NCP), but our understanding on the atmospheric aging process of POA particles and the resulting influences on their optical properties is limited. As part of the Atmospheric Pollution and Human Health in a Chinese Megacity (APHH-Beijing) programme, we collected airborne particles at an urban site (Beijing) and an upwind rural site (Gucheng, Hebei province) in the NCP during 13–27 Nov. 2016 for microscopic analyses. We confirmed that large amounts of light-absorbing spherical POA (i.e., tarball) and irregular POA particles with high viscosity were emitted from the domestic coal and biomass burning at the rural site and were further transported to the urban site during regional wintertime hazes. During the heavily polluted period (PM<sub>2.5</sub> > 200 μg m<sup>−3</sup>), more than 60% of these burning-related POA particles were thickly coated with secondary inorganic aerosols (named as core–shell POA–SIA particle) through the aging process, suggesting that POA particles can provide surfaces for the heterogeneous reactions of SO<sub>2</sub> and NO<sub>x</sub>. As a result, their average particle-to-core diameter ratios at the rural and urban sites in the heavily polluted period increased to 1.60 and 1.67, respectively. Interestingly, we found that the aging process did not change the morphology and sizes of POA cores, indicating that these POA particles are quite inert in the atmosphere and can be transported long distances. Using Mie theory we estimated that the absorption capacity of POA particles was enhanced by ~1.39 times in the heavily polluted period at the rural and urban sites due to the “lensing effect” of secondary inorganic coatings. We highlight that the “lensing effect” on burning-related POA particles should be considered in radiative forcing models and the governments should continue to promote clean energy in rural areas to effectively reduce primary emissions.</p>

2020 ◽  
Author(s):  
Lei Liu ◽  
Jian Zhang ◽  
Yinxiao Zhang ◽  
Yuanyuan Wang ◽  
Liang Xu ◽  
...  

Abstract. Primary organic aerosol (POA) is a major component of PM2.5 in the winter polluted air in the North China Plain (NCP), but our understanding on the atmospheric aging process of POA particles and the resulting influences on their optical properties is limited. As part of the Atmospheric Pollution and Human Health in a Chinese Megacity (APHH-Beijing) programme, we collected airborne particles at an urban site (Beijing) and an upwind rural site (Gucheng, Hebei province) in the NCP during 13–27 November 2016 for microscopic analyses. We confirmed that a distinct group of spherical or irregular POA particles with high viscosity, defined as primary organic tar (POT) particles, was emitted from the domestic coal and biomass burning at the rural site and was further transported to the urban site during the regional wintertime hazes. During the heavily polluted period (PM2.5 > 200 μg m−3), more than 60 % of the POT particles were thickly coated with secondary inorganic aerosols (named as core–shell POT-SIA particle) through the aging process, suggesting that POT particles can provide surfaces for the heterogeneous reactions of SO2 and NOx. As a result, their average particle-to-core ratios at the rural and urban sites in the heavily polluted period increased to 1.60 and 1.67, respectively. Interestingly, we found that the aging process did not change the morphology and sizes of the POT cores, indicating that POT particles are quite inert in the atmosphere and can be transported long distances. We using the Mie theory estimated that the light absorption of individual POT particles was enhanced by ~ 1.39 times in the heavily polluted period at the rural and urban sites due to the lensing effect of secondary inorganic coatings. We highlight that the lensing effect on POT particles should be considered in radiative forcing models and the governments should continue to promote clean energy in rural areas to effectively reduce primary emissions.


2021 ◽  
Vol 21 (3) ◽  
pp. 2251-2265
Author(s):  
Lei Liu ◽  
Jian Zhang ◽  
Yinxiao Zhang ◽  
Yuanyuan Wang ◽  
Liang Xu ◽  
...  

Abstract. Primary organic aerosols (POAs) are a major component of PM2.5 in winter polluted air in the North China Plain (NCP), but our understanding of the atmospheric aging processes of POA particles and the resulting influences on their optical properties is limited. As part of the Atmospheric Pollution and Human Health in a Chinese Megacity (APHH-Beijing) program, we collected airborne particles at an urban site (Beijing) and an upwind rural site (Gucheng, Hebei province) in the NCP during 13–27 November 2016 for microscopic analyses. We confirmed that large numbers of light-absorbing spherical POA (i.e., tarball) and irregular POA particles with high viscosity were emitted from domestic coal and biomass burning at the rural site and were further transported to the urban site during regional wintertime hazes. During the heavily polluted period (PM2.5 > 200 µg m−3), more than 60 % of these burning-related POA particles were thickly coated with secondary inorganic aerosols (named as core–shell POA–SIA particles) through the aging process, suggesting that POA particles can provide surfaces for the heterogeneous reactions of SO2 and NOx. As a result, during the heavily polluted period, their average particle-to-core diameter ratios at the rural and urban sites increased to 1.60 and 1.67, respectively. Interestingly, we found that the aging process did not change the morphology and sizes of POA cores, indicating that the burning-related POA particles are quite inert in the atmosphere and can be transported over long distances. Using Mie theory we estimated that the absorption capacity of these POA particles was enhanced by ∼ 1.39 times in the heavily polluted period at the rural and urban sites due to the “lensing effect” of secondary inorganic coatings. We highlight that the lensing effect on burning-related POA particles should be considered in radiative forcing models and authorities should continue to promote clean energy in rural areas to effectively reduce primary emissions.


2016 ◽  
Vol 16 (2) ◽  
pp. 1139-1160 ◽  
Author(s):  
L. Xu ◽  
L. R. Williams ◽  
D. E. Young ◽  
J. D. Allan ◽  
H. Coe ◽  
...  

Abstract. The composition of PM1 (particulate matter with diameter less than 1 µm) in the greater London area was characterized during the Clean Air for London (ClearfLo) project in winter 2012. Two high-resolution time-of-flight aerosol mass spectrometers (HR-ToF-AMS) were deployed at a rural site (Detling, Kent) and an urban site (North Kensington, London). The simultaneous and high-temporal resolution measurements at the two sites provide a unique opportunity to investigate the spatial distribution of PM1. We find that the organic aerosol (OA) concentration is comparable between the rural and urban sites, but the contribution from different sources is distinctly different between the two sites. The concentration of solid fuel OA at the urban site is about twice as high as at the rural site, due to elevated domestic heating in the urban area. While the concentrations of oxygenated OA (OOA) are well-correlated between the two sites, the OOA concentration at the rural site is almost twice that of the urban site. At the rural site, more than 70 % of the carbon in OOA is estimated to be non-fossil, which suggests that OOA is likely related to aged biomass burning considering the small amount of biogenic SOA in winter. Thus, it is possible that the biomass burning OA contributes a larger fraction of ambient OA in wintertime than what previous field studies have suggested. A suite of instruments was deployed downstream of a thermal denuder (TD) to investigate the volatility of PM1 species at the rural Detling site. After heating at 250 °C in the TD, 40 % of the residual mass is OA, indicating the presence of non-volatile organics in the aerosol. Although the OA associated with refractory black carbon (rBC; measured by a soot-particle aerosol mass spectrometer) only accounts for < 10 % of the total OA (measured by a HR-ToF-AMS) at 250 °C, the two measurements are well-correlated, suggesting that the non-volatile organics have similar sources or have undergone similar chemical processing as rBC in the atmosphere. Although the atomic O : C ratio of OOA is substantially larger than that of solid fuel OA and hydrocarbon-like OA, these three factors have similar volatility, which is inferred from the change in mass concentration after heating at 120 °C. Finally, we discuss the relationship between the mass fraction remaining (MFR) of OA after heating in the TD and atomic O : C of OA and find that particles with a wide range of O : C could have similar MFR after heating. This analysis emphasizes the importance of understanding the distribution of volatility and O : C in bulk OA.


2013 ◽  
Vol 13 (11) ◽  
pp. 29685-29720 ◽  
Author(s):  
H. Che ◽  
X. Xia ◽  
J. Zhu ◽  
Z. Li ◽  
O. Dubovic ◽  
...  

Abstract. In January 2013, North China Plain experienced several serious haze events. Cimel sunphotometer measurements at seven sites over rural, suburban and urban regions of North China Plain from 1 to 30 January 2013 were used to further our understanding of spatial-temporal variation of aerosol optical parameters and aerosol radiative forcing (ARF). It was found that Aerosol Optical Depth at 500 nm (AOD500 nm) during non-pollution periods at all stations was lower than 0.30 and increased significantly to greater than 1.00 as pollution events developed. The Angstrom exponent (Alpha) was larger than 0.80 for all stations most of the time. AOD500 nm averages increased from north to south during both polluted and non-polluted periods on the three urban sites in Beijing. The fine mode AOD during pollution periods is about a factor of 2.5 times larger than that during the non-pollution period at urban sites but a factor of 5.0 at suburban and rural sites. The fine mode fraction of AOD675 nm was higher than 80% for all sites during January 2013. The absorption AOD675 nm at rural sites was only about 0.01 during pollution periods, while ~0.03–0.07 and 0.01–0.03 during pollution and non-pollution periods at other sites, respectively. Single scattering albedo varied between 0.87 and 0.95 during January 2013 over North China Plain. The size distribution showed an obvious tri-peak pattern during the most serious period. The fine mode effective radius in the pollution period was about 0.01–0.08 μm larger than during non-pollution periods, while the coarse mode radius in pollution periods was about 0.06–0.38 μm less than that during non-pollution periods. The total, fine and coarse mode particle volumes varied by about 0.06–0.34 μm3, 0.03–0.23 μm3, and 0.03–0.10 μm3, respectively, throughout January 2013. During the most intense period (1–16 January), aerosol radiative forcing (ARF) at the surface exceeded −50 W m−2, −180 W m−2, and −200 W m−2 at rural, suburban, and urban sites, respectively. The ARF readings at the top of the atmosphere were approximately −30 W m−2 in rural and −40–60 W m−2 in urban areas. Positive ARF at the top of the atmosphere at the Huimin suburban site was found to be different from others as a result of the high surface albedo due to snow cover.


2019 ◽  
Vol 19 (20) ◽  
pp. 12857-12874 ◽  
Author(s):  
Renmin Yuan ◽  
Xiaoye Zhang ◽  
Hao Liu ◽  
Yu Gui ◽  
Bohao Shao ◽  
...  

Abstract. Due to excessive anthropogenic emissions, heavy aerosol pollution episodes (HPEs) often occur during winter in the Beijing–Tianjin–Hebei (BTH) area of the North China Plain. Extensive observational studies have been carried out to understand the causes of HPEs; however, few measurements of vertical aerosol fluxes exist, despite them being the key to understanding vertical aerosol mixing, specifically during weak turbulence stages in HPEs. In the winter of 2016 and the spring of 2017 aerosol vertical mass fluxes were measured by combining large aperture scintillometer (LAS) observations, surface PM2.5 and PM10 mass concentrations, and meteorological observations, including temperature, relative humidity (RH), and visibility, at a rural site in Gucheng (GC), Hebei Province, and an urban site at the Chinese Academy of Meteorological Sciences (CAMS) in Beijing located 100 km to the northeast. These are based on the light propagation theory and surface-layer similarity theory. The near-ground aerosol mass flux was generally lower in winter than in spring and weaker in rural GC than in urban Beijing. This finding provides direct observational evidence for a weakened turbulence intensity and low vertical aerosol fluxes in winter and polluted areas such as GC. The HPEs included a transport stage (TS), an accumulative stage (AS), and a removal stage (RS). During the HPEs from 25 to 31 January 2017, in Beijing, the mean mass flux decreased by 51 % from 0.0049 mg m−2 s−1 in RSs to 0.0024 mg m−2 s−1 in the TSs. During the ASs, the mean mass flux decreased further to 0.00087 mg m−2 s−1, accounting for approximately one-third of the flux in the TSs. A similar reduction from the TSs to ASs was observed in the HPE from 16 to 22 December 2016 in GC. It can be seen that from the TS to the AS, the aerosol vertical turbulent flux decreased, but the aerosol particle concentration within the surface layer increased, and it is inferred that in addition to the contribution of regional transport from upwind areas during the TS, suppression of vertical turbulence mixing confining aerosols to a shallow boundary layer increased accumulation.


2020 ◽  
Author(s):  
Weiqi Xu ◽  
Chun Chen ◽  
Yanmei Qiu ◽  
Ying Li ◽  
Zhiqiang Zhang ◽  
...  

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.


2020 ◽  
Author(s):  
Renmin Yuan

&lt;p&gt;Due to excessive anthropogenic emissions, heavy aerosol pollution episodes (HPEs) often occur during winter in the Beijing-Tianjin-Hebei (BTH) area of the North China Plain. Extensive observational studies have been carried out to understand the causes of HPEs; however, few measurements of vertical aerosol fluxes exist, despite them being the key to understanding vertical aerosol mixing, specifically during weak turbulence stages in HPEs. In the winter of 2016 and the spring of 2017 aerosol vertical mass fluxes were measured by combining large aperture scintillometer (LAS) observations, surface PM&lt;sub&gt;2.5&lt;/sub&gt; and PM&lt;sub&gt;10&lt;/sub&gt; mass concentrations, and meteorological observations, including temperature, relative humidity (RH), and visibility, at a rural site in Gucheng (GC), Hebei Province, and an urban site at the Chinese Academy of Meteorological Sciences (CAMS) in Beijing located 100 km to the northeast. These are based on the light propagation theory and surface-layer similarity theory. The near-ground aerosol mass flux was generally lower in winter than in spring and weaker in rural GC than in urban Beijing. This finding provides direct observational evidence for a weakened turbulence intensity and low vertical aerosol fluxes in winter and polluted areas such as GC. The HPEs included a transport stage (TS), an accumulative stage (AS), and a removal stage (RS). During the HPEs from 25 January 2017 to January 31, 2017, in Beijing, the mean mass flux decreased by 51% from 0.0049 mg m&lt;sup&gt;-2&lt;/sup&gt;s&lt;sup&gt;-1&lt;/sup&gt; in RSs to 0.0024 mg m&lt;sup&gt;-2&lt;/sup&gt;s&lt;sup&gt;-1&lt;/sup&gt; in the TSs. During the ASs, the mean mass flux decreased further to 0.00087 mg m&lt;sup&gt;-2&lt;/sup&gt;s&lt;sup&gt;-1&lt;/sup&gt;, accounting for approximately 1/3 of the flux in the TSs. A similar reduction from the TSs to ASs was observed in the HPE from 16 December 2016 to 22 December 2016 in GC. It can be seen that from the TS to the AS, the aerosol vertical turbulent flux decreased, but the aerosol particle concentration within surface layer increased, and it is inferred that in addition to the contribution of regional transport from upwind areas during the TS, suppression of vertical turbulence mixing confining aerosols to a shallow boundary layer increased accumulation.&lt;/p&gt;


2019 ◽  
Author(s):  
Renmin Yuan ◽  
Xiaoye Zhang ◽  
Hao Liu ◽  
Yu Gui ◽  
Bohao Shao ◽  
...  

Abstract. Due to excessive anthropogenic emissions, heavy aerosol pollution episodes (HPEs) often occur during winter in the Beijing-Tianjin-Hebei (BTH) area of the North China Plain. Extensive observational studies have been carried out to understand the causes of HPEs; however, few measurements of aerosol vertical fluxes exist, despite them being the key to understanding vertical aerosol mixing, specifically during weak turbulence stages in HPEs. In the winter of 2016 and the spring of 2017, based on the light propagation theory and surface-layer similarity theory, aerosol vertical mass fluxes were measured by combining large aperture scintillometer (LAS) observations, surface PM2.5 and PM10 mass concentrations, and meteorological observations, including temperature, relative humidity (RH), and visibility, at a rural site in Gucheng (GC), Hebei Province, and an urban site at the Chinese Academy of Meteorological Sciences (CAMS) in Beijing located 100 km to the northeast. The near-ground aerosol mass flux was generally lower in winter than in spring and weaker in rural GC than in urban Beijing. This finding provides direct observational evidence from the perspective of vertical aerosol fluxes for a weakened turbulence intensity in winter and in polluted areas such as GC. The HPEs included a transport stage (TS), an accumulative stage (AS), and a removal stage (RS). During the HPEs from January 25, 2017 to January 31, 2017, in Beijing, the mean mass flux decreased by 51 % from 0.0049 mg m−2 s−1 in RSs to 0.0024 mg m−2 s−1 in the TSs. During the ASs, the mean mass flux decreased further to 0.00087 mg m−2 s−1, accounting for approximately 1/3 of the flux in the TSs. A similar reduction from the TSs to ASs was observed in the HPE from December 16, 2016 to December 22, 2016 in GC. The weakened mass flux indicates that the already weak turbulence would be further weakened by aerosol pollution to a certain extent, which would further facilitate aerosol accumulation.


2021 ◽  
Vol 21 (7) ◽  
pp. 5463-5476
Author(s):  
Weiqi Xu ◽  
Chun Chen ◽  
Yanmei Qiu ◽  
Ying Li ◽  
Zhiqiang Zhang ◽  
...  

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.


2021 ◽  
Author(s):  
Jackie Kleynhans ◽  
Stefano Tempia ◽  
Nicole Wolter ◽  
Anne von Gottberg ◽  
Jinal N. Bhiman ◽  
...  

Background SARS-CoV-2 infections may be underestimated due to limited testing access, particularly in sub-Saharan Africa. South Africa experienced two SARS-CoV-2 waves, the second associated with emergence of variant 501Y.V2. In this study, we report longitudinal SARS-CoV-2 seroprevalence in cohorts in two communities in South Africa. Methods We measured SARS-CoV-2 seroprevalence two monthly in randomly selected household cohorts in a rural and an urban community (July 2020-March 2021). We compared seroprevalence to laboratory-confirmed infections, hospitalisations and deaths reported in the districts to calculate infection-case (ICR), infection-hospitalisation (IHR) and infection-fatality ratio (IFR) in the two waves of infection. Findings Seroprevalence after the second wave ranged from 18% (95%CrI 10-26%) and 28% (95%CrI 17-41%) in children <5 years to 37% (95%CrI 28-47%) in adults aged 19-34 years and 59% (95%CrI 49-68%) in adults aged 35-59 years in the rural and urban community respectively. Individuals infected in the second wave were more likely to be from the rural site (aOR 4.7, 95%CI 2.9-7.6), and 5-12 years (aOR 2.1, 95%CI 1.1-4.2) or ≥60 years (aOR 2.8, 95%CI 1.1-7.0), compared to 35-59 years. The in-hospital IFR in the urban site was significantly increased in the second wave 0.36% (95%CI 0.28-0.57%) compared to the first wave 0.17% (95%CI 0.15-0.20%). ICR ranged from 3.69% (95%CI 2.59-6.40%) in second wave at urban community, to 5.55% (95%CI 3.40-11.23%) in first wave in rural community. Interpretation The second wave was associated with a shift in age distribution of cases from individuals aged to 35-59 to individuals at the extremes of age, higher attack rates in the rural community and a higher IFR in the urban community. Approximately 95% of SARS-CoV-2 infections in these two communities were not reported to the national surveillance system, which has implications for contact tracing and infection containment. Funding US Centers for Disease Control and Prevention


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