scholarly journals Physical and chemical constraints on transformation and mass-increase of fine aerosols in northeast Asia

2021 ◽  
Author(s):  
Saehee Lim ◽  
Meehye Lee ◽  
Paolo Laj ◽  
Sang-Woo Kim ◽  
Kang-Ho Ahn ◽  
...  

Abstract. Over the past few decades, northeast Asia has suffered from the extreme levels of PM2.5 (particulate matter with an aerodynamic diameter smaller than 2.5 μm). Despite extensive efforts and the scientific advances in understanding PM2.5 pollution, the fundamental mechanisms responsible for the occurrence of high PM2.5 concentrations have not been comprehensively understood. In this study, we investigated the physical and chemical drivers for the formation and transformation of atmospheric particles using a four-year dataset of nanoparticle number size distributions, PM2.5 chemical composition, gaseous precursors, and meteorological variables in northeast Asia outflows. The empirical orthogonal function (EOF) analyses of size-separated particle numbers extracted two modes representing a burst of nanoparticles (EOF1) and an increase in PM2.5 mass (EOF2) associated with persistent anticyclone and synoptic-scale stagnation, respectively. The vertical structure of the particles demonstrated that the synoptic conditions also affected the daily evolution of boundary layer, promoting either the formation of nanoparticles through deep mixing or conversion into accumulation-mode particles in shallow mixed layers. In the haze-development episode equivalent to EOF2 during the KORUS-AQ (KORea-US Air Quality) campaign, the PM2.5 mass reached 63 μg m−3 with the highest contribution from inorganic constituents, which was accompanied by a thick coating of refractory black carbon (rBC) that linearly increased with condensation-mode particles. This observational evidence suggests that the thick coating of rBC resulted from an active conversion of condensable gases into particle-phase on the BC surface, thereby increasing the mass of the accumulation-mode aerosol. Consequently, this result complies with the strategy to reduce black carbon as a way to effectively mitigate haze pollution as well as climate change in northeast Asia.

Atmosphere ◽  
2021 ◽  
Vol 12 (7) ◽  
pp. 870
Author(s):  
Fangfang Wang ◽  
Jialuo Xu ◽  
Yinzhi Huang ◽  
Guangli Xiu

Ozone and PM2.5 (all particulate matter with diameter of 2.5 µm or smaller) are currently two disturbing environmental issues in most cities of China. Black carbon (BC), mainly from incomplete combustion, is one of the most important components of PM2.5 because it can absorb light and contribute to haze pollution and global warming. Meanwhile, volatile organic compounds (VOCs) have become a major air pollutant due to their association with haze, ozone (O3), global warming and human health by direct or indirect processes. In this study, one year-long observation campaign of BC, VOCs and other conventional air pollutants was conducted in the Northern Region of the Hangzhou Bay (NRHB) in Shanghai, China. The results indicated that higher concentration of BC mainly occurred in the autumn and winter, especially in December. In December, higher BC concentrations were found when the air mass came from northwest where there is an important local freeway, or southwest where some adjacent southwest chemical industrial parks are located. Different from the characteristics of BC in urban areas reported by previous studies, the diurnal variation of BC exhibited three peaks, two of which coincided with the morning and evening rush hours which are related to the heavy diesel traffic from a nearby freeway, and the third peak was often found late at night, around 2 am, which might be associated with abnormal emissions from an industrial park or marine traffic in the ocean waterway. BC had weakly negative correlation with O3 and NO, and a strongly positive correlation with PM2.5, SO2, NO2 and NOx, which implies that some incomplete combustion sources might occur in the nearby regions. With regard to VOCs, BC had a strong positive correlation with alkane, alkenes, alkynes, aromatic and non-sulfur VOCs, particularly with aromatic organic matter. Unlike the stronger correlation with aromatics in the morning rush hours, a stronger correlation between BC and alkenes and alkynes during the evening rush hour was observed. The relationships between BC and VOCs, particularly with some specific VOCs species related to the neighboring chemical industrial park, demonstrated that the contribution of the surrounding chemical industrial parks to BC should not be neglected.


2017 ◽  
Author(s):  
Zilin Wang ◽  
Xin Huang ◽  
Aijun Ding

Abstract. Black carbon (BC) has been identified to play a critical role in aerosol-planet boundary layer (PBL) interaction and further deterioration of near-surface air pollution in megacities, which has been named as its dome effect. However, the impacts of key factors that influence this effect, such as the vertical distribution and aging processes of BC, and also the underlying land surface, have not been quantitatively explored yet. Here, based on available in-situ measurements of meteorology and atmospheric aerosols together with the meteorology-chemistry online coupled model, WRF-Chem, we conduct a set of parallel simulations to quantify the roles of these factors in influencing the BC's dome effect and surface haze pollution, and discuss the main implications of the results to air pollution mitigation in China. We found that the impact of BC on PBL is very sensitive to the altitude of aerosol layer. The upper level BC, especially those near the capping inversion, is more essential in suppressing the PBL height and weakening the turbulence mixing. The dome effect of BC tends to be significantly intensified as BC aerosol mixed with scattering aerosols during winter haze events, resulting in a decrease of PBL height by more than 25 %. In addition, the dome effect is more substantial (up to 15 %) in rural areas than that in the urban areas with the same BC loading, indicating an unexpected regional impact of such kind of effect to air quality in countryside. This study suggests that China's regional air pollution would greatly benefit from BC emission reductions, especially those from the elevated sources from the chimneys and also the domestic combustions in rural areas, through weakening the aerosol-boundary layer interactions that triggered by BC.


2018 ◽  
Author(s):  
Jinhui Gao ◽  
Bin Zhu ◽  
Hui Xiao ◽  
Hanqing Kang ◽  
Chen Pan

Abstract. As an important solar-radiation absorbing aerosol, the effect of black carbon (BC) on surface ozone, by influencing photolysis rate, has been widely discussed by offline model studies. However, BC-boundary layer (BL) interactions also influence surface ozone. Using the online model simulations and processes analysis, we demonstrate the significant impact of BC-BL interaction on surface ozone. The absorbing effect of BC heats the air above the BL and suppresses BL development, which eventually leads to changes in the contributions of ozone through chemical and physical processes (photochemistry, vertical mixing, and advection). Different from previous offline model studies, BL suppression leads large amounts of ozone precursors being confined below the BL which offsetting the influence from the reduction of photolysis rate, thus enhancing ozone photochemical formation before noon. Furthermore, the changes in physical process show a more significant influence on surface ozone. The weakened turbulence entrains much less ozone from the overlying ozone-rich air down to surface. As a result, the net contribution of ozone from physical and chemical processes leads to surface ozone reduction before noon. The maximum reduction reaches to 16.4 ppb at 12:00. In the afternoon, the changes in chemical process are small which influence inconspicuously to surface ozone. However, physical process still influences the surface ozone significantly. Due to the delayed development of the BL, less vertically mixed BL continues to show an obvious ozone gradient near the top of the BL. Therefore, more ozone aloft can be entrained down to the surface, offsetting the surface ozone reduction. Comparing all the changes in the contributions of processes, the change in the contribution of vertical mixing plays a more important role in impacting surface ozone. Our results show the great impacts of BC-BL interactions on surface ozone. And more attention should be paid on the mechanism of aerosol-BL interactions when we deal with the ozone pollution control in China.


2016 ◽  
Author(s):  
Osamu Uchino ◽  
Tetsu Sakai ◽  
Toshiharu Izumi ◽  
Tomohiro Nagai ◽  
Isamu Morino ◽  
...  

Abstract. To validate products of the Greenhouse gases Observing SATellite (GOSAT), we observed vertical profiles of aerosols, thin cirrus clouds, and tropospheric ozone with a mobile lidar system that consisted of a two-wavelength (532 and 1064 nm) polarization lidar and a tropospheric ozone Differential Absorption Lidar (DIAL). We used these lidars to make continuous measurements over Saga (33.24° N, 130.29° E) during 20–31 March 2015. High ozone and high aerosol concentrations were observed almost simultaneously in the altitude range 0.5–1.5 km from 03:00 to 20:00 Japan Standard Time on 22 March 2015. The maximum ozone volume mixing ratio was ~ 110 ppbv. The maxima of the aerosol extinction coefficient and optical depth at 532 nm were 1.2 km−1 and 2.1, respectively. Backward trajectory analysis indicated that an air mass with high ozone and aerosol concentrations could have been transported from Northeast Asia. Based on the lidar data and the ground-based in-situ measurements at Saga, this air mass could have been transported to the surface by vertical mixing when the planetary boundary layer developed in the daytime. This plume, which contained high ozone and aerosol pollutant concentrations, impacted surface air quality substantially. After some modifications of its physical and chemical parameters, the Meteorological Research Institute Chemistry-Climate Model, version 2 (MRI-CCM2) approximately reproduced the high-ozone volume-mixing ratio. The Model of Aerosol Species IN the Global AtmospheRe (MASINGAR) mk-2 successfully predicted high aerosol concentrations, but the predicted peak aerosol optical thickness was about one-third of the observed value.


2019 ◽  
Author(s):  
Qiuji Ding ◽  
Jianning Sun ◽  
Xin Huang ◽  
Aijun Ding ◽  
Jun Zou ◽  
...  

Abstract. Aerosols can not only participate in fog formation by acting as condensation nuclei of droplets but also modify the meteorological conditions such as air temperature and moisture, planetary boundary layer height (PBLH) and regional circulation during haze event. The impact of aerosols on fog formation, yet to be revealed, can be critical in understanding and predicting of fog-haze event. In this study, we used the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) to investigate a heavy fog event during a multiday intense haze pollution episode in early December 2013 in the Yangtze River Delta (YRD) region in eastern China. Using the WRF-Chem model, we conducted four parallel numerical experiments to evaluate the roles of aerosol-radiation interaction (ARI), aerosol-cloud interaction (ACI), black carbon (BC) and none BC (non-BC) aerosols in the formation and maintenance of the heavy fog event. Only when the aerosols' feedback processes are considered can the model well capture the haze pollution and the fog event. We find that the ARI dominates this fog-haze episode while the effects of ACI are negligible. Our analyses shows that BC plays a more important role in fog formation than non-BC aerosols. The dome effect of BC leads to an increase of air moisture over the sea by reducing PBLH and weakening vertical mixing, thereby confining more water vapor in the near-surface layer. The strengthened daytime onshore flow by a cyclonic wind anomaly, induced by contrast temperature perturbation over land and sea, transports moister air to the YRD region, where the suppressed PBLH and weakened daytime vertical mixing maintain the high moisture level. Then the heave fog forms due to the surface cooling at night in this region. This study highlights the importance of anthropogenic emissions in the formation of advection-radiation fog in the polluted coastal areas.


2016 ◽  
Vol 16 (7) ◽  
pp. 4693-4706 ◽  
Author(s):  
Megan D. Willis ◽  
Robert M. Healy ◽  
Nicole Riemer ◽  
Matthew West ◽  
Jon M. Wang ◽  
...  

Abstract. The climatic impacts of black carbon (BC) aerosol, an important absorber of solar radiation in the atmosphere, remain poorly constrained and are intimately related to its particle-scale physical and chemical properties. Using particle-resolved modelling informed by quantitative measurements from a soot-particle aerosol mass spectrometer, we confirm that the mixing state (the distribution of co-emitted aerosol amongst fresh BC-containing particles) at the time of emission significantly affects BC-aerosol optical properties even after a day of atmospheric processing. Both single particle and ensemble aerosol mass spectrometry observations indicate that BC near the point of emission co-exists with hydrocarbon-like organic aerosol (HOA) in two distinct particle types: HOA-rich and BC-rich particles. The average mass fraction of black carbon in HOA-rich and BC-rich particle classes was  < 0.1 and 0.8, respectively. Notably, approximately 90 % of BC mass resides in BC-rich particles. This new measurement capability provides quantitative insight into the physical and chemical nature of BC-containing particles and is used to drive a particle-resolved aerosol box model. Significant differences in calculated single scattering albedo (an increase of 0.1) arise from accurate treatment of initial particle mixing state as compared to the assumption of uniform aerosol composition at the point of BC injection into the atmosphere.


2021 ◽  
Vol 21 (4) ◽  
pp. 3143-3162
Author(s):  
Yingying Yan ◽  
Yue Zhou ◽  
Shaofei Kong ◽  
Jintai Lin ◽  
Jian Wu ◽  
...  

Abstract. Currently, mitigating severe particle pollution in autumn and winter is the key to further improving the air quality of China. The source contributions and transboundary transport of fine particles (PM2.5) in pollution episodes are closely related to large-scale or synoptic-scale atmospheric circulation. How to effectively reduce emissions to control haze pollution under different synoptic conditions is rarely reported. In this study, we classify the synoptic conditions over central China from 2013 to 2018 by using Lamb–Jenkinson method and the National Centers for Environmental Prediction/National Center for Atmospheric Research (NCEP/NCAR) Final (FNL) operational global analysis data. The effectiveness of emission control to reduce PM2.5 pollution during winter haze episodes under potential synoptic controls is simulated by GEOS-Chem model. Among the 10 identified synoptic patterns, four types account for 87 % of the total pollution days. Two typical synoptic modes are characterized by low surface wind speed and stable weather conditions or high relative humidity (A or C type) over central China due to a high-pressure system or a southwest trough and low-pressure system, blocking pollutants dispersion. Sensitivity simulations show that these two heavy pollution processes are mainly contributed by local emission sources with ∼82 % for A type and ∼85 % for C type, respectively. The other two patterns lead to pollution of transport characteristics affected by northerly or southerly winds (NW or SW type), carrying air pollution from northern or southern China to central China. The contribution of pollution transmission from northern and southern China is 36.9 % and 7.6 %, respectively of PM2.5, and local emission sources contribute 41 % and 69 %, respectively. We also estimate the effectiveness of emission reduction in these four typical severe pollution synoptic processes. By only reducing SO2 and NOx emission and not controlling NH3, the enhanced nitrate counteracts the effect of sulfate reduction on PM2.5 mitigation, with a less than 4 % decrease in PM2.5. In addition, to effectively mitigate haze pollution of NW- and SW-type synoptic-controlled episodes, local emission control actions should be in coordination with regional collaborative actions.


Sign in / Sign up

Export Citation Format

Share Document