Aerosol Composition in Relation to Air Mass Movements in North China

Author(s):  
JOHN W. WINCHESTER ◽  
MICHAEL DARZI ◽  
ALISTAIR C. D. LESLIE ◽  
WANG MINGXING ◽  
REN LIXIN ◽  
...  
2020 ◽  
Author(s):  
Jiayun Li ◽  
Liming Cao ◽  
Wenkang Gao ◽  
Lingyan He ◽  
Yingchao Yan ◽  
...  

Abstract. For the first time in the North China Plain (NCP), we investigated the seasonal variations of submicron particles (NR-PM1) and its chemical composition at a background mountain station using Aerodyne high-resolution time-of-flight aerosol mass spectrometry (HR-ToF-AMS). The averaged NR-PM1 were highest in autumn (15.1 μg m−3) and lowest in summer (12.4 μg m−3), with the abundance of more nitrate in spring (34 %), winter (31 %), and autumn (34 %), and elevated organics (40 %) and sulfate (38 %) proportion in summer. The submicron particles were almost neutralized by excess ammonium in all four seasons except summer, when the aerosol particles appeared to be slightly acidic. The size distribution of all PM1 species showed a consistent accumulation mode peaked at approximately 600–800 nm (dva), indicating the highly aged and internally mixed nature of the background aerosols, which further supported by the source appointment using multilinear engine (ME-2) and significant contributions of aged secondary organic aerosol (SOA) in organic aerosol (OA) were resolved in all seasons (> 77 %), especially in summer (95 %). The oxidation degree and evolution process of OAs in the four seasons were further investigated, and enhanced carbon oxidation state (−0.45–0.10), O / C (0.54–0.75) and OM / OC (1.86–2.13) ratios compared with urban studies were observed, with the highest oxidation degree of which appeared in summer, likely due to the relatively stronger photochemical processing which dominated the processes of both less oxidized OA (LO-OOA) and more oxidized OA (MO-OOA) formations. Aqueous-phase processing also contributed to the SOA formation but prevailed in autumn and winter and the role of which to MO-OOA and LO-OOA also varied in different seasons. In addition, compared with the urban atmosphere, LO-OOA formation in the background atmosphere exhibited more regional characteristics, as photochemical and aqueous-phase processing enhanced during the transport in summer and autumn, respectively. Furthermore, the backward trajectories analysis showed that higher submicron particles were associated with air mass for short distance transported from the southern regions in four seasons, while the long-range transport from Inner Mongolia (west and north regions) also contributed to the summer particle pollutions in the background areas of NCP. Our results illustrate the background particles in NCP are influenced significantly by aging processing and transport, and the more neutralized state of submicron particles with the abundance of nitrate compared with those in the background atmosphere in southern and western China, highlighting the regional reductions in emissions of nitrogen oxide and ammonia are critical for remedying the increased occurrence of nitrate-dominated haze event in the NCP.


2018 ◽  
Vol 18 (3) ◽  
pp. 1535-1554 ◽  
Author(s):  
Fengcheng Wu ◽  
Pinhua Xie ◽  
Ang Li ◽  
Fusheng Mou ◽  
Hao Chen ◽  
...  

Abstract. Recently, Chinese cities have suffered severe events of haze air pollution, particularly in the North China Plain (NCP). Investigating the temporal and spatial distribution of pollutants, emissions, and pollution transport is necessary to better understand the effect of various sources on air quality. We report on mobile differential optical absorption spectroscopy (mobile DOAS) observations of precursors SO2 and NO2 vertical columns in the NCP in the summer of 2013 (from 11 June to 7 July) in this study. The different temporal and spatial distributions of SO2 and NO2 vertical column density (VCD) over this area are characterized under various wind fields. The results show that transport from the southern NCP strongly affects air quality in Beijing, and the transport route, particularly SO2 transport on the route of Shijiazhuang–Baoding–Beijing, is identified. In addition, the major contributors to SO2 along the route of Shijiazhuang–Baoding–Beijing are elevated sources compared to low area sources for the route of Dezhou–Cangzhou–Tianjin–Beijing; this is found using the interrelated analysis between in situ and mobile DOAS observations during the measurement periods. Furthermore, the discussions on hot spots near the city of JiNan show that average observed width of polluted air mass is 11.83 and 17.23 km associated with air mass diffusion, which is approximately 60 km away from emission sources based on geometrical estimation. Finally, a reasonable agreement exists between the Ozone Monitoring Instrument (OMI) and mobile DOAS observations, with a correlation coefficient (R2) of 0.65 for NO2 VCDs. Both datasets also have a similar spatial pattern. The fitted slope of 0.55 is significantly less than unity, which can reflect the contamination of local sources, and OMI observations are needed to improve the sensitivities to the near-surface emission sources through improvements of the retrieval algorithm or the resolution of satellites.


2012 ◽  
Vol 12 (13) ◽  
pp. 5963-5983 ◽  
Author(s):  
N. H. Robinson ◽  
J. D. Allan ◽  
J. A. Trembath ◽  
P. D. Rosenberg ◽  
G. Allen ◽  
...  

Abstract. Vertical profiles of aerosol chemical composition, number concentration and size were measured throughout the lower troposphere of Borneo, a large tropical island in the western Pacific Ocean. Aerosol composition, size and number concentration measurements (using an Aerodyne Aerosol Mass Spectrometer, Passive Cavity Aerosol Spectrometer Probe and Condensation Particle Counter, respectively) were made both upwind and downwind of Borneo, as well as over the island itself, on board the UK BAe-146 research aircraft as part of the OP3 project. Two meteorological regimes were identified – one dominated by isolated terrestrial convection (ITC) which peaked in the afternoon, and the other characterised by more regionally active mesoscale convective systems (MCS). Upwind profiles show aerosol to be confined to a shallow marine boundary layer below 930 ± 10 hPa (~760 m above sea level, a.s.l.). As this air mass advects over the island with the mean free troposphere synoptic flow during the ITC-dominated regime, it is convectively lofted above the terrestrial surface mixed layer to heights of between 945 ± 22 (~630 m a.s.l.) and 740 ± 44 hPa (~2740 m a.s.l.), consistent with a coupling between the synoptic steering level flow and island sea breeze circulations. Terrestrial aerosol was observed to be lofted into this higher layer through both moist convective uplift and transport through turbulent diurnal sea-breeze cells. At the peak of convective activity in the mid-afternoons, organic aerosol loadings in the lofted layer were observed to be substantially higher than in the morning (by a mean factor of three). This organic matter is dominated by secondary aerosol from processing of biogenic gas phase precursors. Aerosol number concentration profiles suggest formation of new particles aloft in the atmosphere. By the time the air mass reaches the west coast of the island, terrestrial aerosol is enhanced in the lofted layer. Such uplift of aerosol in Borneo is expected to increase aerosol lifetimes in the lower free troposphere downwind, as they are above the boundary layer and therefore less likely to be lost by wet or dry deposition. It is also likely to change the role they play in the semi-direct and direct aerosol effects. The long chain of islands extending from Malaysia to Australia may all similarly be expected to present an orographic barrier to low level mean flow. This would lead to significant transport of aerosol into the tropical free troposphere across the Western Pacific region.


2020 ◽  
Vol 20 (11) ◽  
pp. 6953-6971 ◽  
Author(s):  
Zainab Arub ◽  
Sahil Bhandari ◽  
Shahzad Gani ◽  
Joshua S. Apte ◽  
Lea Hildebrandt Ruiz ◽  
...  

Abstract. Delhi is a megacity subject to high local anthropogenic emissions and long-range transport of pollutants. This work presents for the first time time-resolved estimates of hygroscopicity parameter (κ) and cloud condensation nuclei (CCN), spanning for more than a year, derived from chemical composition and size distribution data. As a part of the Delhi Aerosol Supersite (DAS) campaign, the characterization of aerosol composition and size distribution was conducted from January 2017 to March 2018. Air masses originating from the Arabian Sea (AS), Bay of Bengal (BB), and southern Asia (SA) exhibited distinct characteristics of time-resolved sub-micron non-refractory PM1 (NRPM1) species, size distributions, and CCN number concentrations. The SA air mass had the highest NRPM1 loading with high chloride and organics, followed by the BB air mass, which was more contaminated than AS, with a higher organic fraction and nitrate. The primary sources were identified as biomass-burning, thermal power plant emissions, industrial emissions, and vehicular emissions. The average hygroscopicity parameter (κ), calculated by the mixing rule, was approximately 0.3 (varying between 0.13 and 0.77) for all the air masses (0.32±0.06 for AS, 0.31±0.06 for BB, and 0.32±0.10 for SA). The diurnal variations in κ were impacted by the chemical properties and thus source activities. The total, Aitken, and accumulation mode number concentrations were higher for SA, followed by BB and AS. The mean values of estimated CCN number concentration (NCCN; 3669–28926 cm−3) and the activated fraction (af; 0.19–0.87), for supersaturations varying from 0.1 % to 0.8 %, also showed the same trend, implying that these were highest in SA, followed by those in BB and then those in AS. The size turned out to be more important than chemical composition directly, and the NCCN was governed by either the Aitken or accumulation modes, depending upon the supersaturation (SS) and critical diameter (Dc). af was governed mainly by the geometric mean diameter (GMD), and such a high af (0.71±0.14 for the most dominant sub-branch of the SA air mass – R1 – at 0.4 % SS) has not been seen anywhere in the world for a continental site. The high af was a consequence of very low Dc (25–130 nm, for SS ranging from 0.1 % to 0.8 %) observed for Delhi. Indirectly, the chemical properties also impacted CCN and af by impacting the diurnal patterns of Aitken and accumulation modes, κ and Dc. The high-hygroscopic nature of aerosols, high NCCN, and high af can severely impact the precipitation patterns of the Indian monsoon in Delhi, impact the radiation budget, and have indirect effects and need to be investigated to quantify this impact.


2017 ◽  
Author(s):  
Fengcheng Wu ◽  
Pinhua Xie ◽  
Ang Li ◽  
Fusheng Mou ◽  
Hao Chen ◽  
...  

Abstract. Recently, Chinese cities have suffered severe events of haze air pollution, particularly in the North China Plain (NCP). Investigating the temporal and spatial distribution of pollutants, emissions, and pollution transport is necessary to better understand the effect of various sources on air quality. We report on mobile differential optical absorption spectroscopy (mobile DOAS) observations of precursors SO2 and NO2 vertical columns in NCP in summer of 2013 (from 11 June to 7 July) in this study. The different temporal and spatial distributions of SO2 and NO2 vertical column density (VCD) over this area are characterized under various wind fields. The results show that the transport from southern NCP strongly affects the air quality in Beijing, and the transport route, particularly SO2 transport of Shijiazhuang–Baoding–Beijing is identified. In addition, the major contributors to SO2 along the route of Shijiazhuang–Baoding–Beijing are elevated sources and low area sources for the route of Dezhou–Cangzhou–Tianjin–Beijing are found using the interrelated analysis between in situ and mobile DOAS observations during the measurement periods. Furthermore, the discussion of hot spot near Ji’nan City shows that the average observed width of polluted air mass is 11.83 km and 17.23 km associated with air mass diffusion, which is approximately 60 km away from emission sources based on geometrical estimation. Finally, a reasonable agreement exists between OMI and mobile DOAS observations with correlation coefficient (R2) of 0.65 for NO2 VCDs. Both datasets also have similar spatial pattern. The fitted slop of 0.55 is significantly less than unity can reflect the contamination of local sources and OMI observations need to improve the sensitivities to the near-surface emission sources through the improvements of retrieval algorithm or resolution of satellites.


1981 ◽  
Vol 15 (6) ◽  
pp. 933-937 ◽  
Author(s):  
John W. Winchester ◽  
Lü Weixiu ◽  
Ren Lixin ◽  
Wang Mingxing ◽  
Willy Maenhaut

2019 ◽  
Author(s):  
Zainab Arub ◽  
Sahil Bhandari ◽  
Shahzad Gani ◽  
Joshua S. Apte ◽  
Lea Hildebrandt Ruiz ◽  
...  

Abstract. This work presents for the first time long term and time-resolved estimates of hygroscopicty parameter (κ) and CCN for Delhi, a megacity that is subjected to high local anthropogenic emissions and long-range transport of pollutants. As a part of the Delhi Aerosol Supersite (DAS) campaign, characterisation of aerosol composition and size distribution were conducted from January 2017–March 2018. Air masses originating from the Arabian Sea (AS), Bay of Bengal (BB) and South Asia (SA) exhibited distinct characteristics of time-resolved sub-micron non-refractory PM1 (NRPM1) species, size distributions, and CCN number concentrations. SA air mass had the highest NRPM1 loading with high chloride and organics followed by BB air mass which was relatively more contaminated than AS with a higher organic fraction and nitrate. The primary sources were identified as biomass-burning, thermal power plant emissions, industrial and vehicular emissions. The average hygroscopicty parameter (κ), calculated by the mixing rule was ~ 0.3 (varying between 0.13 and 0.77) for all the air masses (0.32 ± 0.06 for AS, 0.31 ± 0.06 for BB and 0.32 ± 0.10 for SA). The diurnal variations of κ were impacted by the chemical properties and thus source activities. The total, Aitken, and Accumulation mode number concentrations were higher for SA, followed by BB and AS. The mean values of estimated CCN number concentration (NCCN, 3669–28 926 cm−3) and the activated fraction (af, 0.19–0.87) for supersaturations varying from 0.1–0.8 % also showed the same trend (SA > BB > AS). The size turned out to be more important than chemical composition directly, and the NCCN was governed by either the Aitken or Accumulation modes depending upon the supersaturation (SS) and critical diameter (Dc). The af was governed mainly by the Geometric Mean Diameter (GMD), and such a high af (0.71 ± 0.14 for the most dominant sub-branch of SA air mass (R1) at 0.4 % SS) has not been seen anywhere in the world. The high af was a consequence of very low Dc (25–130 nm for SS ranging from 0.1 %–0.8 %) observed for Delhi. Indirectly, the chemical properties also impacted CCN and af by impacting the diurnal patterns of Aitken and accumulation modes, κ and Dc. The high hygroscopic nature of aerosols, high NCCN and high af can severely impact the precipitation patterns of the Indian Monsoon in Delhi, the radiation budget and the indirect effect and need to be investigated to quantify the impacts.


2016 ◽  
Author(s):  
Justin H. Dingle ◽  
Kennedy Vu ◽  
Roya Bahreini ◽  
Eric C. Apel ◽  
Teresa L. Campos ◽  
...  

Abstract. Summertime aerosol optical extinction (βext) was measured in the Colorado Front Range and Denver Metropolitan Area as part of the Front Range Air Pollution and Photochemistry Experiment (FRAPPÉ) campaign during July–August 2014. An Aerodyne Cavity Attenuated Phase Shift particle light extinction monitor (CAPS-PMex) was deployed to measure dry, βext of submicron aerosols at λ = 632 nm at 1 Hz. Data from a suite of gas-phase instrumentation were used to interpret βext behavior under various categories of air masses and sources. Extinction enhancement ratios relative to CO (Δβext/ΔCO) were significantly increased in highly aged air masses compared to fresh air masses by 50–60 %. The resulting increase in Δβext/ΔCO under highly aged air masses was accompanied by formation of secondary organic aerosols (SOA). In addition, the impacts of aerosol composition on βext in air masses under the influence of urban, natural oil and gas operations (O&G), and agriculture and livestock operations were evaluated. Estimated non-refractory mass extinction efficiency (MEE) values for different air mass types ranged from 1.83–3.30 m2 g−1, with the minimum and maximum values observed in agriculture and urban + O&G influenced air masses, respectively. The mass distribution for organic, nitrate, and sulfate aerosols presented distinct profiles in different air mass types. During Aug. 11–12, regional influence of a biomass burning event was observed, increasing the background βext by 10–15 Mm−1 and the estimated MEE and Δβext/ΔCO values in the Front Range.


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