scholarly journals Measurement report: Vertical distribution of atmospheric particulate matter within the urban boundary layer in southern China – size-segregated chemical composition and secondary formation through cloud processing and heterogeneous reactions

2020 ◽  
Vol 20 (11) ◽  
pp. 6435-6453 ◽  
Author(s):  
Shengzhen Zhou ◽  
Luolin Wu ◽  
Junchen Guo ◽  
Weihua Chen ◽  
Xuemei Wang ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Particulate Matter ◽  
Vertical Distribution ◽  
Aqueous Phase ◽  
Ground Level ◽  
Urban Boundary Layer ◽  
Water Soluble ◽  
Heterogeneous Reactions ◽  
Formation Mechanisms ◽  
Autumn And Winter

Abstract. Many studies have recently been done on understanding the sources and formation mechanisms of atmospheric aerosols at ground level. However, vertical profiles and sources of size-resolved particulate matter within the urban boundary layer are still lacking. In this study, vertical distribution characteristics of size-segregated particles were investigated at three observation platforms (ground level, 118 m, and 488 m) on the 610 m high Canton Tower in Guangzhou, China. Size-segregated aerosol samples were simultaneously collected at the three levels in autumn and winter. Major aerosol components, including water-soluble ions, organic carbon, and elemental carbon, were measured. The results showed that daily average fine-particle concentrations generally decreased with height. Concentrations of sulfate and ammonium in fine particles displayed shallow vertical gradients, and nitrate concentrations increased with height in autumn, while the chemical components showed greater variations in winter than in autumn. The size distributions of sulfate and ammonium in both seasons were characterized by a dominant unimodal mode with peaks in the size range of 0.44–1.0 µm. In autumn, the nitrate size distribution was bimodal, peaking at 0.44–1.0 and 2.5–10 µm, while in winter it was unimodal, implying that the formation mechanisms for nitrate particles were different in the two seasons. Our results suggest that the majority of the sulfate and nitrate is formed from aqueous-phase reactions, and we attribute coarse-mode nitrate formation at the measurement site to the heterogeneous reactions of gaseous nitric acid on existing sea-derived coarse particles in autumn. Case studies further showed that atmospheric aqueous-phase and heterogeneous reactions could be important mechanisms for sulfate and nitrate formation, which, in combination with adverse weather conditions such as temperature inversion and calm wind, led to haze formation during autumn and winter in the Pearl River Delta (PRD) region.

scholarly journals Vertical distribution of atmospheric particulate matters within urban boundary layer in southern China: size-segregated chemical composition and secondary formation through cloud processing and heterogeneous reactions

2019 ◽  
Author(s):  
Shengzhen Zhou ◽  
Luolin Wu ◽  
Junchen Guo ◽  
Weihua Chen ◽  
Xuemei Wang ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Vertical Distribution ◽  
Aqueous Phase ◽  
Urban Boundary Layer ◽  
Water Soluble ◽  
Heterogeneous Reactions ◽  
Formation Mechanisms ◽  
Haze Pollution ◽  
Adverse Weather ◽  
Autumn And Winter

Abstract. Great progress has been made recently in the understanding of the sources and formation mechanisms of atmospheric aerosols at the ground level. However, vertical profiles and sources of size-resolved particulate matter within the urban boundary layer are still lacking. In this study, vertical distribution characteristics of size-segregated particles were investigated at three observation platforms (ground, 118 m and 488 m) on the 610-meter-high Canton Tower in Guangzhou, China. Size-segregated aerosol samples were simultaneously collected at the three levels on the Canton Tower in autumn and winter, respectively. Major aerosol components, including water-soluble ions, organic carbon and elemental carbon, were measured. The results showed that daily average fine-particle concentrations generally decreased with height. Concentrations of sulfate and ammonium in fine particles displayed small vertical gradients and nitrate concentrations increased with height in autumn, while the above chemical components showed greater variations in winter than in autumn. The size distributions of sulfate and ammonium in both seasons were characterized by dominant unimodal droplet modes with a peak at the size range of 0.44–1.0 μm. In autumn, the nitrate size distribution was bi-modal, peaking at 0.44–1.0 μm and 2.5–10 μm, while it was unimodal in winter, implying that the formation mechanisms for nitrate particles were different in the two seasons. Our results suggest droplet mode sulfate and nitrate are likely formed from aqueous-phase reactions and coarse mode nitrate formation is attributed to heterogeneous reactions of gaseous nitric acid on existing sea-derived coarse particles in autumn at the measurement site. The results from pollution cases study further showed that atmospheric aqueous-phase and heterogeneous reactions together with adverse weather conditions, such as temperature inversion and calm wind, resulted in the autumn and winter haze pollution in the PRD region.

scholarly journals Vertical distribution of particle-phase dicarboxylic acids, oxoacids and α-dicarbonyls in the urban boundary layer based on the 325-meter tower in Beijing

2020 ◽  
Author(s):  
Wanyu Zhao ◽  
Hong Ren ◽  
Kimitaka Kawamura ◽  
Huiyun Du ◽  
Xueshun Chen ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Oxalic Acid ◽  
Vertical Distribution ◽  
Organic Acids ◽  
Anthropogenic Activities ◽  
Ground Surface ◽  
Dicarboxylic Acids ◽  
Ground Level ◽  
Water Soluble ◽  
Motor Vehicles

Abstract. Vertical distribution of dicarboxylic acids, oxoacids, α-dicarbonyls, and other organic tracer compounds in fine aerosols (PM2.5) was investigated from the ground surface (8 m) to 260 m at a 325-meter meteorological tower in Beijing in the summer of 2015. Results showed that the concentrations of oxalic acid (C2), the predominant diacid, were more abundant at 120 m (210 ± 154 ng m−3) and 260 m (220 ± 140 ng m−3) than those at the ground level (160 ± 90 ng m−3). Concentrations of phthalic acid (Ph) decreased with the increase of heights, demonstrating that the vehicular exhausts at the ground surface was the main contributor. Positive correlations were noteworthy for C2/total diacids with mass ratios of C2 to main oxoacids (Pyr, ωC2) and α-dicarbonyls (Gly, MeGly) in polluted days (0.42 ≤ r2 ≤ 0.65), especially at the ground level. In clean days, the ratios of carbon content in oxalic acid to water soluble organic carbon (C2-C/WSOC) showed larger values at 120 m and 260 m than those at the ground surface. However, in polluted days, the C2-C/WSOC ratio mainly reached its maximum at the ground level. These phenomena may indicate the enhanced contribution of aqueous-phase oxidation to oxalic acid in polluted days. Combined with the influence of wind field, total diacids, oxoacids and α-dicarbonyls decreased by 22 %–58 % under the control on anthropogenic activities during the 2015 Victory Parade period. Furthermore, the PMF results showed that the secondary formation routes (secondary sulfate formation and secondary nitrate formation) were the dominant contributors (37–44 %) to organic acids, followed by biomass burning (25–30 %) and motor vehicles (18–24 %). In this study, the organic acids at the ground level were largely associated with local traffic emissions, while the long-range atmospheric transport followed by photochemical aging contributed more to diacids and related compounds in the boundary layer over Beijing than the ground surface.

scholarly journals Vertical distribution of particle-phase dicarboxylic acids, oxoacids and <i>α</i>-dicarbonyls in the urban boundary layer based on the 325 m tower in Beijing

2020 ◽  
Vol 20 (17) ◽  
pp. 10331-10350
Author(s):  
Wanyu Zhao ◽  
Hong Ren ◽  
Kimitaka Kawamura ◽  
Huiyun Du ◽  
Xueshun Chen ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Oxalic Acid ◽  
Organic Acids ◽  
Anthropogenic Activities ◽  
Ground Surface ◽  
Dicarboxylic Acids ◽  
Ground Level ◽  
Urban Boundary Layer ◽  
Water Soluble ◽  
Motor Vehicles

Abstract. Vertical distributions of dicarboxylic acids, oxoacids, α-dicarbonyls and other organic tracer compounds in fine aerosols (PM2.5) were investigated at three heights (8, 120 and 260 m) based on a 325 m meteorological tower in urban Beijing in the summer of 2015. Results showed that the concentrations of oxalic acid (C2), the predominant diacid, were more abundant at 120 m (210±154 ng m−3) and 260 m (220±140 ng m−3) than those at the ground surface (160±90 ng m−3). Concentrations of phthalic acid (Ph) decreased with the increase in height, indicating that local vehicular exhausts were the main contributor. Positive correlations were noteworthy for C2 ∕ total diacids with mass ratios of C2 to main oxoacids (Pyr and ωC2) and α-dicarbonyls (Gly and MeGly) in polluted days (0.42≤r2≤0.65), especially at the ground level. In clean days, the ratios of carbon content in oxalic acid to water-soluble organic carbon (C2−C ∕ WSOC) showed larger values at 120 and 260 m than those at the ground surface. However, in polluted days, the C2−C ∕ WSOC ratio mainly reached its maximum at ground level. These phenomena may indicate the enhanced contribution of aqueous-phase oxidation to oxalic acid in polluted days. Combined with the influence of wind field, total diacids, oxoacids and α-dicarbonyls decreased by 22 %–58 % under the control on anthropogenic activities during the 2015 Victory Parade period. Furthermore, the positive matrix factorisation (PMF) results showed that the secondary formation routes (secondary sulfate formation and secondary nitrate formation) were the dominant contributors (37 %–44 %) to organic acids, followed by biomass burning (25 %–30 %) and motor vehicles (18 %–24 %). In this study, the organic acids at ground level were largely associated with local traffic emissions, while the long-range atmospheric transport followed by photochemical ageing contributed more to diacids and related compounds in the urban boundary layer than the ground surface in Beijing.

scholarly journals High resolution vertical distribution and sources of HONO and NO<sub>2</sub> in the nocturnal boundary layer in urban Beijing, China

2019 ◽  
Author(s):  
Fanhao Meng ◽  
Min Qin ◽  
Ke Tang ◽  
Jun Duan ◽  
Wu Fang ◽  
...  
Keyword(s):  
Boundary Layer ◽  
High Resolution ◽  
Vertical Distribution ◽  
Heterogeneous Reaction ◽  
Ground Surface ◽  
Ground Level ◽  
Urban Atmosphere ◽  
Surface Measurement ◽  
Enhanced Absorption ◽  
Haze Episode

Abstract. The production of HONO on aerosol surfaces and ground surfaces in urban atmosphere is of interests. However, ground surface measurement commonly in our society is not able to distinguish these two parts. Here, for the first time, we reported high-resolution vertical profile measurements of HONO and NO2 in urban Beijing at night using an incoherent broadband cavity enhanced absorption spectrometer (IBBCEAS) amounted on a movable container which attached to a meteorological tower of 325 m high. The mixing ratios of HONO during one haze episode (E1), the clean episode (C2) and another haze episode (E3) were 4.26 ± 2.08, 0.83 ± 0.65, and 3.54 ± 0.91 ppb, respectively. High-resolution vertical profiles revealed that the vertical distribution of HONO is consistent with stratification and layering in the nocturnal urban atmosphere below 250 m. Direct emissions from combustion processes contributed 51.1 % to ambient HONO concentration at night. The HONO production from the heterogeneous conversion of NO2 on the aerosol surfaces cannot explain HONO vertical measurements at night, indicating that the heterogeneous reaction of NO2 on ground surfaces dominated the nocturnal HONO production. The nocturnal HONO in the boundary layer is primarily derived from the heterogeneous conversion of NO2 at ground level and direct emissions; it is then transported throughout the column by vertical convection. ϕNO2 → HONO, the HONO yield from deposited NO2, is used to evaluate HONO production from the heterogeneous conversion of NO2 at night. The derived ϕNO2 → HONO values on 9 (C2), 10 (C2) and 11 December (E3) were 0.10, 0.08, and 0.09, respectively, indicating a significant production of HONO from heterogeneous reaction of NO2 at ground level. The similar ϕNO2 → HONO values measured during clean and haze episodes suggest that the heterogeneous conversion potential of NO2 at ground level is consistent at night. Furthermore, the dry deposition loss of HONO to the ground surface and vertical mixing effects associated with convection reached a near steady state at midnight on 11–12 December, indicating that significant quantities of HONO are deposited to the ground surface at night, and the ground surface is the source and sink of HONO at night.

scholarly journals Current challenges in modelling far-range air pollution induced by the 2014–2015 Bárðarbunga fissure eruption (Iceland)

2016 ◽  
Vol 16 (17) ◽  
pp. 10831-10845 ◽  
Author(s):  
Marie Boichu ◽  
Isabelle Chiapello ◽  
Colette Brogniez ◽  
Jean-Christophe Péré ◽  
Francois Thieuleux ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Air Pollution ◽  
Vertical Distribution ◽  
Planetary Boundary Layer ◽  
Large Scale ◽  
Temporal Dynamics ◽  
Ground Level ◽  
Optical Absorption Spectroscopy ◽  
Sulfate Aerosols ◽  
Volcanic Cloud

Abstract. The 2014–2015 Holuhraun lava-flood eruption of Bárðarbunga volcano (Iceland) emitted prodigious amounts of sulfur dioxide into the atmosphere. This eruption caused a large-scale episode of air pollution throughout Western Europe in September 2014, the first event of this magnitude recorded in the modern era. We gathered chemistry-transport simulations and a wealth of complementary observations from satellite sensors (OMI, IASI), ground-based remote sensing (lidar, sunphotometry, differential optical absorption spectroscopy) and ground-level air quality monitoring networks to characterize both the spatial-temporal distributions of volcanic SO2 and sulfate aerosols as well as the dynamics of the planetary boundary layer. Time variations of dynamical and microphysical properties of sulfate aerosols in the aged low-tropospheric volcanic cloud, including loading, vertical distribution, size distribution and single scattering albedo, are provided. Retrospective chemistry-transport simulations at low horizontal resolution (25 km  ×  25 km) capture the correct temporal dynamics of this far-range air pollution event but fail to reproduce the correct magnitude of SO2 concentration at ground-level. Simulations at higher spatial resolution, relying on two nested domains with finest resolution of 7.3 km  ×  7.3 km, improve substantially the far-range vertical distribution of the volcanic cloud and subsequently the description of ground-level SO2 concentrations. However, remaining discrepancies between model and observations are shown to result from an inaccurate representation of the planetary boundary layer (PBL) dynamics. Comparison with lidar observations points out a systematic under-estimation of the PBL height by the model, whichever the PBL parameterization scheme. Such a shortcoming impedes the capture of the overlying Bárðarbunga cloud into the PBL at the right time and in sufficient quantities. This study therefore demonstrates the key role played by the PBL dynamics in accurately modelling large-scale volcanogenic air pollution.

scholarly journals How well do tall-tower measurements characterize the CO<sub>2</sub> mole fraction distribution in the planetary boundary layer?

2015 ◽  
Vol 8 (4) ◽  
pp. 1657-1671 ◽  
Author(s):  
L. Haszpra ◽  
Z. Barcza ◽  
T. Haszpra ◽  
Zs. Pátkai ◽  
K. J. Davis
Keyword(s):  
Boundary Layer ◽  
Vertical Distribution ◽  
Planetary Boundary Layer ◽  
Mole Fraction ◽  
Lower Troposphere ◽  
Co2 Flux ◽  
Ground Level ◽  
Rural Site ◽  
Mole Fraction Profile ◽  
Tall Tower

Abstract. Planetary boundary layer (PBL) CO2 mole fraction data are needed by transport models and carbon budget models as both input and reference for validation. The height of in situ CO2 mole fraction measurements is usually different from that of the model levels where the data are needed; data from short towers, in particular, are difficult to utilize in atmospheric models that do not simulate the surface layer well. Tall-tower CO2 mole fraction measurements observed at heights ranging from 10 to 115 m above ground level at a rural site in Hungary and regular airborne vertical mole fraction profile measurements (136 vertical profiles) above the tower allowed us to estimate how well a tower of a given height could estimate the CO2 mole fraction above the tower in the PBL. The statistical evaluation of the height-dependent bias between the real PBL CO2 mole fraction profile (measured by the aircraft) and the measurement at a given elevation above the ground was performed separately for the summer and winter half years to take into account the different dynamics of the lower troposphere and the different surface CO2 flux in the different seasons. The paper presents (1) how accurately the vertical distribution of CO2 in the PBL can be estimated from the measurements on the top of a tower of height H; (2) how tall of a tower would be needed for the satisfaction of different requirements on the accuracy of the estimation of the CO2 vertical distribution; (3) how accurate of a CO2 vertical distribution estimation can be expected from the existing towers; and (4) how much improvement can be achieved in the accuracy of the estimation of CO2 vertical distribution by applying the virtual tall-tower concept.

scholarly journals Vertical distribution of ozone and VOCs in the low boundary layer of Mexico City

2008 ◽  
Vol 8 (12) ◽  
pp. 3061-3079 ◽  
Author(s):  
E. Velasco ◽  
C. Márquez ◽  
E. Bueno ◽  
R. M. Bernabé ◽  
A. Sánchez ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Vertical Distribution ◽  
Mexico City ◽  
Atmospheric Stability ◽  
Ground Level ◽  
Residual Layer ◽  
Background Concentration ◽  
Complex Interactions ◽  
Unstable Layer

Abstract. The evolution of ozone (O3) and 13 volatile organic compounds (VOCs) in the boundary layer of Mexico City was investigated during 2000–2004 to improve our understanding of the complex interactions between those trace gases and meteorological variables, and their influence on the air quality of a polluted megacity. A tethered balloon, fitted with electrochemical and meteorological sondes, was used to obtain detailed vertical profiles of O3 and meteorological parameters up to 1000 m above ground during part of the diurnal cycle (02:00–18:00 h). VOCs samples were collected up to 200 m by pumping air to canisters with a Teflon tube attached to the tether line. Overall, features of these profiles were found to be consistent with the formation of an upper residual layer during nighttime carrying over a fraction of the O3 from the previous day that contributes to the background concentration in surrounding regions. At the same time the release of heat stored in the urban surface forms a shallow unstable layer close to the ground, where the nocturnal emissions are trapped. After sunrise an O3 balance is determined by photochemical production, entrainment from the upper residual layer and destruction by titration with nitric oxide, delaying the ground-level O3 rise by 2 h. The subsequent evolution of the conductive boundary layer and vertical distribution of pollutants are discussed in terms of the energy balance, the presence of turbulence and the atmospheric stability.

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