Particle number concentration, size distribution and chemical composition during haze and photochemical smog episodes in Shanghai

2014 ◽  
Vol 26 (9) ◽  
pp. 1894-1902 ◽  
Author(s):  
Xuemei Wang ◽  
Jianmin Chen ◽  
Tiantao Cheng ◽  
Renyi Zhang ◽  
Xinming Wang
2015 ◽  
Vol 15 (21) ◽  
pp. 12283-12313 ◽  
Author(s):  
A. Lupascu ◽  
R. Easter ◽  
R. Zaveri ◽  
M. Shrivastava ◽  
M. Pekour ◽  
...  

Abstract. Accurate representation of the aerosol lifecycle requires adequate modeling of the particle number concentration and size distribution in addition to their mass, which is often the focus of aerosol modeling studies. This paper compares particle number concentrations and size distributions as predicted by three empirical nucleation parameterizations in the Weather Research and Forecast coupled with chemistry (WRF-Chem) regional model using 20 discrete size bins ranging from 1 nm to 10 μm. Two of the parameterizations are based on H2SO4, while one is based on both H2SO4 and organic vapors. Budget diagnostic terms for transport, dry deposition, emissions, condensational growth, nucleation, and coagulation of aerosol particles have been added to the model and are used to analyze the differences in how the new particle formation parameterizations influence the evolving aerosol size distribution. The simulations are evaluated using measurements collected at surface sites and from a research aircraft during the Carbonaceous Aerosol and Radiative Effects Study (CARES) conducted in the vicinity of Sacramento, California. While all three parameterizations captured the temporal variation of the size distribution during observed nucleation events as well as the spatial variability in aerosol number, all overestimated by up to a factor of 2.5 the total particle number concentration for particle diameters greater than 10 nm. Using the budget diagnostic terms, we demonstrate that the combined H2SO4 and low-volatility organic vapor parameterization leads to a different diurnal variability of new particle formation and growth to larger sizes compared to the parameterizations based on only H2SO4. At the CARES urban ground site, peak nucleation rates are predicted to occur around 12:00 Pacific (local) standard time (PST) for the H2SO4 parameterizations, whereas the highest rates were predicted at 08:00 and 16:00 PST when low-volatility organic gases are included in the parameterization. This can be explained by higher anthropogenic emissions of organic vapors at these times as well as lower boundary-layer heights that reduce vertical mixing. The higher nucleation rates in the H2SO4-organic parameterization at these times were largely offset by losses due to coagulation. Despite the different budget terms for ultrafine particles, the 10–40 nm diameter particle number concentrations from all three parameterizations increased from 10:00 to 14:00 PST and then decreased later in the afternoon, consistent with changes in the observed size and number distribution. We found that newly formed particles could explain up to 20–30 % of predicted cloud condensation nuclei at 0.5 % supersaturation, depending on location and the specific nucleation parameterization. A sensitivity simulation using 12 discrete size bins ranging from 1 nm to 10 μm diameter gave a reasonable estimate of particle number and size distribution compared to the 20 size bin simulation, while reducing the associated computational cost by ~ 36 %.


2016 ◽  
Vol 9 (1) ◽  
pp. 103-114 ◽  
Author(s):  
G. I. Gkatzelis ◽  
D. K. Papanastasiou ◽  
K. Florou ◽  
C. Kaltsonoudis ◽  
E. Louvaris ◽  
...  

Abstract. An experimental methodology was developed to measure the nonvolatile particle number concentration using a thermodenuder (TD). The TD was coupled with a high-resolution time-of-flight aerosol mass spectrometer, measuring the chemical composition and mass size distribution of the submicrometer aerosol and a scanning mobility particle sizer (SMPS) that provided the number size distribution of the aerosol in the range from 10 to 500 nm. The method was evaluated with a set of smog chamber experiments and achieved almost complete evaporation (> 98 %) of secondary organic as well as freshly nucleated particles, using a TD temperature of 400 °C and a centerline residence time of 15 s. This experimental approach was applied in a winter field campaign in Athens and provided a direct measurement of number concentration and size distribution for particles emitted from major pollution sources. During periods in which the contribution of biomass burning sources was dominant, more than 80 % of particle number concentration remained after passing through the thermodenuder, suggesting that nearly all biomass burning particles had a nonvolatile core. These remaining particles consisted mostly of black carbon (60 % mass contribution) and organic aerosol (OA; 40 %). Organics that had not evaporated through the TD were mostly biomass burning OA (BBOA) and oxygenated OA (OOA) as determined from AMS source apportionment analysis. For periods during which traffic contribution was dominant 50–60 % of the particles had a nonvolatile core while the rest evaporated at 400 °C. The remaining particle mass consisted mostly of black carbon with an 80 % contribution, while OA was responsible for another 15–20 %. Organics were mostly hydrocarbon-like OA (HOA) and OOA. These results suggest that even at 400 °C some fraction of the OA does not evaporate from particles emitted from common combustion processes, such as biomass burning and car engines, indicating that a fraction of this type of OA is of extremely low volatility.


2011 ◽  
Vol 11 (8) ◽  
pp. 3823-3833 ◽  
Author(s):  
H. C. Cheung ◽  
L. Morawska ◽  
Z. D. Ristovski

Abstract. The aim of this study was to characterise the new particle formation events in a subtropical urban environment in the Southern Hemisphere. The study measured the number concentration of particles and its size distribution in Brisbane, Australia during 2009. The variation of particle number concentration and nucleation burst events were characterised as well as the particle growth rate which was first reported in urban environment of Australia. The annual average NUFP, NAitken and NNuc were 9.3×103, 3.7×103 and 5.6×103 cm−3, respectively. Weak seasonal variation in number concentration was observed. Local traffic exhaust emissions were a major contributor of the pollution (NUFP) observed in morning which was dominated by the Aitken mode particles, while particles formed by secondary formation processes contributed to the particle number concentration during afternoon. Overall, 65 nucleation burst events were identified during the study period. Nucleation burst events were classified into two groups, with and without particles growth after the burst of nucleation mode particles observed. The average particle growth rate of the nucleation events was 4.6 nm h−1 (ranged from 1.79–7.78 nm h−1). Case studies of the nucleation burst events were characterised including (i) the nucleation burst with particle growth which is associated with the particle precursor emitted from local traffic exhaust emission, (ii) the nucleation burst without particle growth which is due to the transport of industrial emissions from the coast to Brisbane city or other possible sources with unfavourable conditions which suppressed particle growth and (iii) interplay between the above two cases which demonstrated the impact of the vehicle and industrial emissions on the variation of particle number concentration and its size distribution during the same day.


2021 ◽  
Vol 21 (12) ◽  
pp. 9343-9366
Author(s):  
Xueshun Chen ◽  
Fangqun Yu ◽  
Wenyi Yang ◽  
Yele Sun ◽  
Huansheng Chen ◽  
...  

Abstract. Aerosol microphysical processes are essential for the next generation of global and regional climate and air quality models to determine particle size distribution. The contribution of organic aerosols (OAs) to particle formation, mass, and number concentration is one of the major uncertainties in current models. A new global–regional nested aerosol model was developed to simulate detailed microphysical processes. The model combines an advanced particle microphysics (APM) module and a volatility basis set (VBS) OA module to calculate the kinetic condensation of low-volatility organic compounds and equilibrium partitioning of semi-volatile organic compounds in a 3-D framework using global–regional nested domain. In addition to the condensation of sulfuric acid, the equilibrium partitioning of nitrate and ammonium, and the coagulation process of particles, the microphysical processes of the OAs are realistically represented in our new model. The model uses high-resolution size bins to calculate the size distribution of new particles formed through nucleation and subsequent growth. The multi-scale nesting enables the model to perform high-resolution simulations of the particle formation processes in the urban atmosphere in the background of regional and global environments. By using the nested domains, the model reasonably reproduced the OA components obtained from the analysis of aerosol mass spectrometry measurements through positive matrix factorization and the particle number size distribution in the megacity of Beijing during a period of approximately a month. Anthropogenic organic species accounted for 67 % of the OAs of secondary particles formed by nucleation and subsequent growth, which is considerably larger than that of biogenic OAs. On the global scale, the model well predicted the particle number concentration in various environments. The microphysical module combined with the VBS simulated the universal distribution of organic components among the different aerosol populations. The model results strongly suggest the importance of anthropogenic organic species in aerosol particle formation and growth at polluted urban sites and over the whole globe.


2015 ◽  
Vol 6 (5) ◽  
pp. 877-885 ◽  
Author(s):  
Ismael Luis Schneider ◽  
Elba Calesso Teixeira ◽  
Luis Felipe Silva Oliveira ◽  
Flavio Wiegand

2013 ◽  
Vol 2013 ◽  
pp. 1-7 ◽  
Author(s):  
Fangyang Yuan ◽  
Fujun Gan

The method of moments is employed to predict the evolution of aerosol particles in the rainfall process. To describe the dynamic properties of particle size distribution, the population balance equation is converted to moment equations by the method of moments and the converted equations are solved numerically. The variations of particle number concentration, geometric mean diameter, and geometric standard deviation are given in the cases that the Brownian diffusion and inertial impaction of particles dominate, respectively. The effects of raindrop size distribution on particle size distribution are analyzed in nine cases. The results show that the particle number concentration decreases as time goes by, and particles dominated by Brownian diffusion are removed more significantly. The particle number concentration decreases much more rapidly when particle geometric mean diameter is smaller, and the particle size distribution tends to be monodisperse. For the same water content, the raindrops with small geometric mean diameters can remove particles with much higher efficiency than those with large geometric mean diameters. Particles in the “Greenfield gap” are relatively difficult to scavenge, and a new method is needed to remove it from the air.


2015 ◽  
Vol 8 (6) ◽  
pp. 6355-6393 ◽  
Author(s):  
G. I. Gkatzelis ◽  
D. K. Papanastasiou ◽  
K. Florou ◽  
C. Kaltsonoudis ◽  
E. Louvaris ◽  
...  

Abstract. An experimental methodology was developed to measure the non-volatile particle number concentration using a thermodenuder (TD). The TD was coupled with a high-resolution time-of-flight aerosol mass spectrometer, measuring the chemical composition and mass size distribution of the submicrometer aerosol and a scanning mobility particle sizer (SMPS) that provided the number size distribution of the aerosol in the range from 10 to 500 nm. The method was evaluated with a set of smog chamber experiments and achieved almost complete evaporation (> 98 %) of secondary organic as well as freshly nucleated particles, using a TD temperature of 400 °C and a centerline residence time of 15 s. This experimental approach was applied in a winter field campaign in Athens and provided a direct measurement of number concentration and size distribution for particles emitted from major pollution sources. During periods in which the contribution of biomass burning sources was dominant, more than 80 % of particle number concentration remained after passing through the thermodenuder, suggesting that nearly all biomass burning particles had a non-volatile core. These remaining particles consisted mostly of black carbon (60 % mass contribution) and organic aerosol, OA (40 %). Organics that had not evaporated through the TD were mostly biomass burning OA (BBOA) and oxygenated OA (OOA) as determined from AMS source apportionment analysis. For periods during which traffic contribution was dominant 50–60 % of the particles had a non-volatile core while the rest evaporated at 400 °C. The remaining particle mass consisted mostly of black carbon (BC) with an 80 % contribution, while OA was responsible for another 15–20 %. Organics were mostly hydrocarbon-like OA (HOA) and OOA. These results suggest that even at 400 °C some fraction of the OA does not evaporate from particles emitted from common combustion processes, such as biomass burning and car engines, indicating that a fraction of this type of OA is of extremely low volatility.


2006 ◽  
Vol 6 (3) ◽  
pp. 4081-4107 ◽  
Author(s):  
J. Voigtländer ◽  
T. Tuch ◽  
W. Birmili ◽  
A. Wiedensohler

Abstract. Combustion of fossil fuel in gasoline and diesel powered vehicles is a major source of aerosol particles in a city. In a street canyon, the number concentration of particles smaller than 300 nm in diameter, which can be inhaled and cause serious health effects, is dominated by particles originating from this source. In this study we measured both, particle number size distribution and traffic density continuously in a characteristic street canyon in Germany for a time period of 6 months. The street canyon with multistory buildings and 4 traffic lanes is very typical for larger cities. Thus, the measurements are also representative for many other street canyons. In contrast to previous studies, we measured and analyzed the particle number size distribution with high size resolution using a Twin Differential Mobility Analyzer (TDMPS). The measured size range was from 3 to 800 nm, separated into 40 size channels. Correlation coefficients between particle number concentration for integrated size ranges and traffic up to 0.5 counts were determined. Correlations were also calculated for each of the 40 size channels of the DMPS system, respectively. We found two maxima of the correlation coefficient for particles about 10 nm and in the size range 60–80 nm in diameter. Furthermore, correlations between traffic and particles in dependence of meteorological data were calculated. Relevant parameters were identified by a multiple regression method. In our experiment only wind parameters have influenced the particle number concentration significantly. Very high correlation coefficients (up to 0.85) could be observed in the lee side of the street canyon as well as particles in the range between 60 and 80 nm in diameter. These values are significantly higher than correlation coefficients for other wind directions and other particle sizes. A minimum was found in the luff side of the street. These findings are in good agreement with theory of fluid dynamics in street canyons.


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