Xiaojing Shen

Mixing state and hygroscopicity of dust and haze particles before leaving Asian continent

Pollutants during haze and Asian dust storms are transported out of the Asian continent, affecting the regional climate and the hydrological and biogeochemical cycles. Understanding the physicochemical properties of aerosol particles is essential to quantify their impacts. In order to determine physicochemical properties of aerosols before leaving the Asian continent, we carried out a field campaign from 14 April to 2 May 2011 at a background site in the path of Asian dust and haze outflows. We measured concentrations of gaseous pollutants (SO2, NO2, NO, O3, and CO), black carbon (BC), and particle number in situ and collected airborne particles for microscopic analysis. Pollutant concentrations (BC, 4 µg m−3; CO, 808 ppb; SO2, 24 ppb; NO2, 37 ppb) were highest during haze periods, except for PM2.5 mass, which was highest (162 µg m−3) during a dust storm. Seventy-one percent of haze particles were coated with organic films and 32% were internal mixtures of sulfates and refractory particles (e.g., soot, metal/fly ash, and mineral). Seventy-nine percent of haze particles have deliquescence relative humidity at 68–70%. During a dust storm, soot particles were observed among dust particles. Most dust particles were hydrophobic, and no Ca(NO3)2 was observed in dust particles collected during the dust storms, but up to 32% of dust particles were found to be coated with Ca(NO3)2 after the main dust storm moved out of the sampling area. These results indicated that both natural and anthropogenic aerosol particles in Asian outflow can undergo significant physicochemical processes before leaving the Asian continent.

Seasonal characterization of components and size distributions for submicron aerosols in Beijing

Submicron aerosols (PM1) in Beijing were studied using an Aerodyne aerosol mass spectrometer (AMS) from January to October 2008. This paper presents seasonal variations of different chemical components (sulfate, nitrate, ammonium, chloride and organics) and size distributions of PM1. Results show that mass concentration of PM1 was highest in summer, and lowest in autumn. Organics represented the dominant species in all seasons, accounting for 36%–58% of PM1, and their concentrations were highest in winter. Concentrations of inorganic components, sulfate, nitrate, and ammonium were highest in summer. Based on principal component analysis, organics were deconvolved and quantified as hydrocarbon-like and oxygenated organic aerosol (HOA and OOA, respectively). HOA was highest in winter, accounting for about 70% of organics. However, OOA was highest in summer, and had lower values in autumn and winter. A similar diurnal pattern of various components was observed, which is higher at nighttime and lower during daytime. HOA increased more dramatically than other species between 17:00 and 21:00 and peaked at noon, which could be related to cooking emissions. OOA, sulfate, nitrate, ammonium and chloride varied with the same trend. Their concentrations increased with solar radiation from 9:00 to 13:00, and declined with weakening solar radiation. Size distributions of all species showed apparent peaks in the range 500–600 nm. Size distributions of organics were much broader than other species, particularly in autumn and winter. Distributions of sulfate, nitrate and ammonium had similar patterns, broadening in winter. Contributions of different species were size-dependent; the finer the particle, the greater the contribution of organics. Organics represented more than 60% of particles smaller than 200 nm, contributing 50% to PM1 in winter. In spring and summer, HOA was the dominant organic fraction for particles smaller than 200 nm, while OOA contributed more to particles larger than 300 nm. In winter, HOA contributed more than OOA to all PM1 particles.

Relative contributions of boundary-layer meteorological factors to the explosive growth of PM 2.5 during the red-alert heavy pollution episodes in Beijing in December 2016

Based on observations of urban mass concentration of fine particulate matter smaller than 2.5 μm in diameter (PM2.5), ground meteorological data, vertical measurements of winds, temperature, and relative humidity (RH), and ECMWF reanalysis data, the major changes in the vertical structures of meteorological factors in the boundary layer (BL) during the heavy aerosol pollution episodes (HPEs) that occurred in winter 2016 in the urban Beijing area were analyzed. The HPEs are divided into two stages: the transport of pollutants under prevailing southerly winds, known as the transport stage (TS), and the PM2.5 explosive growth and pollution accumulation period characterized by a temperature inversion with low winds and high RH in the lower BL, known as the cumulative stage (CS). During the TS, a surface high lies south of Beijing, and pollutants are transported northwards. During the CS, a stable BL forms and is characterized by weak winds, temperature inversion, and moisture accumulation. Stable atmospheric stratification featured with light/calm winds and accumulated moisture (RH > 80%) below 250 m at the beginning of the CS is closely associated with the inversion, which is strengthened by the considerable decrease in near-surface air temperature due to the interaction between aerosols and radiation after the aerosol pollution occurs. A significant increase in the PLAM (Parameter Linking Aerosol Pollution and Meteorological Elements) index is found, which is linearly related to PM mass change. During the first 10 h of the CS, the more stable BL contributes approximately 84% of the explosive growth of PM2.5 mass. Additional accumulated near-surface moisture caused by the ground temperature decrease, weak turbulent diffusion, low BL height, and inhibited vertical mixing of water vapor is conducive to the secondary aerosol formation through chemical reactions, including liquid phase and heterogeneous reactions, which further increases the PM2.5 concentration levels. The contribution of these reaction mechanisms to the explosive growth of PM2.5 mass during the early CS and subsequent pollution accumulation requires further investigation.

Key features of new particle formation events at background sites in China and their influence on cloud condensation nuclei

Long-term continuous measurements of particle number size distributions with mobility diameter sizes ranging from 3 to 800 nm were performed to study new particle formation (NPF) events at Shangdianzi (SDZ), Mt. Tai (TS), and Lin’an (LAN) stations representing the background atmospheric conditions in the North China Plain (NCP), Central East China (CEC), and Yangtze River Delta (YRD) regions, respectively. The mean formation rate of 3-nm particles was 6.3, 3.7, and 5.8 cm–3∙s–1, and the mean particle growth rate was 3.6, 6.0, and 6.2 nm∙h–1 at SDZ, TS, and LAN, respectively. The NPF event characteristics at the three sites indicate that there may be a stronger source of low volatile vapors and higher condensational sink of pre-existing particles in the YRD region. The formation rate of NPF events at these sites, as well as the condensation sink, is approximately 10 times higher than some results reported at rural/urban sites in western countries. However, the growth rates appear to be 1–2 times higher. Approximately 12%–17% of all NPF events with nucleated particles grow to a climaterelevant size (>50 nm). These kinds of NPF events were normally observed with higher growth rate than the other NPF cases. Generally, the cloud condensation nuclei (CCN) number concentration can be enhanced by approximately a factor of 2–6 on these event days. The mean value of the enhancement factor is lowest at LAN (2–3) and highest at SDZ (~4). NPF events have also been found to have greater impact on CCN production in China at the regional scale than in the other background sites worldwide.Graphical abstract

Characteristics of chemical composition and role of meteorological factors during heavy aerosol pollution episodes in northern Beijing area in autumn and winter of 2015

Abstract Heavy aerosol pollution episodes (HPEs) usually start from late autumn and become more serious in winter in Beijing and its vicinity (BIV). In this study, we examine the reasons for the formation and change of HPEs in the areas of northern BIV. The size-resolved chemical components of PM1 and meteorological conditions were investigated during HPEs in autumn and winter of 2015. Stable regional atmosphere and higher atmospheric condensation processes associated with southerly and lower speed wind led to the formation of HPEs. After the start of these HPEs, the concentration of fine particles increased more than twice in several hours. ~80% of the ‘explosive’ growth in PM mass can be considered as a positive feedback of meteorological factors that come from even more stable atmosphere and larger condensation rate of water vapour, which was derived from the interaction between formed aerosol pollution and the meteorological factors within boundary layer. Nitrate was the largest fraction of PM1 in autumn, and the most significantly increased component during HPEs relative to clean period during both of autumn and winter. The proportion of organic aerosol (OA) was similar to that of nitrate in autumn, but its rise in HPE was much smaller, mainly because of the high concentration of OA existed during clean periods. Compared with the largest increase of nitrate, the similar uplift was found for ammonium production, showing that a large amount of ammonium was mainly formed by the combination of in HPEs, rather than . In addition to the lower southerly wind carrying pollutants from southern part of BIV, westerly wind from central Inner Mongolia and north Shanxi can also bring air pollutants originating from coal combustion, contributing to the heavy pollution in the northern BIV area in winter, and resulting in higher sulphate, nitrate and OA masses.

Comparison of Submicron Particles at a Rural and an Urban Site in the North China Plain during the December 2016 Heavy Pollution Episodes

An extensive field experiment for measurement of physical and chemical properties of aerosols was conducted at an urban site in the Chinese Academy of Meteorological Sciences (CAMS) in Beijing and at a rural site in Gucheng (GC), Hebei Province in December 2016. This paper compares the number size distribution of submicron particle matter (PM1, diameter < 1 μm) between the two sites. The results show that the mean PM1 number concentration at GC was twice that at CAMS, and the mass concentration was three times the amount at CAMS. It is found that the accumulation mode (100–850 nm) particles constituted the largest fraction of PM1 at GC, which was significantly correlated with the local coal combustion, as confirmed by a significant relationship between the accumulation mode and the absorption coefficient of soot particles. The high PM1 concentration at GC prevented the occurrence of new particle formation (NPF) events, while eight such events were observed at CAMS. During the NPF events, the mass fraction of sulfate increased significantly, indicating that sulfate played an important role in NPF. The contribution of regional transport to PM1 mass concentration was approximately 50% at both sites, same as that of the local emission. However, during the red-alert period when emission control took place, the contribution of regional transport was notably higher.

Chemical Components, Variation, and Source Identification of PM1 during the Heavy Air Pollution Episodes in Beijing in December 2016

Air pollution is a current global concern. The heavy air pollution episodes (HPEs) in Beijing in December 2016 severely influenced visibility and public health. This study aims to survey the chemical compositions, sources, and formation processes of the HPEs. An aerodyne quadruple aerosol mass spectrometer (Q-AMS) was utilized to measure the non-refractory PM1 (NR-PM1) mass concentration and size distributions of the main chemical components including organics, sulfate, nitrate, ammonium, and chloride in situ during 15–23 December 2016. The NR-PM1 mass concentration was found to increase from 6 to 188 μg m–3 within 5 days. During the most serious polluted episode, the PM1 mass concentration was about 2.6 times that during the first pollution stage and even 40 times that of the clean days. The formation rates of PM2.5 in the five pollution stages were 26, 22, 22, 32, and 67 μg m–3 h–1, respectively. Organics and nitrate occupied the largest proportion in the polluted episodes, whereas organics and sulfate dominated the submicron aerosol during the clean days. The size distribution of organics is always broader than those of other species, especially in the clean episodes. The peak sizes of the interested species grew gradually during different HPEs. Aqueous reaction might be important in forming sulfate and chloride, and nitrate was formed via oxidization and condensation processes. PMF (positive matrix factorization) analysis on AMS mass spectra was employed to separate the organics into different subtypes. Two types of secondary organic aerosol with different degrees of oxidation consisted of 43% of total organics. By contrast, primary organics from cooking, coal combustion, and traffic emissions comprised 57% of the organic aerosols during the HPEs.

Aerosol Hygroscopicity during the Haze Red-Alert Period in December 2016 at a Rural Site of the North China Plain

A humidification system was deployed to measure aerosol hygroscopicity at a rural site of the North China Plain during the haze red-alert period 17–22 December 2016. The aerosol scattering coefficients under dry [relative humidity (RH) < 30%] and wet (RH in the range of 40%–85%) conditions were simultaneously measured at wavelengths of 450, 550, and 700 nm. It is found that the aerosol scattering coefficient and backscattering coefficient increased by only 29% and 10%, respectively when RH went up from 40% to 80%, while the hemispheric backscatter fraction went down by 14%, implying that the aerosol hygroscopicity represented by the aerosol scattering enhancement factor f(RH) is relatively low and RH exerted little effects on the aerosol light scattering in this case. The scattering enhancement factors do not show significant differences at the three wavelengths, only with an approximate 2% variation, suggesting that the aerosol hygroscopicity is independent of the wavelength. Aerosol hygroscopicity is highly dependent on the aerosol chemical composition. When there is a large mass fraction of inorganics and a small mass fraction of organic matter, f(RH) reaches a high value. The fraction of NO3– was strongly correlated with the aerosol scattering coefficient at RH = 80%, which suggests that NO3– played an important role in aerosol hygroscopic growth during the heavy pollution period.