scholarly journals Measurement report: On the difference of aerosol hygroscopicity between high and low RH conditions in the North China Plain

2022 ◽  
Author(s):  
Jingnan Shi ◽  
Juan Hong ◽  
Nan Ma ◽  
Qingwei Luo ◽  
Yao He ◽  
...  

Abstract. Atmospheric processes, including both primary emissions and secondary formation, may exert complex effects on aerosol hygroscopicity, which is of significant importance in understanding and quantifying the effect of aerosols on climate and human health. In order to explore the influence of local emissions and secondary formation processes on aerosol hygroscopicity, we investigated the hygroscopic properties of submicron aerosol particles at a rural site in the North China Plain (NCP) in winter 2018. This was conducted by simultaneous measurements of aerosol hygroscopicity and chemical composition, using a self-assembled hygroscopic tandem differential mobility analyzer (HTDMA) and a capture-vaporizer time-of-flight aerosol chemical speciation monitor (CV-ToF-ACSM). The hygroscopicity results showed that the particles during the entire campaign were mainly externally mixed, with a more hygroscopic (MH) mode and a less hygroscopic (LH) particles mode. The mean hygroscopicity parameter values (κmean) derived from hygroscopicity measurements for particles at 60, 100, 150, and 200 nm were 0.16, 0.18, 0.16, and 0.15, respectively. During this study, we classified two distinct episodes with different RH/T conditions, indicative of different primary emissions and secondary formation processes. It was observed that aerosols at all measured sizes were more hygroscopic under the high RH (HRH) episode than those under the low RH (LRH) episode. During the LRH, κ decreased with increasing particle size, which may be explained by the enhanced domestic heating at low temperature, causing large emissions of non- or less-hygroscopic primary aerosols. This is particularly obvious for 200 nm particles, with a dominant number fraction (> 50 %) of LH mode particles. Using O : C-dependent hygroscopic parameters of secondary organic compounds (κSOA), closure analysis between the HTDMA_measured κ and the ACSM_derived κ was carried out. The results showed that κSOA under the LRH episode was less sensitive to the changes in organic oxidation level, while κSOA under the HRH had a relatively stronger dependency on the organic O : C. This feature suggests that the different sources and aerosol evolution processes, partly resulting from the variation in atmospheric RH/T conditions, may lead to significant changes in aerosol chemical composition, which will further influence their corresponding physical properties.

2021 ◽  
Author(s):  
Jingnan Shi ◽  
Juan Hong ◽  
Nan Ma ◽  
Qingwei Luo ◽  
Hanbing Xu ◽  
...  

<p>Simultaneous measurements of aerosol hygroscopicity and chemical composition were performed at a suburban site in the North China Plain in winter 2018 using a self-assembled hygroscopic tandem differential mobility analyzer (H-TDMA) and a capture-vaporizer time-of-flight aerosol chemical speciation monitor (CV-ToF-ACSM), respectively. During the experimental period, aerosol particles usually show an external mixture in terms of hygroscopicity, with a less hygroscopic particles mode (LH) and a more hygroscopic mode (MH). The average ensemble mean hygroscopicity parameter (κ<sub>mean</sub>) are 0.16, 0.18, 0.16, and 0.15 for 60, 100, 150, and 200 nm particles, respectively. Two episodes with different RH/T conditions and secondary aerosol formations are distinguished. Higher aerosol hygroscopicity is observed for all measured sizes in the high RH episode (HRH) than in the low RH episode (LRH). In LRH, κ decreases as the particle size increases, which may be explained by the large contribution of non- or less-hygroscopic primary compounds in large particles due to the enhanced domestic heating emissions at low temperature. The number fraction of LH mode at 200 nm even exceeds 50%. Closure analysis is carried out between the HTDMA-measured κ and the ACSM-derived hygroscopicity using different approximations for the hygroscopic parameters of organic compounds (κ<sub>org</sub>). The results indicate that κ<sub>org</sub> is less sensitive towards the variation of its oxidation level under HRH conditions but has a stronger O: C-dependency under LRH conditions. The difference in the chemical composition and their corresponding physical properties under different RH/T conditions reflects potentially different formation mechanisms of secondary organic aerosols at those two distinct episodes.</p>


2014 ◽  
Vol 14 (5) ◽  
pp. 2525-2539 ◽  
Author(s):  
H. J. Liu ◽  
C. S. Zhao ◽  
B. Nekat ◽  
N. Ma ◽  
A. Wiedensohler ◽  
...  

Abstract. Hygroscopic growth of aerosol particles is of significant importance in quantifying the aerosol radiative effect in the atmosphere. In this study, hygroscopic properties of ambient particles are investigated based on particle chemical composition at a suburban site in the North China Plain during the HaChi campaign (Haze in China) in summer 2009. The size-segregated aerosol particulate mass concentration as well as the particle components such as inorganic ions, organic carbon and water-soluble organic carbon (WSOC) are identified from aerosol particle samples collected with a ten-stage impactor. An iterative algorithm is developed to evaluate the hygroscopicity parameter κ from the measured chemical composition of particles. During the HaChi summer campaign, almost half of the mass concentration of particles between 150 nm and 1 μm is contributed by inorganic species. Organic matter (OM) is abundant in ultrafine particles, and 77% of the particulate mass with diameter (Dp) of around 30 nm is composed of OM. A large fraction of coarse particle mass is undetermined and is assumed to be insoluble mineral dust and liquid water. The campaign's average size distribution of κ values shows three distinct modes: a less hygroscopic mode (Dp < 150 nm) with κ slightly above 0.2, a highly hygroscopic mode (150 nm < Dp < 1 μm) with κ greater than 0.3 and a nearly hydrophobic mode (Dp > 1 μm) with κ of about 0.1. The peak of the κ curve appears around 450 nm with a maximum value of 0.35. The derived κ values are consistent with results measured with a high humidity tandem differential mobility analyzer within the size range of 50–250 nm. Inorganics are the predominant species contributing to particle hygroscopicity, especially for particles between 150 nm and 1 μm. For example, NH4NO3, H2SO4, NH4HSO4 and (NH4)2SO4 account for nearly 90% of κ for particles of around 900 nm. For ultrafine particles, WSOC plays a critical role in particle hygroscopicity due to the predominant mass fraction of OM in ultrafine particles. WSOC for particles of around 30 nm contribute 52% of κ. Aerosol hygroscopicity is related to synoptic transport patterns. When southerly wind dominates, particles are more hygroscopic; when northerly wind dominates, particles are less hygroscopic. Aerosol hygroscopicity also has a diurnal variation, which can be explained by the diurnal evolution of planetary boundary layer, photochemical aging processes during daytime and enhanced black carbon emission at night. κ is highly correlated with mass fractions of SO42−, NO3− and NH4+ for all sampled particles as well as with the mass fraction of WSOC for particles of less than 100 nm. A parameterization scheme for κ is developed using mass fractions of SO42−, NO3−, NH4+ and WSOC due to their high correlations with κ, and κ calculated from the parameterization agrees well with κ derived from the particle's chemical composition. Further analysis shows that the parameterization scheme is applicable to other aerosol studies in China.


2021 ◽  
Vol 21 (7) ◽  
pp. 5463-5476
Author(s):  
Weiqi Xu ◽  
Chun Chen ◽  
Yanmei Qiu ◽  
Ying Li ◽  
Zhiqiang Zhang ◽  
...  

Abstract. Volatility and viscosity have substantial impacts on gas–particle partitioning, formation and evolution of aerosol and hence the predictions of aerosol-related air quality and climate effects. Here aerosol volatility and viscosity at a rural site (Gucheng) and an urban site (Beijing) in the North China Plain (NCP) in summer and winter were investigated by using a thermodenuder coupled with a high-resolution aerosol mass spectrometer. The effective saturation concentration (C*) of organic aerosol (OA) in summer was smaller than that in winter (0.55 µg m−3 vs. 0.71–0.75 µg m−3), indicating that OA in winter in the NCP is more volatile due to enhanced primary emissions from coal combustion and biomass burning. The volatility distributions varied and were largely different among different OA factors. In particular, we found that hydrocarbon-like OA (HOA) contained more nonvolatile compounds compared to coal-combustion-related OA. The more oxidized oxygenated OA (MO-OOA) showed overall lower volatility than less oxidized OOA (LO-OOA) in both summer and winter, yet the volatility of MO-OOA was found to be relative humidity (RH) dependent showing more volatile properties at higher RH. Our results demonstrated the different composition and chemical formation pathways of MO-OOA under different RH levels. The glass transition temperature (Tg) and viscosity of OA in summer and winter are estimated using the recently developed parameterization formula. Our results showed that the Tg of OA in summer in Beijing (291.5 K) was higher than that in winter (289.7–290.0 K), while it varied greatly among different OA factors. The viscosity suggested that OA existed mainly as solid in winter in Beijing (RH = 29 ± 17 %), but as semisolids in Beijing in summer (RH = 48 ± 25 %) and Gucheng in winter (RH = 68 ± 24 %). These results have the important implication that kinetically limited gas–particle partitioning may need to be considered when simulating secondary OA formation in the NCP.


2018 ◽  
Vol 32 (1) ◽  
pp. 38-48 ◽  
Author(s):  
Xuefei Qi ◽  
Junying Sun ◽  
Lu Zhang ◽  
Xiaojing Shen ◽  
Xiaoye Zhang ◽  
...  

Atmosphere ◽  
2020 ◽  
Vol 11 (2) ◽  
pp. 179 ◽  
Author(s):  
Lei Liu ◽  
Yusi Liu ◽  
Wei Wen ◽  
Linlin Liang ◽  
Xin Ma ◽  
...  

An intensive sampling of PM2.5 was conducted at a rural site (Gucheng) in the North China Plain from 22 October to 23 November 2016. A total of 25 elements (Al, Na, Cl, Mg, P, S, K, Ca, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, As, Se, Br, Sr, Cd, Ba, Pb, and Sb) from PM2.5 filter samples collected daily were measured using a wavelength dispersive X-ray fluorescence spectrometer. Cl, S, and K were the most abundant elements, with average concentrations of 2077.66 ng m−3 (range 118.88–4638.96 ng m−3), 1748.78 ng m−3 (range 276.67–4335.59 ng m−3), and 1287.07 ng m−3 (range 254.90–2748.63 ng m−3), respectively. Among noncrustal trace metal elements, the concentration of Zn was the highest, with an average of 397.74 ng m−3 (range 36.45–1602.96 ng m−3), followed by Sb and Pb, on average, of 299.20 ng m−3 and 184.52 ng m−3, respectively. The morphologies of PM2.5 samples were observed using scanning electron microscopy. The shape of the particles was predominantly spherical, chain-like, and irregular. Positive matrix factorization analysis revealed that soil dust, following by industry, secondary formation, vehicle emissions, biomass and waste burning, and coal combustion, were the main sources of PM2.5. The results of cluster, potential source contribution function, and concentration weighted trajectory analyses suggested that local emissions from Hebei Province, as well as regional transport from Beijing, Tianjin, Shandong, and Shanxi Province, and long-range transport from Inner Mongolia, were the main contributors to PM2.5 pollution.


2019 ◽  
Vol 19 (20) ◽  
pp. 12857-12874 ◽  
Author(s):  
Renmin Yuan ◽  
Xiaoye Zhang ◽  
Hao Liu ◽  
Yu Gui ◽  
Bohao Shao ◽  
...  

Abstract. Due to excessive anthropogenic emissions, heavy aerosol pollution episodes (HPEs) often occur during winter in the Beijing–Tianjin–Hebei (BTH) area of the North China Plain. Extensive observational studies have been carried out to understand the causes of HPEs; however, few measurements of vertical aerosol fluxes exist, despite them being the key to understanding vertical aerosol mixing, specifically during weak turbulence stages in HPEs. In the winter of 2016 and the spring of 2017 aerosol vertical mass fluxes were measured by combining large aperture scintillometer (LAS) observations, surface PM2.5 and PM10 mass concentrations, and meteorological observations, including temperature, relative humidity (RH), and visibility, at a rural site in Gucheng (GC), Hebei Province, and an urban site at the Chinese Academy of Meteorological Sciences (CAMS) in Beijing located 100 km to the northeast. These are based on the light propagation theory and surface-layer similarity theory. The near-ground aerosol mass flux was generally lower in winter than in spring and weaker in rural GC than in urban Beijing. This finding provides direct observational evidence for a weakened turbulence intensity and low vertical aerosol fluxes in winter and polluted areas such as GC. The HPEs included a transport stage (TS), an accumulative stage (AS), and a removal stage (RS). During the HPEs from 25 to 31 January 2017, in Beijing, the mean mass flux decreased by 51 % from 0.0049 mg m−2 s−1 in RSs to 0.0024 mg m−2 s−1 in the TSs. During the ASs, the mean mass flux decreased further to 0.00087 mg m−2 s−1, accounting for approximately one-third of the flux in the TSs. A similar reduction from the TSs to ASs was observed in the HPE from 16 to 22 December 2016 in GC. It can be seen that from the TS to the AS, the aerosol vertical turbulent flux decreased, but the aerosol particle concentration within the surface layer increased, and it is inferred that in addition to the contribution of regional transport from upwind areas during the TS, suppression of vertical turbulence mixing confining aerosols to a shallow boundary layer increased accumulation.


2008 ◽  
Vol 8 (21) ◽  
pp. 6355-6363 ◽  
Author(s):  
Y. Wang ◽  
M. B. McElroy ◽  
J. W. Munger ◽  
J. Hao ◽  
H. Ma ◽  
...  

Abstract. Large intra-season differences in mixing ratios of CO and O3 were detected at Miyun, a rural site north of Beijing, in summer 2006. Despite an increase in mean daytime mixing ratio of CO from 500 ppbv in June to 700 ppbv in July, mean daytime O3 dropped from 67 ppbv in June to 50 ppbv in July and August. The observed changes in CO and O3 are attributed to the influence of the summer monsoonal circulation that develops over the North China Plain in July. Photochemical production of O3 is reduced as a consequence of increased cloudiness during July and August, as indicated by the strong negative correlation observed between O3 and satellite observations of cloud optical depth, with cloudiness having little effect on CO. The analysis suggests a strategy for emission controls that could be implemented in an economically efficient manner to minimize the frequency of high levels of O3 during summer in Beijing.


2016 ◽  
Vol 16 (17) ◽  
pp. 10985-11000 ◽  
Author(s):  
Yin Wang ◽  
Zhongming Chen ◽  
Qinqin Wu ◽  
Hao Liang ◽  
Liubin Huang ◽  
...  

Abstract. Measurements of atmospheric peroxides were made during Wangdu Campaign 2014 at Wangdu, a rural site in the North China Plain (NCP) in summer 2014. The predominant peroxides were detected to be hydrogen peroxide (H2O2), methyl hydroperoxide (MHP) and peroxyacetic acid (PAA). The observed H2O2 reached up to 11.3 ppbv, which was the highest value compared with previous observations in China at summer time. A box model simulation based on the Master Chemical Mechanism and constrained by the simultaneous observations of physical parameters and chemical species was performed to explore the chemical budget of atmospheric peroxides. Photochemical oxidation of alkenes was found to be the major secondary formation pathway of atmospheric peroxides, while contributions from alkanes and aromatics were of minor importance. The comparison of modeled and measured peroxide concentrations revealed an underestimation during biomass burning events and an overestimation on haze days, which were ascribed to the direct production of peroxides from biomass burning and the heterogeneous uptake of peroxides by aerosols, respectively. The strengths of the primary emissions from biomass burning were on the same order of the known secondary production rates of atmospheric peroxides during the biomass burning events. The heterogeneous process on aerosol particles was suggested to be the predominant sink for atmospheric peroxides. The atmospheric lifetime of peroxides on haze days in summer in the NCP was about 2–3 h, which is in good agreement with the laboratory studies. Further comprehensive investigations are necessary to better understand the impact of biomass burning and heterogeneous uptake on the concentration of peroxides in the atmosphere.


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