scholarly journals Measurement report: Fast photochemical production of peroxyacetyl nitrate (PAN) over the rural North China Plain during haze events in autumn

2021 ◽  
Vol 21 (23) ◽  
pp. 17995-18010
Author(s):  
Yulu Qiu ◽  
Zhiqiang Ma ◽  
Ke Li ◽  
Mengyu Huang ◽  
Jiujiang Sheng ◽  
...  
Keyword(s):  
North China Plain ◽  
North China ◽  
Cold Season ◽  
Rural Site ◽  
Dominant Factor ◽  
Urban Region ◽  
Chemical Production ◽  
Peroxyacetyl Nitrate ◽  
Photochemical Pollution ◽  
Acetaldehyde Oxidation

Abstract. Photochemical pollution over the North China Plain (NCP) is attracting much concern. We usually view peroxyacetyl nitrate (PAN) as the second most important photochemical pollutant featuring high mixing ratios during warm seasons. Our observations at a background site in the NCP identified high PAN concentrations, even during haze events in autumn. The substantial increasing ratios of PAN, by 244 % and 178 %, over the morning hours (08:00–12:00 local time) on 20 and 25 October 2020 were 10.6 and 7.7 times larger than those on clean days. Polluted days are characterized by higher temperature, higher humidity, and anomalous southerly winds compared with clean days. Enhanced local photochemistry has been identified as being the dominant factor that controls the PAN increase in the morning at the rural site, as the time when prevailing wind turns to a southerly wind is too late to promote direct transport of PAN from the polluted urban region. By removing the effect of direct transport of PAN, we provide a quantitative assessment of net PAN chemical production rate of 0.45 ppb h−1 for the mornings of polluted days, also demonstrating the strong local photochemistry. Using observations and calculated photolysis rates, we find that acetaldehyde oxidation by hydroxyl radical (OH) is the primary pathway of peroxyacetyl radical formation at the rural site. Acetaldehyde concentrations and production rates of HOx (HOx= OH + HO2) on polluted days are 2.8 and 2 times as large as those on clean days, leading to a remarkable increase in PAN in the morning. Formaldehyde (HCHO) photolysis dominates the daytime HOx production, thus contributing to fast photochemistry of PAN. Our observational results suggest the cause of a rapid increase in PAN during haze events in autumn at a rural site of the NCP and provide evidence of important role of HCHO photolysis in secondary pollutants at lower nitrogen oxide emissions. This highlights the urgency of carrying out strict volatile organic compound controls over the NCP during the cold season and not just in summer.

scholarly journals Measurement report: Fast photochemical production of peroxyacetyl nitrate (PAN) over the rural North China Plain during cold-season haze events

2021 ◽  
Author(s):  
Yulu Qiu ◽  
Zhiqiang Ma ◽  
Ke Li ◽  
Mengyu Huang ◽  
Jiujiang Sheng ◽  
...  
Keyword(s):  
North China Plain ◽  
North China ◽  
Cold Season ◽  
Rural Site ◽  
Dominant Factor ◽  
Urban Region ◽  
Chemical Production ◽  
Peroxyacetyl Nitrate ◽  
Photochemical Pollution ◽  
Mixing Ratios

Abstract. Photochemical pollution over the North China Plain (NCP) are attracting considerable concern. Peroxyacetyl nitrate (PAN) is usually viewed as the second most important photochemical pollutant featuring high mixing ratios during warm seasons. Our observations at a background site in the NCP identified high PAN concentrations even during cold-season haze events. The abrupt increasing rates of PAN by 244 % and 178 % over the morning hours (8:00–12:00) on 10/20 and 10/25, 2020 were 10.6 and 7.7 times those on clean days. The pollution days were characterized by higher temperature and humidity, accompanied by anomalous southerlies. Enhanced local photochemistry has been identified as the dominant factor that controls PAN increase in the morning at the rural site, as the time when prevailing wind turned to southerlies was too late to facilitate direct transport of PAN from the polluted urban region. By removing the effect of direct transport of PAN, we provide a quantitative assessment of net PAN chemical production rate of 0.45 ppb h−1 on the polluted morning, also demonstrating the strong local photochemistry. Using observations and calculated photolysis rates, we find that oxidation of acetaldehyde by hydroxyl radical (OH) is the primary pathway of peroxyacetyl radical formation at the rural site. Acetaldehyde concentrations and production rates of HOx (HOx = OH + HO2) radical on pollution days were 2.8 and 2 times that on clean days, respectively, leading to the abrupt increase of PAN in the morning. Formaldehyde (HCHO) photolysis dominates the daytime HOx production thus contributing to fast photochemistry of PAN. Our observational results fully explain the cause of rapid increase of PAN during cold days at a rural site of the NCP, as well as provide the evidence of important role of HCHO photolysis in secondary pollutants at lower nitrogen oxide emissions. This highlights the imperative to implement strict volatile organic compounds controls out of summer seasons over the NCP.

Size-resolved effective density of submicron aerosol particles in the North China Plain

2021 ◽  
Author(s):  
Yaqing Zhou ◽  
Nan Ma ◽  
Zhibin Wang ◽  
Jiangchuan Tao ◽  
Juan Hong ◽  
...  
Keyword(s):  
North China Plain ◽  
North China ◽  
Aerosol Particles ◽  
Cold Season ◽  
Effective Density ◽  
Spherical Particles ◽  
Rural Site ◽  
Mass Analyzer ◽  
The North ◽  
The North China Plain

<p>Effective density is one of the most important physical properties of atmospheric aerosol particles, and is linked to particle formation and aging process. Combined characterization of aerosol density, chemical composition, emission and aging processes may provide crucial information for better understanding their interactions and effects on environment and climate. In autumn of 2019, the effective density of sub-micrometer aerosol particles was measured in-situ at a heavily polluted rural site in the North China Plain (NCP). A tandem technique coupling a Centrifugal Particle Mass Analyzer (CPMA) with a differential mobility analyzer (DMA) and a Condensation Particle Counter (CPC) were used to determine the effective density of ambient aerosol particles with diameters of 50, 100, 150, 220 and 300 nm. The probability distribution of effective density exhibits double peak modes in majority cases, with a higher density mode (main-density) and a lower density mode (sub-density). The existence of sub-density particles normally ascribed to freshly emitted or partial aged black carbon (BC) with non-spherical morphology. The number fraction of sub-density mode varies from 4% to 67%, with mean of 22-27% at five particle sizes. Due to the higher aging degree of larger particles, the main-density exhibits an evident ascending trend with particle size. However, the sub-density decreases as mobility size increases, from 0.89 g/cm<sup>3</sup> at 50 nm to 0.62 g/cm<sup>3</sup> at 300 nm, since larger fresh soot particles usually present a more agglomerated morphology than small particles. A comparison was carried out between the mean effective density at 300 nm and ACSM-derived density using different approximations of BC density. The best agreement is achieved when assuming a BC density of 0.6 g/cm<sup>3</sup>, indicating that BC typically exists as non-spherical particles with fractal-like or porous morphology in the NCP in cold season.</p>

Aerosol Promotes Peroxyacetyl Nitrate Formation During Winter in the North China Plain

2021 ◽  
Author(s):  
Wanyun Xu ◽  
Gen Zhang ◽  
Ying Wang ◽  
Shengrui Tong ◽  
Wenqian Zhang ◽  
...  
Keyword(s):  
North China Plain ◽  
North China ◽  
Peroxyacetyl Nitrate ◽  
The North ◽  
The North China Plain

scholarly journals Measuring the Vertical Profiles of Aerosol Extinction in the Lower Troposphere by MAX-DOAS at a Rural Site in the North China Plain

Atmosphere ◽  
2020 ◽  
Vol 11 (10) ◽  
pp. 1037
Author(s):  
Siyang Cheng ◽  
Junli Jin ◽  
Jianzhong Ma ◽  
Xiaobin Xu ◽  
Liang Ran ◽  
...  
Keyword(s):  
North China Plain ◽  
North China ◽  
Lower Troposphere ◽  
Temporal Variations ◽  
Rural Site ◽  
Optical Absorption Spectroscopy ◽  
Aerosol Extinction ◽  
Vertical Profiles ◽  
Near Surface ◽  
The North

Ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements were performed during the summer (13 June–20 August) of 2014 at a rural site in North China Plain. The vertical profiles of aerosol extinction (AE) in the lower troposphere were retrieved to analyze the temporal variations of AE profiles, near-surface AE, and aerosol optical depth (AOD). The average AOD and near-surface AE over the period of study were 0.51 ± 0.26 and 0.33 ± 0.18 km−1 during the effective observation period, respectively. High AE events and elevated AE layers were identified based on the time series of hourly AE profiles, near-surface AEs and AODs. It is found that in addition to the planetary boundary layer height (PBLH) and relative humidity (RH), the variations in the wind field have large impacts on the near-surface AE, AOD, and AE profile. Among 16 wind sectors, higher AOD or AE occur mostly in the directions of the cities upstream. The diurnal variations of the AE profiles, AODs and near-surface AEs are significant and influenced mainly by the source emissions, PBLH, and RH. The AE profile shape from MAX-DOAS measurement is generally in agreement with that from light detection and ranging (lidar) observations, although the AE absolute levels are different. Overall, ground-based MAX-DOAS can serve as a supplement to measure the AE vertical profiles in the lower troposphere.

scholarly journals Aerosol vertical mass flux measurements during heavy aerosol pollution episodes at a rural site and an urban site in the Beijing area of the North China Plain

2019 ◽  
Vol 19 (20) ◽  
pp. 12857-12874 ◽  
Author(s):  
Renmin Yuan ◽  
Xiaoye Zhang ◽  
Hao Liu ◽  
Yu Gui ◽  
Bohao Shao ◽  
...  
Keyword(s):  
Mass Flux ◽  
North China Plain ◽  
North China ◽  
Rural Site ◽  
Urban Site ◽  
The North ◽  
The North China Plain ◽  
Aerosol Pollution ◽  
The Mean ◽  
Pollution Episodes

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.

Observation of ambient NO3 radicals by LP-DOAS at a rural site in North China Plain

2022 ◽  
Vol 804 ◽  
pp. 149680
Author(s):  
Xue Lu ◽  
Min Qin ◽  
Pinhua Xie ◽  
Jun Duan ◽  
Wu Fang ◽  
...  
Keyword(s):  
North China Plain ◽  
North China ◽  
Rural Site

scholarly journals Lower tropospheric distributions of O<sub>3</sub> and aerosol over Raoyang, a rural site in the North China Plain

2017 ◽  
Vol 17 (6) ◽  
pp. 3891-3903 ◽  
Author(s):  
Rui Wang ◽  
Xiaobin Xu ◽  
Shihui Jia ◽  
Ruisheng Ma ◽  
Liang Ran ◽  
...  
Keyword(s):  
Mixed Layer ◽  
North China Plain ◽  
Lower Troposphere ◽  
Number Concentration ◽  
Residual Layer ◽  
Rural Site ◽  
Vertical Profiles ◽  
Photochemical Pollution ◽  
The North ◽  
Aerosol Number Concentration

Abstract. The North China Plain (NCP) has become one of the most polluted regions in China, with the rapidly increasing economic growth in the past decades. High concentrations of ambient O3 and aerosol have been observed at urban as well as rural sites in the NCP. Most of the in situ observations of air pollutants have been conducted near the ground so that current knowledge about the vertical distributions of tropospheric O3 and aerosol over the NCP region is still limited. In this study, vertical profiles of O3 and size-resolved aerosol concentrations below 2.5 km were measured in summer 2014 over a rural site in the NCP, using an unmanned aerial vehicle (UAV) equipped with miniature analyzers. In addition, vertical profiles of aerosol scattering property in the lower troposphere and vertical profiles of O3 below 1 km were also observed at the site using a lidar and tethered balloon, respectively. The depths of the mixed layer and residual layer were determined according to the vertical gradients of lidar particle extinction and aerosol number concentration. Average O3 and size-resolved aerosol number concentration in both the mixed and residual layer were obtained from the data observed in seven UAV flights. The results show that during most of the flights the O3 levels above the top of mixed layer were higher than those below. Such a positive gradient in the vertical distribution of O3 makes the residual layer an important source of O3 in the mixed layer, particularly during the morning when the top of mixed layer is rapidly elevated. In contrast to O3, aerosol number concentration was normally higher in the mixed layer than in the residual layer, particularly in the early morning. Aerosol particles were overwhelmingly distributed in the size range  <  1 µm, showing slight differences between the mixed and residual layers. Our measurements confirm that the lower troposphere over the rural area of the NCP is largely impacted by anthropogenic pollutants locally emitted or transported from urban areas. Compared with the historic O3 vertical profiles over Beijing from the Measurement of Ozone and Water Vapor by Airbus In-Service Aircraft (MOZAIC), a strong increase in O3 can be found at all heights below 2.5 km in the decade from 2004 to 2014, with the largest enhancement of about 41.6 ppb. This indicates that the lower troposphere over the northern part of the NCP has experienced rapidly worsening photochemical pollution. This worsening trend in photochemical pollution deserves more attention in the future.

scholarly journals Variations of O<sub>3</sub> and CO in summertime at a rural site near Beijing

2008 ◽  
Vol 8 (21) ◽  
pp. 6355-6363 ◽  
Author(s):  
Y. Wang ◽  
M. B. McElroy ◽  
J. W. Munger ◽  
J. Hao ◽  
H. Ma ◽  
...  
Keyword(s):  
North China Plain ◽  
North China ◽  
Rural Site ◽  
Mixing Ratio ◽  
Efficient Manner ◽  
Strong Negative Correlation ◽  
Cloud Optical Depth ◽  
Mixing Ratios ◽  
The North ◽  
The North China Plain

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.

scholarly journals Organic aerosol volatility and viscosity in North China Plain: Contrast between summer and winter

2020 ◽  
Author(s):  
Weiqi Xu ◽  
Chun Chen ◽  
Yanmei Qiu ◽  
Ying Li ◽  
Zhiqiang Zhang ◽  
...  
Keyword(s):  
Coal Combustion ◽  
North China Plain ◽  
North China ◽  
Organic Aerosol ◽  
Rural Site ◽  
Urban Site ◽  
Aerosol Mass ◽  
Effective Saturation ◽  
Formation And Evolution ◽  
Primary Emissions

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 North China Plain (NCP) in summer and winter were investigated by using a thermodenuder coupled with 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 NCP is more volatile due to enhanced primary emissions from coal combustion and biomass burning. The volatility distributions varied largely different among different OA factors. In particular, we found that hydrocarbon-like OA (HOA) contained more non-volatile 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, but as semi-solids in Beijing in summer and Gucheng in winter. These results have important implications that kinetically limited gas-particle partitioning may need to be considered when simulating secondary OA formation in NCP.

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