scholarly journals Seasonal variations in the high time-resolved aerosol composition, sources, and chemical process of background submicron particles in North China Plain

2020 ◽  
Author(s):  
Jiayun Li ◽  
Liming Cao ◽  
Wenkang Gao ◽  
Lingyan He ◽  
Yingchao Yan ◽  
...  
Keyword(s):  
Aqueous Phase ◽  
Seasonal Variations ◽  
North China Plain ◽  
North China ◽  
Organic Aerosol ◽  
Submicron Particles ◽  
Western China ◽  
Aerosol Composition ◽  
Oxidation Degree ◽  
Four Seasons

Abstract. For the first time in the North China Plain (NCP), we investigated the seasonal variations of submicron particles (NR-PM1) and its chemical composition at a background mountain station using Aerodyne high-resolution time-of-flight aerosol mass spectrometry (HR-ToF-AMS). The averaged NR-PM1 were highest in autumn (15.1 μg m−3) and lowest in summer (12.4 μg m−3), with the abundance of more nitrate in spring (34 %), winter (31 %), and autumn (34 %), and elevated organics (40 %) and sulfate (38 %) proportion in summer. The submicron particles were almost neutralized by excess ammonium in all four seasons except summer, when the aerosol particles appeared to be slightly acidic. The size distribution of all PM1 species showed a consistent accumulation mode peaked at approximately 600–800 nm (dva), indicating the highly aged and internally mixed nature of the background aerosols, which further supported by the source appointment using multilinear engine (ME-2) and significant contributions of aged secondary organic aerosol (SOA) in organic aerosol (OA) were resolved in all seasons (> 77 %), especially in summer (95 %). The oxidation degree and evolution process of OAs in the four seasons were further investigated, and enhanced carbon oxidation state (−0.45–0.10), O / C (0.54–0.75) and OM / OC (1.86–2.13) ratios compared with urban studies were observed, with the highest oxidation degree of which appeared in summer, likely due to the relatively stronger photochemical processing which dominated the processes of both less oxidized OA (LO-OOA) and more oxidized OA (MO-OOA) formations. Aqueous-phase processing also contributed to the SOA formation but prevailed in autumn and winter and the role of which to MO-OOA and LO-OOA also varied in different seasons. In addition, compared with the urban atmosphere, LO-OOA formation in the background atmosphere exhibited more regional characteristics, as photochemical and aqueous-phase processing enhanced during the transport in summer and autumn, respectively. Furthermore, the backward trajectories analysis showed that higher submicron particles were associated with air mass for short distance transported from the southern regions in four seasons, while the long-range transport from Inner Mongolia (west and north regions) also contributed to the summer particle pollutions in the background areas of NCP. Our results illustrate the background particles in NCP are influenced significantly by aging processing and transport, and the more neutralized state of submicron particles with the abundance of nitrate compared with those in the background atmosphere in southern and western China, highlighting the regional reductions in emissions of nitrogen oxide and ammonia are critical for remedying the increased occurrence of nitrate-dominated haze event in the NCP.

scholarly journals Seasonal variations in the highly time-resolved aerosol composition, sources and chemical processes of background submicron particles in the North China Plain

2021 ◽  
Vol 21 (6) ◽  
pp. 4521-4539
Author(s):  
Jiayun Li ◽  
Liming Cao ◽  
Wenkang Gao ◽  
Lingyan He ◽  
Yingchao Yan ◽  
...  
Keyword(s):  
Oxidation State ◽  
Seasonal Variations ◽  
North China Plain ◽  
North China ◽  
Organic Aerosol ◽  
Submicron Particles ◽  
Regional Transport ◽  
The North ◽  
The North China Plain ◽  
Four Seasons

Abstract. For the first time in the North China Plain (NCP) region, we investigated the seasonal variations in submicron particles (NR-PM1) and their chemical composition at a background mountainous site of Xinglong using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer. The average concentration of NR-PM1 was highest in autumn (15.1 µg m−3) and lowest in summer (12.4 µg m−3), with a greater abundance of nitrate in spring (34 %), winter (31 %) and autumn (34 %) and elevated organics (40 %) and sulfate (38 %) in summer. PM1 in Xinglong showed higher acidity in summer and moderate acidity in spring, autumn and winter, with average pH values of 2.7±0.6, 4.2±0.7, 3.5±0.5 and 3.7±0.6, respectively, which is higher than those estimated in the United States and Europe. The size distribution of all PM1 species showed a consistent accumulation mode peaking at approximately 600–800 nm (dva), indicating a highly aged and internally mixed nature of the background aerosols, which was further supported by the source appointment results using positive matrix factorization and multilinear engine analysis. Significant contributions of aged secondary organic aerosol (SOA) in organic aerosol (OA) were resolved in all seasons (>77 %), especially in summer. The oxidation state and the process of evolution of OAs in the four seasons were further investigated, and an enhanced carbon oxidation state (−0.45–0.10) and O/C (0.54–0.75) and OM/OC (1.86–2.13) ratios – compared with urban studies – were observed, with the highest oxidation state appearing in summer, likely because of the relatively stronger photochemical processing that dominated the formation processes of both less oxidized OA (LO-OOA) and more oxidized OA (MO-OOA). Aqueous-phase processing also contributed to the SOA formation and prevailed in winter, with the share to MO-OOA being more important than that to LO-OOA. In addition, regional transport also played an important role in the variations in SOA. Especially in summer, continuous increases in SOA concentration as a function of odd oxygen (Ox=O3+NO2) were found to be associated with the increases in wind speed. Furthermore, backward trajectory analysis showed that higher concentrations of submicron particles were associated with air masses transported short distances from the southern regions in all four seasons, while long-range transport from Inner Mongolia (western and northern regions) also contributed to summertime particulate pollution in the background areas of the NCP. Our results illustrate that the background particles in the NCP are influenced significantly by aging processes and regional transport, and the increased contribution of aerosol nitrate highlights how regional reductions in nitrogen oxide emissions are critical for remedying occurrence of nitrate-dominated haze events over the NCP.

Photochemical Aqueous-Phase Reactions Induce Rapid Daytime Formation of Oxygenated Organic Aerosol on the North China Plain

2020 ◽  
Vol 54 (7) ◽  
pp. 3849-3860 ◽  
Author(s):  
Ye Kuang ◽  
Yao He ◽  
Wanyun Xu ◽  
Bin Yuan ◽  
Gen Zhang ◽  
...  
Keyword(s):  
Aqueous Phase ◽  
North China Plain ◽  
North China ◽  
Organic Aerosol ◽  
The North ◽  
The North China Plain

scholarly journals Size-resolved characterization of organic aerosol in the North China Plain: new insights from high resolution spectral analysis

2021 ◽  
Author(s):  
Weiqi Xu ◽  
Chun Chen ◽  
Yanmei Qiu ◽  
Conghui Xie ◽  
Yunle Chen ◽  
...  
Keyword(s):  
Radiative Forcing ◽  
North China Plain ◽  
North China ◽  
Fine Particles ◽  
Large Fraction ◽  
Organic Aerosol ◽  
Size Distributions ◽  
The North ◽  
The Impact

Organic aerosol (OA), a large fraction of fine particles, has a large impact on climate radiative forcing and human health, and the impact depends strongly on size distributions. Here we...

scholarly journals Diurnal variations of organic molecular tracers and stable carbon isotopic compositions in atmospheric aerosols over Mt. Tai in North China Plain: an influence of biomass burning

2012 ◽  
Vol 12 (4) ◽  
pp. 9079-9124
Author(s):  
P. Q. Fu ◽  
K. Kawamura ◽  
J. Chen ◽  
J. Li ◽  
Y. L. Sun ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Biomass Burning ◽  
North China Plain ◽  
North China ◽  
Secondary Organic Aerosol ◽  
Organic Aerosol ◽  
Total Carbon ◽  
Stable Carbon ◽  
Isotopic Compositions ◽  
Carbon Isotopic

Abstract. Organic tracer compounds of tropospheric aerosols, as well as organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC), and stable carbon isotope ratios (δ13C) of total carbon (TC) have been investigated for aerosol samples collected during early and late periods of Mount Tai eXperiment 2006 (MTX2006) field campaign in North China Plain. Total solvent extracts were investigated by gas chromatography/mass spectrometry. More than 130 organic compounds were detected in the aerosol samples. They were grouped into twelve organic compound classes, including biomass burning tracers, biogenic primary sugars, biogenic secondary organic aerosol (SOA) tracers, and anthropogenic tracers such as phthalates, hopanes and polycyclic aromatic hydrocarbons (PAHs). In early June when the field burning activities of wheat straws in North China Plain were very active, the total identified organics (2090 ± 1170 ng m−3) were double those in late June (926 ± 574 ng m−3). All the compound classes were more abundant in early June than in late June, except phthalate esters, which were higher in late June. Levoglucosan (88–1210 ng m−3, 403 ng m−3) was found as the most abundant single compound in early June, while diisobutyl phthalate was the predominant species in late June. During the biomass-burning period in early June, the diurnal trends of most of the primary and secondary organic aerosol tracers were characterized by the concentration peaks observed at mid-night or in early morning, while in late June most of the organic species peaked in late afternoon. This suggests that smoke plumes from biomass burning can uplift the aerosol particulate matter to a certain altitude and then transported to and encountered the summit of Mt. Tai during nighttime. On the basis of the tracer-based method for the estimation of biomass-burning OC, fungal-spore OC and biogenic secondary organic carbon (SOC), we estimate that an average of 24% (up to 64%) of the OC in the Mt. Tai aerosols was due to biomass burning in early June, followed by the contribution of isoprene SOC (mean 4.3%). In contrast, isoprene SOC was the main contributor (6.6%) to OC, and only 3.0% of the OC was due to biomass burning in late June. In early June, δ13C of TC (−26.6‰ to −23.2‰, mean −25.0‰) were lower than those (−23.9‰ to −21.9‰, mean −22.9‰) in late June. In addition, a strong anti-correlation was found between levoglucosan and δ13C values. This study demonstrates that crop-residue burning activities can significantly enhance the organic aerosol loading and alter the organic molecular compositions and stable carbon isotopic compositions of aerosol particles in the troposphere over North China Plain.

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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