scholarly journals Explosive Secondary Aerosol Formation during Severe Haze in the North China Plain

2021 ◽  
Vol 55 (4) ◽  
pp. 2189-2207
Author(s):  
Jianfei Peng ◽  
Min Hu ◽  
Dongjie Shang ◽  
Zhijun Wu ◽  
Zhuofei Du ◽  
...  
2019 ◽  
Vol 6 (9) ◽  
pp. 1675-1693 ◽  
Author(s):  
Baozhu Ge ◽  
Xiaobin Xu ◽  
Zhiqiang Ma ◽  
Xiaole Pan ◽  
Zhe Wang ◽  
...  

2020 ◽  
Vol 257 ◽  
pp. 113621 ◽  
Author(s):  
Ye Kuang ◽  
Wanyun Xu ◽  
Weili Lin ◽  
Zhaoyang Meng ◽  
Huarong Zhao ◽  
...  

2020 ◽  
Author(s):  
Tao Ma ◽  
Hiroshi Furutani ◽  
Fengkui Duan ◽  
Takashi Kimoto ◽  
Jingkun Jiang ◽  
...  

Abstract. Severe winter hazes accompanied by high concentrations of fine particulate matter (PM2.5) occur frequently in the North China Plain and threaten public health. Organic matter (OM) and sulfate are recognized as major components of PM2.5, while atmospheric models often fail to predict their high concentrations during severe winter hazes due to incomplete understanding of secondary aerosol formation mechanisms. By using a novel combination of single particle mass spectrometer and optimized ion chromatography measurement, here we show that hydroxymethanesulfonate (HMS), formed by the reaction between formaldehyde (HCHO) and dissolved SO2 in aerosol water, is ubiquitous in Beijing winter. The HMS concentration and the molar ratio of HMS to sulfate increased with the deterioration of winter haze. High concentrations of precursors (SO2 and HCHO) coupled with low oxidant levels, low temperature, high relative humidity, and moderately acid pH facilitate the heterogeneous formation of HMS, which could account for up to 15 % of OM in winter haze and lead to 36 % overestimates of sulfate when using traditional ion chromatography measurements. Despite the clean air actions have substantially reduced SO2 emissions, HMS concentration and molar ratio of HMS to sulfate during severe winter hazes increased from 2015 to 2016 with the growth of HCHO concentration. Our findings illustrate the significant contribution of heterogeneous HMS chemistry to severe winter hazes in Beijing, which help to improve the prediction of OM and sulfate, and suggest that the reduction in HCHO can help to mitigate haze pollution.


2013 ◽  
Vol 13 (24) ◽  
pp. 12495-12506 ◽  
Author(s):  
Z. B. Wang ◽  
M. Hu ◽  
J. Y. Sun ◽  
Z. J. Wu ◽  
D. L. Yue ◽  
...  

Abstract. Long-term measurements of particle number size distributions were carried out both at an urban background site (Peking University, PKU) and a regional Global Atmospheric Watch station (Shangdianzi, SDZ) from March to November in 2008. In total, 52 new particle formation (NPF) events were observed simultaneously at both sites, indicating that this is a regional phenomenon in the North China Plain. On average, the mean condensation sink value before the nucleation events started was 0.025 s−1 in the urban environment, which was 1.6 times higher than that at regional site. However, higher particle formation and growth rates were observed at PKU (10.8 cm−3 s−1 and 5.2 nm h−1) compared with those at SDZ (4.9 cm−3 s−1 and 4.0 nm h−1). These results implied that precursors were much more abundant in the polluted urban environment. Different from the observations in cleaner environments, the background conditions of the observed particle homogeneous nucleation events in the North China Plain could be characterized as the co-existing of a stronger source of precursor gases and a higher condensational sink of pre-existing aerosol particles. Secondary aerosol formation following nucleation events results in an increase of particle mass concentration, particle light scattering coefficient, and cloud condensation nuclei (CCN) number concentration, with consequences on visibility, radiative effects, and air quality. Typical regional NPF events with significant particle nucleation rates and subsequent particle growth over a sufficiently long time period at both sites were chosen to investigate the influence of NPF on the number concentration of "potential" CCN. As a result, the NPF and the subsequent condensable growth increased the CCN number concentration in the North China Plain by factors in the range from 5.6 to 8.7. Moreover, the potential contribution of anthropogenic emissions to the CCN number concentration was more than 50%, to which more attention should be drawn in regional and global climate modeling, especially in the polluted urban areas.


2017 ◽  
Vol 17 (20) ◽  
pp. 12361-12378 ◽  
Author(s):  
Zhe Wang ◽  
Weihao Wang ◽  
Yee Jun Tham ◽  
Qinyi Li ◽  
Hao Wang ◽  
...  

Abstract. Dinitrogen pentoxide (N2O5) and nitryl chloride (ClNO2) are key species in nocturnal tropospheric chemistry and have significant effects on particulate nitrate formation and the following day's photochemistry through chlorine radical production and NOx recycling upon photolysis of ClNO2. To better understand the roles of N2O5 and ClNO2 in the high-aerosol-loading environment of northern China, an intensive field study was carried out at a high-altitude site (Mt. Tai, 1465 m a.s.l.) in the North China Plain (NCP) during the summer of 2014. Elevated ClNO2 plumes were frequently observed in the nocturnal residual layer with a maximum mixing ratio of 2.1 ppbv (1 min), whilst N2O5 was typically present at very low levels (< 30 pptv), indicating fast heterogeneous N2O5 hydrolysis. Combined analyses of chemical characteristics and backward trajectories indicated that the ClNO2-laden air was caused by the transport of NOx-rich plumes from the coal-fired industry and power plants in the NCP. The heterogeneous N2O5 uptake coefficient (γ) and ClNO2 yield (ϕ) were estimated from steady-state analysis and observed growth rate of ClNO2. The derived γ and ϕ exhibited high variability, with means of 0.061 ± 0.025 and 0.28 ± 0.24, respectively. These values are higher than those derived from previous laboratory and field studies in other regions and cannot be well characterized by model parameterizations. Fast heterogeneous N2O5 reactions dominated the nocturnal NOx loss in the residual layer over this region and contributed to substantial nitrate formation of up to 17 µg m−3. The estimated nocturnal nitrate formation rates ranged from 0.2 to 4.8 µg m−3 h−1 in various plumes, with a mean of 2.2  ± 1.4 µg m−3 h−1. The results demonstrate the significance of heterogeneous N2O5 reactivity and chlorine activation in the NCP, and their unique and universal roles in fine aerosol formation and NOx transformation, and thus their potential impacts on regional haze pollution in northern China.


2020 ◽  
Vol 20 (10) ◽  
pp. 5887-5897 ◽  
Author(s):  
Tao Ma ◽  
Hiroshi Furutani ◽  
Fengkui Duan ◽  
Takashi Kimoto ◽  
Jingkun Jiang ◽  
...  

Abstract. Severe winter haze accompanied by high concentrations of fine particulate matter (PM2.5) occurs frequently in the North China Plain and threatens public health. Organic matter (OM) and sulfate are recognized as major components of PM2.5, while atmospheric models often fail to predict their high concentrations during severe winter haze due to incomplete understanding of secondary aerosol formation mechanisms. By using a novel combination of single-particle mass spectrometry and an optimized ion chromatography method, here we show that hydroxymethanesulfonate (HMS), formed by the reaction between formaldehyde (HCHO) and dissolved SO2 in aerosol water, is ubiquitous in Beijing during winter. The HMS concentration and the molar ratio of HMS to sulfate increased with the deterioration of winter haze. High concentrations of precursors (SO2 and HCHO) coupled with low oxidant levels, low temperature, high relative humidity, and moderately acidic pH facilitate the heterogeneous formation of HMS, which could account for up to 15 % of OM in winter haze and lead to up to 36 % overestimates of sulfate when using traditional ion chromatography. Despite the clean air actions having substantially reduced SO2 emissions, the HMS concentration and molar ratio of HMS to sulfate during severe winter haze increased from 2015 to 2016 with the growth in HCHO concentration. Our findings illustrate the significant contribution of heterogeneous HMS chemistry to severe winter haze in Beijing, which helps to improve the prediction of OM and sulfate and suggests that the reduction in HCHO can help to mitigate haze pollution.


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