The promotion effect of nitrous acid on aerosol formation in wintertime in Beijing: the possible contribution of traffic-related emissions

Liu, Yongchun; Zhang, Yusheng; Lian, Chaofan; Yan, Chao; Feng, Zeming; Zheng, Feixue; Fan, Xiaolong; Wang, Weigang; Chu, Biwu; Wang, Yonghong; Cai, Jing; Du, Wei; Daellenbach, Kaspar R.; Kangasluoma, Juha; Bianchi, Federico; Kujansuu, Joni; Petäj̈ä, Tuukka; Wang, Xuefei; Hu, Bo; Wang, Yuesi; Ge, Maofa; He, Hong; Kulmala, Markku

doi:10.5194/acp-20-13023-2020

Cited by 47 publications

(47 citation statements)

References 109 publications

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“…Several studies have proposed out that NO 2 can promote the oxidation of SO 2 on particle surfaces and in aqueous phase. For example, laboratory studies have found that parts per million (ppm) levels of NO 2 can promote sulfate formation on the surface of dust through NO + NO − 3 which is disproportionated from N 2 O 4 intermediate (He et al, 2014;Liu et al, 2012;Ma et al, 2008) or parts per million levels of NO 2 can promote the oxidation of SO 2 in the deliquesced oxalic acid (Wang et al, 2016). This is supported by the evidence that a high fraction of sulfate in PM 2.5 is positively correlated with NO 2 concentration (Xie et al, 2015) and that a high PM 2.5 concentration is accompanied with high ratio of NO 2 /SO 2 in several case studies (He et al, 2014).…”

Section: Influence Of Other Factors On Sulfate Formationmentioning

confidence: 99%

Ammonium nitrate promotes sulfate formation through uptake kinetic regime

et al. 2021

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Abstract. Although the anthropogenic emissions of SO2 have decreased significantly in China, the decrease in SO42- in PM2.5 is much smaller than that of SO2. This implies an enhanced formation rate of SO42- in the ambient air, and the mechanism is still under debate. This work investigated the formation mechanism of particulate sulfate based on statistical analysis of long-term observations in Shijiazhuang and Beijing supported with flow tube experiments. Our main finding was that the sulfur oxidation ratio (SOR) was exponentially correlated with ambient RH in Shijiazhuang (SOR = 0.15+0.0032×exp⁡(RH/16.2)) and Beijing (SOR = -0.045+0.12×exp⁡(RH/37.8)). In Shijiazhuang, the SOR is linearly correlated with the ratio of aerosol water content (AWC) in PM2.5 (SOR = 0.15+0.40×AWC/PM2.5). Our results suggest that uptake of SO2 instead of oxidation of S(IV) in the particle phase is the rate-determining step for sulfate formation. NH4NO3 plays an important role in the AWC and the change of particle state, which is a crucial factor determining the uptake kinetics of SO2 and the enhanced SOR during haze days. Our results show that NH3 significantly promoted the uptake of SO2 and subsequently the SOR, while NO2 had little influence on SO2 uptake and SOR in the presence of NH3.

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Section: Influence Of Other Factors On Sulfate Formationmentioning

confidence: 99%

Ammonium nitrate promotes sulfate formation through uptake kinetic regime

et al. 2021

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“…High concentrations of aerosol particles obscure downward radiation, as a result of which the surface temperature and sensitive heat flux decrease and the development of mixing layer height is sup-pressed. Recent studies have gradually realised that the facilitation of various chemical processes plays a non-negligible role in the aerosol-radiation-boundary layer feedback (Liu et al, 2018;Z. Liu.…”

Section: Typical Case Of Rapid Aerosol Mass Growth Episodes Affected By Aerosol-chemistry-boundary Layer Interactionsmentioning

confidence: 99%

“…During winter haze episodes, a rapid growth of the aerosol mass concentration has commonly been observed, and this phenomenon seems to be directly affected by meteorological factors (J. Liu et al, 2018;Z. Liu et al, 2019;.…”

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confidence: 99%

Rapid mass growth and enhanced light extinction of atmospheric aerosols during the heating season haze episodes in Beijing revealed by aerosol–chemistry–radiation–boundary layer interaction

et al. 2021

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Abstract. Despite the numerous studies investigating haze formation mechanism in China, it is still puzzling that intensive haze episodes could form within hours directly following relatively clean periods. Haze has been suggested to be initiated by the variation of meteorological parameters and then to be substantially enhanced by aerosol–radiation–boundary layer feedback. However, knowledge on the detailed chemical processes and the driving factors for extensive aerosol mass accumulation during the feedback is still scarce. Here, the dependency of the aerosol number size distribution, mass concentration and chemical composition on the daytime mixing layer height (MLH) in urban Beijing is investigated. The size distribution and chemical composition-resolved dry aerosol light extinction is also explored. The results indicate that the aerosol mass concentration and fraction of nitrate increased dramatically when the MLH decreased from high to low conditions, corresponding to relatively clean and polluted conditions, respectively. Particles having their dry diameters in the size of ∼400–700 nm, and especially particle-phase ammonium nitrate and liquid water, contributed greatly to visibility degradation during the winter haze periods. The dependency of aerosol composition on the MLH revealed that ammonium nitrate and aerosol water content increased the most during low MLH conditions, which may have further triggered enhanced formation of sulfate and organic aerosol via heterogeneous reactions. As a result, more sulfate, nitrate and water-soluble organics were formed, leading to an enhanced water uptake ability and increased light extinction by the aerosols. The results of this study contribute towards a more detailed understanding of the aerosol–chemistry–radiation–boundary layer feedback that is likely to be responsible for explosive aerosol mass growth events in urban Beijing.

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“…Up to 33-92 % OH formation can be attributed to HONO photolysis in both rural and urban sites Michoud et al, 2012;Tan et al, 2017;Hendrick et al, 2014). However, the detailed formation mechanisms of HONO are still not well understood and the observed HONO concentrations cannot be completely explained by current research (Sörgel et al, 2011a;Sarwar et al, 2008;Liu et al, 2019a;Liu et al, 2020c).…”

Section: Introductionmentioning

confidence: 96%

“…Discussion started: 3 May 2021 c Author(s) 2021. CC BY 4.0 License Slater et al, 2020;Liu et al, 2020c). Taiwan (Lin et al, 2006) andHebei (Xue et al, 2020).…”

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Budget of nitrous acid (HONO) and its impacts on atmospheric oxidation capacity at an urban site in the fall season of Guangzhou, China

Cheng

et al. 2021

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Abstract. Nitrous acid (HONO) can produce hydroxyl radicals (OH) by photolysis and plays an important role in atmospheric photochemistry. Over the years, high concentrations of HONO have been observed in the Pearl River Delta region (PRD) of China, which may be one reason for the elevated atmospheric oxidation capacity. A comprehensive atmospheric observation campaign was conducted at an urban site in Guangzhou from 27 September to 9 November 2018. During the period, HONO was measured from 0.02 to 4.43 ppbv with an average of 0.74 ± 0.70 ppbv. The emission ratios (HONO/NOx) of 0.9 ± 0.4 % were derived from 11 fresh plumes. The primary emission rates of HONO at night were calculated to be between 0.04 ± 0.02 ppbv h−1 and 0.30 ± 0.15 ppbv h−1 based on a high-resolution emission inventory. The HONO formation rate by the homogeneous reaction of OH + NO at night was 0.26 ± 0.08 ppbv h−1, which can be seen as secondary results from primary emission. They were both much higher than the increase rate of HONO (0.02 ppbv h−1) during night. Soil emission rate of HONO at night was calculated to be 0.019 ± 0.001 ppbv h−1. Assuming dry deposition as the dominant removal process of HONO at night, and a deposition velocity of at least ~2.5 cm s−1 is required to balance the direct emissions and OH + NO reaction. Correlation analysis shows that NH3 and relative humidity (RH) may participate in the heterogeneous transformation from NO2 to HONO at night. In the daytime, the average primary emission Pemis was 0.12 ± 0.01 ppbv h−1, and the homogeneous reaction POH + NO was 0.79 ± 0.61 ppbv h−1, larger than the unknown sources PUnknown (0.65 ± 0.46 ppbv h−1). These results suggest primary emissions as a key factor affecting HONO at our site, both during daytime and nighttime. Similar to previous studies, the daytime unknown source of HONO, PUnknown, appeared to be related to the photo-enhanced conversion of NO2. The daytime average OH production rates by photolysis of HONO was 3.7 × 106 cm−3 s−1, lower than that from O1D + H2O at 4.9 × 106 cm−3 s−1. Simulations of OH and O3 with the Master Chemical Mechanism (MCM) box model suggested strong enhancement effect of HONO on OH and O3 by 59 % and 68.8 %, respectively, showing a remarkable contribution of HONO to the atmospheric oxidation in the fall season of Guangzhou.

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The promotion effect of nitrous acid on aerosol formation in wintertime in Beijing: the possible contribution of traffic-related emissions

Cited by 47 publications

References 109 publications

Ammonium nitrate promotes sulfate formation through uptake kinetic regime

Ammonium nitrate promotes sulfate formation through uptake kinetic regime

Rapid mass growth and enhanced light extinction of atmospheric aerosols during the heating season haze episodes in Beijing revealed by aerosol–chemistry–radiation–boundary layer interaction

Budget of nitrous acid (HONO) and its impacts on atmospheric oxidation capacity at an urban site in the fall season of Guangzhou, China

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