Particle acidity and sulfate production during severe haze events in China cannot be reliably inferred by assuming a mixture of inorganic salts

Wang, Gehui; Zhang, Fang; Peng, Jianfei; Duan, Lian; Ji, Yuemeng; Marrero-Ortiz, Wilmarie; Wang, Jiayuan; Li, Jianjun; Wu, Chengdong; Cao, Cong; Wang, Yuan; Zheng, Jun; Secrest, Jeremiah; Li, Yixin; Wang, Yuying; Li, Hong; Li, Na; Zhang, Renyi

doi:10.5194/acp-18-10123-2018

Cited by 90 publications

(82 citation statements)

References 48 publications

(65 reference statements)

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“…3 ) in the SPAMS mass spectra (Whiteaker and Prather, 2003). The observed number concentration of HMS-containing particles (N HMS ) was closely correlated with AWC (r = 0.86, P < 0.001), supporting the production of HMS in aerosol droplets.…”

Section: Hms Is Likely the Major Os Speciesmentioning

confidence: 65%

“…3 ) with no significant interference from other species in previous laboratory and field studies (Lee et al, 2003;Whiteaker and Prather, 2003;Dall'Osto et al, 2009;Zhang et al, 2012). HMS-containing particles were identified by the presence of a peak at m/z −111 with the absolute and relative peak areas greater than 50 % and 0.5 %, respectively.…”

Section: Spams Measurementsmentioning

confidence: 90%

“…3b). Although the SPAMS data showed a significant percentage (∼ 10 % during haze periods) of HMS-containing particles in the total particle counts, a quantitative estimate of HMS mass concentration is not available here because HMS may be fragmented into smaller ions, such as HSO − 3 and SO − 3 , depending on the countercations in particles (i.e., matrix effects) (Neubauer et al, 1997;Whiteaker and Prather, 2003). These ions coexist with the HMS peak in the SPAMS mass spectra (Fig.…”

Section: Hms Is Likely the Major Os Speciesmentioning

confidence: 94%

“…Several heterogeneous reaction pathways have been proposed (He et al, 2014;Cheng et al, 2016;Wang et al, 2016;Li et al, 2017a;Hung et al, 2018;Qin et al, 2018;Yu et al, 2018), including the oxidation of SO 2 in aerosol water (by NO 2 , transition-metal-catalyzed O 2 , or H 2 O 2 ) and on aerosol surfaces (by NO 2 and/or O 2 ). Their relative importance for sulfate production in winter haze, however, is unknown due to uncertainties in relevant reaction rates and estimates for aerosol water pH values (most reaction pathways are pH-dependent) (Guo et al, 2017b;Liu et al, 2017a;Li et al, 2018b;Wang et al, 2018;Zhao et al, 2018). For example, Wang et al (2016Wang et al ( , 2018 found in laboratory experiments that the rate for the oxidation of SO 2 by NO 2 strongly depended on the types of seed particles.…”

Section: Introductionmentioning

confidence: 99%

“…Their relative importance for sulfate production in winter haze, however, is unknown due to uncertainties in relevant reaction rates and estimates for aerosol water pH values (most reaction pathways are pH-dependent) (Guo et al, 2017b;Liu et al, 2017a;Li et al, 2018b;Wang et al, 2018;Zhao et al, 2018). For example, Wang et al (2016Wang et al ( , 2018 found in laboratory experiments that the rate for the oxidation of SO 2 by NO 2 strongly depended on the types of seed particles. In another example, Cheng et al (2016) suggested that reactions of SO 2 with NO 2 in aerosol water could be the source of missing sulfate given the neutralized feature of haze aerosols (with a pH value of about 6 estimated with the ISORROPIA-II thermodynamic equilibrium model).…”

Section: Introductionmentioning

confidence: 99%

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Possible heterogeneous chemistry of hydroxymethanesulfonate (HMS) in northern China winter haze

et al. 2019

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Abstract. The chemical mechanisms responsible for rapid sulfate production, an important driver of winter haze formation in northern China, remain unclear. Here, we propose a potentially important heterogeneous hydroxymethanesulfonate (HMS) chemical mechanism. Through analyzing field measurements with aerosol mass spectrometry, we show evidence for a possible significant existence in haze aerosols of organosulfur primarily as HMS, misidentified as sulfate in previous observations. We estimate that HMS can account for up to about one-third of the sulfate concentrations unexplained by current air quality models. Heterogeneous production of HMS by SO2 and formaldehyde is favored under northern China winter haze conditions due to high aerosol water content, moderately acidic pH values, high gaseous precursor levels, and low temperature. These analyses identify an unappreciated importance of formaldehyde in secondary aerosol formation and call for more research on sources and on the chemistry of formaldehyde in northern China winter.

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Section: Hms Is Likely the Major Os Speciesmentioning

confidence: 65%

Section: Spams Measurementsmentioning

confidence: 90%

Section: Hms Is Likely the Major Os Speciesmentioning

confidence: 94%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Possible heterogeneous chemistry of hydroxymethanesulfonate (HMS) in northern China winter haze

et al. 2019

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Characteristics of Chemical Speciation in PM1 in Six Representative Regions in China

Bai

et al. 2021

Adv. Atmos. Sci.

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A better knowledge of aerosol properties is of great significance for elucidating the complex mechanisms behind frequently occurring haze pollution events. In this study, we examine the temporal and spatial variations in both PM 1 and its major chemical constituents using three-year field measurements that were collected in six representative regions in China between 2012 and 2014. Our results show that both PM 1 and its chemical compositions varied significantly in space and time, with high PM 1 loadings mainly observed in the winter. By comparing chemical constituents between clean and polluted episodes, we find that the elevated PM 1 mass concentration during pollution events should be largely attributable to significant increases in organic matter (OM) and inorganic aerosols like sulfate, nitrate, and ammonium (SNA), indicative of the critical role of primary emissions and secondary aerosols in elevating PM 1 pollution levels. The ratios of PM 1 /PM 2.5 are found to be generally high in Shanghai and Guangzhou, while relatively low ratios are seen in Xi’an and Chengdu, indicating anthropogenic emissions were more likely to accumulate in forms of finer particles. With respect to the relative importance of chemical components and meteorological factors quantified via statistical modeling practices, we find that primary emissions and secondary aerosols were the two leading factors contributing to PM 1 variations, though meteorological factors also played important roles in regulating the dispersion of atmospheric PM.

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Particulate Amines in the Background Atmosphere of the Yangtze River Delta, China: Concentration, Size Distribution, and Sources

Wang

Yang

et al. 2021

Adv. Atmos. Sci.

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Amines are important for new particle formation and subsequent growth in the atmosphere. Consequently, the processes involved are receiving more attention in recent years. Here, we conduct a field observation in order to investigate the atmospheric particulate amines at a background site in the Yangtze River Delta (YRD) during the summer of 2018. Four amines in PM 2.5 , i.e., methylamine (MA), dimethylamine (DMA), diethylamine (DEA), and trimethylamine (TMA), were collected, twice daily and analyzed. During the campaign, our measurements found the concentrations of MA, DMA, DEA, and TMA of 15.0 ± 15.0, 6.3 ± 6.9, 20.4 ± 30.1, and 4.0 ± 5.9 ng m -3 , respectively, and the four amines correlated well with each other. The concentration of amines appear to be independent of whether they were collected during the day or night. Both MA and DMA exhibited a bimodal size distribution that had peaks at 0.67 and 1.1 μm, suggesting amines preferably distribute on submicron particles. Boundary layer height (BLH), relative humidity, and pH of aerosols were found have a negative relationship with amines, while aerosol liquid water content (ALWC) was found to have a positive relationship with amines. The PMF (positive matrix factorization) source apportionment results showed that the main source of amines in Chongming Island was of anthropogenic origin such as industrial and biomass emission, followed by marine sources including sea salt and marine biogenic sources. Given that the YRD region is still suffering from complex atmospheric pollution and that the knowledge on aerosol amines is still limited, more field studies are in urgent need for a better understanding of the pollution characteristics of amines.

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Particle acidity and sulfate production during severe haze events in China cannot be reliably inferred by assuming a mixture of inorganic salts

Cited by 90 publications

References 48 publications

Possible heterogeneous chemistry of hydroxymethanesulfonate (HMS) in northern China winter haze

Possible heterogeneous chemistry of hydroxymethanesulfonate (HMS) in northern China winter haze

Characteristics of Chemical Speciation in PM1 in Six Representative Regions in China

Particulate Amines in the Background Atmosphere of the Yangtze River Delta, China: Concentration, Size Distribution, and Sources

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