Organosulfates in Ambient Aerosol: State of Knowledge and Future Research Directions on Formation, Abundance, Fate, and Importance

Brüggemann, Martin; Xu, Rongshuang; Tilgner, Andreas; Kwong, Kai Chung; Mutzel, Anke; Poon, Hon Yin; Otto, Tobias; Schaefer, Thomas; Poulain, Laurent; Chan, Man Nin; Herrmann, Hartmut

doi:10.1021/acs.est.9b06751

Cited by 148 publications

(218 citation statements)

References 151 publications

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“…5a, b). A similar result was also found in Beijing, where most OS species were correlated strongly with the product of ozone and particulate sulfate ([O 3 ] • [SO 2− 4 ]) (Bryant et al, 2020). In addition, an overall positive correlation was observed between the OS concentration and ALWC (Fig.…”

Section: Factors Influencing Organosulfate Formationsupporting

confidence: 83%

“…The dramatically larger ratios of 2-MTS/2-MAS in summer than in other seasons, therefore, strongly suggest that the low-NO x oxidation pathways dominated the production of isoprene-derived SOAs in summer, while the processes favorable under high-NO x conditions were important for SOA formation in other seasons. We note that the 2-MTS/2-MAS ratios observed in summertime Shanghai are smaller than those (17.0-33.8) observed in less polluted environments such as the southeastern United States (Hettiyadura et al, 2019;Budisulistiorini et al, 2015;Riva et al, 2019) but significantly larger than those (0.55-1.57) observed in Beijing Bryant et al, 2020) and the PRD region of China (He et al, 2018).…”

Section: Isoprene-derived Organosulfatescontrasting

confidence: 53%

“…This implies that the O x level is a driving factor for OS formation in ambient aerosols in Shanghai. Very recently, a similar oxidant effect on OS formation was also observed in urban Beijing (Bryant et al, 2020). Therefore, mitigation of O x pollution may effectively reduce the production of OSs and SOAs in Chinese megacities.…”

Section: Factors Influencing Organosulfate Formationmentioning

confidence: 56%

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Organosulfates in atmospheric aerosols in Shanghai, China: seasonal and interannual variability, origin, and formation mechanisms

et al. 2021

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Abstract. Organosulfates (OSs) are ubiquitous in the atmosphere and serve as important tracers for secondary organic aerosols (SOAs). Despite intense research over the years, the abundance, origin, and formation mechanisms of OSs in ambient aerosols, particularly in regions with severe anthropogenic pollution, are still not well understood. In this study, we collected filter samples of ambient fine particulate matter (PM2.5) over four seasons in both 2015–2016 and 2018–2019 at an urban site in Shanghai, China, and comprehensively characterized the OS species in these PM2.5 samples using an ultra-performance liquid chromatography quadrupole time-of-flight mass spectrometer equipped with an electrospray ionization (ESI) source (UPLC-ESI-QToFMS). Overall, we find that while the concentration of organic aerosols (OAs) decreased by 29 % in 2018–2019 compared to that in 2015–2016, mainly as a result of the reduction of anthropogenic pollutant emissions in eastern China, the annually averaged concentrations of 35 quantified OSs were similar in both years (65.5 ± 77.5 ng m−3, 0.57 % ± 0.56 % of OA in 2015–2016 vs. 59.4 ± 79.7 ng m−3, 0.66 % ± 0.56 % of OA in 2018–2019), suggesting an increased contribution of SOAs to OAs in 2018–2019 compared to 2015–2016. Isoprene- and monoterpene-derived OSs were the two most abundant OS families, on average, accounting for 36.3 % and 31.0 % of the quantified OS concentrations, respectively, during both sampling years, suggesting an important contribution of biogenic emissions to the production of OSs and SOAs in Shanghai. The abundance of biogenic OSs, particularly those arising from isoprene, exhibited strong seasonality (peaked in summer) but no significant interannual variability. In contrast, the quantified anthropogenic OSs had little seasonal variability and declined in 2018–2019 compared with those in 2015–2016. The C2 and C3 OS species that have both biogenic and anthropogenic origins contributed, on average, 19.0 % of the quantified OSs, with C2H3O6S−, C3H5O5S−, and C3H5O6S− being the most abundant species, together accounting for 76 % of the C2 and C3 OS concentrations in 2015–2016 and 2018–2019. 2-Methyltetrol sulfate (2-MTS, C5H11O7S−) and monoterpene-derived C10H16NO7S− were the most abundant OSs and nitrooxy OSs in summer, on average, contributing 31 % and 5 % of the quantified OSs, respectively, during the summertime of the sampling years. The substantially larger concentration ratio of 2-MTS to 2-methylglyceric acid sulfate (2-MAS, C4H7O7S−) in summer (6.8–7.8) compared to the other seasons (0.31–0.78) implies that low-NOx oxidation pathways played a dominant role in isoprene-derived SOA formation in summer, while high-NOx reaction pathways were more important in other seasons. We further find that the production of OSs was largely controlled by the level of Ox (Ox= O3+ NO2), namely the photochemistry of OS precursors, particularly in summer, though sulfate concentration, aerosol acidity, and aerosol liquid water content (ALWC) that could affect the heterogeneous chemistry of reactive intermediates leading to OS formation also played a role. Our study provides valuable insights into the characteristics and mechanisms of OS formation in a typical Chinese megacity and implies that the mitigation of Ox pollution can effectively reduce the production of OSs and SOAs in eastern China.

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Section: Factors Influencing Organosulfate Formationsupporting

confidence: 83%

Section: Isoprene-derived Organosulfatescontrasting

confidence: 53%

Section: Factors Influencing Organosulfate Formationmentioning

confidence: 56%

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Organosulfates in atmospheric aerosols in Shanghai, China: seasonal and interannual variability, origin, and formation mechanisms

et al. 2021

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“…The OSs affect the physicochemical properties of aerosols such as hygroscopicity, acidity, and viscosity, and ultimately the climate and health effects of aerosols (Surratt et al, 2007;Farmer et al, 2010;Sorooshian et al, 2015;Estillore et al, 2016;Riva et al, 2019). The identified OSs include organosulfates (ROSO 3 − ), sulfoxides (RSOR'), sulfones (RSO 2 R'), and sulfonates (RSO 3 − ) (Brüggemann et al, 2020).…”

Section: Introductionmentioning

confidence: 99%

“…levels, and spatiotemporal distributions. Organosulfates and MSA are the two most studied OSs species or classes (Bates et al, 1992;Huang et al, 2017;Brüggemann et al, 2020). Organosulfates are primarily formed by the reactive uptake of gasphase epoxides on acidic sulfate particles (Froyd et al, 2010;Surratt et al, 2010;Xu et al, 2015).…”

Section: Introductionmentioning

confidence: 99%

Global modeling of heterogeneous hydroxymethanesulfonate chemistry

Song¹,

Ma²,

Zhang³

et al. 2020

Preprint

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Abstract. Hydroxymethanesulfonate (HMS) has recently been identified as an abundant organosulfur compound in aerosols during winter haze episodes in northern China. It has also been detected in other regions, although the concentrations are low. Because of the sparse field measurements, the global significance of HMS and its spatial and seasonal patterns remain unclear. Here, we implement HMS chemistry into the GEOS-Chem chemical transport model and conduct multiple global simulations. The developed model accounts for cloud entrainment and gas–aqueous mass transfer within the rate expressions for heterogeneous sulfur chemistry. Our simulations can generally reproduce the available HMS observations, and show that East Asia has the highest HMS concentration, followed by Europe and North America. The simulated HMS shows a seasonal pattern with higher values in the colder period. Photochemical oxidizing capacity affects the competition of formaldehyde with oxidants (such as ozone and hydrogen peroxide) for sulfur dioxide and is a key factor influencing the seasonality of HMS. The highest average HMS concentration (1–3 μg m−3) and HMS/sulfate molar ratio (0.1–0.2) are found in northern China winter. The simulations suggest that aqueous clouds act as the major medium for HMS chemistry while aerosol liquid water may play a role if its rate constant for HMS formation is greatly enhanced compared to cloud water.

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Photochemical Degradation of Organic Matter in the Atmosphere

Liu

et al. 2021

Advanced Sustainable Systems

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Organosulfates in Ambient Aerosol: State of Knowledge and Future Research Directions on Formation, Abundance, Fate, and Importance

Cited by 148 publications

References 151 publications

Organosulfates in atmospheric aerosols in Shanghai, China: seasonal and interannual variability, origin, and formation mechanisms

Organosulfates in atmospheric aerosols in Shanghai, China: seasonal and interannual variability, origin, and formation mechanisms

Global modeling of heterogeneous hydroxymethanesulfonate chemistry

Photochemical Degradation of Organic Matter in the Atmosphere

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