Organosulfates in Atlanta, Georgia: anthropogenic influences on biogenic secondary organic aerosol formation

Hettiyadura, Anusha P. S.; Al-Naiema, Ibrahim M.; Hughes, Dagen D.; Fang, Ting; Stone, Elizabeth A.

doi:10.5194/acp-19-3191-2019

Cited by 94 publications

(167 citation statements)

References 62 publications

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“…Remarkably, at both sites, the concentrations of single and total MT-OSs were considerably lower than previously reported for isoprene-derived OS in urban summertime PM 2.5 from the south-eastern United States. As described by Hettiyadura et al (2019), an average concentration of 1792 ng m À3 was determined for methyltetrol sulfate, which accounted for 12.6 % of PM 2.5 OC alone. Other isoprene-derived OSs showed significantly lower concentrations of 1-131 ng m À3 , which were still larger than most of the MT-OS concentrations determined for MEL and NCP.…”

Section: Quantification Of Terpenoid Ossmentioning

confidence: 99%

“…Nonetheless, more recent studies have shown that, in particular, the application of new developments in separation techniques, such as hydrophilic interaction LC (also referred to as HILIC), can substantially increase the number of detectable isoprene OS and facilitate their identification and quantification (Cui et al 2018;Hettiyadura et al 2015Hettiyadura et al , 2017Hettiyadura et al , 2019.…”

Section: Introductionmentioning

confidence: 99%

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Quantification of known and unknown terpenoid organosulfates in PM10 using untargeted LC–HRMS/MS: contrasting summertime rural Germany and the North China Plain

et al. 2019

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Environmental context. Secondary organic aerosols account for a major fraction of atmospheric particulate matter, affecting both climate and human health. Organosulfates, abundant compounds in organic aerosols, are difficult to measure because of the lack of authentic standards. Here we quantify terpene-derived organosulfates in atmospheric particulate matter at a rural site in Germany and at the North China Plain using a combined target/non-target high-resolution mass spectrometry approach.Abstract. Organosulfates (OSs) are a ubiquitous class of compounds in atmospheric aerosol particles. However, a detailed quantification of OSs is commonly hampered because of missing authentic standards and the abundance of unknown OSs. Using a combined targeted and untargeted approach of high-resolution liquid chromatography-Orbitrap mass spectrometry (LC-Orbitrap MS), we quantified for the first time the total concentrations of known and unknown monoterpene (MT) and sesquiterpene (SQT) OSs in summertime PM 10 particulate matter from field studies in rural Germany (MEL) and the North China Plain (NCP). At each site, we observed more than 50 MT-OSs, 13 of which were detectable at both sites. For both locations, median concentrations of MT-OSs were in the range of 10 to 40 ng m À3 , to which the 13 common MT-OSs contributed on average .50 %. The main contributor to MT-OSs was C 9 H 16 O 7 S (MT-OS 267) with average mass concentrations of 2.23 and 6.38 ng m À3 for MEL and NCP respectively. The concentrations of MT-OSs correlated with the concentrations of MT oxidation products only for MEL. For NCP, the low concentrations of MT oxidation products (i.e. typically ,1 ng m À3 ) suggested a suppression of carboxylic acid formation under high concentrations of NO x and particulate sulfate. Furthermore, we observed 17 SQT-OSs for the MEL samples, whereas 40 SQT-OSs were detected in the NCP samples. Only five of these SQT-OSs were detectable at both sites. Correspondingly, the total concentrations of SQT-OSs were larger for NCP than for MEL, which suggested large differences in the particle chemistry. In particular, aerosol acidity was found to be a key factor during SQT-OS formation, and was probably not sufficient in the PM 10 from MEL.

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Section: Quantification Of Terpenoid Ossmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Quantification of known and unknown terpenoid organosulfates in PM10 using untargeted LC–HRMS/MS: contrasting summertime rural Germany and the North China Plain

et al. 2019

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“…Identification of OSs in aerosol samples has been performed by using various measurement techniques, including liquid chromatography (LC) (also including hydrophilic interaction LC) mass spectrometry (MS) (Cui et al, 2018; Hettiyadura et al, 2017; Hettiyadura et al, 2019; Stone et al, 2012), single particle MS (Hatch et al, 2011), particle analysis laser mass spectrometer (Liao et al, 2015), Raman microspectroscopy (Bondy et al, 2018), electrospray ionization coupled with ultra‐high‐resolution MS (Lin, Yu, et al, 2012; O'Brien et al, 2014; Tao et al, 2014), and ultra‐high‐performance liquid chromatography (UHPLC) coupled to Orbitrap MS (Huang, Cochran, et al, 2018; Wang et al, 2016; Wang, Zhang, et al, 2019). However, due to a lack of authentic standards, quantification of OSs is still challenging, which results in studies on OSs largely remaining at the qualitative level (O'Brien et al, 2014; Tao et al, 2014; Wang et al, 2016).…”

Section: Introductionmentioning

confidence: 99%

“…Semiquantification methods in some research showed that OSs accounted for 4–30% of organic matter (OM) (Hawkins et al, 2010; Surratt et al, 2008; Tolocka & Turpin, 2012) and 4–14% of total sulfate (Lukacs et al, 2009; Stone et al, 2012) in fine particles. Most previous work regarding OSs were examined in Europe (Frossard et al, 2011; Iinuma et al, 2007; Kristensen & Glasius, 2011; Lukacs et al, 2009; Nguyen et al, 2014) and the United States (Glasius, Bering, et al, 2018; Hettiyadura et al, 2019; Hughes & Stone, 2019; Olson et al, 2011; Riva et al, 2015; Riva et al, 2019; Tolocka & Turpin, 2012), but only a few studies were conducted in Asia (Huang, Cao, et al, 2018; Ma et al, 2014; Stone et al, 2012; Wang, Ma, et al, 2019), especially in China.…”

Section: Introductionmentioning

confidence: 99%

Molecular Characterization of Organosulfates in Highly Polluted Atmosphere Using Ultra‐High‐Resolution Mass Spectrometry

et al. 2020

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Organosulfates (OSs) have recently been observed to be a potentially important constituent of secondary organic aerosol (SOA); however, their molecular characterization in highly polluted atmospheres has not been probed in detail. This study thoroughly presents the characterization of OSs in polluted air and demonstrates their seasonal and diurnal variations, formation mechanisms, and contributions to organic aerosol. Atmospheric PM 2.5 samples were collected from an urban Shanghai site across the winter and summer of 2017. OSs were characterized by ultra-high-performance liquid chromatography (UHPLC) coupled with Orbitrap mass spectrometry (MS). Based on exact mass formulae in conjunction with previous chamber studies, hundreds of sulfur-containing compounds were tentatively identified as OSs. The number and abundance of OSs increased significantly during pollution episodes. The OSs in the clean aerosol samples were dominant in biogenic products, whereas the OSs in the polluted winter samples had distinctive anthropogenic characteristics. Aromatics and long-chain alkanes from anthropogenic emissions might be their precursors. By using synthesized standards, the total concentrations of 14 quantified OSs ranged 21.6-161 ng m −3 in summer and 5.85-84.3 ng m −3 in winter, respectively. Among these OSs, glycolic acid sulfate was the most abundant species (1.13-122 ng m −3 ). Further analysis of their seasonal and diurnal variations suggests possible contributions from multiple formation mechanisms, including acid-catalyzed and NO 3 -initiated oxidation reactions. Our results highlight that increased anthropogenic pollutant emissions (e.g., NO x and SO 2 ) can significantly enhance the SOA burden in biogenically influenced urban areas.

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“…from diverse environmental sources have been reported to act as precursors of organic aerosols (Hallquist et al, 2009;Tao et al, 2017;Volkamer et al, 2009;Carlton et al, 2009;Ziemann and Atkinson, 2012;Gentner et al, 2017;Hettiyadura et al, 2019;Majdi et al, 2019;Lim et al, 2019;Maclean et al, 2017). Numerical simulations have been carried out at the molecular level to gain insights into the morphology of aerosols and the energetics of their nucleation from VOCs (Chakraborty and Zachariah, 2011;Li et al, 2010;Ma et al, 2011;Zhao et al, 2019;Hede et al, 2011).…”

mentioning

confidence: 99%

Role of black carbon in the formation of primary organic aerosols: Insights from molecular dynamics simulations

Zhou

Picaud

et al. 2020

Preprint

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Abstract. Many studies on the mixing state of suspended particulate matters (PM) have pointed to the role of carbon particles as nucleation seeds in the formation of atmospheric aerosols. However, the underlying physicochemical mechanisms remain unclear, particularly concerning the involvement of volatile organic compounds (VOCs) at the primary stage of clustering. Here we gain insights into those microscopic formation mechanisms through molecular dynamics simulations of the physisorption of gaseous organic molecules on the surface of a carbon nanoparticle (NP). Six different organic species are selected among the VOCs dominating the atmospheric pollutants of several megacities, to interact with an onion-shell NP that mimics the primary soot particle. We consider organic molecules at various densities on the surface of a NP, as well as the same molecules in a freestanding configuration without any NP. The molecular clusters formed on the NP are found to be energetically more stable than those formed in the gas phase for all the six organic compounds. This points to a catalytic role of black carbon in the primary formation of aerosols from VOCs. Morphology analysis reveals different manners of clustering of aromatic and aliphatic compounds, which lead to different values of the binding energy and thus different thermal stability. Simulation results also suggest a layer-by-layer formation process of aerosol PM, consistent with previous transmission electron microscopy observations. These results shed light on the microscopic mechanisms of the primary formation of aerosol particulate matters, and are correlated with a variety of experimental measurements.

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Organosulfates in Atlanta, Georgia: anthropogenic influences on biogenic secondary organic aerosol formation

Cited by 94 publications

References 62 publications

Quantification of known and unknown terpenoid organosulfates in PM10 using untargeted LC–HRMS/MS: contrasting summertime rural Germany and the North China Plain

Quantification of known and unknown terpenoid organosulfates in PM10 using untargeted LC–HRMS/MS: contrasting summertime rural Germany and the North China Plain

Molecular Characterization of Organosulfates in Highly Polluted Atmosphere Using Ultra‐High‐Resolution Mass Spectrometry

Role of black carbon in the formation of primary organic aerosols: Insights from molecular dynamics simulations

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