SOA Formation from Partitioning and Heterogeneous Reactions:  Model Study in the Presence of Inorganic Species

Jang, Myoseon; Czoschke, Nadine M.; Northcross, Amanda; Cao, Gang; Shaof, David

doi:10.1021/es0511220

Cited by 48 publications

(55 citation statements)

References 42 publications

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“…Furthermore, no major enhancement in particle growth was observed for the acidic seed, suggesting that the large glyoxal uptake was not a result of particle acidity but rather of ionic strength of the seed. These results are in contrast to those reported by Jang et al (2006a) and further work is clearly required to resolve this discrepancy. The proposed reaction mechanisms for acid-catalyzed reactions of aldehydes include hydration, hemiacetal/acetal formation, trioxane formation, aldol condensation, carbocationic rearrangement, and cross-linking in aerosol media, as shown in Fig.…”

Section: Laboratory Studies Of Aerosol Growth By Acid-catalyzed Reactcontrasting

confidence: 99%

The formation, properties and impact of secondary organic aerosol: current and emerging issues

et al. 2009

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Abstract. Secondary organic aerosol (SOA) accounts for a significant fraction of ambient tropospheric aerosol and a detailed knowledge of the formation, properties and transformation of SOA is therefore required to evaluate its impact on atmospheric processes, climate and human health. The chemical and physical processes associated with SOA formation are complex and varied, and, despite considerable progress in recent years, a quantitative and predictive understanding of SOA formation does not exist and therefore represents a major research challenge in atmospheric science. This review begins with an update on the current state of knowledge on the global SOA budget and is followed by an overview of the atmospheric degradation mechanisms for SOA precursors, gas-particle partitioning theory and the analytical techniques used to determine the chemical composition of SOA. A survey of recent laboratory, field and modeling studies is also presented. The following topical and emerging issues are highlighted and discussed in detail: molecular characterization of biogenic SOA constituents, condensed phase reactions and oligomerization, the interaction of atmospheric organic components with sulfuric acid, the chemical and photochemical processing of organics in the atmospheric aqueous phase, aerosol formation from real plant emissions, interaction of atmospheric organic components with water, thermodynamics and mixtures in atmospheric models. Finally, the major challenges ahead in laboratory, field and modeling studies of SOA are discussed and recommendations for future research directions are proposed.

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Section: Laboratory Studies Of Aerosol Growth By Acid-catalyzed Reactcontrasting

confidence: 99%

The formation, properties and impact of secondary organic aerosol: current and emerging issues

et al. 2009

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“…3.1), and pK BH + of i m,n in the aerosol phase, [H + ] and LWC (activity of water, a w ) from the inorganic thermodynamic model (Sect. 3.2), and the excess acidity, X (Im et al, 2014;Jang et al, 2006).…”

Section: Om From Aerosol Phase Reactions (Om Ar )mentioning

confidence: 99%

Simulating the SOA formation of isoprene from partitioning and aerosol phase reactions in the presence of inorganics

Beardsley

Jang

2016

Atmos. Chem. Phys.

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Abstract. The secondary organic aerosol (SOA) produced by the photooxidation of isoprene with and without inorganic seed is simulated using the Unified Partitioning Aerosol Phase Reaction (UNIPAR) model. Recent work has found the SOA formation of isoprene to be sensitive to both aerosol acidity ([H + ], mol L −1 ) and aerosol liquid water content (LWC) with the presence of either leading to significant aerosol phase organic mass generation and large growth in SOA yields (Y SOA ). Classical partitioning models alone are insufficient to predict isoprene SOA formation due to the high volatility of photooxidation products and sensitivity of their mass yields to variations in inorganic aerosol composition. UNIPAR utilizes the chemical structures provided by a near-explicit chemical mechanism to estimate the thermodynamic properties of the gas phase products, which are lumped based on their calculated vapor pressure (eight groups) and aerosol phase reactivity (six groups). UNIPAR then determines the SOA formation of each lumping group from both partitioning and aerosol phase reactions (oligomerization, acid-catalyzed reactions and organosulfate formation) assuming a single homogeneously mixed organic-inorganic phase as a function of inorganic composition and VOC / NO x (VOC -volatile organic compound). The model is validated using isoprene photooxidation experiments performed in the dual, outdoor University of Florida Atmospheric PHotochemical Outdoor Reactor (UF APHOR) chambers. UNI-PAR is able to predict the experimental SOA formation of isoprene without seed, with H 2 SO 4 seed gradually titrated by ammonia, and with the acidic seed generated by SO 2 oxidation. Oligomeric mass is predicted to account for more than 65 % of the total organic mass formed in all cases and over 85 % in the presence of strongly acidic seed. The model is run to determine the sensitivity of Y SOA to [H + ], LWC and VOC / NO x , and it is determined that the SOA formation of isoprene is most strongly related to [H + ] but is dynamically related to all three parameters. For VOC / NO x > 10, with increasing NO x both experimental and simulated Y SOA increase and are found to be more sensitive to [H + ] and LWC. For atmospherically relevant conditions, Y SOA is found to be more than 150 % higher in partially titrated acidic seeds (NH 4 HSO 4 ) than in effloresced inorganics or in isoprene only.

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“…The volatile organic compounds involved in such studies were well-known aerosol precursors such as α-pinene (Czoschke et al, 2003;Gao et al, 2004a, b;Iinuma et al, 2004;Tolocka et al, 2004;Kleindienst et al, 2006;Czoschke and Jang, 2006;Jang et al, 2006), β-pinene (Iinuma et al, 2007b;Northcross and Jang, 2007), limonene (Iinuma et al, 2007a;Northcross and Jang, 2007), and isoprene (Czoschke et al, 2003;Edney et al, 2005;Surratt et al, 2007b), or directly their semi-volatile photooxidation products like pinonaldehyde (Liggio and Li, 2006a, b), glyoxal (Kroll et al, 2005;Liggio et al, 2005), or other carbonyls (Jang et al, , 2005. In the case of hydroxy compounds organosulfates are formed by esterification with sulfuric acid, while in the case of carbonyl compounds esterification occurs after gem-diol formation.…”

Section: Introductionmentioning

confidence: 99%

Quantitative assessment of organosulfates in size-segregated rural fine aerosol

Lukács

Gelencsér²,

Hoffer

et al. 2009

Atmos. Chem. Phys.

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Abstract.Organosulfates have recently come into the focus of organic aerosol research as potentially important components of water-soluble secondary organic aerosol (SOA) which now dominate tropospheric fine aerosol. Their presence has been confirmed by the identification of sulfate esters of abundant biogenic carbonyl compounds in both smog chamber and continental aerosol. However, none of the studies have been able to determine the mass contribution of organosulfates to SOA.In this paper, as possibly the very first attempt to quantify organosulfates in ambient aerosol, we inferred the mass concentrations of organosulfates by concurrently determining mass concentrations of total sulfur, sulfate and methanesulfonate in rural fine aerosol using two highly sensitive analytical techniques. Although uncertainties were relatively large, we found that mass concentrations of organosulfates in water-soluble fine aerosol ranged from 0.02 µgS m −3 to 0.09 µgS m −3 yielding a mass contribution of 6-12% to bulk sulfur concentrations (or 6-14% to sulfate concentrations). The inferred size distribution of organosulfates suggested that they possibly form in heterogeneous reactions from semi-volatile carbonyl compounds with subsequent or concurrent condensation of gaseous sulfuric acid producing a refractory organic film on particle surfaces.

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SOA Formation from Partitioning and Heterogeneous Reactions: Model Study in the Presence of Inorganic Species

Cited by 48 publications

References 42 publications

The formation, properties and impact of secondary organic aerosol: current and emerging issues

The formation, properties and impact of secondary organic aerosol: current and emerging issues

Simulating the SOA formation of isoprene from partitioning and aerosol phase reactions in the presence of inorganics

Quantitative assessment of organosulfates in size-segregated rural fine aerosol

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