In-cloud processes of methacrolein under simulated conditions – Part 2: Formation of secondary organic aerosol

Haddad, Imad El; Liu, Yao; Nieto-Gligorovski, L.; Michaud, V.; Temime-Roussel, Brice; Quivet, Étienne; Marchand, Nicolas; Sellegri, Karine; Monod, Anne

doi:10.5194/acp-9-5107-2009

Cited by 80 publications

(69 citation statements)

References 34 publications

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“…It was suggested that SOA can be produced through cloud and fog processing of carbonyls, monocarboxylic acids, alcohols and organic peroxides to form dicarboxylic acids, functionalized acids, functionalized carbonyls, esters, polyols, amines, amino acids, and organosulfur compounds. Subsequently, a number of studies have been performed on the transformation of various oxygenated organic species in the aqueous phase and at its interface in order to elucidate the key processes and mechanisms involved (Blando and Turpin, 2000;Warneck, 2003;Ervens et al, 2004aErvens et al, , b, 2008Altieri et al, 2006Altieri et al, , 2008Altieri et al, , 2009Carlton et al, 2006;Poulain et al, 2007;Tilgner et al, 2008;El Haddad et al, 2009;Liu et al, 2009). …”

Section: Chemical and Photochemical Processing Of Organics In The Atmmentioning

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: Chemical and Photochemical Processing Of Organics In The Atmmentioning

confidence: 99%

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

et al. 2009

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“…oxalate, glycolate, oligomers, epoxide sulfates and imidazoles). [1][2][3][4][5][6][7][8][9][10][11] As a result, gas-phase followed by aqueous-phase chemistry contributes to secondary organic aerosol (SOA). [12,13] SOA is also formed when semiand low-volatility products of gas-phase chemistry sorb to particulate organic matter [14,15] (here SOA gas is used to denote SOA formed by this latter pathway and SOA aq to denote SOA formed with a contribution from aqueous-phase chemistry).…”

Section: Introductionmentioning

confidence: 99%

Glyoxal secondary organic aerosol chemistry: effects of dilute nitrate and ammonium and support for organic radical–radical oligomer formation

Kirkland¹,

Lim²,

Tan³

et al. 2013

Environ. Chem.

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Environmental context. Atmospheric waters (clouds, fogs and wet aerosols) are media in which gases can be converted into particulate matter. This work explores aqueous transformations of glyoxal, a water-soluble gas with anthropogenic and biogenic sources. Results provide new evidence in support of previously proposed chemical mechanisms. These mechanisms are beginning to be incorporated into transport models that link emissions to air pollution concentrations and behaviour.Abstract. Glyoxal (GLY) is ubiquitous in the atmosphere and an important aqueous secondary organic aerosol (SOA) precursor. At dilute (cloud-relevant) organic concentrations, OH radical oxidation of GLY has been shown to produce oxalate. GLY has also been used as a surrogate species to gain insight into radical and non-radical reactions in wet aerosols, where organic and inorganic concentrations are very high (in the molar region). The work herein demonstrates, for the first time, that tartarate forms from GLY þ OH . Tartarate is a key product in a previously proposed organic radical-radical reaction mechanism for oligomer formation from GLY oxidation. Previously published model predictions that include this GLY oxidation pathway suggest that oligomers are major products of OH radical oxidation at the high organic concentrations found in wet aerosols. The tartarate measurements herein provide support for this proposed oligomer formation mechanism. This paper also demonstrates, for the first time, that dilute (cloud or fog-relevant) concentrations of inorganic nitrogen (i.e. ammonium and nitrate) have little effect on the GLY þ OH chemistry leading to oxalate formation in clouds. This, and results from previous experiments conducted with acidic sulfate, increase confidence that the currently understood dilute GLY þ OH chemistry can be used to predict GLY SOA formation in clouds and fogs. It should be recognised that organic-inorganic interactions can play an important role in droplet evaporation chemistry and in wet aerosols. The chemistry leading to SOA formation in these environments is complex and remains poorly understood.

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“…In aqueous environments with sufficiently high organic concentrations, polyfunctional carbonyl compounds react to form high-molecular-weight species, polymers, and oligomers, yet the reaction mechanisms responsible for these aqueous phase reactions remain elusive targets for investigation (5,6,13,(19)(20)(21). This investigation provides fundamental laboratory results and mechanisms for the photochemistry of pyruvic acid (PA) in an aqueous solution.…”

mentioning

confidence: 99%

Photochemistry of aqueous pyruvic acid

Griffith

Carpenter

Shoemaker³

et al. 2013

Proc. Natl. Acad. Sci. U.S.A.

126

289

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The study of organic chemistry in atmospheric aerosols and cloud formation is of interest in predictions of air quality and climate change. It is now known that aqueous phase chemistry is important in the formation of secondary organic aerosols. Here, the photoreactivity of pyruvic acid (PA; CH 3 COCOOH) is investigated in aqueous environments characteristic of atmospheric aerosols. PA is currently used as a proxy for α-dicarbonyls in atmospheric models and is abundant in both the gas phase and the aqueous phase (atmospheric aerosols, fog, and clouds) in the atmosphere. The photoreactivity of PA in these phases, however, is very different, thus prompting the need for a mechanistic understanding of its reactivity in different environments. Although the decarboxylation of aqueous phase PA through UV excitation has been studied for many years, its mechanism and products remain controversial. In this work, photolysis of aqueous PA is shown to produce acetoin (CH 3 CHOHCOCH 3 ), lactic acid (CH 3 CHOHCOOH), acetic acid (CH 3 COOH), and oligomers, illustrating the progression from a three-carbon molecule to four-carbon and even six-carbon molecules through direct photolysis. These products are detected using vibrational and electronic spectroscopy, NMR, and MS, and a reaction mechanism is presented accounting for all products detected. The relevance of sunlight-initiated PA chemistry in aqueous environments is then discussed in the context of processes occurring on atmospheric aerosols.

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In-cloud processes of methacrolein under simulated conditions – Part 2: Formation of secondary organic aerosol

Cited by 80 publications

References 34 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

Glyoxal secondary organic aerosol chemistry: effects of dilute nitrate and ammonium and support for organic radical–radical oligomer formation

Photochemistry of aqueous pyruvic acid

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