Isoprene Forms Secondary Organic Aerosol through Cloud Processing:  Model Simulations

Lim, Ho-Jin; Carlton, Annmarie G.; Turpin, Barbara J.

doi:10.1021/es048039h

Cited by 427 publications

(533 citation statements)

References 44 publications

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“…S2) because OH produced by nitrate photolysis reacts with nitrite radicals to regenerate nitric acid. [52] The production of oxalate was much slower in GLY þ HNO 3 þ UV control experiments (Fig. S6) compared with OH radical experiments, also suggesting that OH radical production by HNO 3 photochemistry was modest (Fig.…”

Section: Resultsmentioning

confidence: 93%

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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Section: Resultsmentioning

confidence: 93%

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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“…The hydrated MeGly is further reacted with oxidants, resulting in Pyr, acetic acid, hydrated ωC 2 , and finally C 2 . Similarly, hydrated Gly can be converted to ωC 2 , and then C 2 (Lim et al, 2005;Sorooshian et al, 2007).…”

Section: Possible Production Of Oxalic Acid In Nighttimementioning

confidence: 99%

Diurnal and temporal variations of water-soluble dicarboxylic acids and related compounds in aerosols from the northern vicinity of Beijing: Implication for photochemical aging during atmospheric transport

He¹,

Kawamura²,

Okuzawa³

et al. 2014

Science of The Total Environment

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Abstract:Aerosol samples were collected in autumn 2007 on day-and nighttime basis in the northern receptor site of Beijing, China. The samples were analyzed for total carbon (TC) and water-soluble dicarboxylic acids (C 2 -C 12 ), oxocarboxylic acids (C 2 -C 9 ), glyoxal and methylglyoxal to better understand the photochemical aging of organic aerosols in the vicinity of Beijing. Concentrations of TC are 50% greater in daytime when winds come from Beijing than in nighttime when winds come from the northern forest areas. Most diacids showed higher concentrations in daytime, suggesting that the organics emitted from the urban Beijing and delivered to the northern vicinity in daytime are subjected to photo-oxidation to result in diacids.However, oxalic acid (C 2 ), which is the most abundant diacid followed by C 3 or C 4 , became on average 30% more abundant in nighttime together with azelaic, ω-oxooctanoic and ω-oxononanoic acids, which are specific oxidation products of biogenic unsaturated fatty acids.Methylglyoxal, an oxidation product of isoprene and a precursor of oxalic acid, also became 29% more abundant in nighttime. Based on a positive correlation between C 2 and glyoxylic acid (ωC 2 ) in nighttime when relative humidity significantly enhanced, we propose a nighttime aqueous phase production of C 2 via the oxidation of ωC 2 . We found an increase in the contribution of diacids to TC by 3 folds during consecutive clear days. This study demonstrates that diacids and related compounds are largely produced in the northern vicinity of Beijing via photochemical processing of organic precursors emitted from urban center and forest areas.

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“…-Dicarbonyls are produced by photochemical oxidation of biogenic (isoprene) and anthropogenic (aromatic) hydrocarbons and are further oxidized to keotacids and then to oxalic acid (Lim et al, 2005;Warneck, 2003).…”

Section: Relative Abundance Of Wsoc Diacids Ketoacids and -Dicarbomentioning

confidence: 99%

Time-resolved variations in the distributions of inorganic ions, carbonaceous components, dicarboxylic acids and related compounds in atmospheric aerosols from Sapporo, northern Japan during summertime

Pavuluri

Kawamura

Kikuta

et al. 2012

Atmospheric Environment

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To better understand time-resolved variations of water-soluble organic aerosols in the atmosphere, we collected atmospheric particles (TSP) every 3 h during summertime (8-10 August, 2005) in Sapporo, northern Japan. We measured inorganic ions, carbonaceous components, dicarboxylic acids, ketoacids and α-dicarbonyls in TSP. SO4^[2-] was found as the most abundant ionic species (57 ± 9% of total ions determined) followed by NH4+ and NO3-. However, none of the ionic species showed any diurnal trend throughout the campaign. Organic carbon (OC) ranged from 2.1 to 12.1 μg m^[-3] whereas elemental carbon (EC) was negligible in most of the samples (0.31 ± 0.56 μg m^[-3]). Oxalic (C2) acid was the most abundant diacid species, followed by malonic (C3) and succinic (C4) acids. Water-soluble OC (WSOC), water-insoluble OC (WIOC) and OC as well as dominant diacids (C2-C4), total diacids, ketoacids and α-dicarbonyls did not show diurnal trend on 8 August, but they showed clear diurnal distributions during 9-10 August following the changes in ambient temperature (and radiation). Detailed analyses of time-resolved aerosols demonstrate that diurnal variations of organic aerosol compositions are caused by local in situ photochemical production, but are significantly superimposed by long-range atmospheric transport of aerosols, particularly when the air masses are enriched with emissions from higher plants and/or biomass burning, and their photochemical processing during the transport

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Isoprene Forms Secondary Organic Aerosol through Cloud Processing: Model Simulations

Cited by 427 publications

References 44 publications

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

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

Diurnal and temporal variations of water-soluble dicarboxylic acids and related compounds in aerosols from the northern vicinity of Beijing: Implication for photochemical aging during atmospheric transport

Time-resolved variations in the distributions of inorganic ions, carbonaceous components, dicarboxylic acids and related compounds in atmospheric aerosols from Sapporo, northern Japan during summertime

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