Aqueous-phase photolysis of biacetyl (An α-dicarbonyl compound): A sink for biacetyl, and a source of acetic acid, peroxyacetic acid, hydrogen peroxide, and the highly oxidizing acetylperoxyl radical in aqueous aerosols, fogs, and clouds

Faust, Bruce C.; Powell, Kendall; Rao, C. J.; Anastasio, Cort

doi:10.1016/s1352-2310(96)00171-9

Cited by 54 publications

(40 citation statements)

References 52 publications

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“…Even if the role of this complex is the subject of debate, the irradiation of cloud water leads to an increase in the concentration of H 2 O 2 and Fe(II) [84]. The photolysis of phenolic compounds [85] and biacetyl compounds [86] was also proposed as a source of H 2 O 2 . Zuo and Deng observed that substantial amounts of H 2 O 2 were produced by lightning activities during thunderstorms [87].…”

Section: Main Oxidants In Cloud Watermentioning

confidence: 99%

Photochemistry of the Cloud Aqueous Phase: A Review

et al. 2020

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This review paper describes briefly the cloud aqueous phase composition and deeply its reactivity in the dark and mainly under solar radiation. The role of the main oxidants (hydrogen peroxide, nitrate radical, and hydroxyl radical) is presented with a focus on the hydroxyl radical, which drives the oxidation capacity during the day. Its sources in the aqueous phase, mainly through photochemical mechanisms with H2O2, iron complexes, or nitrate/nitrite ions, are presented in detail. The formation rate of hydroxyl radical and its steady state concentration evaluated by different authors are listed and compared. Finally, a paragraph is also dedicated to the sinks and the reactivity of the HO• radical with the main compounds found in the cloud aqueous phase. This review presents an assessment of the reactivity in the cloud aqueous phase and shows the significant potential impact that this medium can have on the chemistry of the atmosphere and more generally on the climate.

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Section: Main Oxidants In Cloud Watermentioning

confidence: 99%

Photochemistry of the Cloud Aqueous Phase: A Review

et al. 2020

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“…There are few data available for the photolysis processes of carbonyl compounds in the aqueous phase. Based on a study by Faust et al [1997] it can be estimated that these processes do not represent a significant loss for these species in the aqueous phase since their photolysis rates (j max ≈ 2 · 10 −4 s −1 ) are too small to compete with the simultaneous OH reactions.…”

Section: Chemical Mechanismmentioning

confidence: 99%

A modeling study of aqueous production of dicarboxylic acids: 1. Chemical pathways and speciated organic mass production

Feingold²,

et al. 2004

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While the formation pathways and thermodynamic properties of inorganic species (e.g., sulphate) in atmospheric aerosols are well understood, many more uncertainties exist about organics. In the present study we present oxidation pathways of organic gas phase species that lead to low volatility organic compounds (C2‐C6 dicarboxylic acids, pyruvic acid) in both the aqueous and gas phases. This mechanism is implemented in a cloud parcel model initialized with pure (NH4)2SO4 particles in 10 discrete sizes. Under clean continental conditions a few cloud processing cycles produce a total organic mass addition of ∼150 ng m−3. Individual resuspended aerosol size classes contain significant organic fractions, sometimes higher than 50%. These are likely upper bound estimates of organic mass production. In a polluted, i.e., SO2‐rich scenario, about 400 ng m−3 organic material is produced after about eight cloud cycles. Since the initial conditions in this latter case favor significant production of sulphate, the organic fraction of the aerosol mass after cloud processing represents a much lower percentage of the total aerosol mass. Oxalic, glutaric, adipic, and pyruvic acids are the main contributors to the organic fraction in both cases. In agreement with observations, the oxalate fraction in processed particles exceeds the fractions of other dicarboxylic acids since it represents an end product in the oxidation of several organic gas phase species. The study suggests that cloud processing may act as a significant source of small dicarboxylic acids, some fraction of which can be retained in the aerosol phase upon drop evaporation.

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“…Further, a small amount of PAA can be formed by the reaction of acetyl peroxy radical (CH 3 C(O)OO) with high concentrations of "H-atom donors" commonly found in atmospheric aqueous phase, like formate, formaldehyde, glyoxal and phenolic compounds (Reaction R3) (Faust et al, 1997). Sinks of PAA include photolysis, reaction with the hydroxy radical (OH), and loss by physical deposition to the ground (Reactions R4, R5) (Jackson and Hewitt, 1999).…”

Section: Introductionmentioning

confidence: 99%

Peroxyacetic acid in urban and rural atmosphere: concentration, feedback on PAN-NO<sub>x</sub> cycle and implication on radical chemistry

Zhang

Chen

et al. 2010

Atmos. Chem. Phys.

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Abstract. Peroxyacetic acid (PAA) is one of the most important atmospheric organic peroxides, which have received increasing attention for their potential contribution to the oxidation capacity of the troposphere and the formation of secondary aerosols. We report here, for the first time, a series of data for atmospheric PAA concentrations at urban and rural sites, from five field campaigns carried out in China in summer 2006, 2007 and 2008. For these five measurements, daytime mean (08:00-20:00 LT) PAA concentrations on sunlit days were 21.4-148.0 pptv with a maximum level of ∼1 ppbv. The various meteorological and chemical parameters influencing PAA concentrations were examined using Principal Factor Analysis. This statistical analysis shows that the local photochemical production was the major source of PAA, and its concentration increased with increasing temperature, solar radiation and ozone but decreased with increasing NO x (NO and NO 2 ), CO, SO 2 , and relative humidity. Based on the dataset, several issues are highlighted in this study: (i) Because PAA is a product from the photochemical oxidation of some specific volatile organic compounds (VOCs) that lead to acetyl peroxy radicals, the importance of various VOCs with respect to the PAA formation is therefore ranked using the incremental reactivity method. (ii) The contribution of PAN thermal degradation to PAA formation under conditions of different NO x concentrations is estimated based on the chemical kinetics analysis. The result shows that PAN seems to play an important role in the formation of PAA when the NO/NO 2 concentration ratio was less than 0.2 and PAA would correspondingly have feedback on the PAN-NO x cycle. (iii) PAA and other peroxides, such as methyl Correspondence to: Z. M. Chen (zmchen@pku.edu.cn) hydroperoxide (MHP) and H 2 O 2 , usually exhibited a similar asymmetric shape typically shifted to the afternoon. However, under some conditions, H 2 O 2 diurnal cycle was out of phase with MHP and PAA. The combination of linear regression and kinetics analysis indicate that the formation and removal processes of H 2 O 2 may be different from those of MHP and PAA. (iv) Considering that PAA is the reservior of free radicals, its fate is expected to have an effect on the free radical budget in the atmosphere. A box model based on the CBM-IV mechanism has been performed to access its influence on the radical budget. We suggest that the detailed information on PAA in the atmosphere is of importance to better understand the free radical chemistry.

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Aqueous-phase photolysis of biacetyl (An α-dicarbonyl compound): A sink for biacetyl, and a source of acetic acid, peroxyacetic acid, hydrogen peroxide, and the highly oxidizing acetylperoxyl radical in aqueous aerosols, fogs, and clouds

Cited by 54 publications

References 52 publications

Photochemistry of the Cloud Aqueous Phase: A Review

Photochemistry of the Cloud Aqueous Phase: A Review

A modeling study of aqueous production of dicarboxylic acids: 1. Chemical pathways and speciated organic mass production

Peroxyacetic acid in urban and rural atmosphere: concentration, feedback on PAN-NO<sub>x</sub> cycle and implication on radical chemistry

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Aqueous-phase photolysis of biacetyl (An α-dicarbonyl compound): A sink for biacetyl, and a source of acetic acid, peroxyacetic acid, hydrogen peroxide, and the highly oxidizing acetylperoxyl radical in aqueous aerosols, fogs, and clouds

Cited by 54 publications

References 52 publications

Photochemistry of the Cloud Aqueous Phase: A Review

Photochemistry of the Cloud Aqueous Phase: A Review

A modeling study of aqueous production of dicarboxylic acids: 1. Chemical pathways and speciated organic mass production

Peroxyacetic acid in urban and rural atmosphere: concentration, feedback on PAN-NO&lt;sub&gt;x&lt;/sub&gt; cycle and implication on radical chemistry

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Peroxyacetic acid in urban and rural atmosphere: concentration, feedback on PAN-NO<sub>x</sub> cycle and implication on radical chemistry