Methylglyoxal Uptake Coefficients on Aqueous Aerosol Surfaces

Haan, David O. De; Jimenez, Natalie G.; Loera, Alexia de; Cazaunau, Mathieu; Gratien, Aline; Pangui, Edouard; Doussin, Jean‐François

doi:10.1021/acs.jpca.8b00533

Cited by 23 publications

(20 citation statements)

References 43 publications

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“…Other pathways for the formations of SOAs, such as the uptake of isoprene epoxides on the surface of aerosols (Lal et al, 2012;Lin et al, 2013), the aging mechanism of semivolatile primary organic aerosols (Shrivastava et al, 2008), and the oxidation of primary semi-and intermediate VOCs, are not considered in this model. Besides, recent studies (e.g., Galloway et al, 2009;De Haan et al, 2018) have presented that the reactive uptake of glyoxal and methylglyoxal can be reversible, especially methylglyoxal, but we do not consider that in this study.…”

Section: Model Results and Analysesmentioning

confidence: 86%

“…For example, the reactive uptake of dicarbonyls in this study has been processed as irreversible reactions. However, several recent studies (e.g., Galloway et al, 2009;De Haan et al, 2018) have presented that the uptake processes can be reversible, but we do not consider this. As another example, the uptake coefficient of dicarbonyls has been reported to vary between different surfaces by Curry et al (2018), including the differences between the cloud droplet and aqueous aerosol and between each aerosol component.…”

Section: Discussionmentioning

confidence: 92%

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Assessment of dicarbonyl contributions to secondary organic aerosols over China using RAMS-CMAQ

Zhang

Tang

et al. 2019

Atmos. Chem. Phys.

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Abstract. The concentration of secondary organic aerosol (SOA) is underestimated in current model studies. Recent research suggests that the reactive uptake of dicarbonyls contributes to the production of SOA, although few models have included this pathway. Glyoxal, an important representative component of dicarbonyls in models, is significantly underestimated. We therefore incorporated the reactive uptake of dicarbonyls into the regional air quality modeling system RAMS-CMAQ (the Regional Atmospheric Modeling System-Community Multiscale Air Quality) to evaluate the contribution of dicarbonyls to SOA, and we then assess the impact of the underestimation of glyoxal on the production of SOA in China during two time periods: 3 June to 11 July 2014 (episode 1) and 14 October to 14 November 2014 (episode 2). When the reactive uptake process was added, the modeled mean concentration of SOA in episode 1 increased by 3.65 µg m−3, which explained 34.8 % of the unaccounted-for source of SOA. Meanwhile the increase in the concentration of SOA in episode 2 was 1.82 µg m−3 as a result of the lower liquid water content and the lower amount of dicarbonyls produced from biogenic precursors in the fall. On this basis, when the glyoxal simulation was improved, the modeled mean dicarbonyl-derived SOA (AAQ) increased by more than a factor of 2 in both episodes relative to case 1. AAQ in episode 1 contributed, on average, 60.6 % of the total concentration of SOA and the increase in this contribution represented 69.1 % of the unaccounted-for concentration of SOA, whereas the mean AAQ in episode 2 accounted for 64.5 % of total concentration of SOA. Based on the results, the mean AAQ over China was generally higher in the east than in the west during the two episodes. The highest value (10–15 µg m−3) of episode 1 appeared in the areas around the lower reaches of the Yellow River, whereas the highest value of 5–10 µg m−3 in episode 2 was concentrated over regions from south of the lower reaches of the Yellow River to the south of Guangzhou Province as well as the Sichuan Basin. The contribution of AAQ to the concentration of SOA in episode 1 varied from 10 % to 90 % throughout China, with the highest contributions (70 %–90 %) in the coastal regions and offshore along the East China Sea to the South China Sea and in the southwestern regions. The fraction of AAQ to SOA in episode 2 was in the range of 10 %–80 % over China, with the fraction up to 80 % in a small portion of northeastern China.

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Section: Model Results and Analysesmentioning

confidence: 86%

Section: Discussionmentioning

confidence: 92%

Assessment of dicarbonyl contributions to secondary organic aerosols over China using RAMS-CMAQ

Zhang

Tang

et al. 2019

Atmos. Chem. Phys.

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“…As for the atmospheric sink for Gly and Mgly, the photolysis, reaction with OH, dry deposition and heterogenous processes are considered as the main loss pathways, among which aerosol uptake is most complicated and needs more comprehensive exploration (De Haan et al, 2018;McNeill, 2015;Knote et al, 2014;Fu et al, 2008). The uptake of Gly and Mgly onto inorganic or organic particles has been studied in laboratory experiments under controlled conditions (De Haan et al, 2018;Liggio et al, 2005), and uptake coefficients (γ ) were measured by the loss of gas-phase concentration or the increase in particle organic mass, within the range of ∼ 10 −4 to 10 −2 (De Haan et al, 2018;Pye et al, 2017;Liggio et al, 2005). The lower γ value was probably related to the kinetic limitations (Ervens and Volkman, 2010), while the higher γ value may be associated with the increased particle acidity (Liggio et al, 2005), relative humidity (De Haan et al, 2018;Corrigan et al, 2008) and ionic strength (Kroll et al, 2005).…”

mentioning

confidence: 99%

“…The uptake of Gly and Mgly onto inorganic or organic particles has been studied in laboratory experiments under controlled conditions (De Haan et al, 2018;Liggio et al, 2005), and uptake coefficients (γ ) were measured by the loss of gas-phase concentration or the increase in particle organic mass, within the range of ∼ 10 −4 to 10 −2 (De Haan et al, 2018;Pye et al, 2017;Liggio et al, 2005). The lower γ value was probably related to the kinetic limitations (Ervens and Volkman, 2010), while the higher γ value may be associated with the increased particle acidity (Liggio et al, 2005), relative humidity (De Haan et al, 2018;Corrigan et al, 2008) and ionic strength (Kroll et al, 2005). In addition, ammonium-catalyzed and OH reactions were found to have significant influences on the surface uptake of dicarbonyls (Knote et al, 2014;Kampf et al, 2013;Noziere et al, 2008), and the rate coefficients were found to increase with the increasing ammonium ion activity (a NH + 4 ) and pH (Noziere et al, 2008).…”

mentioning

confidence: 99%

“…Li et al, 2013). However, only the simple parameterization of surface uptake of Gly and Mgly without detailed physical and chemical processes (e.g., reversible partitioning of Gly and Mgly into deliquesced droplets) in the model could bias the evolution of Gly and Mgly, leading to the poor understanding of the budgets of Gly and Mgly, their relationship with precursors, and the contributions of precursors to SOA formation in the PRD (De Haan et al, 2018;Waxman et al, 2015;Knote et al, 2014;N. Li et al, 2013;Li et al, 2014;Lu et al, 2013).…”

mentioning

confidence: 99%

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Formation and sink of glyoxal and methylglyoxal in a polluted subtropical environment: observation-based photochemical analysis and impact evaluation

et al. 2020

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Abstract. The dicarbonyls glyoxal (Gly) and methylglyoxal (Mgly) have been recognized as important precursors of secondary organic aerosols (SOAs) through the atmospheric heterogeneous process. In this study, field measurement was conducted at a receptor site in the Pearl River Delta (PRD) region in southern China, and an observation-based photochemical box model was subsequently applied to investigate the production and evolution of Gly and Mgly as well as their contributions to SOA formation. The model was coupled with a detailed gas-phase oxidation mechanism of volatile organic compounds (VOCs) (i.e., Master Chemical Mechanism, MCM, v3.2), heterogeneous processes of Gly and Mgly (i.e., reversible partitioning in aqueous phase, irreversible volume reactions and irreversible surface uptake processes), and the gas–particle partitioning of oxidation products. The results suggested that without considering the heterogeneous processes of Gly and Mgly on aerosol surfaces, the model would overpredict the mixing ratios of Gly and Mgly by factors of 3.3 and 3.5 compared to the observed levels. The agreement between observation and simulation improved significantly when the irreversible uptake and the reversible partitioning were incorporated into the model, which in total both contributed ∼ 62 % to the destruction of Gly and Mgly during daytime. Further analysis of the photochemical budget of Gly and Mgly showed that the oxidation of aromatics by the OH radical was the major pathway producing Gly and Mgly, followed by degradation of alkynes and alkenes. Furthermore, based on the improved model mechanism, the contributions of VOC oxidation to SOA formed from gas–particle partitioning (SOAgp) and from heterogeneous processes of Gly and Mgly (SOAhet) were also quantified. It was found that o-xylene was the most significant contributor to SOAgp formation (∼ 29 %), while m,p-xylene and toluene made dominant contributions to SOAhet formation. Overall, the heterogeneous processes of Gly and Mgly can explain ∼ 21 % of SOA mass in the PRD region. The results of this study demonstrated the important roles of heterogeneous processes of Gly and Mgly in SOA formation and highlighted the need for a better understanding of the evolution of intermediate oxidation products.

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A new method for the determination of imidazole-like brown carbons using gas chromatography-mass spectrometry

Chen

Lin

2023

Atmospheric Pollution Research

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Methylglyoxal Uptake Coefficients on Aqueous Aerosol Surfaces

Cited by 23 publications

References 43 publications

Assessment of dicarbonyl contributions to secondary organic aerosols over China using RAMS-CMAQ

Assessment of dicarbonyl contributions to secondary organic aerosols over China using RAMS-CMAQ

Formation and sink of glyoxal and methylglyoxal in a polluted subtropical environment: observation-based photochemical analysis and impact evaluation

A new method for the determination of imidazole-like brown carbons using gas chromatography-mass spectrometry

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