Aqueous chemistry and its role in secondary organic aerosol (SOA) formation

Lim, Yong Bin; Tan, Yinling; Perri, Mark J.; Seitzinger, Sybil P.; Turpin, Barbara J.

doi:10.5194/acp-10-10521-2010

Cited by 555 publications

(772 citation statements)

References 110 publications

(218 reference statements)

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“…The released OH radicals within particles or cloud droplets can oxidize other organic compounds, producing low-volatility products, including organic acids, peroxides and oligomers (Lim et al, 2010;McNeill et al, 2012;Ervens, 2015;Herrmann et al, 2015). Autoxidation in the condensed phase might be triggered by OH radicals forming highly oxidized compounds .…”

Section: Discussionmentioning

confidence: 99%

Quantification of environmentally persistent free radicals and reactive oxygen species in atmospheric aerosol particles

et al. 2016

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Abstract. Fine particulate matter plays a central role in the adverse health effects of air pollution. Inhalation and deposition of aerosol particles in the respiratory tract can lead to the release of reactive oxygen species (ROS), which may cause oxidative stress. In this study, we have detected and quantified a wide range of particle-associated radicals using electron paramagnetic resonance (EPR) spectroscopy. Ambient particle samples were collected using a cascade impactor at a semi-urban site in central Europe, Mainz, Germany, in May-June 2015. Concentrations of environmentally persistent free radicals (EPFR), most likely semiquinone radicals, were found to be in the range of (1-7) × 10 11 spins µg −1 for particles in the accumulation mode, whereas coarse particles with a diameter larger than 1 µm did not contain substantial amounts of EPFR. Using a spin trapping technique followed by deconvolution of EPR spectra, we have also characterized and quantified ROS, including OH, superoxide (O − 2 ) and carbon-and oxygen-centered organic radicals, which were formed upon extraction of the particle samples in water. Total ROS amounts of (0.1-3) ×10 11 spins µg −1 were released by submicron particle samples and the relative contributions of OH, O − 2 , C-centered and O-centered organic radicals were ∼ 11-31, ∼ 2-8, ∼ 41-72 and ∼ 0-25 %, respectively, depending on particle sizes. OH was the dominant species for coarse particles. Based on comparisons of the EPR spectra of ambient particulate matter with those of mixtures of organic hydroperoxides, quinones and iron ions followed by chemical analysis using liquid chromatography mass spectrometry (LC-MS), we suggest that the particle-associated ROS were formed by decomposition of organic hydroperoxides interacting with transition metal ions and quinones contained in atmospheric humic-like substances (HULIS).

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Section: Discussionmentioning

confidence: 99%

Quantification of environmentally persistent free radicals and reactive oxygen species in atmospheric aerosol particles

et al. 2016

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“…In general, most models use both gas and aqueous-phase mechanisms, with relatively more detail in the gas phase mechanisms. The more explicit treatment of liquid-phase chemistry is included in limited area models that simulate interactions with cloud systems (Tilgner et al, 2010;Lim et al, 2010). Lim et al (2010) showed the importance of aqueous-phase chemistry in the production of secondary organic aerosol (SOA).…”

Section: Atmospheric Chemical Mechanisms: Gas and Aqueous-phasementioning

confidence: 99%

Online coupled regional meteorology chemistry models in Europe: current status and prospects

et al. 2014

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Published by Copernicus Publications on behalf of the European Geosciences Union. A. Baklanov et al.: Online coupled regional meteorology chemistry models in EuropeAbstract. Online coupled mesoscale meteorology atmospheric chemistry models have undergone a rapid evolution in recent years. Although mainly developed by the air quality modelling community, these models are also of interest for numerical weather prediction and regional climate modelling as they can consider not only the effects of meteorology on air quality, but also the potentially important effects of atmospheric composition on weather. Two ways of online coupling can be distinguished: online integrated and online access coupling. Online integrated models simulate meteorology and chemistry over the same grid in one model using one main time step for integration. Online access models use independent meteorology and chemistry modules that might even have different grids, but exchange meteorology and chemistry data on a regular and frequent basis. This article offers a comprehensive review of the current research status of online coupled meteorology and atmospheric chemistry modelling within Europe. Eighteen regional online coupled models developed or being used in Europe are described and compared. Topics discussed include a survey of processes relevant to the interactions between atmospheric physics, dynamics and composition; a brief overview of existing online mesoscale models and European model developments; an analysis on how feedback processes are treated in these models; numerical issues associated with coupled models; and several case studies and model performance evaluation methods. Finally, this article highlights selected scientific issues and emerging challenges that require proper consideration to improve the reliability and usability of these models for the three scientific communities: air quality, numerical meteorology modelling (including weather prediction) and climate modelling. This review will be of particular interest to model developers and users in all three fields as it presents a synthesis of scientific progress and provides recommendations for future research directions and priorities in the development, application and evaluation of online coupled models.

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“…From an environmental health perspective, deposition of LMWOAs may have ecosystem impacts as they have been shown to be toxic to various marine invertebrates (Staples et al, 2000;Sverdrup et al, 2001), phytotoxic (Himanen et al, 2012;Lynch, 1977), and interfere with the uptake and mobilization of heavy metals by microbial communities in soils (Song et al, 2016;Menezes-Blackburn et al, 2016). However, studies on the human toxicity of LMWOAs are sparse and the results are unclear (Rydzynski, 1997;Azuma et al, 2016).…”

Section: Introductionmentioning

confidence: 99%

“…They are key participants in the aqueous-phase chemistry of clouds and contribute to SOA formation through various reactions within the aqueous portion of the particle phase (Carlton et al, 2007;Ervens et al, 2004;Lim et al, 2010). Furthermore, since organic acids can be photochemical products, they can also serve as indicators of atmospheric transformation processes.…”

Section: Introductionmentioning

confidence: 99%

Understanding the primary emissions and secondary formation of gaseous organic acids in the oil sands region of Alberta, Canada

et al. 2017

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Abstract. Organic acids are known to be emitted from combustion processes and are key photochemical products of biogenic and anthropogenic precursors. Despite their multiple environmental impacts, such as on acid deposition and human-ecosystem health, little is known regarding their emission magnitudes or detailed chemical formation mechanisms. In the current work, airborne measurements of 18 gas-phase low-molecular-weight organic acids were made in the summer of 2013 over the oil sands region of Alberta, Canada, an area of intense unconventional oil extraction. The data from these measurements were used in conjunction with emission retrieval algorithms to derive the total and speciated primary organic acid emission rates, as well as secondary formation rates downwind of oil sands operations. The results of the analysis indicate that approximately 12 t day −1 of low-molecular-weight organic acids, dominated by C 1 -C 5 acids, were emitted directly from off-road diesel vehicles within open pit mines. Although there are no specific reporting requirements for primary organic acids, the measured emissions were similar in magnitude to primary oxygenated hydrocarbon emissions, for which there are reporting thresholds, measured previously (≈ 20 t day −1 ). Conversely, photochemical production of gaseous organic acids significantly exceeded the primary sources, with formation rates of up to ≈ 184 t day −1 downwind of the oil sands facilities. The formation and evolution of organic acids from a Lagrangian flight were modelled with a box model, incorporating a detailed hydrocarbon reaction mechanism extracted from the Master Chemical Mechanism (v3.3). Despite evidence of significant secondary organic acid formation, the explicit chemical box model largely underestimated their formation in the oil sands plumes, accounting for 39, 46, 26, and 23 % of the measured formic, acetic, acrylic, and propionic acids respectively and with little contributions from biogenic VOC precursors. The model results, together with an examination of the carbon mass balance between the organic acids formed and the primary VOCs emitted from oil sands operations, suggest the existence of significant missing secondary sources and precursor emissions related to oil sands and/or an incomplete mechanistic and quantitative understanding of how they are processed in the atmosphere.

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Aqueous chemistry and its role in secondary organic aerosol (SOA) formation

Cited by 555 publications

References 110 publications

Quantification of environmentally persistent free radicals and reactive oxygen species in atmospheric aerosol particles

Quantification of environmentally persistent free radicals and reactive oxygen species in atmospheric aerosol particles

Online coupled regional meteorology chemistry models in Europe: current status and prospects

Understanding the primary emissions and secondary formation of gaseous organic acids in the oil sands region of Alberta, Canada

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