How alkaline compounds control atmospheric aerosol acidity

Karydis, Vlassis A.; Tsimpidi, Alexandra P.; Pozzer, Andrea; Lelieveld, Jos

doi:10.5194/acp-2020-1222

Cited by 3 publications

(1 citation statement)

References 79 publications

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“…Nevertheless, in the case of the forward and reverse reactions, they typically occur fast and thus the concentrations of the reactants and the products are generally assumed to be in equilibrium in the global model due to its relatively long timestep and large model grid. Note, however, that recent modeling studies showed that the metastable assumption applied here could lead to an increase of aerosols' acidity (i.e., regionally up to 2 pH-units in the presence of crustal elements over dust sources, and roughly 0.5 pH units globally; Karydis et al, 2020) compared to the stable aerosol state assumption (i.e., the aerosols both in solid and liquid phases).…”

Section: Thermodynamic Equilibrium and Atmospheric Acidity Calculationsmentioning

confidence: 68%

Multiphase processes in the EC-Earth Earth System model and their relevance to the atmospheric oxalate, sulfate, and iron cycles

Myriokefalitakis

Bergas‐Massó

Gonçalves

et al. 2021

Preprint

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Abstract. Understanding how multiphase processes affect the iron-containing aerosol cycle is key to predict ocean biogeochemistry changes and hence the feedback effects on climate. For this work, the EC-Earth Earth system model in its climate-chemistry configuration is used to simulate the global atmospheric oxalate (OXL), sulfate (SO42−), and iron (Fe) cycles, after incorporating a comprehensive representation of the multiphase chemistry in cloud droplets and aerosol water. The model considers a detailed gas-phase chemistry scheme, all major aerosol components, and the partitioning of gases in aerosol and atmospheric water phases. The dissolution of Fe-containing aerosols accounts kinetically for the solution’s acidity, oxalic acid, and irradiation. Aerosol acidity is explicitly calculated in the model, both for accumulation and coarse modes, accounting for thermodynamic processes involving inorganic and crustal species from sea salt and dust. Simulations for present-day conditions (2000–2014) have been carried out with both EC-Earth and the atmospheric composition component of the model in standalone mode driven by meteorological fields from ECMWF’s ERA-Interim reanalysis. The calculated global budgets are presented and the links between the 1) aqueous-phase processes, 2) aerosol dissolution, and 3) atmospheric composition, are demonstrated and quantified. The model results are supported by comparison to available observations. We obtain an average global OXL net chemical production of 12.61 ± 0.06 Tg yr−1 in EC-Earth, with glyoxal being by far the most important precursor of oxalic acid. In comparison to the ERA-Interim simulation, differences in atmospheric dynamics as well as the simulated weaker oxidizing capacity in EC-Earth result overall in a ~30 % lower OXL source. On the other hand, the more explicit representation of the aqueous-phase chemistry in EC-Earth compared to the previous versions of the model leads to an overall ~20 % higher sulfate production, but still well correlated with atmospheric observations. The total Fe dissolution rate in EC-Earth is calculated at 0.806 ± 0.014 Tg Fe yr−1 and is added to the primary dissolved Fe (DFe) sources from dust and combustion aerosols in the model (0.072 ± 0.001 Tg Fe yr−1). The simulated DFe concentrations show a satisfactory comparison with available observations, indicating an atmospheric burden of ∼0.007 Tg Fe, and overall resulting in an atmospheric deposition flux into the global ocean of 0.376 ± 0.005 Tg Fe yr−1, well within the range reported in the literature. All in all, this work is a first step towards the development of EC-Earth into an Earth System Model with fully interactive bioavailable atmospheric Fe inputs to the marine biogeochemistry component of the model.

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Section: Thermodynamic Equilibrium and Atmospheric Acidity Calculationsmentioning

confidence: 68%

Multiphase processes in the EC-Earth Earth System model and their relevance to the atmospheric oxalate, sulfate, and iron cycles

Myriokefalitakis

Bergas‐Massó

Gonçalves

et al. 2021

Preprint

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Impacts of the East Asia monsoon on the PM2.5 acidity in Hanoi

Hien,

Vuong,

Anh

et al. 2024

Atmospheric Pollution Research

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Seasonal adjustment of particulate matter pollution in coastal East Asia during the 2020 COVID lockdown

2021

Environ. Res. Lett.

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Seasonally, the East Asian particulate matter (PM) level is higher in the winter–spring period than in summer, at which time the level rapidly decreases due to the summer monsoon migration. Attempting to attribute East Asian PM pollution to a source without considering such natural factors is challenging. However, to what degree the effect of season on an attribution bias remains controversial; the bias may even be implicated in PM-related health effects. This study examined seasonal dynamics including the unusual precipitation evolution during 2020—a year in which coronavirus-related lockdowns occurred frequently worldwide—and suggested a large-scale effect from the removal of PM pollutants from most of the coastal cities in East Asia. In winter–spring 2020, compared with that of previous years, a deeper and farther southward intrusion of the East Asian coastal trough and a stronger surface monsoon flow acted jointly to transport air pollutants over the Korea–Japan region. In summer 2020, the strength and migration of the western North Pacific (WNP) high increased precipitation and removed air pollutants in mid-latitude East Asia, whereas it reduced precipitation in the subtropical WNP. Consequently, the reduced PM level in the subtropical region (including Taiwan) may be irrelevant to the anomalous seasonal pattern. Although an artificial effect is conceivable and may be primarily responsible for the marked decrease in 2020 East Asian PM pollutants in some subtropical cities, the modulation of a large-scale and precipitating effect also deserves consideration.

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How alkaline compounds control atmospheric aerosol acidity

Cited by 3 publications

References 79 publications

Multiphase processes in the EC-Earth Earth System model and their relevance to the atmospheric oxalate, sulfate, and iron cycles

Multiphase processes in the EC-Earth Earth System model and their relevance to the atmospheric oxalate, sulfate, and iron cycles

Impacts of the East Asia monsoon on the PM2.5 acidity in Hanoi

Seasonal adjustment of particulate matter pollution in coastal East Asia during the 2020 COVID lockdown

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