Tilgner, A., Bräuer, P. orcid.org/0000-0002-3815-7631, Wolke, R. et al. (1 more author) (2013) Modelling multiphase chemistry in deliquescent aerosols and clouds using CAPRAM3.0i. Journal of Atmospheric Chemistry. pp. 221-256. ISSN 0167-7764
Abstract
Modelling studies were performed with the multiphase mechanism RACM- MIM2ext/CAPRAM 3.0i to investigate the tropospheric multiphase chemistry in deli- quesced particles and non-precipitating clouds using the SPACCIM model framework. Simulations using a non-permanent cloud scenario were carried out for two different environmental conditions focusing on the multiphase chemistry of oxidants and other linked chemical subsystems. Model results were analysed by time-resolved reaction flux analyses allowing advanced interpretations. The model shows significant effects of multiphase chemical interactions on the tropospheric budget of gas-phase oxidants and organic com- pounds. In-cloud gas-phase OH radical concentration reductions of about 90 % and 75 % were modelled for urban and remote conditions, respectively. The reduced in-cloud gas- phase oxidation budget increases the tropospheric residence time of organic trace gases by up to about 30 %. Aqueous-phase oxidations of methylglyoxal and 1,4-butenedial were identified as important OH radical sinks under polluted conditions. The model revealed that the organic C3 and C4 chemistry contributes with about 38 %/48 % and 8 %/9 % consid- erably to the urban and remote cloud / aqueous particle OH sinks. Furthermore, the simulations clearly implicate the potential role of deliquescent particles to operate as a reactive chemical medium due to an efficient TMI/HOx,y chemical processing including e.g. an effective in-situ formation of OH radicals. Considerable chemical differences be- tween deliquescent particles and cloud droplets, e.g. a circa 2 times more efficient daytime iron processing in the urban deliquescent particles, were identified. The in-cloud oxidation of methylglyoxal and its oxidation products is identified as efficient sink for NO3 radicals in the aqueous phase.
Metadata
Item Type: | Article |
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Authors/Creators: |
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Dates: |
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Institution: | The University of York |
Academic Units: | The University of York > Faculty of Sciences (York) > Chemistry (York) |
Depositing User: | Pure (York) |
Date Deposited: | 28 Oct 2016 08:58 |
Last Modified: | 03 Apr 2025 23:09 |
Published Version: | https://doi.org/10.1007/s10874-013-9267-4 |
Status: | Published |
Refereed: | Yes |
Identification Number: | 10.1007/s10874-013-9267-4 |
Open Archives Initiative ID (OAI ID): | oai:eprints.whiterose.ac.uk:106202 |
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