CLEPS 1.0: A new protocol for cloud aqueous phase oxidation of VOC mechanisms
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Published:2017-03-29
Issue:3
Volume:10
Page:1339-1362
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ISSN:1991-9603
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Container-title:Geoscientific Model Development
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language:en
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Short-container-title:Geosci. Model Dev.
Author:
Mouchel-Vallon Camille, Deguillaume Laurent, Monod Anne, Perroux Hélène, Rose ClémenceORCID, Ghigo Giovanni, Long Yoann, Leriche Maud, Aumont BernardORCID, Patryl Luc, Armand Patrick, Chaumerliac Nadine
Abstract
Abstract. A new detailed aqueous phase mechanism named the Cloud Explicit Physico-chemical Scheme (CLEPS 1.0) is proposed to describe the oxidation of water soluble organic compounds resulting from isoprene oxidation. It is based on structure activity relationships (SARs) which provide global rate constants together with branching ratios for HO⋅ abstraction and addition on atmospheric organic compounds. The GROMHE SAR allows the evaluation of Henry's law constants for undocumented organic compounds. This new aqueous phase mechanism is coupled with the MCM v3.3.1 gas phase mechanism through a mass transfer scheme between gas phase and aqueous phase. The resulting multiphase mechanism has then been implemented in a model based on the Dynamically Simple Model for Atmospheric Chemical Complexity (DSMACC) using the Kinetic PreProcessor (KPP) that can serve to analyze data from cloud chamber experiments and field campaigns. The simulation of permanent cloud under low-NOx conditions describes the formation of oxidized monoacids and diacids in the aqueous phase as well as a significant influence on the gas phase chemistry and composition and shows that the aqueous phase reactivity leads to an efficient fragmentation and functionalization of organic compounds.
Publisher
Copernicus GmbH
Reference127 articles.
1. Alfassi, Z. B. (Ed.): The Chemistry of Free Radicals: Peroxyl Radicals, Wiley, New York, 1997. 2. Arakaki, T., Anastasio, C., Kuroki, Y., Nakajima, H., Okada, K., Kotani, Y., Handa, D., Azechi, S., Kimura, T., Tsuhako, A., and Miyagi, Y.: A general scavenging rate constant for reaction of hydroxyl radical with organic carbon in atmospheric waters, Environ. Sci. Technol., 47, 8196–8203, https://doi.org/10.1021/es401927b, 2013. 3. Asmus, K. D., Moeckel, H., and Henglein, A.: Pulse radiolytic study of the site of hydroxyl radical attack on aliphatic alcohols in aqueous solution, J. Phys. Chem., 77, 1218–1221, https://doi.org/10.1021/j100629a007, 1973. 4. Aumont, B., Szopa, S., and Madronich, S.: Modelling the evolution of organic carbon during its gas-phase tropospheric oxidation: development of an explicit model based on a self generating approach, Atmos. Chem. Phys., 5, 2497–2517, https://doi.org/10.5194/acp-5-2497-2005, 2005. 5. Barth, M. C., Sillman, S., Hudman, R., Jacobson, M. Z., Kim, C. H., Monod, A., and Liang, J.: Summary of the cloud chemistry modeling intercomparison: Photochemical box model simulation, J. Geophys. Res., 108, 4214, https://doi.org/10.1029/2002JD002673, 2003.
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