CLEPS 1.0: A new protocol for cloud aqueous phase oxidation of VOC mechanisms

Mouchel‐Vallon, Camille; Deguillaume, Laurent; Monod, Anne; Perroux, Hélène; Rose, Clémence; Ghigo, Giovanni; Long, Y.; Leriche, Maud; Aumont, Bernard; Patryl, Luc; Armand, Patrick; Chaumerliac, Nadine

doi:10.5194/gmd-10-1339-2017

Cited by 40 publications

(51 citation statements)

References 117 publications

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“…Vallon and coworkers focused on oxidation processes, paying particular attention to the competition between fragmentation and functionalization (Mouchel-Vallon et al, 2017). They developed a protocol to build CLEPS 1.0 (Cloud Explicit Physico-chemical Scheme), a new detailed aqueousphase oxidation mechanism for low-NO x conditions that is able to describe multiple oxidation pathways for each of the considered C 1 -C 4 organic species.…”

Section: Rose Et Al: Modeling the Partitioning Of Organic Chemicamentioning

confidence: 99%

“…The coupled model can also provide insights into the processing of these particle-originating organic species in the cloud aqueous phase. To make the most of these opportunities, the oxidation pathways of several additional C 4 dicarboxylic acids were implemented in CLEPS (V1.1) compared to the initial version of the mechanism introduced in Mouchel-Vallon et al (2017). In addition to abovementioned nucleation-scavenging-related aspects, the model also allows for the evaluation of the importance of cloud microphysical processes in the redistribution of the reactive compounds among the different phases (gas, cloud and rain) (Leriche et al, 2001).…”

Section: Rose Et Al: Modeling the Partitioning Of Organic Chemicamentioning

confidence: 99%

“…The ability of the coupled model to predict concentrations in the range of those measured during cloud events at the PUY station is finally tested. The recent cloud chemistry model based on the explicit aqueous-phase oxidation mechanism CLEPS 1.0 was first introduced in Mouchel-Vallon et al (2017), where a detailed description can be found. In addition to the inorganic chemical scheme previously described in Deguillaume et al (2004) and in Leriche et al (2007), CLEPS 1.0 describes the HO q and NO 3 q oxidation pathways of C 1-4 organic compounds following the methodology developed by Mouchel-Vallon et al (2017).…”

Section: Rose Et Al: Modeling the Partitioning Of Organic Chemicamentioning

confidence: 99%

“…The recent cloud chemistry model based on the explicit aqueous-phase oxidation mechanism CLEPS 1.0 was first introduced in Mouchel-Vallon et al (2017), where a detailed description can be found. In addition to the inorganic chemical scheme previously described in Deguillaume et al (2004) and in Leriche et al (2007), CLEPS 1.0 describes the HO q and NO 3 q oxidation pathways of C 1-4 organic compounds following the methodology developed by Mouchel-Vallon et al (2017). CLEPS 1.0 relies on recent improvements in the estimation of kinetic and thermodynamic parameters based on structure-activity relationships (SARs) derived from experimental data (Doussin and Monod, 2013;Minakata et al, 2009;Monod and Doussin, 2008;Raventos-Duran et al, 2010).…”

Section: Rose Et Al: Modeling the Partitioning Of Organic Chemicamentioning

confidence: 99%

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Modeling the partitioning of organic chemical species in cloud phases with CLEPS (1.1)

Chaumerliac¹,

Deguillaume²,

Perroux³

et al. 2018

Atmos. Chem. Phys.

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Abstract. The new detailed aqueous-phase mechanism Cloud Explicit Physico-chemical Scheme (CLEPS 1.0), which describes the oxidation of isoprene-derived watersoluble organic compounds, is coupled with a warm microphysical module simulating the activation of aerosol particles into cloud droplets. CLEPS 1.0 was then extended to CLEPS 1.1 to include the chemistry of the newly added dicarboxylic acids dissolved from the particulate phase. The resulting coupled model allows the prediction of the aqueousphase concentrations of chemical compounds originating from particle scavenging, mass transfer from the gas-phase and in-cloud aqueous chemical reactivity. The aim of the present study was more particularly to investigate the effect of particle scavenging on cloud chemistry. Several simulations were performed to assess the influence of various parameters on model predictions and to interpret long-term measurements conducted at the top of Puy de Dôme (PUY, France) in marine air masses. Specific attention was paid to carboxylic acids, whose predicted concentrations are on average in the lower range of the observations, with the exception of formic acid, which is rather overestimated in the model. The different sensitivity runs highlight the fact that formic and acetic acids mainly originate from the gas phase and have highly variable aqueous-phase reactivity depending on the cloud acidity, whereas C 3 -C 4 carboxylic acids mainly originate from the particulate phase and are supersaturated in the cloud.

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Section: Rose Et Al: Modeling the Partitioning Of Organic Chemicamentioning

confidence: 99%

Section: Rose Et Al: Modeling the Partitioning Of Organic Chemicamentioning

confidence: 99%

Section: Rose Et Al: Modeling the Partitioning Of Organic Chemicamentioning

confidence: 99%

Section: Rose Et Al: Modeling the Partitioning Of Organic Chemicamentioning

confidence: 99%

See 2 more Smart Citations

Modeling the partitioning of organic chemical species in cloud phases with CLEPS (1.1)

Chaumerliac¹,

Deguillaume²,

Perroux³

et al. 2018

Atmos. Chem. Phys.

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“…The dissolution of particles into liquid phase after nucleation depends on several factors: the solubility of trace metals is radical via the photolysis of Fe(III) and the Fenton reaction in some kind of catalytic cycle where it is regenerated [1]. These reactions are considered in cloud chemistry models [21][22][23], but the ability of iron to control the oxidative budget depends on the presence of carboxylate compounds that can complex the iron [24,25]. Recently, siderophore molecules, like pyoverdine, produced by microbial activity are likely to complex Fe [26,27].…”

Section: Introductionmentioning

confidence: 99%

Trace Metals in Cloud Water Sampled at the Puy De Dôme Station

et al. 2017

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Concentrations of 33 metal elements were determined by ICP-MS (Inductively CoupledPlasma Mass Spectrometry) analysis for 24 cloud water samples (corresponding to 10 cloud events) collected at the puy de Dôme station. Clouds present contrasted chemical composition with mainly marine and continental characteristics; for some cloud events, a further anthropogenic source can be superimposed on the background level. In this context, measurements of trace metals may help to evaluate the impact of anthropogenic and natural sources on the cloud and to better discriminate the origin of the air masses. The metal concentrations in the samples are low (between 16.4 µg L −1 and 1.46 mg L −1 ). This could be explained by the remoteness of the puy de Dôme site from local sources. Trace metals are then used to confirm and refine a previous sample classification. A principal component analysis (PCA) using the pH value and the concentrations of Cl − , NO 3 − , SO 4 2− , Na + and NH 4 + is performed considering 24 cloud samples. This first analysis shows that 18 samples are of marine origin and 6 samples are classified as continental. The same statistical approach is used adding trace metal concentration. Zn and Mg elements are the most abundant trace metals for all clouds. A higher concentration of Cd is mainly associated to clouds from marine origins. Cu, As, Tl and Sb elements are rather found in the continental samples than in the marine ones. Mg, V, Mn and Rb elements mainly found in soil particles are also more concentrated in the samples from continental air mass. This new PCA including trace metal confirms the classification between marine and continental air masses but also indicates that one sample presenting low pH and high concentrations of SO 4 2− , Fe, Pb and Cu could be rather attributed to a polluted event.

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