Comment on mathematical models of the uptake of ClONO2 and other gases by atmospheric aerosols

Kolb, C. E.; Worsnop, D. R.; Jayne, John T.; Davidovits, P.

doi:10.1016/s0021-8502(97)10022-2

Cited by 7 publications

(6 citation statements)

References 23 publications

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“…for pressures in the range 14-25 torr) the deviation from the Fuchs-Sutugin formulation is less than 5% and for most experiments even less then 3%. This conclusion is similar to the one reached by Kolb et al (1998). Therefore, we are confident that, under our experimental conditions, Eq.…”

Section: Resultssupporting

confidence: 91%

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Uptake study of ClONO2 and BrONO2 by Halide containing droplets

Deiber

George²,

Calvé

et al. 2004

Atmos. Chem. Phys.

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Abstract. The uptake kinetics of gaseous ClONO 2 and BrONO 2 on aqueous surfaces were measured, as a function of temperature and liquid composition (pure water and NaCl or NaBr containing solutions) using the droplet train technique coupled to a mass spectrometer. The uptake kinetics are driven by the reactivity of these gases and, for both compounds, the uptake rates on pure water or on NaCl solutions (0.1 M) are comparable. The uptake coefficient γ of ClONO 2 does not depend on the temperature while that of BrONO 2 increases slightly when the temperature is raised from 272 to 280 K. For ClONO 2 and BrONO 2 , the uptake rates increase on NaBr-doped droplets, enabling the estimation of the mass accommodation coefficient α. The corresponding values for α are 0.108±0.033 for ClONO 2 and 0.063±0.021 for BrONO 2 where the statistical errors correspond to ±2σ .The reactions of ClONO 2 and BrONO 2 on NaCl solutions lead respectively to the formation of Cl 2 and BrCl. The uptake of ClONO 2 on NaBr solutions generates BrCl as primary product, which in turn can react with NaBr to produce Br 2 . As expected, the only product of BrONO 2 reaction on NaBr solution is Br 2 .

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Section: Resultssupporting

confidence: 91%

“…The application of Eq. (8) was recently the subject of some discussion (Kolb et al, 1998;Widmann and Davis, 1997), especially the diffusion correction formulation which is based on the work of Schwartz (1986) who derived in a "simple but effective" manner the background leading to Eq. (8).…”

Section: Resultsmentioning

confidence: 99%

Uptake study of ClONO2 and BrONO2 by Halide containing droplets

Deiber

George²,

Calvé

et al. 2004

Atmos. Chem. Phys.

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“…Therefore, the uptake coefficient may be described according to 11 where the term -1/2 accounts for the distortion of the Boltzmann collision rate. 32 The gas-phase diffusion coefficient (D g ) needed have been estimated by the method of Reid et al 35 The application of eq 6 was recently the subject of some discussion, 36,37 especially the diffusion correction formulation which is based on the work of Schwartz 38 who derived in a "simple but effective" manner the background leading to eq 6. As already underlined by several authors, most of the expressions describing the kinetics of mass transport are subject to some criticisms because of the assumptions made in their derivation.…”

Section: Resultsmentioning

confidence: 99%

Experimental Uptake Study of Ethanol by Water Droplets and Its Theoretical Modeling of Cluster Formation at the Interface

Katrib¹,

Mirabel²,

Calvé³

et al. 2002

J. Phys. Chem. B

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Uptake measurements of ethanol were performed to provide experimental values for a theoretical approach of its incorporation into a water droplet. The uptake coefficients of ethanol on pure water were therefore measured as a function of temperature, using the droplet train technique coupled to a mass spectrometric detection. They were found to be independent of the aqueous phase composition and of the gas-liquid contact times. Their values show a negative temperature dependence, varying from 3.8 × 10 -2 to 2.1 × 10 -2 in the temperature range 266-280 K. From these kinetic data, the mass accommodation coefficient R was derived and was found to vary from 4.6 × 10 -2 to 2.4 × 10 -2 for the same temperature range. The results are used to discuss the uptake process involved in the incorporation of ethanol into an aqueous phase, using nucleation theory and quantum mechanical calculations. The small value of the experimental N* motivated calculations on very small clusters of the type ethanol-(H 2 O) n)1,3 . This theoretical work shows the specific role of a cluster containing the ethanol molecule and only one water molecule. It could be a step toward either the growing of the cluster or its uptake by the surface of the droplet. Both the experimental and the theoretical works show that ethanol and methanol behave similarly.

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“…We note that the term "reacto-diffusive" traditionally referred to bulk reaction systems with a strong gradient in X and no gradient in Y (see e.g. Danckwerts, 1951;Schwartz, 1986;Hanson et al, 1994;Davidovits et al, 1995;Ravishankara, 1997;Kolb et al, 1998;Ravishankara and Longfellow, 1999;Davidovits et al, 2006;Pöschl et al, 2007;Kolb et al, 2010). Throughout this paper we will refer to this case as the "traditional reacto-diffusive case".…”

Section: Mass Transportmentioning

confidence: 99%

Kinetic regimes and limiting cases of gas uptake and heterogeneous reactions in atmospheric aerosols and clouds: a general classification scheme

et al. 2013

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Abstract. Heterogeneous reactions are important to atmospheric chemistry and are therefore an area of intense research. In multiphase systems such as aerosols and clouds, chemical reactions are usually strongly coupled to a complex sequence of mass transport processes and results are often not easy to interpret. Here we present a systematic classification scheme for gas uptake by aerosol or cloud particles which distinguishes two major regimes: a reaction-diffusion regime and a mass transfer regime. Each of these regimes includes four distinct limiting cases, characterised by a dominant reaction location (surface or bulk) and a single rate-limiting process: chemical reaction, bulk diffusion, gas-phase diffusion or mass accommodation. The conceptual framework enables efficient comparison of different studies and reaction systems, going beyond the scope of previous classification schemes by explicitly resolving interfacial transport processes and surface reactions limited by mass transfer from the gas phase. The use of kinetic multi-layer models instead of resistor model approaches increases the flexibility and enables a broader treatment of the subject, including cases which do not fit into the strict limiting cases typical of most resistor model formulations. The relative importance of different kinetic parameters such as diffusion, reaction rate and accommodation coefficients in this system is evaluated by a quantitative global sensitivity analysis. We outline the characteristic features of each limiting case and discuss the potential relevance of different regimes and limiting cases for various reaction systems. In particular, the classification scheme is applied to three different datasets for the benchmark system of oleic acid reacting with ozone in order to demonstrate utility and highlight potential issues. In light of these results, future directions of research needed to elucidate the multiphase chemical kinetics in this and other reaction systems are discussed.

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Comment on mathematical models of the uptake of ClONO2 and other gases by atmospheric aerosols

Cited by 7 publications

References 23 publications

Uptake study of ClONO<sub>2</sub> and BrONO<sub>2</sub> by Halide containing droplets

Uptake study of ClONO<sub>2</sub> and BrONO<sub>2</sub> by Halide containing droplets

Experimental Uptake Study of Ethanol by Water Droplets and Its Theoretical Modeling of Cluster Formation at the Interface

Kinetic regimes and limiting cases of gas uptake and heterogeneous reactions in atmospheric aerosols and clouds: a general classification scheme

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Comment on mathematical models of the uptake of ClONO2 and other gases by atmospheric aerosols

Cited by 7 publications

References 23 publications

Uptake study of ClONO&lt;sub&gt;2&lt;/sub&gt; and BrONO&lt;sub&gt;2&lt;/sub&gt; by Halide containing droplets

Uptake study of ClONO&lt;sub&gt;2&lt;/sub&gt; and BrONO&lt;sub&gt;2&lt;/sub&gt; by Halide containing droplets

Experimental Uptake Study of Ethanol by Water Droplets and Its Theoretical Modeling of Cluster Formation at the Interface

Kinetic regimes and limiting cases of gas uptake and heterogeneous reactions in atmospheric aerosols and clouds: a general classification scheme

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Product

Resources

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Uptake study of ClONO<sub>2</sub> and BrONO<sub>2</sub> by Halide containing droplets

Uptake study of ClONO<sub>2</sub> and BrONO<sub>2</sub> by Halide containing droplets