2002
DOI: 10.1029/2002gl015542
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A chemical kinetic model for reactive transformations of aerosol particles

Abstract: [1] A simple formalism is presented to model chemical interactions between aerosols and reactive trace gases over a wide range of conditions. The model takes into account gas phase diffusion, mass accommodation, bulk phase chemical reactions, surface reactions and particle phase reactant diffusion from the aerosol interior toward the surface. While previous models have focused on the heterogeneous uptake of trace gases by atmospheric droplets and particles, this model focuses on the reactive transformation of … Show more

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Cited by 144 publications
(253 citation statements)
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References 17 publications
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“…that the surface is refreshed via mixing within the particle and/or OH can undergo substantial diffusion into the particle. However, a model based on reactive uptake of OH to a liquid particle, that includes the assumption that every OH colliding with the particle surface would encounter the initial particle component (Worsnop et al, 2002), does not reproduce the majority of our data well.…”
Section: Oxidation Of Pure Palmitic Acid Particlescontrasting
confidence: 44%
See 1 more Smart Citation
“…that the surface is refreshed via mixing within the particle and/or OH can undergo substantial diffusion into the particle. However, a model based on reactive uptake of OH to a liquid particle, that includes the assumption that every OH colliding with the particle surface would encounter the initial particle component (Worsnop et al, 2002), does not reproduce the majority of our data well.…”
Section: Oxidation Of Pure Palmitic Acid Particlescontrasting
confidence: 44%
“…Schematic of the experimental set-up as those that are supercooled or structured (Hearn and Smith, 2005;Katrib et al, 2005;Knopf et al, 2005). Therefore, the reactive zone for OH oxidation, which is expected to be fast (Bertram et al, 2001;Molina et al, 2004;Lambe et al, 2007;George et al, 2007), may be confined to the particle surface or near-surface region (Hanson et al, 1994;Worsnop et al, 2002) leading to differences in the transformation rates between the surface and bulk (Maria et al, 2004). To our knowledge, this aspect has not been thoroughly examined by laboratory studies.…”
Section: Introductionmentioning
confidence: 98%
“…We postulate that the reacto-diffusion length L in a wellmixed particle is more appropriately defined as L= √ 2 D orgn ∆ t coll , where Dorgn is the onedimensional, radial self-diffusion coefficient of the organic component of the particle, and the time interval is determined by the reactive collision frequency of OH with the particle surface. This is distinct from several other definitions in the literature 22,24,61 in an important conceptual way. Relationships have been proposed that utilize the reaction rate constant between the gas molecule and the organic species in the aerosol, whether at the surface or in the bulk, to provide a fundamental clock in the coupled reaction-diffusion system.…”
Section: Discussionmentioning
confidence: 65%
“…The value of γ 0 calculated from experimental measurements using Eq. (1) was corrected for gas-phase diffusion by applying an empirical formulation by Fuchs and Sutugin (Fuchs and Sutugin, 1970;Worsnop et al, 2002 (Massman, 1998), which was calculated to be D OH =0.260 cm 2 s −1 for our flow conditions. This value is close to the experimental D OH value measured in dry air (Ivanov et al, 2007).…”
Section: Kinetic Studiesmentioning
confidence: 99%