Uptake of gas molecules by liquids: a model

Davidovits, P.; Jayne, J. T.; Duan, Suqing; Worsnop, Douglas R.; Zahniser, M. S.; Kolb, C. E.

doi:10.1021/j100169a048

Cited by 98 publications

(146 citation statements)

References 0 publications

Supporting

Mentioning

132

Contrasting

Order By: Relevance

“…Concentration of trace-gas molecules in the interface can be explained by the ''cluster'' model developed in the work of Davidovits et al [1]. The model is based on the nucleation theory, in which gas molecules participate in a nucleation process, where clusters that form of a critical size undergo growth by condensation and merge with the bulk liquid.…”

Section: Governing Equations Results and Discussionmentioning

confidence: 99%

Langmuir approach in the study of interface mass transfer

Remorov

Bardwell

2005

Surface Science

View full text Add to dashboard Cite

Section: Governing Equations Results and Discussionmentioning

confidence: 99%

Langmuir approach in the study of interface mass transfer

Remorov

Bardwell

2005

Surface Science

View full text Add to dashboard Cite

“…35-37). Moreover, the cluster-nucleation model proposed by Davidovits et al (1991) and similar approaches of describing surface-to-bulk transfer could be used to determine and parameterize k s,b,Xi (Remorov and Bardwell, 2005;Remorov and George, 2006). The bulk-to-surface transfer rate coefficient k b,s,Xi has dimensions of unit length per unit time and can be regarded as a transfer velocity, analogous to the deposition velocity (adsorption rate coefficient k a,Xi ) on the gas phase side.…”

Section: Overall Chemical Production and Loss Of Surface Layer Componmentioning

confidence: 99%

“…(e.g. Jayne et al, 1990;Davidovits et al, 1991;Mozurkewich, 1993;Tabazadeh and Turco, 1993;Tabor et al, 1994;Davidovits et al, 1995;Kolb et al, 1995;Nathanson et al, 1996;Atkinson et al, 1997;Carslaw and Peter, 1997;Hanson, 1997;Jayne et al, 1997;Pöschl et al, 1998;Bertram et al, 2001;Clegg and Abbatt, 2001;Grassian, 2001;Katrib et al, 2001;Vesala et al, 2001;Adams et al, 2002;Hynes et al, 2002;Remorov et al, 2002;Sander et al, 2002;Smith et al, 2002;Worsnop et al, 2002;Ammann et al, 2003;da Rosa et al, 2003;Djikaev and Tabazadeh, 2003;Folkers et al, 2003;Reid and Sayer, 2003;Strekowski et al, 2003;Frinak et al, 2004;Kwamena et al, 2004Kwamena et al, , 2006Kwamena et al, , 2007Thornberry and Abbatt, 2004;Adams et al, 2005;Al-Hosney and Grassian, 2005;Gustafsson et al, 2005;Kleffmann and Wiesen, 2005;Remorov and Bardwell, 2005;…”

Section: Introductionmentioning

confidence: 99%

Kinetic model framework for aerosol and cloud surface chemistry and gas-particle interactions – Part 1: General equations, parameters, and terminology

2007

View full text Add to dashboard Cite

Abstract. Aerosols and clouds play central roles in atmospheric chemistry and physics, climate, air pollution, and public health. The mechanistic understanding and predictability of aerosol and cloud properties, interactions, transformations, and effects are, however, still very limited. This is due not only to the limited availability of measurement data, but also to the limited applicability and compatibility of model formalisms used for the analysis, interpretation, and description of heterogeneous and multiphase processes. To support the investigation and elucidation of atmospheric aerosol and cloud surface chemistry and gasparticle interactions, we present a comprehensive kinetic model framework with consistent and unambiguous terminology and universally applicable rate equations and parameters. It enables a detailed description of mass transport and chemical reactions at the gas-particle interface, and it allows linking aerosol and cloud surface processes with gas phase and particle bulk processes in systems with multiple chemical components and competing physicochemical processes.The key elements and essential aspects of the presented framework are: a simple and descriptive double-layer surface model (sorption layer and quasi-static layer); straightforward flux-based mass balance and rate equations; clear separation of mass transport and chemical reactions; well-defined and consistent rate parameters (uptake and accommodation coefficients, reaction and transport rate coefficients); clear distinction between gas phase, gas-surface, and surfacebulk transport (gas phase diffusion, surface and bulk accommodation); clear distinction between gas-surface, surface layer, and surface-bulk reactions (Langmuir-Hinshelwood and Eley-Rideal mechanisms); mechanistic description of The outlined double-layer surface concept and formalisms represent a minimum of model complexity required for a consistent description of the non-linear concentration and time dependences observed in experimental studies of atmospheric multiphase processes (competitive co-adsorption and surface saturation effects, etc.). Exemplary practical applications and model calculations illustrating the relevance of the above aspects are presented in a companion paper (Ammann and Pöschl, 2007).We expect that the presented model framework will serve as a useful tool and basis for experimental and theoretical studies investigating and describing atmospheric aerosol and cloud surface chemistry and gas-particle interactions. It shall help to end the "Babylonian confusion" that seems to inhibit scientific progress in the understanding of heterogeneous chemical reactions and other multiphase processes in aerosols and clouds. In particular, it shall support the planning and design of laboratory experiments for the elucidation and determination of fundamental kinetic parameters; the establishment, evaluation, and quality assurance of comprehensive and self-consistent collections of rate parameters; and the development of detailed master mechanisms for process mo...

show abstract

“…The formalism developed by adapts the model of uptake of gaseous species by liquids (Davidovits et al, 1991;Hanson, 1997;Hanson and Lovejoy, 1995;Kolb et al, 2002;Shi et al, 1999) to reactive transforms of the condensed-phase organic species because the particle MS methods monitor the loss of the organic substrate. In the OL-O 3 HRS, this involves monitoring OL loss and using this loss to calculate the uptake coefficient, γ .…”

Section: Models Of Reactive Uptakementioning

confidence: 99%

The oleic acid-ozone heterogeneous reaction system: products, kinetics, secondary chemistry, and atmospheric implications of a model system – a review

2007

View full text Add to dashboard Cite

Abstract. The heterogeneous processing of organic aerosols by trace oxidants has many implications to atmospheric chemistry and climate regulation. This review covers a model heterogeneous reaction system (HRS): the oleic acidozone HRS and other reaction systems featuring fatty acids, and their derivatives. The analysis of the commonly observed aldehyde and organic acid products of ozonolysis (azelaic acid, nonanoic acid, 9-oxononanoic acid, nonanal) is described. The relative product yields are noted and explained by the observation of secondary chemical reactions. The secondary reaction products arising from reactive Criegee intermediates are mainly peroxidic, notably secondary ozonides and α-acyloxyalkyl hydroperoxide oligomers and polymers, and their formation is in accord with solution and liquidphase ozonolysis. These highly oxygenated products are of low volatility and hydrophilic which may enhance the ability of particles to act as cloud condensation nuclei (CCN). The kinetic description of this HRS is critically reviewed. Most kinetic studies suggest this oxidative processing is either a near surface reaction that is limited by the diffusion of ozone or a surface based reaction. Internally mixed particles and coatings represent the next stage in the progression towards more realistic proxies of tropospheric organic aerosols and a description of the products and the kinetics resulting from the ozonolysis of these proxies, which are based on fatty acids or their derivatives, is presented. Finally, the main atmospheric implications of oxidative processing of particulate containing fatty acids are presented. These implications include the extended lifetime of unsaturated species in the troposphere facilitated by the presence of solids, semi-solids or viscous phases, and an enhanced rate of ozone uptake by particulate unsaturates compared to corresponding gas-phase organics.Correspondence to: G. A. Petrucci (giuseppe.petrucci@uvm.edu) Ozonolysis of oleic acid enhances its CCN activity, which implies that oxidatively processed particulate may contribute to indirect forcing of radiation.

show abstract

Uptake of gas molecules by liquids: a model

Cited by 98 publications

References 0 publications

Langmuir approach in the study of interface mass transfer

Langmuir approach in the study of interface mass transfer

Kinetic model framework for aerosol and cloud surface chemistry and gas-particle interactions – Part 1: General equations, parameters, and terminology

The oleic acid-ozone heterogeneous reaction system: products, kinetics, secondary chemistry, and atmospheric implications of a model system – a review

Contact Info

Product

Resources

About