Mass-Transport Considerations Pertinent to Aqueous Phase Reactions of Gases in Liquid-Water Clouds

Schwartz, Stephen E.

doi:10.1007/978-3-642-70627-1_16

Cited by 485 publications

(476 citation statements)

References 41 publications

Supporting

Mentioning

465

Contrasting

Unclassified

Order By: Relevance

“…The g were chosen on the basis of available recommendations [e.g., Jacob, 2000] or on available experimental results as further discussed in the following. The gas to particle transfer rate K (s À1 ) is calculated for each reaction following Schwartz [1986]:…”

Section: Heterogeneous Chemistrymentioning

confidence: 99%

Trace gas and aerosol interactions in the fully coupled model of aerosol‐chemistry‐climate ECHAM5‐HAMMOZ: 1. Model description and insights from the spring 2001 TRACE‐P experiment

et al. 2008

View full text Add to dashboard Cite

[1] In this paper, we introduce the ECHAM5-HAMMOZ aerosol-chemistry-climate model that includes fully interactive simulations of Ox-NOx-hydrocarbons chemistry and of aerosol microphysics (including prognostic size distribution and mixing state of aerosols) implemented in the General Circulation Model ECHAM5. The photolysis rates used in the gas chemistry account for aerosol and cloud distributions and a comprehensive set of heterogeneous reactions is implemented. The model is evaluated with trace gas and aerosol observations provided by the TRACE-P aircraft experiment. Sulfate concentrations are well captured but black carbon concentrations are underestimated. The number concentrations, surface areas, and optical properties are reproduced fairly well near the surface but underestimated in the upper troposphere. CO concentrations are well reproduced in general while O 3 concentrations are overestimated by 10-20 ppbv. We find that heterogeneous chemistry significantly influences the regional and global distributions of a number of key trace gases. Heterogeneous reactions reduce the ozone surface concentrations by 18-23% over the TRACE-P region and the global annual mean O 3 burden by 7%. The annual global mean OH concentration decreases by 10% inducing a 7% increase in the global CO burden. Annual global mean HNO 3 surface concentration decreases by 15% because of heterogenous reaction on mineral dust. A comparison of our results to those from previous studies suggests that the choice of uptake coefficients for a given species is the critical parameter that determines the global impact of heterogeneous chemistry on a trace gas (rather than the description of aerosol properties and distributions). A prognostic description of the size distribution and mixing state of the aerosols is important, however, to account for the effect of heterogeneous chemistry on aerosols as further discussed in the second part of this two-part series.Citation: Pozzoli, L., I. Bey, S. Rast, M. G. Schultz, P. Stier, and J. Feichter (2008), Trace gas and aerosol interactions in the fully coupled model of aerosol-chemistry-climate ECHAM5-HAMMOZ: 1. Model description and insights from the spring 2001 TRACE-P experiment,

show abstract

Section: Heterogeneous Chemistrymentioning

confidence: 99%

Trace gas and aerosol interactions in the fully coupled model of aerosol‐chemistry‐climate ECHAM5‐HAMMOZ: 1. Model description and insights from the spring 2001 TRACE‐P experiment

et al. 2008

View full text Add to dashboard Cite

show abstract

“…The transfer coefficients kt includes both the effects of gas phase diffusion (kag) and of mass transport across the gas-aqueous interface (ki) [Schwartz, 1986] (Table 5), Dg is the gas phase diffusivity (in gm 2 s'l) ß introducing •, the mean free path for a gas phase species taken equal to 0.1 gm, the gas phase diffusivity is …”

Section: Heff ( T ) X R X Rmentioning

confidence: 99%

A general circulation model based calculation of HCl and ClNO₂ production from sea salt dechlorination: Reactive Chlorine Emissions Inventory

Erickson¹,

Seuzaret²,

Keene³

et al. 1999

J. Geophys. Res.

119

139

View full text Add to dashboard Cite

Tg C1 yr -1 and 0.06 Tg C1 yr -1, respectively; virtually all in the Northern Hemisphere. Largest HC1 and C1NO2 fluxes occur in northern hemisphere winter due to high sea salt loading and elevated HNO3, SO2 and N205 concentrations. 70% of the HC1 dechlorination occurs on particles between 0.75 gm and 4 gm radius; C1NO2 volatilized from slightly larger particles. The aerosol pH of each particle size bin equilibrates towards the same value once the alkalinity has been titrated.

show abstract

“…The gas-to-liquid mass transfer of NO3, N205, SO2, HO2, and H202 was calculated using the formalism derived by Schwartz [1984Schwartz [ , 1986, which maintained dynamic exchange between the gas and the condensed phases. The liquid-phase rate coefficients were corrected for the nonuniform concentration of NO3 throughout the droplet, which is caused by the slower rate of diffusion compared to the reaction in the liquid phase [Schwartz, 1986].…”

Section: The Modelmentioning

confidence: 99%

“…The liquid-phase rate coefficients were corrected for the nonuniform concentration of NO3 throughout the droplet, which is caused by the slower rate of diffusion compared to the reaction in the liquid phase [Schwartz, 1986]. The correction was essential to avoid overestimation of the reactive loss of NO3 in the droplet, and it was calculated for each reactant, as the simulation progressed.…”

Section: The Modelmentioning

confidence: 99%

Multiphase chemistry of NO₃ in the remote troposphere

Rudich¹,

Talukdar²,

Ravishankara³

1998

J. Geophys. Res.

View full text Add to dashboard Cite

Abstract. The effect of NO 3 uptake at night into marine aerosol and cloud droplets on (1) sulfur oxidation, (2) NO 3 ambient concentrations, and (3) NO 3 atmospheric lifetime is examined using a simple chemical kinetics model. It is shown that the atmospheric lifetime toward multiphase removal of NO 3 is < 10 min in presence of cloud droplets. We also show that at low mixing ratios of H202 (<150 pmol/mol), NO 3 can enhance sulfur oxidation in clouds via a catalytic cycle with a chain length of~8. Finally, in presence of sea-salt aerosol, the uptake of NO 3 leads to low ambient concentrations of NO3, efficient S(IV) oxidation, and possibly, to release of halogens from the aerosol. The results of this study imply that the multiphase reaction of NO 3 may be important in the remote marine boundary layer.

show abstract

Mass-Transport Considerations Pertinent to Aqueous Phase Reactions of Gases in Liquid-Water Clouds

Cited by 485 publications

References 41 publications

Trace gas and aerosol interactions in the fully coupled model of aerosol‐chemistry‐climate ECHAM5‐HAMMOZ: 1. Model description and insights from the spring 2001 TRACE‐P experiment

Trace gas and aerosol interactions in the fully coupled model of aerosol‐chemistry‐climate ECHAM5‐HAMMOZ: 1. Model description and insights from the spring 2001 TRACE‐P experiment

A general circulation model based calculation of HCl and ClNO₂ production from sea salt dechlorination: Reactive Chlorine Emissions Inventory

Multiphase chemistry of NO₃ in the remote troposphere

Contact Info

Product

Resources

About

Mass-Transport Considerations Pertinent to Aqueous Phase Reactions of Gases in Liquid-Water Clouds

Cited by 485 publications

References 41 publications

Trace gas and aerosol interactions in the fully coupled model of aerosol‐chemistry‐climate ECHAM5‐HAMMOZ: 1. Model description and insights from the spring 2001 TRACE‐P experiment

Trace gas and aerosol interactions in the fully coupled model of aerosol‐chemistry‐climate ECHAM5‐HAMMOZ: 1. Model description and insights from the spring 2001 TRACE‐P experiment

A general circulation model based calculation of HCl and ClNO2 production from sea salt dechlorination: Reactive Chlorine Emissions Inventory

Multiphase chemistry of NO3 in the remote troposphere

Contact Info

Product

Resources

About

A general circulation model based calculation of HCl and ClNO₂ production from sea salt dechlorination: Reactive Chlorine Emissions Inventory

Multiphase chemistry of NO₃ in the remote troposphere