TRAPPING OF TRACE GASES BY ATMOSPHERIC AEROSOLS
Abstract and keywords
Abstract (English):
A theory of trapping gaseous reactants by aerosol particles is developed for arbitrary regimes of reactant transport. The dependence of the trapping efficiency on the particle size is found as a function of sticking probability of the reactant molecules to the particle surface. The key point of this consideration is the solution of the transport equation in the free-molecule zone (where the collisions between the reactant molecules and the molecules of the carrier gas can be ignored) and further matching the reactant concentration profiles at the interface separating the free-molecule and diffusion zones. The flux conservation allows for the formulation of the boundary condition that determines the reactant surface concentration. The latter depends on the total flux of the reactant and thus the trapping efficiency of the reactant molecules occurs to be dependent on the nature of in-particle chemical processes. The first-order chemical reaction serves as a good example of such dependence, where all characteristics of the trapping efficiency can be found analytically.

Keywords:
Nanoaerosols in the atmosphere, absorption, trace gases, transition regime
Text
Publication text (PDF): Read Download
References

1. Ammann, Kinetic model framework for aerosol and cloud surface chemistry and gas--particle interactions -- Part 2: Exemplary practical applications and numerical simulations, Atmospheric Chemistry and Physics, v. 7, 2007., doi: 10.5194/acp-7-6025-2007

2. Clement, Theoretical consideration on sticking probabilities, Journal of Aerosol Science, v. 27, 1996., doi: 10.1016/0021-8502(96)00032-8

3. Clement, Mass transfer to aerosols, Environmental Chemistry of Aerosols, 2007.

4. Davis, Transport phenomena with single aerosol particles, Aerosol Sci. and Techn., v. 2(C), 1983.

5. Davidovits, Uptake of gas molecules by liquids. A Model, Journal of Physical Chemistry, v. 95, 1991., doi: 10.1021/j100169a048

6. Davidovits, Entry of gas molecules into liquids, Faraday Discussion, v. 100, 1995., doi: 10.1039/fd9950000065

7. Farman, Large losses of total ozone in Antarctica reveal seasonal ClOx/NOx interaction, Nature, v. 315, 1985., doi: 10.1038/315207a0

8. Feng, Micro-heterogeneous catalysis at the surface of electrodynamically levitated particles, Journal of Aerosol Science, v. 32, 2001., doi: 10.1016/S0021-8502(01)00046-5

9. Finlayson-Pitts, Chemistry of the Upper and Lower Atmosphere, 2000.

10. Fuchs, Mechanics of Aerosols,, 1964.

11. Fuchs, High-dispersed aerosols, Topics in Current Aerosol Research, volume 2, 1971.

12. Hidy, The Dynamics of Aerocolloidal Systems, 1971.

13. Kulmala, Mass accommodation and uptake coefficients -- a quantitative comparison, Journal of Aerosol Science, v. 32, 2001., doi: 10.1016/S0021-8502(00)00116-6

14. Laaksonen, Commentary on cloud modelling and mass accommodation coefficient of water, Atmospheric Chemistry and Physics, v. 5, 2005., doi: 10.5194/acp-5-461-2005

15. Li, Aerosol evaporation in the transition regime, Aerosol Science and Technology, v. 25, 1995., doi: 10.1080/02786829608965375

16. Li, Mass and thermal accommodation coefficients of H2O(g) on liquid water as a function of temperature, Journal of Physical Chemistry A., v. 105, 2001., doi: 10.1021/jp012758q

17. Lohman, Global indirect aerosol effects: a review, Atmospheric Chemistry and Physics, v. 5, 2005., doi: 10.5194/acp-5-715-2005

18. Lushnikov, Flux-matching theory of particle charging, Physical Review, v. E70, 2004.

19. P\"oschl, Kinetic model framework for aerosol and cloud surface chemistry and gas--particle interactions -- Part 1: General equations, parameters, and terminology, Atmospheric Chemistry and Physics, v. 7, 2007., doi: 10.5194/acp-7-5989-2007

20. Qu, Droplet evaporation and condensation in the near continuum regime, Journal of Aerosol Science, v. 32, 2001., doi: 10.1016/S0021-8502(00)00112-9

21. Ray, Direct measurements of evaporation rates of single droplets at large Knudsen numbers, Langmuir, v. 4, 1988.

22. Sahni, The effect of black sphere on the flux distribution of an infinite moderator, J. Nucl. Energy, v. 20, 1966.

23. Seinfeld, Atmospheric Chemistry and Physics,, 1998.

24. Smith, Aerosol uptake described by numerical solution of the diffusion-reaction equation in the particle, Journal of Physical Chemistry, v. A107, 2003., doi: 10.1021/jp021843a

25. Wagner, Aerosol growth by condensation, Aerosol Microphysics II, 1982., doi: 10.1007/978-3-642-81805-9_5

26. Weber, Aerosol catalysis on nickel nanoparticles, Journal of Nanoparticle Research, v. 1, 1999.

27. Widmann, Mathematical models of the uptake of ClONO2 and other gases by atmospheric aerosols, Journal of Aerosol Sciience, v. 28, 1997., doi: 10.1016/S0021-8502(96)00060-2

28. Williams, Aerosol Science, Theory and Practice, 1991.

29. Winkler, Mass and thermal accomodation during gas-liquid condensation of water, Physical Review Letter, v. 93, 2004.

30. Winkler, Condensation of water vapor. Experimental determination of mass and thermal accommodation coefficients, Journal of Geophysical Research, v. 111, 2006., doi: 10.1029/2006JD007194

31. Worsnop, A chemical reactive model for reactive transformation of aerosol particles, Geophysical Research Letters, v. 29(20), 2002., doi: 10.1029/2002GL015542

Login or Create
* Forgot password?