A theoretical study of the ion-molecule chemistry of K+.X complexes (X = O, O2, N2, CO2, H2O): implications for the upper atmosphere

The Journal of Physical Chemistry. a
John M C PlaneTimothy G Wright

Abstract

High-level ab initio calculations were carried out on a series of K+.X cluster ions (X = O, O2, N2, CO2, H2O) and X.K+.Y ions. Rice-Ramsberger-Kassel-Markus theory was then used to estimate the rate coefficients for a series of recombination and ligand-switching reactions that govern the ion-molecule chemistry of K+ in the upper mesosphere and lower thermosphere. These rate coefficients were then included in an atmospheric model of potassium chemistry. The important result is that K+ forms weakly bound clusters with N2, O2, and O (the major atmospheric species), with binding energies between 10 and 22 kJ mol(-1). Even under atmospheric conditions (200 K and 10(-3) Torr), these cluster dissociate in less than 1 s. This prevents the formation by ligand-switching of the more stable CO2 and H2O clusters, which could then undergo dissociative recombination with electrons to produce K. The result is that K+ ions have a much longer lifetime against neutralization in the upper atmosphere than other metallic ions such as Na+ and Fe+.

References

Dec 11, 2003·Chemical Reviews·John M C Plane
Apr 20, 1973·Science·R A Goldberg, A C Aikin

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Citations

May 9, 2008·Chemical Communications : Chem Comm·Li WanYong Zhang
Mar 10, 2015·Chemical Reviews·John M C PlaneErin C M Dawkins

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