Uphill diffusion and overshooting in the adsorption of binary mixtures in nanoporous solids

Alexander Lauerer, Tomas Binder, Christian Chmelik, Erich Miersemann, Jürgen Haase, Douglas M. Ruthven and Jörg Kärger ()
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Alexander Lauerer: Faculty of Physics and Earth Sciences, University of Leipzig
Tomas Binder: Faculty of Physics and Earth Sciences, University of Leipzig
Christian Chmelik: Faculty of Physics and Earth Sciences, University of Leipzig
Erich Miersemann: University of Leipzig
Jürgen Haase: Faculty of Physics and Earth Sciences, University of Leipzig
Douglas M. Ruthven: University of Maine
Jörg Kärger: Faculty of Physics and Earth Sciences, University of Leipzig

Nature Communications, 2015, vol. 6, issue 1, 1-9

Abstract: Abstract Under certain conditions, during binary mixture adsorption in nanoporous hosts, the concentration of one component may temporarily exceed its equilibrium value. This implies that, in contrast to Fick’s Law, molecules must diffuse in the direction of increasing rather than decreasing concentration. Although this phenomenon of ‘overshooting’ has been observed previously, it is only recently, using microimaging techniques, that diffusive fluxes in the interior of nanoporous materials have become accessible to direct observation. Here we report the application of interference microscopy to monitor ‘uphill’ fluxes, covering the entire period of overshooting from initiation until final equilibration. It is shown that the evolution of the profiles can be adequately predicted from the single-component diffusivities together with the binary adsorption equilibrium data. The guest molecules studied (carbon dioxide, ethane and propene) and the host material (ZSM-58 or DDR) are of practical interest in relation to the development of kinetically selective adsorption separation processes.

Date: 2015
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DOI: 10.1038/ncomms8697

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