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Diffusion in nanoporous phases: size dependence and levitation effect.

S Yashonath¹, Pradip Kr Ghorai

¹Solid State and Structural Chemistry Unit, Center for Condensed Matter Theory, Indian Institute of Science, Bangalore-560012, India.

The Journal of Physical Chemistry. B

|December 19, 2007

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The levitation effect explains the maximum in self-diffusivity (D) observed across various materials, from liquids to solids. This universal phenomenon arises from force cancellations when diffusant size matches void size, impacting transport properties.

Area of Science:

Condensed Matter Physics
Physical Chemistry
Materials Science

Background:

Self-diffusivity (D) in diverse media like liquids, porous solids, and ionic solutions shows significant size dependence.
Previous theoretical models struggled to universally explain this size dependence across different systems.
Molecular dynamics simulations revealed a key mechanism in guest-porous solids: force cancellation when diffusant and void sizes are comparable.

Purpose of the Study:

To elucidate the universal mechanism behind the size-dependent maximum in self-diffusivity (D).
To explore the origins and implications of the levitation effect (LE) across various condensed matter phases.
To reconcile experimental observations with theoretical understanding of diffusion phenomena.

Main Methods:

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Review and synthesis of theoretical approaches to diffusion.
Analysis of molecular dynamics (MD) simulation data for guest-porous solids and other systems.
Examination of experimental data on ionic conductivity and solute diffusion.

Main Results:

The levitation effect (LE), arising from symmetry-induced force cancellation, explains the diffusivity maximum.
LE is observed in porous solids, uncharged solutes in solvents, and ionic solutions, irrespective of specific pore geometry.
LE leads to the breakdown of established transport relationships like the Stokes-Einstein and Walden's rules over certain size ratios.

Conclusions:

The levitation effect is a universal phenomenon driving diffusivity maxima in condensed matter.
LE originates from van der Waals or electrostatic interactions when diffusant and void/solvent sizes are comparable.
Understanding LE is crucial for predicting and controlling diffusion in a wide range of materials and applications.