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Lattice density functional theory of molecular diffusion.

Daniel Matuszak¹, Gregory L Aranovich, Marc D Donohue

¹Department of Chemical and Biomolecular Engineering, The Johns Hopkins University, Baltimore, Maryland 21218, USA.

The Journal of Chemical Physics

|July 21, 2004

Summary

This study introduces a new density functional theory for diffusion in lattice fluids, accurately modeling molecular transport and predicting phase transitions in nanopores. It offers a unified approach to equilibrium and nonequilibrium diffusion phenomena.

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Area of Science:

Statistical Mechanics
Physical Chemistry
Materials Science

Background:

Understanding diffusion in confined systems is crucial for various applications.
Existing theories often struggle to capture nonequilibrium behavior accurately.
Lattice fluid models provide a simplified yet powerful framework for studying molecular transport.

Purpose of the Study:

To develop a novel density functional theory for diffusion in lattice fluids.
To unify equilibrium and nonequilibrium diffusion descriptions.
To model transport phenomena in nanoporous materials.

Main Methods:

Development of a density functional theory for molecular flux.
Comparison with generalized Ono-Kondo theory at equilibrium.
Application to a model nanopore system.

Main Results:

The theory reproduces Fick's first law under specific conditions.
It deviates from Fickian behavior, aligning with Maxwell-Stefan formulation away from equilibrium.
Nonequilibrium phase transitions and surface diffusion effects were predicted in a nanopore model.

Conclusions:

The developed theory provides a robust framework for studying diffusion in lattice fluids.
It successfully models complex phenomena like nonequilibrium phase transitions in confined environments.
The theory highlights the importance of surface diffusion in capillary condensate transport.