A 3D non-local density functional theory for any pore geometry. (1st June 2020)

• Record Type: Journal Article
• Authors: Bernet, Thomas; Piñeiro, Manuel M.; Plantier, Frédéric; Miqueu, Christelle
• Is Part Of: Molecular physics. Volume 118:Number 9/10(2020)
• Publication Date: 2020-06-01
• Subjects: Density functional theory -- fundamental-measure theory -- discrete geometry; Molecules -- Periodicals; Chemistry, Physical and theoretical -- Periodicals; Molécules -- Périodiques; Chimie physique et théorique -- Périodiques; 539.6.05
• DOI: 10.1080/00268976.2020.1767308
• Languages: English
• ISSNs: 0026-8976

Abstract

Abstract : A general framework of classical non-local density functional theory (NLDFT) is presented, in order to consider the adsorption of spherical molecules in porous materials of any geometry. Fluid-fluid interactions and fluid-solid interactions can be repulsive or attractive. Some techniques that have been developed for the computation of weighted densities of hard-spheres are extended to attractive ones, in order to deal with an arbitrary pore geometry. This way, the computation method introduced in this work is validated by a comparison with analytical results for simple cases, and is directly applied to more complex systems. Density distributions depending on multi-dimensional effects are presented, and some radial distribution functions are recovered from NLDFT computations. Finally, the case of attractive continuous curved walls is detailed, which represents a large variety of real systems (e.g. micro and mesoporous silica, zeolites, carbonaceous nanoporous materials, etc.). With the new way of computation proposed, a general solution is presented, valid for any shape of continuous pore surface, by considering mathematical properties of discrete geometry due to the discretisation of the computational space with FFT computations. GRAPHICAL ABSTRACT: