Detailed Characterization of Rough Surfaces for Silica Materials

TL;DR

This paper introduces a novel method using random surface density functional theory to accurately characterize the nanoscale roughness of silica materials from low-pressure adsorption data, aiding in material design.

Contribution

It presents a new approach combining correlated random surface models with RS-DFT to extract detailed surface geometry from experimental adsorption data.

Findings

The method accurately reproduces surface roughness parameters.

Surface fractal dimensions align with experimental observations.

Provides insights into adsorption mechanisms on rough silica surfaces.

Abstract

We propose a new approach to obtain the nanoscale morphology of rough surfaces from low-temperature adsorption experiments. Our method is based on one of the most realistic models of rough surfaces formulated in terms of random correlated processes and random surface density functional theory (RS-DFT) as a theoretical adsorption model. We consider the roughness in the normal direction, the correlation length of the lateral surface structure and the specific surface area as tuning parameters of RS-DFT to fit the experimental data in the low pressure range, where the influence of the surface geometry is the most crucial. One of the major advantages of the proposed approach over published methods is the best-fit detailed geometry of rough surfaces, which provides full information for further atomistic modeling. The obtained geometry correctly reflects how the nanoroughness of silica materials depends on the synthesis conditions. We demonstrate that the surface fractal dimension observed in many experiments is natural for the correlated random surface model. We investigated the surface geometry of popular silica materials synthesized at different conditions. The obtained roughness parameters and fractal dimensions coincide well with the published experimental data. Analysis of the best fit specific surface area reveals the mechanism of adsorption on rough surfaces and provides a new strategy for the search of optimal storage materials.