Revisiting greenhouse gases adsorption in carbon nanostructures: Advances through a combined first-principles and molecular simulation approach

Author(s)

Cezar, Henrique M. ; Lanna, Teresa D. ; Damasceno, Daniela A. ; Kirch, Alexsandro ; Miranda, Caetano R.

• Document type: Journal article
• Source: Applied Surface Science; v. 671, p. 7-pg., 2024-07-16.

Abstract

Carbon nanostructures are promising materials to improve the performance of current gas separation membrane technologies. From the molecular modeling perspective, an accurate description of the interfacial interactions is mandatory to understand the gas selectivity in the context of greenhouse gases applications. Most of the molecular dynamics simulations studies considered available force fields with the standard Lorentz-Berthelot (LB) mixing rules to describe the interaction among carbon dioxide (CO2), methane (CH4) and carbon structures. We performed a systematic study in which we showed the LB underestimates the interaction energies compared to the density functional theory (DFT) results. To improve the classical description, we propose a new parametrization for the cross-terms of the Lenard-Jones potential by fitting DFT forces and energies. The effects of the new parametrization on the gases adsorption within single-walled carbon nanotubes (SWCNTs), are investigated with Grand Canonical Monte Carlo simulations. We observed considerable differences in the CO2 and CH4 density within SWCNTs compared to those obtained with the standard approach. Our study highlights the importance of going beyond the traditional LB mixing rules in studies involving solid/fluid interfaces of confined systems. The revised mixing terms enhanced fluid/carbon interface description with excellent transferability ranging from SWCNTs to graphene. (AU)

• FAPESP's process: 20/15230-5 - Research Centre for Greenhouse Gas Innovation - RCG2I
• Grantee: Julio Romano Meneghini
• Support Opportunities: Research Grants - Research Centers in Engineering Program
• FAPESP's process: 20/01558-9 - Computational design of natural gas separation nanomaterials
• Grantee: Daniela Andrade Damasceno
• Support Opportunities: Scholarships in Brazil - Post-Doctoral
• FAPESP's process: 17/02317-2 - Interfaces in materials: electronic, magnetic, structural and transport properties
• Grantee: Adalberto Fazzio
• Support Opportunities: Research Projects - Thematic Grants
• FAPESP's process: 14/50279-4 - Brasil Research Centre for Gas Innovation
• Grantee: Julio Romano Meneghini
• Support Opportunities: Research Grants - Research Centers in Engineering Program
• FAPESP's process: 19/21430-0 - Computational nanofluidics studies on the confinement effects on fluid-solid interfaces
• Grantee: Henrique Musseli Cezar
• Support Opportunities: Scholarships in Brazil - Post-Doctoral