DFT-MD simulations and experimental validation of graphene-CO₂ interaction energies and structural dynamics for enhanced CO₂ adsorption

Graphene-based materials have garnered significant interest for CO₂ capture due to their unique physicochemical properties and tunable surface characteristics. This study combines Density Functional Theory (DFT) and Molecular Dynamics (MD) simulations with experimental validation to investigate the interaction energies and structural dynamics of graphene-CO₂ systems under varying conditions. Simulations assumed complete surface accessibility of graphene for CO₂ binding, while experimental setups revealed an actual surface coverage of approximately 50 %-80 % due to constraints in coating homogeneity. Both DFT and MD simulations revealed an increase in adsorption energy with the application of an electric field, corroborated by experimental data which exhibited enhanced CO₂ uptake under similar conditions. The close agreement between simulation and experimental outcomes under an electric field confirms the accuracy of the adopted model, demonstrating its relevance for optimizing graphene-based CO₂ capture systems. This integrated approach provides deeper insights into the design of efficient graphene-based adsorbents for sustainable carbon capture applications.