Comparison of 3D-cDFT and GCMC Simulations for Fluid-Structure Analysis in Amorphous Carbon Nanoporous Materials

Abstract Investigating fluid behavior in nanoporous materials is essential for gas storage, separation, and catalysis applications. Here, we present a comparison of two computational methods for fluid-structure analysis in amorphous nanoporous carbon materials: three-dimensional (3D) classical Density Functional Theory (cDFT) and Grand Canonical Monte Carlo (GCMC) simulations. We extended our recent development of 3D-cDFT to allow density-profile analysis without symmetry assumptions, enhancing its applicability to a broader range of porous materials. We provide a theoretical overview and discuss the advantages and limitations of each method. Our results highlight the accuracy of both 3D-cDFT and GCMC simulations while emphasizing differences in computational cost, precision, and scope. We also explore the impact of the non-crystalline structure of amorphous carbon nanopores on fluid structure and adsorption isotherms, as well as fluid-fluid and fluid-solid interactions. We offer insights for selecting computational methods in fluid structure analysis of nanoporous materials, guiding future research and optimization in advanced material development for diverse applications.