Computational Study of Metal‐Organic Frameworks for Hydrogen Sulfide Adsorption: Grand Canonical Monte Carlo and Molecular Dynamics Simulations

Abstract Hydrogen sulfide (H 2 S) is a highly toxic, and flammable acid gas that is widely present in confined spaces. However, conventional adsorption materials are inefficient and have poor reuse properties. Metal‐organic frameworks (MOFs) show potential viability as novel materials in gas adsorption. Herein, mainstream MOFs were investigated based on molecular simulation techniques to explore the differences contributing to H 2 S adsorption. The adsorption process of H 2 S in MOFs was simulated by Grand Canonical Monte Carlo (GCMC) method, and the diffusion behavior was investigated based on molecular dynamics (MD) simulations. The results showed that the interaction energy and isosteric heat of adsorption were important criteria for determining the adsorption performance of H 2 S. The regulation of open metal sites could help to further enhance the adsorption of H 2 S, and the pore structure of MOFs affected the capture of H 2 S. A higher self‐diffusion rate implies faster H 2 S capture. Hydrogen bonds affect the trapping efficiency of MOFs for H 2 S and the relative positions of ligands in the benzene ring cause subtle differences in adsorption. This study provides design strategies for the improvement of new high‐performing MOFs for H 2 S adsorption in confined spaces.