CO₂ Capture in MOFs: Connecting Experiments, Multiscale Simulations, and Data-Driven Approaches

Metal-organic frameworks (MOFs) have emerged as promising porous materials for CO₂ capture due to their tunable pore structures and chemically versatile adsorption sites. However, achieving efficient capture at low CO₂ concentrations while balancing adsorption strength, regeneration, and structural stability remains challenging. Existing reviews often treat experimental and computational investigations separately, limiting the development of unified design principles. This review integrates experimental insights with multiscale computational approaches, including density functional theory (DFT), grand canonical Monte Carlo, molecular dynamics, and computational fluid dynamics (CFD). DFT calculations provide molecular-level understanding of adsorption behavior, highlighting the role of electronic structure at open metal sites and functionalized pores. Classical simulations predict adsorption capacity, selectivity, and diffusion, while CFD extends these insights to macroscopic transport and process-level performance, enabling direct comparison with experiments. In addition, emerging data-driven approaches are discussed to uncover structure-property relationships and accelerate performance prediction across large materials spaces. The integration of these methods establishes a closed-loop framework linking theory, simulation, and experiment, guiding the rational design of efficient and stable porous materials for practical CO₂ capture applications.