Benchmarking Selected Density Functionals and Dispersion Corrections for MOF-5 and its Derivatives

Abstract: Accurate computational predictions of metal-organic frameworks (MOFs) and their properties is crucial for discovering optimal compositions and applying them in relevant technological areas. This work benchmarks density functional theory (DFT) approaches, including semi-local, meta-GGA, and hybrid functionals with various dispersion corrections, on MOF-5 and three of its computationally predicted derivatives, analyzing structural, electronic, and vibrational properties. Our results underline the importance of explicitly treating van der Waals interactions for an accurate description of structural and vibrational properties, and indicate the meta-GGA functional R2SCAN as the best balance between accuracy and efficiency for characterizing the electronic structure of these systems, in view of future high-throughput screening studies on MOFs.