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

Area of Science:

• Computational materials science
• Solid-state chemistry

Background:

• Accurate computational predictions of metal-organic frameworks (MOFs) are essential for materials discovery and technological applications.
• Density functional theory (DFT) is a common method for predicting MOF properties.

Purpose of the Study:

• To benchmark different density functional theory (DFT) approaches for MOF property prediction.
• To identify the most accurate and efficient DFT functional for characterizing MOF electronic structures.

Main Methods:

• Benchmarking DFT functionals (semilocal, meta-GGA, hybrid) with dispersion corrections.
• Analysis of structural, electronic, and vibrational properties of MOF-5 and its derivatives.
• Evaluation of van der Waals interaction treatment.

Main Results:

• Explicit treatment of van der Waals interactions is crucial for accurate structural and vibrational properties.
• The meta-GGA functional R2SCAN provides the best balance of accuracy and efficiency for electronic structure calculations.
• R2SCAN is recommended for future high-throughput screening of MOFs.

Conclusions:

• DFT methods, particularly those including van der Waals corrections, are vital for MOF research.
• R2SCAN emerges as a promising functional for computational screening of MOFs.
• This work guides the selection of appropriate computational methods for MOF design.