Predicting Electronic and Photophysical Properties of Photocatalytically Active Metal-Organic Frameworks

Metal-Organic-Frameworks (MOFs) have attracted great interest to be used in photocatalytic applications, such as hydrogen evolution reaction (HER). In this context, an atomistic understanding of their electronic and optical properties is of importance to be translated for the design of new promising materials. MOFs modular and porosity structure provides a platform to assemble photo-active and catalytic-sites building block units that can offer unique photo-physics. This feature is of great interest for H₂ evolution photocatalytic applications. Thus, elucidating and predicting the optical properties of MOFs will have wide implications in the development of MOF-based photocatalysts. Computational studies can be of great aid for the discovery of MOFs photocatalyst. Yet, this is a challenging task for computational chemistry given the complexity of the photophysical properties, the inorganic-organic nature, the number of atoms, and the unit cell size of MOFs. Our goal is to exploit Density functional theory (DFT) and linear-response time-dependent DFT (LR-TDDFT) formalisms for predicting their feasibility for photocatalytic applications this includes light absorption, charge separation, and charge transfer properties of the material. MOFs’ modular nature intrinsically defines a large number of materials to explore where high-throughput screening workflows are required to determine decisive parameters for photocatalytic HER. Our strategy aims to explore key design criteria to pave the way for designing efficient MOFs for photocatalysis.