High-throughput screening of efficient Metal-Organic Frameworks for the generation of reactive oxygen species

Metal-organic frameworks (MOFs) are recognized as promising catalysts for generating reactive oxygen species (ROS) due to their exceptional properties. However, identifying the most efficient MOF candidates remains challenging. In this study, the ROS generation performance of MOFs was predicted using Density Functional Theory (DFT) and a multi-step high-throughput screening process. This screening involved evaluations of structural stability, pore size, adsorption capacity, open metal sites, O₂ activation potential, and free energy simulations of reaction pathways. As a result, several MOFs (i.e., Cu-tris(4-aminophenyl)amine (Cu-MOF), Zn-2-H-MeIM (Zn-MOF), and Ce-2-amino-1,4-benzenedicarboxylic) (Ce-MOF) were identified as potential catalysts for ROS generation under both light and dark conditions. Especially, Cu-MOF was identified as the most efficient catalyst, generating 7.52 ​mmol ​g⁻¹ ​H₂O₂ in 1 ​h under light irradiation, and 2.88 ​mmol ​g⁻¹ ​H₂O₂ in the dark. Furthermore, the polarity of coordination bonds between the metal atoms and ligand atoms in the ligands was found to significantly influence O₂ activation. The ROS generation trend of MOFs was consistent with the polarity of these coordination bonds. The sterilization efficiency of Cu-MOF and Zn-MOF reached 99.9 ​% after 40 ​min of light exposure, while after 100 ​min in the dark, the efficiencies were 99.9 ​% and 41.6 ​%, respectively. This trend was closely related to the variation in the polarity of coordination bonds. This work provides a strategy and methodology for high-throughput screening of MOFs.