The metal-organic framework (MOF) MFU-4l containing Co(II) centers and Cl- ligands has recently shown promising redox activity. Aiming for further improved MOF catalysts for oxidation processes employing molecular oxygen we present a density-functional theory (DFT) based computational screening approach to identify promising metal center and ligand combinations within the MFU-4l structural family. Using the O2 binding energy as a descriptor for the redox property, we show that relative energetic trends in this descriptor can reliably be obtained at the hybrid functional DFT level and using small cluster (scorpionate-type complex) models. Within this efficient computational protocol we screen a range of metal center / ligand combinations and identify several candidate systems that offer more exothermic O2 binding than the original Co/Cl-based MFU-4l framework.
@article{arxiv.1311.6639,
title = {Computational screening study towards redox-active metal-organic frameworks},
author = {Jelena Jelic and Dmytro Denysenko and Dirk Volkmer and Karsten Reuter},
journal= {arXiv preprint arXiv:1311.6639},
year = {2013}
}