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arXiv · 1311.6639

Computational screening study towards redox-active metal-organic frameworks

Jelena Jelic·Dmytro Denysenko·Dirk Volkmer·Karsten Reuter
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Abstract

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.

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Jelena Jelic, Dmytro Denysenko, Dirk Volkmer, Karsten Reuter. 2013-11-26. Computational screening study towards redox-active metal-organic frameworks. https://doi.org/10.1088/1367-2630%2F15%2F11%2F115004

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