Transition metal oxides containing redox-active 3d metal centers are crucial ingredients for generating renewable fuels via two-step, oxide-based, solar thermochemical reactors. However, any predictive modeling, such as using density functional theory (DFT), needs to accurately describe the energetics of redox reactions involving transition metals, if promising new materials are to be discovered via simulation. Recently, we demonstrated that the strongly constrained and appropriately normed (SCAN) exchange-correlation (XC) functional requires an appropriately determined Hubbard U correction to accurately describe the ground-state structure, lattice parameters, magnetic moments, and electronic properties of Ce-, Mn-, and Fe-oxides. Here, we extend our approach of using experimental oxidation enthalpies to identify optimal U values for other 3d oxide systems, such as Ti, V, Cr, Co, Ni, and Cu, within the SCAN+U framework. We find that the addition of U significantly improves ground-state property predictions, particularly for Ti, V, Co, and Ni oxides, with an absolute value of U for all 3d metals lower than with a generalized gradient approximation (GGA)+U or a local density approximation (LDA)+U approach. Thus, the SCAN+Uframework with an appropriately determined U is required to provide accurate ground-state energies and qualitatively consistent electronic structures for most first-row, transition-metal oxides needed to help identify novel oxide materials for energy applications.

Modeling 3d transition metal oxides with optimal U values within a SCAN+U framework

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

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