Published February 13, 2023 | Version v1
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Unraveling the effects of inter-site Hubbard interactions in spinel Li-ion cathode materials

  • 1. Theory and Simulation of Materials (THEOS), and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), École Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland.

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Description

Accurate first-principles predictions of the structural, electronic, magnetic, and electrochemical properties of cathode materials can be key in the design of novel efficient Li-ion batteries. Spinel-type cathode materials LixMn2O4 and LixMn1.5Ni0.5O4 are promising candidates for Li-ion battery technologies, but they present serious challenges when it comes to their first-principles modeling. Here, we use density-functional theory with extended Hubbard functionals - DFT+U+V with on-site U and inter-site V Hubbard interactions - to study the properties of these transition-metal oxides. The Hubbard parameters are computed from first-principles using density-functional perturbation theory. We show that while U is crucial to obtain the right trends in properties of these materials, V is essential for a quantitative description of the structural and electronic properties, as well as the Li-intercalation voltages. This work paves the way for reliable first-principles studies of other families of cathode materials without relying on empirical fitting or calibration procedures.

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References

Preprint (Preprint where the data is discussed)
I. Timrov, M. Kotiuga, N. Marzari, "Unraveling the effects of inter-site Hubbard interactions in spinel Li-ion cathode materials", arXiv:2301.11143

Journal reference (Paper where the data is discussed)
I. Timrov, M. Kotiuga, N. Marzari, "Unraveling the effects of inter-site Hubbard interactions in spinel Li-ion cathode materials", Phys. Chem. Chem. Phys. 25, 9061 (2023)., doi: 10.1039/D3CP00419H

Journal reference (Paper where the data is discussed)
I. Timrov, M. Kotiuga, N. Marzari, "Unraveling the effects of inter-site Hubbard interactions in spinel Li-ion cathode materials", Phys. Chem. Chem. Phys. 25, 9061 (2023).