2026-06-23T08:17:01Z https://archive.materialscloud.org/oai2d

oai:materialscloud.org:1654 2023-02-13T16:26:26Z openaire_data community-mcarchive

Timrov, Iurii Kotiuga, Michele Marzari, Nicola Timrov, Iurii Kotiuga, Michele Marzari, Nicola 2023-02-13 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 Li<sub>x</sub>Mn<sub>2</sub>O<sub>4</sub> and Li<sub>x</sub>Mn<sub>1.5</sub>Ni<sub>0.5</sub>O<sub>4</sub> 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. text/markdown text/plain application/x-tar https://doi.org/10.24435/materialscloud:ry-v5 oai:materialscloud.org:1654 mcid:2023.25 eng Materials Cloud https://arxiv.org/abs/2301.11143 https://doi.org/10.1039/D3CP00419H https://pubs.rsc.org/en/content/articlelanding/2023/cp/d3cp00419h https://archive.materialscloud.org/communities/mcarchive https://doi.org/10.24435/materialscloud:pc-w4 info:eu-repo/semantics/openAccess Creative Commons Attribution 4.0 International https://creativecommons.org/licenses/by/4.0/legalcode DFT+U+V DFT+U Extended Hubbard functionals Spinel cathode materials Li-ion batteries Lithium intercalation voltage MARVEL/OSP CSCS Unraveling the effects of inter-site Hubbard interactions in spinel Li-ion cathode materials info:eu-repo/semantics/other