Iurii Timrov^1*, Michele Kotiuga^1*, Nicola Marzari^1*

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.

* Corresponding authors emails: iurii.timrov@epfl.ch, michele.kotiuga@epfl.ch, nicola.marzari@epfl.ch

DOI10.24435/materialscloud:ry-v5 [version v1]

Publication date: Feb 13, 2023

How to cite this record

Iurii Timrov, Michele Kotiuga, Nicola Marzari, Unraveling the effects of inter-site Hubbard interactions in spinel Li-ion cathode materials, Materials Cloud Archive 2023.25 (2023), https://doi.org/10.24435/materialscloud:ry-v5

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 Li_xMn₂O₄ and Li_xMn_1.5Ni_0.5O₄ 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.

Materials Cloud sections using this data

Files

File name	Size	Description
README.txt MD5md5:09fbec9d6d6cecd4bc5490e523389d08	3.1 KiB	The README.txt file describes the content of the compressed file "Files.tar"
Files.tar MD5md5:0f716e329c1a747d3e0634af7bc91ae4	263.9 MiB	Collection of all files which were used to produce the data of the paper: input files, output files, references to codes which were used, etc.

License

Files and data are licensed under the terms of the following license: Creative Commons Attribution 4.0 International.
Metadata, except for email addresses, are licensed under the Creative Commons Attribution Share-Alike 4.0 International license.

External references

Keywords

DFT+U+V DFT+U Extended Hubbard functionals Spinel cathode materials Li-ion batteries Lithium intercalation voltage MARVEL/OSP CSCS