Journal article
Computational framework for a systematic investigation of anionic redox process in Li-rich compounds
Anionic redox processes play a key role in determining the accessible capacity and cycle life of Li-rich cathode materials for batteries. We present a framework for investigating the anionic redox processes based on data readily available from standard DFT calculations. Our recipe includes a method of classifying different anionic species, counting the number of species present in the structure and a preconditioning scheme to promote anionic redox.
The method is applied to a set of LixMnO3 (1 ≤ x ≤2) structures, with cationic disorder, to identify the evolution of anionic redox processes during cycling. Additionally, we investigate how different choices of exchange-correlation functionals affect the formation of anionic redox species. The preconditioning of the structures is shown to promote the formation of peroxo-like species.
Furthermore, the choice of exchange-correlation functional has a large impact on the type of anionic redox species present, and thus care must be taken when considering localization in anionic species.
Language: | English |
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Publisher: | Nature Publishing Group UK |
Year: | 2020 |
ISSN: | 20573960 |
Types: | Journal article |
DOI: | 10.1038/s41524-020-0335-4 |
ORCIDs: | Tygesen, Alexander Sougaard , Chang, Jinhyun , Vegge, Tejs and García Lastra, Juan Maria |