Theoretical Insights into High-Entropy Ni-Rich Layered Oxide Cathodes for Low-Strain Li-Ion Batteries

Amreen Bano, Malachi Noked, Dan Thomas Major

Research output: Contribution to journalArticlepeer-review

1 Scopus citations


Ni-rich, Co-free layered oxide cathode materials are promising candidates for next-generation Li-ion batteries due to their high energy density. However, these cathode materials suffer from rapid capacity fading during electrochemical cycling. To overcome this shortcoming, so-called high-entropy (HE) materials, which are obtained by incorporating multiple dopants, have been suggested. Recent experimental work has shown that HE Ni-rich cathode materials can offer excellent capacity retention on cycling, although a thorough rationale for this has yet to be provided. Here, we present classical and first-principles calculations to elucidate the salient features of HE layered oxides as cathode materials in Li-ion batteries. We suggest that a combination of five prime factors may be responsible for the enhanced performance of HE Ni-rich layered oxide cathode materials over other Ni-rich cathodes: (1) low crystal lattice variation, (2) invariant local crystal field environment, (3) strong metal-oxygen bonding, (4) low degree of antisite defects, and (5) low operational voltage.

Original languageEnglish
Pages (from-to)8426-8439
Number of pages14
JournalChemistry of Materials
Issue number20
StatePublished - 24 Oct 2023

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