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The origin causing detrimental phase transition in LiNiO2 is discussed through the detailed analysis on LiNiO2 integrated with nanosized Li3PO4, which is derived from a metastable and rocksalt LiNiO2–Li3PO4 solid solution sample. LiNiO2 derived from the metastable rocksalt oxide has approximately 6% anti-site defects between Li and Ni sites, and the particle size growth is suppressed by the presence of uniformly dispersed nanosized Li3PO4. In low crystallinity LiNiO2 with partial structural disordering derived from the rocksalt precursor, the Ni ion migration to tetrahedral sites is effectively suppressed because of repulsive electrostatic interaction from Ni ions located in Li layers. Moreover, on the basis of these findings, non-stoichiometric LiyNiO2 has been directly synthesized without high-energy milling and Li3PO4 integration, and significant improvement of electrode reversibility is achieved for the non-stoichiometric oxide without the addition of non-nickel ions. The unified understanding of deterioration mechanisms for LiNiO2 offers a new criterion to design Co-free LiNiO2 without metal substitution, potentially leading to full utilization of a reversible capacity as layered materials.

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• Creative Commons BY Attribution 4.0 International
  

Keyword: Lithium nickelate, Phase transition, Nickel migration, Structural disordering

Date published: 2024-01-18

Publisher: Elsevier BV

Journal:

• Energy Storage Materials (ISSN: 24058297) vol. 66 103200

Funding:

Manuscript type: Publisher's version (Version of record)

MDR DOI:

First published URL: https://doi.org/10.1016/j.ensm.2024.103200

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Updated at: 2024-08-20 12:30:31 +0900

Published on MDR: 2024-08-20 12:30:31 +0900