Superexchange interaction regulates Ni/Mn spin states triggering Ni-t_2g/O-2p reductive coupling enabling stable lithium-rich cathode.

ABSTRACT: Lithium-rich layer oxides are expected to be high-capacity cathodes for next-generation lithium-ion batteries, but their performance is hindered by irreversible anionic redox, leading to voltage decay, lag, and slow kinetics. In order to solve these problems, we regulate the Ni/Mn spin state in Li_1.2Mn_0.6Ni_0.2O₂ by Be doping, which generates the superexchange interaction and activates Ni-t_2g orbitals. The activation of Ni-t_2g orbitals triggers the reductive coupling mechanism between Ni/O, which improves the reversibility and kinetics of anionic redox. The strong π-type Ni-t_2g/O-2p interaction forms a stable Ni-(O-O) configuration, suppressing excessive anion oxidation. In this work, the Be modified cathodes have

SUBMITTER: Zheng C 

PROVIDER: S-EPMC12022161 | biostudies-literature | 2025 Apr

REPOSITORIES: biostudies-literature