Revisiting doping strategies: The critical role of dopant-host interplay in cobalt-free, high-nickel cathode materials
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초록

Cobalt-free, high-nickel (Ni-rich) layered oxides are promising cathode materials for next-generation lithium-ion batteries, offering high specific capacity while circumventing the economic and ethical issues associated with cobalt. However, the inherent structural and interfacial instabilities of Ni-rich compositions present significant challenges. While doping is a widely adopted strategy to enhance cathode stability, previous studies have predominantly focused on the intrinsic physicochemical properties of the dopants themselves. In contrast, this study reveals that the efficacy of a dopant is critically dependent on the specific composition of the host cathode materials, a factor that becomes particularly pronounced in Co-free, Ni-rich systems. To systematically investigate this compositional dependence, we introduced four common dopants-Al, B, Mg, and Ti-into a Co-free, Nirich layered oxide. Our findings indicate that the stabilizing effects of Al, B, and Mg were diminished due to a functional overlap with the role of manganese (Mn) already present in the host material. Conversely, titanium (Ti) provided a complementary stabilizing function that Mn could not, leading to a significant enhancement in overall performance. Specifically, the Ti-doped cathode material demonstrated superior capacity retention over long-term cycling and effectively suppressed detrimental phenomena such as impedance growth and microcrack formation. This work highlights that the interplay between the dopant and the host material's existing elements is a key design parameter, providing a new, more holistic perspective for developing next-generation, highperformance cathodes.

키워드

Lithium-ion batteriesCo-free Ni-rich cathodesDopingMn interferenceXPS-SURFACE ANALYSISCYCLE STABILITYSEI LAYERSIONOXIDE
제목
Revisiting doping strategies: The critical role of dopant-host interplay in cobalt-free, high-nickel cathode materials
저자
Ahn, Seon HooKwon, Doo SeokKim, Hyun WooBang, Jin Ho
DOI
10.1016/j.cej.2025.168882
발행일
2025-11
유형
Article
저널명
Chemical Engineering Journal
523