Toward a Nanoscale-Defect-Free Ni-Rich Layered Oxide Cathode Through Regulated Pore Evolution for Long-Lifespan Li Rechargeable Batteries

Seok Hyun Song, Hwa Soo Kim, Kyoung Sun Kim, Seokjae Hong, Hyungkwon Jeon, Jun Lim, Young Hwa Jung, Hyungju Ahn, Jong Dae Jang, Man Ho Kim, Jong Hyeok Seo, Ji Hwan Kwon, Dokyung Kim, Young Joo Lee, Young Soo Han, Kyu Young Park, Chunjoong Kim, Seung Ho Yu, Hyeokjun Park, Hyeong Min JinHyungsub Kim

Research output: Contribution to journalArticlepeer-review

Abstract

Ni-rich layered oxides are envisioned as the most promising cathode materials for next-generation lithium-ion batteries; however, their practical adoption is plagued by fast capacity decay originating from chemo-mechanical degradation. The intrinsic chemical–mechanical instability, inherited from atomic- and nanoscale defects generated during synthesis, is not yet resolved. Here, atomic- and nanoscale structural evolution during solid-state synthesis of Ni-rich layered cathode, Li[Ni0.92Co0.03Mn0.05]O2, is investigated using combined X-ray/neutron scattering and electron/X-ray microscopy. The multiscale analyses demonstrate the intertwined correlation between phase transition and microstructural evolution, with atomic-scale defects derived from the decomposition of precursors leading to the creation of intra/inter-granular pores. The nucleation and coalescence mechanism of pore defects during the synthesis of Ni-rich layered cathodes are quantitatively revealed. Furthermore, a modified synthetic route is proposed to effectively circumvent the formation of nanoscale defects in Ni-rich layered cathodes by facilitating uniform synthetic reactions, resulting in superior electrochemical and microstructural stability.

Original languageEnglish
Article number2306654
JournalAdvanced Functional Materials
Volume34
Issue number3
DOIs
Publication statusPublished - 2024 Jan 15

Bibliographical note

Publisher Copyright:
© 2023 Wiley-VCH GmbH.

Keywords

  • Li-ion batteries
  • Ni-rich NCM
  • cathodes
  • defect-free
  • multi-length characterizations
  • pore defects

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • General Chemistry
  • Biomaterials
  • General Materials Science
  • Condensed Matter Physics
  • Electrochemistry

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