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

Song, Seok HyunKim, Hwa SooKim, Kyoung SunHong, SeokjaeJeon, HyungkwonLim, JunJung, Young HwaAhn, HyungjuJang, Jong DaeKim, Man-HoSeo, Jong HyeokKwon, Ji-HwanKim, DokyungLee, Young JooHan, Young-SooPark, Kyu-YoungKim, ChunjoongYu, Seung-HoPark, HyeokjunJin, Hyeong MinKim, Hyungsub
Issue Date
John Wiley & Sons Ltd.
Advanced Functional Materials, v.34, no.3
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. X-ray and neutron scattering experiments provide a new methodology for quantitatively probing the generation of microstructural defects. Based on these findings, a modified synthetic route is proposed that effectively avoids the formation of nanoscale defects in Ni-rich layered cathodes by promoting uniform synthetic reactions.image
cathodes; defect-free; Li-ion batteries; multi-length characterizations; Ni-rich NCM; pore defects
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KIST Article > 2023
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