Song, Seok Hyun Kim, Hwa Soo Kim, Kyoung Sun Hong, Seokjae Jeon, Hyungkwon Lim, Jun Jung, Young Hwa Ahn, Hyungju Jang, Jong Dae Kim, Man-Ho Seo, Jong Hyeok Kwon, Ji-Hwan Kim, Dokyung Lee, Young Joo Han, Young-Soo Park, Kyu-Young Kim, Chunjoong Yu, Seung-Ho Park, Hyeokjun Jin, Hyeong Min Kim, Hyungsub 2024-01-19T08:31:49Z 2024-01-19T08:31:49Z 2023-10-29 2024-01 1616-301X https://pubs.kist.re.kr/handle/201004/113198 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 English John Wiley & Sons Ltd. Toward a Nanoscale-Defect-Free Ni-Rich Layered Oxide Cathode Through Regulated Pore Evolution for Long-Lifespan Li Rechargeable Batteries Article 10.1002/adfm.202306654 1 Advanced Functional Materials, v.34, no.3 Advanced Functional Materials 34 3 N scie scopus 001076464800001 2-s2.0-85173499104 Chemistry, Multidisciplinary Chemistry, Physical Nanoscience & Nanotechnology Materials Science, Multidisciplinary Physics, Applied Physics, Condensed Matter Chemistry Science & Technology - Other Topics Materials Science Physics Article cathodes defect-free Li-ion batteries multi-length characterizations Ni-rich NCM pore defects