described the surface reconstruction and chemical evolution of the rhombohedral layered structure to a cubic spinel structure using high-throughput X-ray absorption spectroscopy 8. investigated the degradation mechanism of the phase transformation induced by cation mixing from the surface to bulk using ex situ structural analysis 7. To better understand these challenges, Jung et al. NI MATE CRACK CRACKWhile the increase of the Ni ratio in NCM contributes to an enhanced specific discharge capacity, it also results in severe capacity degradation caused by cation mixing, surface side reactions, and crack propagation with structural instability 1. Although LiNi 1/3Co 1/3Mn 1/3O 2 (NCM111) has been successfully commercialized, in order to meet the demand for large-scale energy storage applications such as electric vehicles (EVs) and energy storage systems (ESSs), further NCM research and development have been directed toward enhancing its specific capacity by increasing the ratio of the Ni component toward LiNi 0.8Co 0.1Mn 0.1O 2 (NCM811) 4, 5, 6. Ni-rich transition metal layered oxides (LiNi xCo yMn 1− x− yO 2, with x > 0.5, Ni-rich NCM) have been spotlighted during the past decade as the most promising candidates for high capacity cathode materials in Li-ion batteries (LIBs) due to their high energy densities (>200 mAh g −1 until ~4.6 V vs. Further, meso-scale strain distributions show around 5% of anisotropic contraction with lower critical energy release rates, which cause not only micro-crack generations of secondary particles on the interfaces between the contracted primary particles, but also mechanical instability of primary particles from heterogeneous strain changes. Abrupt phase transformations with heterogeneous structural collapse after x = 0.81 (~220 mAh g −1) were identified in the nanodomain. Combined-phase investigations represent the highest phase barrier and steepest chemical potential after x = 0.75, leading to phase transformations to highly Li-deficient phases with an inactive character. Atomic-scale structure analysis demonstrated that opposite changes in the lattice parameters are observed until the inverse Li content x = 0.75 then, structure collapses due to complete extraction of Li from between transition metal layers. For these reasons, we focused on the origins of crack generation from phase transformations and structural distortions in Ni-rich LiNi 0.8Co 0.1Mn 0.1O 2 using multiscale approaches, from first-principles to meso-scale phase-field model. Although its specific capacity is enhanced at higher voltages as Ni ratio increases, its structural degradation due to phase transformations and lattice distortions during cycling becomes severe. Ni-rich LiNi 0.8Co 0.1Mn 0.1O 2 layered oxide cathodes have been highlighted for large-scale energy applications due to their high energy density.
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