Understanding the chemomechanical degradation of layered oxide cathodes is crucial for the development of next-generation lithium-ion battery cathodes. Current understanding of their mechanical failure is limited to cracking, while our study reveals a stress-driven phase degradation mechanism caused by severe lattice bending and interlayer shear. This stress-driven phase transformation is a typical degradation modality widely existing in the material. Our work provides new insights into the mechanical deformation-induced phase transformation in layered oxide cathodes through deep-learning-aided super-resolution imaging and density functional theory calculations.
Understanding chemomechanical degradations of layered oxide cathodes is critical to developing next-generation cathodes for lithium-ion batteries. So far, although the multimodal phase degra-dations in layered cathodes have been extensively studied, current understanding of their mechanical failure is only limited to cracking. Here, by using deep-learning-aided super-resolution imaging, we uncover a stress-driven phase degradation mechanism distinct from a conventional pathway driven by delithiation-induced self -destabilization in a technologically important layered cathode. We show that severe lattice bending caused by chemomechanical stress concentration could directly lead to phase transformation through interlayer shear. The O3 -> O1 transformation forms not only in bending bands but also in bending-induced kink structures, suggest-ing that the stress-driven phase transformation is a typical degrada-tion modality widely existing in the material. Density functional the-ory (DFT) calculations confirm that the bending-induced O3 -> O1 phase transformation in delithiated lattice is energetically favor-able. Our work offers new understanding of the mechanical defor-mation-induced phase transformation in layered oxide cathodes.
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