Journal
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
Volume 915, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.jelechem.2022.116340
Keywords
Transition metal oxide cathodes; Nucleation-merging mechanism; Layered structure; Lithium-ion batteries degradation
Categories
Funding
- Energy Materials and Surface Sciences Unit of the Okinawa Institute of Science and Technology Graduate University
- OIST Proof of Concept (POC) Program
- OIST R&D Cluster Research Program
- Incheon National University Research
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In this study, the surface degradation mechanism of the layered LiNi1/3Co1/3Mn1/3O2 cathode was examined using an operando Raman cell. It was found that the degradation process involves nucleation of degenerated layers and growth/merging between the degenerated layers during charge and discharge, providing key information on how the reconstructed surface can expand during cycling.
The well-defined layered structure for Li+ (de)intercalation of transition metal oxide cathodes plays a crucial role in delivering high capacity for lithium-ion batteries. Therefore, structural deformations of the layered structure are often considered as the evidence of deterioration in the battery performance and stability. In this study, the surface degradation mechanism of the layered LiNi1/3Co1/3Mn1/3O2 cathode is examined on charge-discharge using an operando Raman cell. We revealed the surface degradation process of the cathode with the A1g Raman spectral window (similar to 600 cm(-1)) in the voltage range of 2.8-4.35 V, and proposed the nucleation-merging mechanism. The spectral shifts and mappings have been compared between the early-stage and later-stage cycles (>= 15 cycles). It has been identified that the degradation process not only involves the structural changes (i.e., nucleation of the degenerated layers), but also the growth/merging between the degenerated layers during charge and discharge. This observation provides key information on how the reconstructed surface can expand during cycling.
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