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Abstract Understanding defect evolution and structural transformations constitutes a prominent research frontier for ultimately controlling the electrochemical properties of advanced battery materials. Herein, for the first time, we utilize in situ high-energy Kr ion irradiation with transmission electron microscopy to monitor how defects and microstructures evolve in Na- and Li-layered cathodes with 3d transition metals. Our experimental and theoretical analyses reveal that Li-layered cathodes are more resistant to radiation-induced structural transformations, such as amorphization than Na-layered cathodes. The underlying mechanism is the facile formation of Li-transition metal antisite defects in Li-layered cathodes. The quantitative mathematical analysis of the dynamic bright-field imaging shows that defect clusters preferentially align along the Na/Li ion diffusion channels ( a-b planes), which is likely governed by the formation of dislocation loops. Our study provides critical insights into designing battery materials for extreme irradiation environments and understanding fundamental defect dynamics in layered oxides.

Layered cathode materials (LCMs), because of their high energy density and relatively stable performance, represent an important class of cathode materials for alkali metal ion ( e.g. , Li + and Na + ) batteries. Chemomechanical behaviors of LCMs, which affect battery performance dramatically, have drawn extensive attention in recent years. Most chemomechanical processes have some common chemical and structural origins that are at the center of materials chemistry, for example, defects and local bonding environments in the solid state. In this review, we first discuss the chemomechanical breakdown of LCMs by introducing their categories and negative effects on the battery performance. We then systematically analyze factors that govern the initiation and propagation of chemomechanical breakdown and summarize their formation mechanisms. Strategies that can enhance the chemomechanical properties of LCMs or reduce the destructive effects of chemomechanical breakdown are then discussed. Finally, light is shed on the new state-of-the-art techniques that have been applied to study chemomechanical breakdown. This review virtually includes most aspects of the chemomechanical behaviors of LCMs and provides some insights into the important chemical motifs that determine the chemomechanical properties. Therefore, we believe that advanced design protocols of LCMs can be developed to effectively address themore »chemomechanical breakdown issue of LCMs.« less