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.
Highlights
Understanding defect evolution and structural transformations constitutes a prominent research frontier for controlling the electrochemical properties of advanced battery materials
Our work has unveiled the fundamental mechanisms of defect evolution and structural transformations in Na- and Lilayered cathodes, promoted by high-energy Kr ion irradiation
Our experimental results suggest that Li-layered cathode, for example, LiNiO2 is more resistant to Kr ion irradiation-induced structural damage than Na-layered cathode, for example, Na2/3Fe1/2Mn1/2O2, which can be associated with the easiness of the cationic antisite defect formation in the former
Summary
Understanding defect evolution and structural transformations constitutes a prominent research frontier for controlling the electrochemical properties of advanced battery materials. 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 Naand Li-layered cathodes with 3d transition metals. Our study provides critical insights into designing battery materials for extreme irradiation environments and understanding fundamental defect dynamics in layered oxides. Layered transition metal oxides are extensively utilized as cathodes for the state-of-the-art rechargeable batteries[8,9]. Defects in these materials can be induced by the high-temperature synthesis[10] and electrochemical cycling[11] and can broadly influence battery properties. Ion irradiation in conjunction with TEM has been utilized to understand the irradiation damage in nuclear reactor materials and fuels[27,28,29,30]
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