Defect and structural evolution under high-energy ion irradiation informs battery materials design for extreme environments

• Published in: Nature communications Vol. 11; no. 1; pp. 4548 - 13
• Main Authors: Rahman, Muhammad Mominur, Chen, Wei-Ying, Mu, Linqin, Xu, Zhengrui, Xiao, Ziqi, Li, Meimei, Bai, Xian-Ming, Lin, Feng
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 11.09.2020; Nature Publishing Group; Nature Portfolio
• Subjects: 147/143; 639/301; 639/4077; Amorphization; Antisite defects; Cathodes; Defects; Design defects; Dislocation loops; Electrochemical analysis; Electrochemistry; Energy; ENERGY STORAGE; Evolution; Extreme environments; Humanities and Social Sciences; INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Ion diffusion; Ion irradiation; Irradiation; MATERIALS SCIENCE; Mathematical analysis; multidisciplinary; Radiation; Radiation effects; Radiation tolerance; Science; Science (multidisciplinary); Sodium; Transition metals; Transmission electron microscopy
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-020-18345-4

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. Defect and structural evolution are critical in determining the stability of battery materials. Here, the authors use high-energy Kr ion irradiation to induce rapid defect and study structural evolution in Li- and Na-layered cathodes to find that Li-layered cathodes are more resilient under irradiation.