Defect and Structural Evolution Under High-Energy Ion Irradiation Informs Battery Materials Design for Extreme Environments

Abstract

Defect and structural evolution can have a broad influence on battery materials ranging from electrochemistry to batteries for extreme environments.1–3 In this presentation, the fundamental interplay of defect and structural evolution promoted by high-energy ion irradiation in layered oxide cathodes are discussed. Li and Na layered oxides are subjected to Kr ion irradiation (1 MeV) at various fluences and the transformations of the materials are studied in situ. Our study shows that Li layered oxides are more structurally stable under irradiation than Na layered oxides. The better structural stability of Li layered oxides can be explained in terms of the facile formation of cationic antisite defects because of the smaller size difference between Li and the transition metals. Moreover, a mathematical model is presented to quantitatively probe the defect evolution in these materials under irradiation. Our model shows that the defect clusters induced by ion irradiation preferentially align along the Na/Li diffusion channels in the materials. This study presents critical information for the design of battery materials for extreme environments where materials damage due to irradiation can be significant. Fundamental defect evolution in layered oxide cathodes is also unraveled.1 Acknowledgement This work is primarily supported by The Thomas F. and Kate Miller Jeffress Memorial Trust, Bank of America, Trustee, and the Jeffress Trust Awards Program in Interdisciplinary Research. F.L. and X.-M.B. also acknowledge their startup funds at Virginia Tech. The Na cathode was developed based on a project funded by the National Science Foundation (No. CBET-1912885). The Li cathode was developed based upon work supported by the U.S. Department of Energy’s Office of Energy Efficiency and Renewable Energy (EERE) under the Award Number: DE-EE0008444. The irradiation work at the IVEM User Facility at Argonne National Laboratory was supported by the U.S. Department of Energy, Office of Nuclear Energy under DOE Idaho Operations Office Contract DE-AC07-051D14517 as part of a Nuclear Science User Facilities experiment. X.-M.B. acknowledges the high-performance computing facilities at Virginia Tech’s Advanced Research Computing. Reference M. M. Rahman, W.-Y. Chen, L. Mu, Z. Xu, Z. Xiao, M. Li, X.-M. Bai, and F. Lin, Nat. Commun., 11, 4548 (2020).Z. Xu, D. Hou, D. Kautz, W. Liu, R. Xu, X. Xiao, and F. Lin, Adv. Mater., 32, 2003417 (2020).M. M. Rahman, J. Mao, W. H. Kan, C.-J. Sun, L. Li, Y. Zhang, M. Avdeev, X.-W. Du, and F. Lin, ACS Mater. Lett., 1, 573–581 (2019).