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Intrinsic Defects in LiMn$_{2}$O$_{4}$: First-Principles Calculations

Li, Xu; Wang, Jianchuan; Zhang, Shiwei; Sun, Lixian; Zhang, Weibin; Dang, Feng; Seifert, Hans J.; Du, Yong

Spinel LiMn$_{2}$O$_{4}$ has attracted wide attention due to its advantages of a high-voltage plateau, good capacity, environmental friendliness, and low cost. Due to different experimental synthesis methods and conditions, there are many intrinsic point defects in LiMn$_{2}$O$_{4}$. By means of first-principles calculations based on a reasonable magnetic configuration, we studied the formation energies, local structures, and charge compensation mechanism of intrinsic point defects in LiMn$_{2}$O$_{4}$. The formation energies of defects under the assumed O-rich equilibrium conditions were examined. It was found that O, Li, and Mn vacancies, Mn and Li antisites, and Li interstitial could appear in the lattice at some equilibrium conditions, but Mn interstitial is hard to form. The charge was compensated mainly by adjusting the oxidation state of Mn around the defect, except for the defects at the 8a Wyckoff site. The binding energies between point defects were calculated to shed light on the clustering of point defects. Furthermore, the diffusion of Li ions around the defects was discussed. Cation antisites led to a decrease of the Li diffusion barrier but O vacancy caused an increase of the barrier. ... mehr

Verlagsausgabe §
DOI: 10.5445/IR/1000139426
Veröffentlicht am 26.10.2021
Cover der Publikation
Zugehörige Institution(en) am KIT Institut für Angewandte Materialien - Angewandte Werkstoffphysik (IAM-AWP)
Publikationstyp Zeitschriftenaufsatz
Publikationsmonat/-jahr 08.2021
Sprache Englisch
Identifikator ISSN: 2470-1343, 2470-1343
KITopen-ID: 1000139426
HGF-Programm 38.02.02 (POF IV, LK 01) Components and Cells
Erschienen in ACS omega
Verlag American Chemical Society (ACS)
Band 6
Heft 33
Seiten 21255–21264
Vorab online veröffentlicht am 12.08.2021
Nachgewiesen in Web of Science
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