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Intrinsic Defects in LiMn₂O₄: First-Principles Calculations.

ABSTRACT: Spinel LiMn₂O₄ 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 LiMn₂O₄. 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 LiMn₂O₄. 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. This study provides theoretical support for understanding point defects in spinel LiMn₂O₄.

SUBMITTER: Li X

PROVIDER: S-EPMC8388003 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:In this paper, first principles method was adopted to investigate the point defects, Vanadium-related defects and defect combinations (vacancy (V), substitutional (S) and/or interstitial (I)) in molybdenum β-Mo2C and explore the use of first principles calculation data in analysing the link between different carbides and the effects of doping elements. Supercell models with different defect types were established and optimized, and the formation energy data of defects was developed. The structure evolution during the optimization process is analysed in detail to establish the main characteristics of changes and the relevant electronic properties. The data for different types of intrinsic defects and combined defects complexes was developed and key results is analysed. The results show that carbon vacancy (VC) is stable but does not inevitably exist in pure β-Mo2C. Interstitial site II is a very unstable position for any type of atoms (Mo, V and C), and analysis of the structure evolution shows that the atom always moves to the interface area near the interstitial site I between two layers. In particular, a C atom can expand the lattice structure when it exists between the layer interfaces. One type of the defects studied, the substitution of Mo with V (designated as 'SV-Mo'), is the most stable defect among all single point defects. The data for defect complexes shows that the combination of multiple SV-Mo defects in the super cell being more stable than the combination of other defects (e.g., 'VMo+IC', 'SV-Mo+VC'). The data with increasing SV-Mo in (Mo, V)2C system is developed, and typical data (e.g., formation energy) for Mo-rich carbides and V carbides are correlated and the potential of the data in analysing transition of different carbides is highlighted. The relevance of using first principles calculation data in the studying of V-doping and the complex carbides (V- and Mo-rich carbides) evolution in different materials systems and future focus of continuous work is also discussed.

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Intrinsic Defects in LiMn₂O₄: First-Principles Calculations.

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