Density Functional Theory Studies on Li Metal Electrode/Garnet‐Type Li ₇ La ₃ Zr ₂ O ₁₂ Solid Electrolyte Interfaces for Application in All‐Solid‐State Batteries

Garnet-type Li7La3Zr2O12 (LLZ) and its analogs are considered potential candidates as solid electrolytes for all-solid-state Li metal batteries because their fast Li-ion conductivity chemical stability against anodes result in both safe large energy densities. To date, several computational experimental studies have been performed to obtain a more detailed understanding of the nonreactivity garnet-type LLZ with related phenomena. Herein, first-principles calculations based on density functional theory approach metal/LLZ interfaces elucidate electronic atomistic level aspects. It is confirmed that valence band maximum conduction minimum phase do not cross Fermi corresponding 2s band. In addition, it found defect formation energies associated vacancy interstitial largely reduced. particular, sites, i.e., Li+ insertion into phase, negative, indicating spontaneous likely proceed vicinity Li/LLZ interface. This new suggestion may help further elucidation reported interfacial behavior.