Atomistic Insight into Ion Transport and Conductivity in Ga/Al-Substituted Li7La3Zr2O12 Solid Electrolytes

First-Principles Study of Microscopic Electrochemistry at the LiCoO₂ Cathode/LiNbO₃ Coating/β-Li₃PS₄ Solid Electrolyte Interfaces in an All-Solid-State Battery

Revealing Atomic‐Scale Ionic Stability and Transport around Grain Boundaries of Garnet Li₇La₃Zr₂O₁₂ Solid Electrolyte

AbstractFor real applications of all‐solid‐state batteries (ASSBs) to be realized, understanding and control of the grain boundaries (GBs) are essential. However, the in‐depth insight into the atomic‐scale defect stabilities and transport of ions around GBs is still far from understood. Here, a first‐principles investigation on the promising garnet Li7La3Zr2O12 (LLZO) solid electrolyte (SE) GBs is carried out. The study reveals a GB‐dependent behavior for the Li‐ion transport correlated to the diffusion network. Of particular note, the Σ3(112) tilt GB model exhibits a quite high Li‐ion conductivity comparable to that in bulk, and a fast intergranular diffusion, contrary to former discovered. Moreover, the uncovered preferential electron localization at the Σ3(112) GB leads to an increase in the electronic conductivity at the GB, and the Li accumulation at the coarse GBs is revealed from the negative Li interstitial formation energies. These factors play important roles in the dendrite formation along the GBs during Li plating in the LLZO|Li cell. These findings suggest strategies for the optimization of synthesis conditions and coating materials at the interface for preventing dendrite formation. The present comprehensive simulations provide new insights into the GB effect and engineering of the SE in ASSBs.

Oxysulfide Li2BeSO: A potential new material for solid electrolyte predicted from first principles

Surface-Dependent Stability of the Interface between Garnet Li₇La₃Zr₂O₁₂ and the Li Metal in the All-Solid-State Battery from First-Principles Calculations

Interface structure prediction via CALYPSO method

Li⁺ Transport Mechanism at the Heterogeneous Cathode/Solid Electrolyte Interface in an All-Solid-State Battery via the First-Principles Structure Prediction Scheme

High-Pressure Evolution of Unexpected Chemical Bonding and Promising Superconducting Properties of YB₆

Novel structures of oxygen adsorbed on a Zr(0001) surface predicted from first principles