Screening Topological Quantum Cathode Materials for K‑Ion Batteries by Graph Neural Network and First-Principles Calculations

Among the key parts of metal-ion batteries, cathode materials significantly affect the energy density and cycling stability. However, due to the large size of K+, not much progress has been made on cathode materials for K-ion batteries (KIBs). In this study, using the Atomistic Line Graph Neural Network and first-principles calculations, for the first time we screen cathode materials for KIBs from 7385 topological quantum materials with high electronic conductivity and reversible capacity. The experimentally synthesized K2MnS2 is discovered to have a reversible capacity of 203.8 mAh/g, an energy density of 564.5 Wh/kg, a small volume change of 6.4%, and multiple channels for K+ transport with fast dynamics. Furthermore, K2MnS2 shows high electrochemical interface stability with the reported solid electrolytes of K4V2O7, and K3NbP2O9. These findings suggest that topological quantum materials expand the design space of battery cathodes

Novel Solid-State Electrolyte Na₃La₅Cl₁₈ with High Stability and Fast Ionic Conduction

Motivated by the recent experimental synthesis of a LaCl3-based lithium superionic conductor [Yin, Y.-C.Nature 2023, 616, 77–83], we explore the potential of a LaCl3-based system for a sodium superionic conductor in this work. Using density functional theory combined with molecular dynamics simulation and a grand potential phase diagram analysis, we find that the resulting Na3La5Cl18 exhibits high energetic stability with a small energy-above-hull of 18 meV per atom, a large band gap of 5.58 eV, a wide electrochemical window of 0.41–3.76 V from the cathodic to the anodic limit, and a high Na+ conductivity of 1.3 mS/cm at 300 K. Furthermore, Na3La5Cl18 shows high chemical interface stability with the reported high-potential cathode materials such as NaCoO2, NaCrO2, Na2FePO4F, Na3V2(PO4)3, and Na3V2(PO4)2F3. These findings clearly suggest that the LaCl3-based framework can be used as a building block not only for Li-ion but also for Na-ion batteries