2022/08/30 by Xingyu Guo, Chi Chen, Guo, Xingyu +3 · 2 citations
Engineering · Materials Science · #Advanced Battery Technologies Research #Advancements in Battery Materials #FOS: Physical sciences #Machine Learning in Materials Science #Materials Science (cond-mat.mtrl-sci)
paper · pdf · doi:10.48550/arxiv.2208.14420
openalex publication_date 2022/08/30 · openalex created_date 2022/09/01 · openalex updated_date 2026/07/28
Disordered rocksalt (DRX) Li3V2O5 is a promising candidate for anode in rechargeable lithium-ion batteries because of its ideal low voltage, high rate capability, and superior cycling stability. Herein, we presents a comprehensive study of intercalation chemistry of the DRX-Li3V2O5 anode using density functional theory calculations combined with machine learning cluster expansions and interatomic potentials. The predicted voltage profile of the disordered Li3V2O5 anode at room temperature based on Monte Carlo simulations with a fitted cluster expansion model is in excellent agreement with experiments. In contrast to previous DFT results, we find that Li ions predominately intercalate into tetrahedral sites during charging, while the majority of Li and V ions at octahedral sites remain stable. In addition, MD simulations with a fitted moment tensor potential attribute the fast-charging capability of DRX-Li3V2O5 to the facile diffusivity of Li+ via tetrahedral - octahedral - tetrahedral pathway. We further suggest tuning the Li:V ratio as a means to trade off increased lithiation capacity and decreased anode voltage in this system. This work provides in-depth insights into the high-performance DRX-Li3V2O5 anode, and paves the way to the discovery of other disordered anode materials.