论文标题
无序岩石LI3V2O5阳极的互化化学来自集群扩展和机器学习间原子势
The Intercalation Chemistry of the Disordered RockSalt Li3V2O5 Anode from Cluster Expansions and Machine Learning Interatomic Potentials
论文作者
论文摘要
无序岩石（DRX）Li3V2O5是可充电锂离子电池中阳极的有前途的候选者，因为其理想的低压，高速率能力和出色的循环稳定性。本文中，我们使用密度功能理论计算结合了机器学习群集扩展和原子间电位，对DRX-LI3V2O5阳极的互化化学进行了全面研究。基于蒙特卡洛模拟，带有拟合群集扩展模型的室温下，无序的LI3V2O5阳极的预测电压曲线与实验非常吻合。与先前的DFT结果相反，我们发现在充电过程中，李离子主要插入四面体位点，而八面体部位的大多数Li和V离子保持稳定。此外，具有拟合力矩张力电势的MD模拟将DRX -LI3V2O5的快速充电能力归因于Li+通过四面体 - 八面体 - 四面体途径的易于扩散率。我们进一步建议将LI：V比率调整为折断静脉静脉能力增加并降低该系统中阳极电压的一种手段。这项工作可深入了解高性能DRX-LI3V2O5阳极，并为发现其他无序阳极材料的发现铺平了道路。
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.
