Enhanced Ionic Conductivity Through Crystallization of Li3PS4 Glass by Machine Learning Molecular Dynamics Simulations

IF 3.3 3区 化学 Q2 CHEMISTRY, PHYSICAL
Koji Shimizu*, Parth Bahuguna, Shigeo Mori, Akitoshi Hayashi and Satoshi Watanabe*, 
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Abstract

Understanding the atomistic mechanism of ion conduction in solid electrolytes is critical for the advancement of all-solid-state batteries. Glass-ceramics, which undergo crystallization from a glass state, frequently exhibit unique properties including enhanced ionic conductivities compared to both the original crystalline and glass forms. Despite these distinctive features, specific details regarding the behavior of ion conduction in glass-ceramics, particularly concerning conduction pathways, remain elusive. In this study, we demonstrate the crystallization process of Li3PS4 glass through molecular dynamics simulations employing machine learning interatomic potentials constructed from first-principles calculation data. Our analyses of Li conduction using the obtained partially crystallized structures reveal that the diffusion barriers of Li decrease as the crystallinity in Li3PS4 glass-ceramics increases. Furthermore, Li displacements predominantly occur in the precipitated crystalline portion, suggesting that percolation conduction plays a significant role in enhanced Li conduction. These findings provide valuable insights for the future utilization of glass-ceramic materials.

Abstract Image

Abstract Image

通过机器学习分子动力学模拟提高 Li3PS4 玻璃结晶的离子传导性
了解固体电解质中离子传导的原子机制对于全固态电池的发展至关重要。从玻璃状态结晶而成的玻璃陶瓷经常表现出独特的特性,包括与原始晶体和玻璃形态相比离子传导性更强。尽管玻璃陶瓷具有这些独特的特性,但有关玻璃陶瓷中离子传导行为的具体细节,尤其是传导路径,仍然难以捉摸。在本研究中,我们利用第一原理计算数据构建的机器学习原子间势,通过分子动力学模拟展示了 Li3PS4 玻璃的结晶过程。我们利用所获得的部分结晶结构对锂的传导进行了分析,结果表明,随着 Li3PS4 玻璃陶瓷结晶度的增加,锂的扩散障碍也随之降低。此外,锂的位移主要发生在沉淀结晶部分,这表明渗滤传导在增强锂传导方面发挥了重要作用。这些发现为今后利用玻璃陶瓷材料提供了宝贵的启示。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
The Journal of Physical Chemistry C
The Journal of Physical Chemistry C 化学-材料科学:综合
CiteScore
6.50
自引率
8.10%
发文量
2047
审稿时长
1.8 months
期刊介绍: The Journal of Physical Chemistry A/B/C is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.
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