Koji Shimizu*, Parth Bahuguna, Shigeo Mori, Akitoshi Hayashi and Satoshi Watanabe*,
{"title":"Enhanced Ionic Conductivity Through Crystallization of Li3PS4 Glass by Machine Learning Molecular Dynamics Simulations","authors":"Koji Shimizu*, Parth Bahuguna, Shigeo Mori, Akitoshi Hayashi and Satoshi Watanabe*, ","doi":"10.1021/acs.jpcc.4c01076","DOIUrl":null,"url":null,"abstract":"<p >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 Li<sub>3</sub>PS<sub>4</sub> 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 Li<sub>3</sub>PS<sub>4</sub> 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.</p>","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"128 24","pages":"10139–10145"},"PeriodicalIF":3.3000,"publicationDate":"2024-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"The Journal of Physical Chemistry C","FirstCategoryId":"1","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.jpcc.4c01076","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
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.
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.