4.8 Article

Engineering the Site-Disorder and Lithium Distribution in the Lithium Superionic Argyrodite Li6PS5Br

期刊

ADVANCED ENERGY MATERIALS
卷 11, 期 5, 页码 -

出版社

WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.202003369

关键词

anionic site‐ disorder; diffusion; lithium substructure; solid electrolytes; solid‐ state batteries

资金

  1. Bundesministerium fur Bildung und Forschung (BMBF) [03XP0177A, 03XP0174A]
  2. Projekt DEAL

向作者/读者索取更多资源

The study shows that controlling site-disorder in Li6PS5Br by adjusting synthesis conditions can enhance lithium ion diffusion pathways and increase ionic conductivity. Experimental results and ab initio molecular dynamics simulations corroborate each other, highlighting the importance of this modulation method for design and optimization of argyrodites.
Lithium argyrodite superionic conductors, of the form Li6PS5X (X = Cl, Br, and I), have shown great promise as electrolytes for all-solid-state batteries because of their high ionic conductivity and processability. The ionic conductivity of these materials is highly influenced by the structural disorder of S2-/X- anions; however, it is unclear if and how this affects the Li distribution and how it relates to transport, which is critical for improving conductivities. Here it is shown that the site-disorder once thought to be inherent to given compositions can be carefully controlled in Li6PS5Br by tuning synthesis conditions. The site-disorder increases with temperature and can be frozen in. Neutron diffraction shows this phenomenon to affect the Li+ substructure by decreasing the jump distance between so-called cages of clustered Li+ ions; expansion of these cages makes a more interconnected pathway for Li+ diffusion, thereby increasing ionic conductivity. Additionally, ab initio molecular dynamics simulations provide Li+ diffusion coefficients and time-averaged radial distribution functions as a function of the site-disorder, corroborating the experimental results on Li+ distribution and transport. These approaches of modulating the Li+ substructure can be considered essential for the design and optimization of argyrodites and may be extended to other lithium superionic conductors.

作者

我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。

评论

主要评分

4.8
评分不足

次要评分

新颖性
-
重要性
-
科学严谨性
-
评价这篇论文

推荐

暂无数据
暂无数据