Lithium ion diffusion mechanism in covalent organic framework based solid state electrolyte
Literature Information
Kecheng Zhang, Bingkai Zhang, Mouyi Weng, Jiaxin Zheng, Shunning Li, Feng Pan
Solid state electrolytes (SSEs) based on two dimensional covalent organic frameworks (2D-COFs) with Li salts and solvents impregnated in their large pores have emerged as novel candidate materials for solid state lithium batteries. Here, using ab initio molecular dynamics simulation, we track the atomic-scale structural evolution during Li+ ion diffusion in a 2D-COF SSE composed of COF-5, LiClO4 and tetrahydrofuran (THF). Our simulation results show the transient dynamics of the Li+ diffusion events, the free rotation of ClO4− ions and the essential role of THFs in partitioning between the ions and the solid framework. We find clear evidence that Li+ ion diffusion adopts a one-dimensional (1D) liquid-like behavior with the coordination evolution driven by facile rotation and short-range diffusion of ClO4− ions and THFs. The fast Li+ diffusion pathway in the 1D tunnels of COFs may shed light on future design of high-performance COF based SSEs.
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Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.



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