Multicomponent Covalent Organic Framework Solid Electrolyte Allowing Effective Li-Ion Dissociation and Diffusion for All-Solid-State Batteries
- Title
- Multicomponent Covalent Organic Framework Solid Electrolyte Allowing Effective Li-Ion Dissociation and Diffusion for All-Solid-State Batteries
- Author
- 김종호
- Keywords
- all-solid-state lithium metal battery; and organic solid electrolyte; covalent organic framework; dendrite-free; multicomponent ionic conductor
- Issue Date
- 2023-08
- Publisher
- American Chemical Society
- Citation
- ACS Nano, v. 17, NO. 17, Page. 17372.0-17382.0
- Abstract
- Organic solid electrolytes compatible with all-solid-state Li metal batteries (LMBs) are essential to ensuring battery safety, high energy density, and long-term cycling performance. However, it remains a challenge to develop an approach to provide organic solid electrolytes with capabilities for the facile dissociation of strong Li-ion pairs and fast transport of ionic components. Herein, a diethylene glycol-modified pyridinium covalent organic framework (DEG-PMCOF) with a well-defined periodic structure is prepared as a multicomponent solid electrolyte with a cationic moiety of high polarity, an additional flexible ion-transporter, and an ordered ionic channel for all-solid-state LMBs. The DEG-containing pyridinium groups of DEG-PMCOF allow a lower dissociation energy of Li salts and a smaller energy barrier of Li-ion transport, leading to high ion conductivity (1.71 × 10-4 S cm-1) and a large Li-ion transfer number (0.61) at room temperature in the solid electrolyte. The DEG-PMCOF solid electrolyte exhibits a wide electrochemical stability window and effectively suppresses the formation of Li dendrites and dead Li in all-solid-state LMBs. Molecular dynamics and density functional theory simulations provide insights into the mechanisms for the enhanced Li-ion transport driven by the integrated diffusion process based on hopping motion, vehicle motion, and free diffusion of DEG-PMCOF. The all-solid-state LMB assembled with a DEG-PMCOF solid electrolyte displays a high specific capacity with a retention of 99% and an outstanding Coulombic efficiency of 99% at various C-rates during long-term cycling. This DEG-PMCOF approach can offer an effective route to design various solid-state Li batteries. © 2023 American Chemical Society.
- URI
- https://pubs.acs.org/doi/10.1021/acsnano.3c05405https://repository.hanyang.ac.kr/handle/20.500.11754/187825
- ISSN
- 1936-0851;1936-086X
- DOI
- 10.1021/acsnano.3c05405
- Appears in Collections:
- COLLEGE OF ENGINEERING SCIENCES[E](공학대학) > MATERIALS SCIENCE AND CHEMICAL ENGINEERING(재료화학공학과) > Articles
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