An Ion-Channel-Restructured Zwitterionic Covalent Organic Framework Solid Electrolyte for All-Solid-State Lithium-Metal Batteries
- Authors
- Kang, Tae Woog; Lee, Jun-Hyeong; Lee, Jaewoo; Park, Jung Hyun; Shin, Jae-Hoon; Ju, Jong-Min; Lee, Hajin; Lee, Sang Uck; Kim, Jong-Ho
- Issue Date
- Jun-2023
- Publisher
- WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
- Keywords
- all-solid-state lithium batteries; covalent organic frameworks; lithium-metal batteries; solid electrolytes; zwitterionic ion conductors
- Citation
- Advanced Materials, pp.1 - 10
- Indexed
- SCIE
SCOPUS
- Journal Title
- Advanced Materials
- Start Page
- 1
- End Page
- 10
- URI
- https://scholarworks.bwise.kr/hanyang/handle/2021.sw.hanyang/188135
- DOI
- 10.1002/adma.202301308
- ISSN
- 0935-9648
- Abstract
- Organic solid electrolytes offer an effective route for safe and high-energy-density all-solid-state Li metal batteries. However, it remains a challenge to devise a new strategy to promote the dissociation of strong ion pairs and the transport of ionic components in organic solid electrolytes. Herein, a zwitterionic covalent organic framework (Zwitt-COF) with well-defined chemical and pore structures is prepared as a solid electrolyte capable of accelerating the dissociation and transport of Li ions. The Zwitt-COF solid electrolyte exhibits a high room-temperature ionic conductivity of 1.65 x 10(-4) S cm(-1) with a wide electrochemical stability window. Besides, the Zwitt-COF solid electrolyte displays stable Li plating/stripping behavior via effective inhibition of the formation of Li dendrites and dead Li, leading to superior long-term cycle performance with retention of 99% discharge capacity and 98% Coulombic efficiency in an all-solid-state Li-metal battery. Theoretical simulations reveal that the incorporation of zwitterionic groups into COF can facilitate the dissociation of strong ion pairs and reconstruct the AA-stacking configuration by dissociative adsorption of Li+ ions on Zwitt-COF producing linear hexagonal ion channels in the Zwitt-COF solid electrolyte. This strategy based on Zwitt-COF can provide an alternative way to construct various solid-state Li batteries.
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