Suppressing storage-induced degradation of Li7La3Zr2O12 via encapsulation with hydrophobicity-tailored polymer nanolayer
- Authors
- Jeong, Wooyoung; Joo, Hyeonseo; Kim, Chaejeong; Jung, Kyu-Nam; Lee, Ju-Hyuck; Lee, Jong-Won
- Issue Date
- Jun-2023
- Publisher
- PERGAMON-ELSEVIER SCIENCE LTD
- Keywords
- Biphasic solid electrolytes; Li< sub> 7< /sub> La< sub> 3< /sub> Zr< sub> 2< /sub> O< sub> 12< /sub> ; Lithium carbonates; Polymer encapsulation; Polyurethane
- Citation
- ELECTROCHIMICA ACTA, v.453, pp.1 - 10
- Indexed
- SCIE
SCOPUS
- Journal Title
- ELECTROCHIMICA ACTA
- Volume
- 453
- Start Page
- 1
- End Page
- 10
- URI
- https://scholarworks.bwise.kr/hanyang/handle/2021.sw.hanyang/186043
- DOI
- 10.1016/j.electacta.2023.142358
- ISSN
- 0013-4686
- Abstract
- Solid-state batteries have been proposed as an alternative to conventional lithium-ion batteries to resolve safety issues. Biphasic solid electrolytes (BSEs) based on Li7La3Zr2O12 (LLZO) and a polymer phase have been widely studied because LLZO has high Li+ conductivity and chemical/electrochemical compatibility with Li metal. However, LLZO reacts with H2O and CO2 during storage in air, forming lithium carbonate (Li2CO3) layers on the surface. The extremely low Li+ conductivity of Li2CO3 degrades the Li+-conduction properties of LLZO-based BSEs. Herein, we propose an effective approach to improve the air-stability of LLZO via encapsulation with a hydrophobicity-tailored, Li+-conducting polymer nanolayer. Polyurethane-based polymers are designed to have high hydrophobicity by tuning soft segments and chain extenders and successfully encapsulate the LLZO surface with a thickness of ∼10 nm (P-LLZO). Accelerated durability tests (ADTs) under controlled concentrations of O2, H2O, and CO2 indicate that LLZO encapsulation with hydrophobic polymer effectively mitigates storage-induced degradation by preventing direct contact between LLZO and H2O/CO2. ADT-tested P-LLZO BSE exhibits higher ionic conductivity (σ = 1.3 × 10−4 S cm−1 at 60 °C) compared with that of ADT-tested LLZO BSE (σ = 3.6 × 10−5 S cm−1). A solid-state Li battery with ADT-tested P-LLZO BSE shows enhanced cycling stability than that with ADT-tested LLZO BSE, proving the efficacy of polymer encapsulation. The findings are essential for understanding the role of interfacial engineering in mitigating the degradation of Li+-conduction properties and developing highly conductive LLZO-based BSEs.
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