Improving Room-Temperature Li-Metal Battery Performance by In Situ Creation of Fast Li⁺ Transport Pathways in a Polymer-Ceramic Electrolyte

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Yu, Jing ; Zhou, Guodong ; Li, Yueqing ; Wang, Yuhao ; Chen, Dengjie ; Ciucci, Francesco:
Improving Room-Temperature Li-Metal Battery Performance by In Situ Creation of Fast Li⁺ Transport Pathways in a Polymer-Ceramic Electrolyte.
In: Small. Bd. 19 (2023) Heft 39 . - 2302691.
ISSN 1613-6829
DOI: https://doi.org/10.1002/smll.202302691

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Abstract

Abstract Composite polymer-ceramic electrolytes have shown considerable potential for high-energy-density Li-metal batteries as they combine the benefits of both polymers and ceramics. However, low ionic conductivity and poor contact with electrodes limit their practical usage. In this study, a highly conductive and stable composite electrolyte with a high ceramic loading is developed for high-energy-density Li-metal batteries. The electrolyte, produced through in situ polymerization and composed of a polymer called poly-1,3-dioxolane in a poly(vinylidene fluoride)/ceramic matrix, exhibits excellent room-temperature ionic conductivity of 1.2 mS cm⁻¹ and high stability with Li metal over 1500 h. When tested in a Li|electrolyte|LiFePO₄ battery, the electrolyte delivers excellent cycling performance and rate capability at room temperature, with a discharge capacity of 137 mAh g⁻¹ over 500 cycles at 1 C. Furthermore, the electrolyte not only exhibits a high Li⁺ transference number of 0.76 but also significantly lowers contact resistance (from 157.8 to 2.1 Ω) relative to electrodes. When used in a battery with a high-voltage LiNi0.8Mn0.1Co0.1O₂ cathode, a discharge capacity of 140 mAh g−1 is achieved. These results show the potential of composite polymer-ceramic electrolytes in room-temperature solid-state Li-metal batteries and provide a strategy for designing highly conductive polymer-in-ceramic electrolytes with electrode-compatible interfaces.