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Article 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 and high stability with Li metal over 1500 h. When tested in a Li|electrolyte|LiFePO battery, the electrolyte delivers excellent cycling performance and rate capability at room temperature, with a discharge capacity of 137 mAh g 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 LiNi Mn Co O cathode, a discharge capacity of 140 mAh g 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.

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http://dx.doi.org/10.1002/smll.202302691DOI Listing

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