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In Situ Cross-Linked Plastic Crystal Electrolytes for Wide-Temperature and High-Energy-Density Lithium Metal Batteries

机译:In Situ Cross-Linked Plastic Crystal Electrolytes for Wide-Temperature and High-Energy-Density Lithium Metal Batteries

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摘要

The development of high-energy-density lithium metal batteries hasbeen significantly hampered mainly due to the poor electrolyte–electrodecompatibility, narrow operating temperature range, and stringent safetyconcerns of conventional electrolytes. Here, an in situ cross-linked plasticcrystal-based electrolyte (CPCE) with an optimized composition design isproposed. Based on the interaction of succinonitrile (SN) and ethoxylatedtrimethylolpropane triacrylate (ETPTA) with polar carbonyl groups, CPCEdelivers well-tuned energy levels and a concentrated coordination structure,leading to an improved electrochemical window and stable electrode–electrolyte interface. In addition, the crystallization of SN molecules isalso inhibited, ensuring suitable ion migration in bulky CPCE over a widetemperature range. Moreover, both the nonleakage of cross-linked ETPTAand the nonflammability of the plastic crystal electrolyte (PCE) furtherreinforce the safety of CPCE. As a result, the well-designed CPCE achieveshigh ion conductivity with a wide electrochemical window (≈5.4 V vsLi~+/Li) and a broad operating temperature range (?20 to 100 ℃). It alsodelivers dendrite-free lithium plating with high Coulombic efficiency of up to≈99.1%. The Cu|CPCE|LiNi_(0.8)Co_(0.1)Mn_(0.1)O_2 anode-free pouch cell exhibitshigh energy density (≈1520 Wh L~(-1)) and high safety during abuse tests.This study paves a new pathway to realize the practical application ofhigh-energy-density lithium metal battery energy storage systems.

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