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Stabilizing Solid-state Lithium Metal Batteries through In Situ Generated Janus-heterarchical LiF-rich SEI in Ionic Liquid Confined 3D MOF/Polymer Membranes
Authors:Xingxing Zhang  Qingmei Su  Gaohui Du  Bingshe Xu  Shun Wang  Zhuo Chen  Liming Wang  Wenhuan Huang  Huan Pang
Institution:1. School of Materials Science & Engineering, Shaanxi University of Science and Technology, 710021 Xi'an, P.?R. China

Key Laboratory of Chemical Additives for China National Light Industry, College of Chemistry and Chemical Engineering, Shaanxi University of Science and Technology, 710021 Xi'an, P.?R. China;2. School of Materials Science & Engineering, Shaanxi University of Science and Technology, 710021 Xi'an, P.?R. China;3. Key Laboratory of Chemical Additives for China National Light Industry, College of Chemistry and Chemical Engineering, Shaanxi University of Science and Technology, 710021 Xi'an, P.?R. China;4. School of Chemistry and Chemical Engineering, Institute for Innovative Materials and Energy, Yangzhou University, 225002 Yangzhou, P.?R. China

Abstract:Pursuing high power density lithium metal battery with high safety is essential for developing next-generation energy-storage devices, but uncontrollable electrolyte degradation and the consequence formed unstable solid-electrolyte interface (SEI) make the task really challenging. Herein, an ionic liquid (IL) confined MOF/Polymer 3D-porous membrane was constructed for boosting in situ electrochemical transformations of Janus-heterarchical LiF/Li3N-rich SEI films on the nanofibers. Such a 3D-Janus SEI-incorporated into the separator offers fast Li+ transport routes, showing superior room-temperature ionic conductivity of 8.17×10?4 S cm?1 and Li+ transfer number of 0.82. The cryo-TEM was employed to visually monitor the in situ formed LiF and Li3N nanocrystals in SEI and the deposition of Li dendrites, which is greatly benefit to the theoretical simulation and kinetic analysis of the structural evolution during the battery charge and discharge process. In particular, this membrane with high thermal stability and mechanical strength used in solid-state Li||LiFePO4 and Li||NCM-811 full cells and even in pouch cells showed enhanced rate-performance and ultra-long life spans.
Keywords:Janus-Heterarchical LiF/Li3N-Rich SEI Films  Lithium Metal Battery  Solid-Electrolyte Interface (SEI)
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