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Interface Design for High-Performance All-Solid-State Lithium Batteries
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DOI：10.1002/aenm.202303046.png)
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Abstract
En 中文
All-solid-state batteries suffer from high interface resistance and lithium dendrite growth leading to low Li plating/stripping Coulombic efficiency (CE) of <90% and low critical current density at high capacity. Here, simultaneously addresses both challenges are simultaneously addressed and the Li plating/stripping CE is significantly increased to 99.6% at 0.2 mA cm(-2)/0.2 mAh cm(-2), and critical current density (CCD) of > 3.0 mA cm(-2)/3.0 mAh cm(-2) by inserting a mixed ionic-electronic conductive (MIEC) and lithiophobic LiF-C-Li3N-Bi nanocomposite interlayer between Li6PS5Cl electrolyte and Li anode. The highly lithiophobic LiF-C-Li3N-Bi interlayer with high ionic conductivity (10(-5) S cm(-1)) and low electronic conductivity (3.4x10(-7) S cm(-1)) enables Li to plate on the current collector (CC) surface rather than on Li6PS5Cl surface avoiding Li6PS5Cl electrolyte reduction. During initial Li plating on CC, Li penetrates into porous LiF-C-Li3N-Bi interlayer and lithiates Bi nanoparticles into Li3Bi. The lithiophilic Li3Bi and Li3N nanoparticles in LiF-C-Li3N-Li3Bi sub-interlayer will move to CC along with plated Li, forming LiF-C/Li3N-Li3Bi lithiophobic/lithiophilic sublayer during the following Li stripping. This interlayer enables Co0.1Fe0.9S2/Li6PS5Cl/Li cell with an areal capacity of 1.4 mAh cm(-2) to achieve a cycle life of >850 cycles at 150 mA g(-1). The lithiophobic/lithiophilic interlayer enables solid-state metal batteries to simultaneously achieve high energy and long cycle life.
Keywords:
all-solid-state lithium-metal battery
coulombic efficiency
lithiophobic/lithophilic interlayer
lithium dendrite suppression
mix-conductive interphase
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