Abstract

Composite solid electrolytes (CSEs), composed of sodium superionic conductor (NASICON)-type Li1+xAlxTi2-x(PO4)3 (LATP), poly (vinylidene fluoride-hexafluoro propylene) (PVDF-HFP), and lithium bis (trifluoromethanesulfonyl)imide (LiTFSI) salt, are designed and fabricated for lithium-metal batteries. The effects of the key design parameters (i.e., LiTFSI/LATP ratio, CSE thickness, and carbon content) on the specific capacity, coulombic efficiency, and cyclic stability were systematically investigated. The optimal CSE configuration, superior specific capacity (~160 mAh g-1), low electrode polarization (~0.12 V), and remarkable cyclic stability (a capacity retention of 86.8%) were achieved during extended cycling (>200 cycles). In addition, with the optimal CSE structure, a high ionic conductivity (~2.83 × 10-4 S cm-1) was demonstrated at an ambient temperature. The CSE configuration demonstrated in this work can be employed for designing highly durable CSEs with enhanced ionic conductivity and significantly reduced interfacial electrolyte/electrode resistance.

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