Preprint Article Version 1 Preserved in Portico This version is not peer-reviewed

Solid-State Lithium Batteries with Cathode-Supported Composite Solid Electrolytes Enabling High Rate Capability and Excellent Cyclic Performance

Version 1 : Received: 29 August 2023 / Approved: 29 August 2023 / Online: 30 August 2023 (04:45:13 CEST)

A peer-reviewed article of this Preprint also exists.

Chang, K.-F.; Panda, P.K.; Hsieh, C.-T.; Yang, P.-C.; Kataria, N.; Khoo, K.S. Solid-State Lithium Batteries with Cathode-Supported Composite Solid Electrolytes Enabling High-Rate Capability and Excellent Cyclic Performance. Batteries 2023, 9, 490. Chang, K.-F.; Panda, P.K.; Hsieh, C.-T.; Yang, P.-C.; Kataria, N.; Khoo, K.S. Solid-State Lithium Batteries with Cathode-Supported Composite Solid Electrolytes Enabling High-Rate Capability and Excellent Cyclic Performance. Batteries 2023, 9, 490.

Abstract

In this study, robust composite solid electrolytes were developed and employed them to enhance the performance of Li-metal batteries significantly. The robust composite solid electrolytes are composed of a soft polymer, poly(ethylene oxide), a Li salt, bis(trifluoromethanesulfonyl)imide (LiTFSI), and super ionic conductive ceramic fillers such as Li1.5Al0.5Ti1.5(PO4)3 (LATP), and Li6.4La3Zr1.4Ta0.6O12 (LLZTO). The main goal of this study is to enhance the electrochemical stability and ionic conductivity. The ionic conductivities of the composite solid electrolytes were found to be 2.08 × 10-4 and 1.64 × 10-4 S cm-1 with the introduction of LATP and LLZTO fillers, respectively. The results prove that the fabricated solid electrolyte was electrochemical stable at voltage exceeding 4.25 V vs. Li/Li+. The internal resistance of the solid electrolyte significantly reduced as compare to gel electrolyte. This reduction can be attributed owing to the alleviation of bulk electrolyte, charge-transfer, and interfacial electrolyte/electrode impedance. When LiFePO4 cathode sheets are coated with a composite solid electrolyte containing LATP powders, the resulting Li-metal battery displays high capacity at 5 C (with a capacity retention of 65.2% compared to the original capacity at 0.2 C) as well as superior cyclic stability and excellent Coulombic efficiency (> 99.5%, over 200 cycles). These results confirm that the composite solid electrolyte acts as a protective layer which have ability to prevent the growth of Li dendrites. Consequently, the fabricated electrolyte configuration can be engineered to enable high energy/power density and electrochemical stable cyclability in Li-metal batteries.

Keywords

LATP powders; Composite solid electrolytes; Garnet-type powders; LLZTO powders; Lithium metal batteries

Subject

Engineering, Chemical Engineering

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