Abstract

All-solid-state batteries have gained significant attention as promising candidates to replace liquid electrolytes in lithium-ion batteries for high safety, energy storage performance, and stability under elevated temperature conditions. However, the low ionic conductivity and unsuitability of lithium metal in solid polymer electrolytes is a critical problem. To resolve this, we used a cubic garnet oxide electrolyte (Li7La3Zr2O12 – LLZO) and ionic liquid in combination with a polymer electrolyte to produce a composite electrolyte membrane. By applying a solid polymer electrolyte on symmetric stainless steel, the composite electrolyte membrane shows high ionic conductivity at elevated temperatures. The effect of LLZO in suppressing lithium dendrite growth within the composite electrolyte was confirmed through symmetric lithium stripping/plating tests under various current densities showing small polarization voltages. The full cell with lithium iron phosphate as the cathode active material achieved a highest specific capacity of 137.4 mAh g−1 and a high capacity retention of 98.47% after 100 cycles at a current density of 50 mA g−1 and a temperature of 60°C. Moreover, the specific discharge capacities were 137 and 100.8 mAh g−1 at current densities of 100 and 200 mA g−1, respectively. This research highlights the capability of solid polymer electrolytes to suppress the evolution of lithium dendrites and enhance the performance of all-solid-state batteries.

Highlights

  • Lithium-ion batteries (LIBs) currently play a principal role in energy storage technologies, having a wide range of applications from automotive vehicles to electronic devices, owing to their high energy density, ecological friendliness, fast charging time, and long cycle life (Abdin and Khalilpour, 2019)

  • The battery with PLL electrolyte exhibited outstanding performance with a high specific capacity of 137.4 mAh g−1 at the maximal point and 135.3 mAh g−1 after 100 cycles with 98.47% capacity retention at 50 mA g−1 current density

  • Cubic LLZO was prepared at a low temperature of 800◦C without any impurities and formed a homogeneous structure

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Summary

INTRODUCTION

Lithium-ion batteries (LIBs) currently play a principal role in energy storage technologies, having a wide range of applications from automotive vehicles to electronic devices, owing to their high energy density, ecological friendliness, fast charging time, and long cycle life (Abdin and Khalilpour, 2019). SPEs are typically operated at a high temperature (usually at 60◦C) to achieve good battery performance; under this condition, ionic conductivities can be low, and electrode/electrolyte interfacial resistances may increase To address this issue, ionic liquids can be used as crosslinks onto a PEO polymer matrix; this additive could improve the properties of SPEs, such as minimum volatilization, excellent thermal stability, extensive electrochemical stability window, and great ionic conductivity. The cathode-basis LFP was prepared by mixing LiFePO4, super-P, and PEO-LiTFSI (molar ratio of EO: Li = 8:1) as a binder, with a weight ratio of 8:1:1 This cathode was used to fabricate all-solid-state batteries operating at 60◦C with various SPEs, including PL and PLL, to compare the electrochemical properties of the electrolyte and determine the effect of LLZO within the electrolyte. The active material mass loading of LFP was ∼2 mg cm−2, and the lithium metal chip as anode (MTI Korea) was used with the thickness of 450 μm and the diameter of 16.0 mm

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DATA AVAILABILITY STATEMENT

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