Abstract

We demonstrate that the Li-ion conductivity can be improved by adding a certain amount of Li (x = 0.25–0.5) as a charge carrier to the composition of glass-ceramic Li7+xP3S11. Structural analysis clarified that the structural changes caused by the ratio of ortho-thiophosphate tetrahedra PS43− and pyro-thiophosphate ditetrahedra P2S74− affect the Li-ion conductivity. The ratio of PS43− and P2S74− varies depending on x and the highest Li-ion conductivity (2.5 × 10−3 S cm−1) at x = 0.25. All-solid-state LiNi0.8Co0.15Al0.05O2/Li7.25P3S11/In-metal cell exhibits the discharge capacity of 106.2 mAh g−1. This ion conduction enhancement from excess Li is expected to contribute to the future design of sulfide-type electrolytes.

Highlights

  • The recent explosion of demand for mobile electronic devices such as cell phones and laptop computers has led to the era of Li-ion batteries using organic liquid electrolytes.[1,2,3] despite the good conductivity of Li-ions, organic liquid electrolytes have limitations such as ignition hazards, low specific energy density, and low voltage.[4,5,6,7,8,9] advanced electrolyte technology is required for next-generation automobiles including hybrids, plug-in hybrids, and electric vehicles, which require batteries with high safety, high specific energy density, and high voltage.[10]

  • There have been recent reports related to Li2S–P2S5 (LPS)-based sulfides with Li-ion conductivity of 1 × 10 2 S cm 1, which is equal to or higher than that of liquid electrolytes

  • In 2011, the Li10GeP2S12 crystal structure was obtained by melt-quenching the raw materials Li2S, P2S5, and GeS2 at a molar ratio of 5/1/1 and showed a high bulk ion conductivity of 1.2 × 10 2 S cm 1 at ambient temperatures

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Summary

Introduction

The recent explosion of demand for mobile electronic devices such as cell phones and laptop computers has led to the era of Li-ion batteries using organic liquid electrolytes.[1,2,3] despite the good conductivity of Li-ions, organic liquid electrolytes have limitations such as ignition hazards, low specific energy density, and low voltage.[4,5,6,7,8,9] advanced electrolyte technology is required for next-generation automobiles including hybrids, plug-in hybrids, and electric vehicles, which require batteries with high safety, high specific energy density, and high voltage.[10]. Configuring PSx tetrahedral clusters in Li-excess Li7P3S11 solid electrolyte In 2011, the Li10GeP2S12 crystal structure was obtained by melt-quenching the raw materials Li2S, P2S5, and GeS2 at a molar ratio of 5/1/1 and showed a high bulk ion conductivity of 1.2 × 10 2 S cm 1 at ambient temperatures.

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