Abstract

All-solid-state batteries (ASSB) are considered promising candidates for future energy storage and advanced electric mobility. When compared to conventional Li-ion batteries, the substitution of Li-ion conductive, flammable liquids by a solid electrolyte and the application of Li-metal anodes substantially increase safety and energy density. The solid electrolyte Li1.3Al0.3Ti1.7(PO4)3 (LATP) provides high Li-ion conductivity of about 10−3 S/cm and is considered a highly promising candidate for both the solid electrolyte-separator and the ionically conductive part of the all-solid state composite cathode, consisting of the cathode material, the solid electrolyte, and an electron conductor. Co-sintering of the composite cathode is a sophisticated challenge, because temperatures above 1000 °C are typically required to achieve the maximum ionic conductivity of LATP but provoke reactions with the cathode material, inhibiting proper electrochemical functioning in the ASSB. In the present study, the application of sintering aids with different melting points and their impact on the sinterability and the conductivity of LATP were investigated by means of optical dilatometry and impedance spectroscopy. The microstructure of the samples was analyzed by SEM. The results indicate that the sintering temperature can be reduced below 800 °C while maintaining high ionic conductivity of up to 3.6 × 10−4 S/cm. These insights can be considered a crucial step forward towards enable LATP-based composite cathodes for future ASSB.

Highlights

  • All-solid-state batteries (ASSB) are considered as promising candidates for future energy storage and advanced electric mobility

  • We systematically investigated the reduction of the sintering temperature of solid electrolytes for ASSB with NASICON structure by the application of sintering aids, using the exemplary composition of Li1.3 Al0.3 Ti1.7 (PO4 )3 (LATP)

  • The sintering temperature was significantly reduced and the maximum shrinkage rate was enhanced for all mixtures of LATP with sintering aids when compared to pure LATP

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Summary

Introduction

All-solid-state batteries (ASSB) are considered as promising candidates for future energy storage and advanced electric mobility. Li-ion conductive, flammable liquids by a solid electrolyte and the application of Li-metal anodes substantially increase safety and energy density [1]. Currently used in mobile electronic devices and electric vehicles, the liquid electrolyte is substituted by a solid Li-ion conductor in the ASSB [2]. This includes a solid electrolyte-separator and the ionically conductive part of the all-solid state composite cathode, consisting of a cathode material, the solid electrolyte, and an electron conductor. Oxides are not affected by these restrictions and Crystals 2020, 10, 408; doi:10.3390/cryst10050408 www.mdpi.com/journal/crystals

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