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Lithium Thiosilicophosphate Glassy Solid Electrolytes Synthesized by High-Energy Ball-Milling and Melt-Quenching: Improved Suppression of Lithium Dendrite Growth by Si Doping.

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Due to the volatility of P2S5, the ambient pressure synthesis of Li2S + P2S5 (LPS) has been limited to planetary ball-milling (PBM). As a result, LPS doped with SiS2 has… Click to show full abstract

Due to the volatility of P2S5, the ambient pressure synthesis of Li2S + P2S5 (LPS) has been limited to planetary ball-milling (PBM). As a result, LPS doped with SiS2 has been studied because SiS2 lowers the vapor pressure of the melt and promotes strong glass formation which combined allows for greater ease in synthesis. In this work, we have examined the struc-tures and electrochemical properties of the lithium thiosilicophosphate (LTSP) 0.6 Li2S + 0.4 [x SiS2 + 1.5 (1-x) PS5/2] glassy solid electrolytes (GSEs) prepared by PBM and melt-quenching (MQ). It is shown that the critical current density (CCD) improved after incorporating SiS2, reaching 1.5 mA/cm2 for the x = 0.8 composition. However, the interfacial reaction of the MQed GSE with Lithium metal (LM) introduced micro-cracks, which shows a need to further explore more stable glass compositions. These fundamental results can help to understand the interface reaction and formation and as such can provide a guide to design improved GSEs with SiS2 as a glass former.

Keywords: ball milling; lithium thiosilicophosphate; melt quenching; lithium; solid electrolytes; glassy solid

Journal Title: ACS applied materials & interfaces
Year Published: 2019

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