Lithium Ion Conducting Glasses and Glass-Ceramics in the Systems Li2S-MxSy (M=Al, Si and P) Prepared by Mechanical Milling

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Amorphous solid electrolytes in the system Li2S-Al2S3 were prepared by a mechanical milling technique for the first time. The 60Li2S•40AlS1.5 (mol%) amorphous solid electrolyte showed the maximum conductivity of 3.4×10-5 S cm-1 at room temperature in tablet shape. The Li2S-Al2S3 system proved to show lower conductivity than the Li2S-SiS2 and Li2S-P2S5 systems in an amorphous state because the latter two systems exhibited the conductivities of 10-4 S cm-1 at room temperature. Glass-ceramics in the system Li2S-Al2S3 were directly obtained by mechanical milling at a higher rotation speed, suggesting that glass-ceramic electrolytes as well as glassy ones were prepared by controlling the milling conditions. The crystal Li5AlS4 precipitated from the system Li2S-Al2S3 lowered the conductivity. On the contrary, the conductivity enhancement by crystallization was observed for the 67Li2S•33PS2.5 (mol%) glass and the obtained glass-ceramic exhibited high ambient temperature conductivity of about 10-3 S cm-1. The crystallization of a superionic crystal analogous to the thio-LISICON Li3.25Ge0.25P0.75S4 was responsible for the marked conductivity enhancement.
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