Abstract

Highly lithium ion conducting glass–ceramics in the system Li 2S P 2S 5 were successfully prepared by a heat treatment of the mechanochmically prepared sulfide glasses. The 80Li 2S·20P 2S 5 (mol.%) glass–ceramic mainly composed of the crystal analogous to the highly conductive thio-LISICON II phase in the system Li 4− x Ge 1− x P x S 4 showed conductivity as high as 10 −3 S cm −1 at room temperature. The 70Li 2S·30P 2S 5 glass–ceramic, in which the highly ion conductive new metastable phase was formed on heating, showed the highest conductivity of 3.2 × 10 −3 S cm −1 and the lowest activation energy of 12 kJ mol −1 for conduction. The all-solid-state battery In/80Li 2S·20P 2S 5 glass–ceramic/LiCoO 2 exhibited excellent cycling performance of over 500 times with no decrease in the charge–discharge capacity (100 mAh g −1). The SnS P 2S 5 glasses as active materials were mechanochemically prepared from SnS and P 2S 5. High performance of these glassy electrode materials was observed in the rechargeable cell of 80SnS·20P 2S 5/80Li 2S·20P 2S 5 glass–ceramic/LiCoO 2, in which a continuous sulfide network between electrode and electrolyte was successfully formed. The effects of conductive additives in composite electrodes on charge–discharge behavior of all-solid-state cells with Li 2S P 2S 5 glass–ceramics as a solid electrolyte were investigated. Under a current density over 1 mA cm −2, the cell with vapor grown carbon fiber kept larger discharge capacities during 50 cycles than the cell with acetylene black. The design of continuous electron conducting path from a point of view of morphology for conductive additives is important to improve cell performances of all-solid-state lithium secondary batteries.

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