Abstract

At present, fabrication of all-solid-state lithium-ion batteries using garnet-type electrolytes is still challenging due to issues with interfacial stability and interfacial impedance caused by the high-temperature sintering process. In this work, we employ Li2CO3 as additive to mitigate high-temperature side reactions and prepare an all-solid-state battery LNM|LLZT|LTO using spinel-structured LiNi0.5Mn1.5O4 (LNM) and Li4Ti5O12 (LTO) as electrodes and garnet-type Li6.4La3Zr1.4Ta0.6O12 (LLZT) as the electrolyte. The battery voltage reaches beyond 3 V and can be charged and discharged for 5 cycles at a rate of C/10. The three-electrode setup of the battery allows the separation of positive and negative electrodes in their voltage profiles and impedance responses during cycling. Our results suggest that the high-voltage electrode LNM can work with LLZT in a solid-state-battery configuration and the negative electrode is the performance-limiting component.

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