All-Solid-State Batteries (ASSBs) that use oxide-based solid electrolytes (SEs) have been considered as a promising energy-storage platform to meet an increasing demand for Li-ion batteries (LIBs) with improved energy density and superior safety. However, high interfacial resistance between particles in the composite electrode and between electrodes and the use of Li metal in the ASBS hinder their practical utilization. Here, we review recent research progress on oxide-based SEs for the ASSBs with respect to the use of Li metal. We especially focus on research progress on garnet-type solid electrolytes (Li
7
La
3
Zr
2
O
12
) because they have high ionic conductivity, good chemical stability with Li metal, and a wide electrochemical potential window. This review will also discuss Li dendritic behavior in the oxide-based SEs and its relationship with critical current density (CCD). We close with remarks on prospects of ASSB.
Here, we, for the first time, report on the simultaneous enhancement in cubic phase stability and Li-ion conductivity of garnettype solid electrolytes (SEs) by adding excess Li/Al. The excess Al/Li creates very large grains of up to 170 μm via the segregation of Al at the grain boundaries and enables preferential Al occupation at 96h sites over 24d sites, a behavior contrary to previous observations. The resulting SE shows improved Li-ion conductivity due to the large grain size and less blocking Li pathway caused by different preferential Al occupation. Surprisingly, it is observed that the cubic phase of the garnet-type SE is transformed to the tetragonal phase on the surface and in the bulk under the applied voltage, and the preferential Al occupation enables its cubic phase stability. Under battery operating conditions, the LLZO SE with excess Li/Al can maintain high ionic conductivity due to the cubic phase stability and large grain size. We clearly demonstrate that the cubic phase stability and ionic conductivity of LLZO can be simultaneously improved by excess Li/Al without any post-treatments. The findings and understanding will provide new insights into practical use of the garnet-type SEs for advanced all solid-state batteries.
Since the electrification of vehicles has been extended, solid-state batteries have been attracting a lot of interest because of their superior safety. Especially, polymer, sulfide, and oxide based materials are being studied as solid electrolytes, and each type of materials has advantaged and disadvantages over others. Oxide electrolytes has higher chemical and electrochemical stability compared to the other types of electrolytes. However, ionic conductivity isn't high enough as much as that of organic liquid electrolytes. Also, there are many difficulties of fabricating solidstate batteries with oxide based electrolytes because they require a sintering process at very high temperature (above ~800 ℃). Herein, we review recent studies of solid-state batteries with oxide based electrolytes about the ionic conductivity, interfacial reactions with Li metal, and preparation of solid-state cell.
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