As the most promising candidate of the solid electrolyte materials for future lithium batteries, oxide electrolytes with highlithium-ion conductivity have experienced a rapid development in the past few decades. Existing oxide electrolytes are divided into two groups, i.e., crystalline group including NASICON, perovskite, garnet, and some newly developing structures, and amorphous/glass group including Li 2 O-MO x (M = Si, B, P, etc.) and LiPON-related materials. After a historical perspective on the general development of oxide electrolytes, we try to give a comprehensive review on the oxide electrolytes with high-lithium-ion conductivity, with special emphasis on the aspect of materials selection and design for applications as solid electrolytes in lithium batteries. Some successful examples and meaningful attempts on the incorporation of oxide electrolytes in lithium batteries are also presented. In the conclusion part, an outlook for the future direction of oxide electrolytes development is given.

All-solid-state bulk-type lithium ion batteries (LIBs) are considered ultimate solutions to the safety issues associated with conventional LIBs using flammable liquid electrolyte. The development of bulk-type all-solid-state LIBs has been hindered by the low loading of active cathode materials, hence low specific surface capacity, and by the high interface resistance, which results in low rate and cyclic performance. In this contribution, we propose and demonstrate a synergistic all-composite approach to fabricating flexible all-solid-state LIBs. PEO-based composite cathode layers (filled with LiFePO particles) of ∼300 μm in thickness and composite electrolyte layers (filled with Al-LLZTO particles) are stacked layer-by-layer with lithium foils as negative layer and hot-pressed into a monolithic all-solid-state LIB. The flexible LIB delivers a high specific discharge capacity of 155 mAh/g, which corresponds to an ultrahigh surface capacity of 10.8 mAh/cm, exhibits excellent capacity retention up to at least 10 cycles and could work properly under harsh operating conditions such as bending or being sectioned into pieces. The all-composite approach is favorable for improving both mesoscopic and microscopic interfaces inside the all-solid-state LIB and may provide a new toolbox for design and fabrication of all-solid-state LIBs.

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Highly Li-ion conductive 78LiS-22PS glass-ceramic electrolytes were prepared by simple heat treatment of the glass phase obtained via mechanical ball milling. A high ionic conductivity of ∼1.78 × 10 S cm is achieved at room temperature and is attributed to the formation of a crystalline phase of high lithium-ion conduction. All-solid-state lithium-ion batteries based on these glass-ceramic electrolytes are assembled by using LiS nanoparticles or low-cost commercially available FeS as active cathode materials and Li-In alloys as anode. A high discharge capacity of 535 mAh g is achieved after at least 50 cycles for the all-solid-state cells with LiS as cathode materials, suggesting a rather high capacity retention of 97.4%. Even for the cells using low-cost FeS as cathode materials, same high discharge capacity of 560 mAh g is also achieved after at least 50 cycles. Moreover, the Coulombic efficiency remain at ∼99% for these all-solid-state cells during the charge-discharge cycles.

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