Abstract
Today, all-solid-state secondary lithium-ion batteries have attracted attention in research and development all over the world as a next-generation energy storage device. A key material for the all-solid-state lithium batteries is inorganic solid electrolyte, including oxide and sulfide materials. Among the oxide electrolytes, garnet-type oxide exhibits the highest lithium-ion conductivity and a wide electrochemical potential window. However, they have major problems for practical realization. One of the major problems is an internal short-circuit in charging and discharging. In the polycrystalline garnet-type oxide electrolyte, dendrites of lithium metal easily grow through the void or impurity in grain boundaries of the sintered body, which causes serious internal short-circuits in the battery system. To solve these problems, we present an all-solid-state battery system using a single-crystal oxide electrolyte. We are the first to successfully grow centimeter-sized single crystals of garnet-type by the floating zone method. The single-crystal solid electrolyte exhibits an extremely high lithium-ion conductivity of 10−3 S cm−1 at 298 K. The garnet-type single-crystal electrolyte has an advantageous bulk nature to realize the bulk conductivity without grain boundaries such as in a sintered polycrystalline body, and will be a game-changing technology for achieving highly safe advanced battery systems.
Highlights
Research and development on all-solid-state secondary lithium-ion batteries (LIBs) are being actively carried out as next-generation batteries in order to realize high energy density, high power density, and high safety[1,2,3]
In the polycrystalline garnet-type oxide electrolyte, lithium metal dendrites grow through the void or impurity in grain boundaries of the sintered body, which causes serious internal short-circuits in the battery system[9,10,12,21]
A detailed crystal structure analysis using single-crystal X-ray and single-crystal neutron diffraction data revealed that Li ions occupied two kinds of 96 h sites in the interspaces of the garnet-type framework structure
Summary
The short Li-Li distance, Li site disordering, and partial occupation of the Li atoms were reported as a key role of lithium ion diffusion in the garnet-type structure. This result suggests that the LLZNb05 single-crystal plate functions as a solid electrolyte and a separator without short-circuiting to 0.5 mA cm−2, and the lithium metal dissolution and deposition reaction repeats reversibly. The battery of this time has many problems because it consists only of active material for positive electrode, we think that many problems can be improved by combining solid electrolyte and conductive material
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