Abstract
Cyclable lithium batteries with a lithium metal anode are of great interest for future mobile and stationary applications due to their high potential energy density. To suppress lithium dendrite formation and growth, solid electrolytes (all‐solid‐state‐batteries) are an alternative for liquid electrolytes. Compared with all other solid electrolytes, the ceramic lithium garnet solid electrolyte Li7La3Zr2O12 (LLZO) features a high thermal, electrochemical, and chemical stability. Due to its nonflammable nature, it is beneficial for battery cell safety. Despite major research efforts, an industrially applicable process route to produce the ceramic solid electrolyte has not been identified yet. Herein, film fabrication at room temperature of Al0.2Li6.025La3Zr1.625Ta0.375O12 (ALLZTO) via powder aerosol deposition (PAD) on a scalable apparatus is investigated. In addition to the description of synthesis and process conditions regarding industrial scalability, the sprayed 30 μm‐thick PAD films are examined optically and electrochemically in half cells and symmetrical cells with lithium metal electrodes. By categorizing the process data and the electrochemical results compared with common reported production methods, a statement about the suitability for the industrial production of ceramic solid electrolytes using PAD is provided.
Highlights
As Powder Aerosol Deposition (PAD) is a promising technique to produce ceramic electrolytes for future lithium metal batteries, we describe the deposition method in detail and provide technical process data to compare the fabrication method to competing methods
The Al0.2Li6.025La3Zr1.625Ta0.375O12 powder was synthesized in the cubic garnet type structure at 1000 C, as shown in the Xray diffraction (XRD) pattern in Figure 2a, with two secondary phases
Considering that coating temperatures between 500 and 600 C will lead to insulating layers at cathode interfaces with a spinel structure,[77,78] films sprayed by the powder aerosol deposition method (PADM) and annealed at 400 C for 1 h show the highest reported ionic conductivity
Summary
Lithium metal batteries with solid-state electrolytes (SSEs) are of several hundred micrometers allows remarkable current densities of up to 6 mA cmÀ2 at 60 C with high solid electrolyte conductivities of up to 10À3 S cmÀ1 at room temperature, a compromising as electrochemical storage devices for future station- mercial industrial large-scale production with high throughput ary or mobile applications due to their potentially high specific energy density and increased safety compared with lithium-ion batteries with a liquid electrolyte.[1,2] Different types of polymer rates in combination with moisture-free processing is challenging.[9,10,11] Ideally, the thickness of the electrolyte should be in the range of 5–20 μm to reduce the risk of short circuits on the oneT. Much research has been conducted, the thickness range for LLZO films significantly
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