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Solid–state batteries based on Li7La3Zr2O12 (LLZO) garnet electrolyte are a robust and safe alternative to conventional lithium‐ion batteries. However, the large‐scale implementation of ceramic composite cathodes is still challenging due to a complex multistep manufacturing process. A new one‐step route for the direct synthesis of LLZO during the manufacturing of LLZO/LiCoO2 (LCO) composite cathodes based on cheap precursors and utilizing the industrially established tape casting process is presented. It is shown that Al, Ta:LLZO can be formed directly in the presence of LCO from metal oxide precursors (LiOH, La2O3, ZrO2, Al2O3, and Ta2O5) by heating to 1050 °C, eliminating the time‐ and energy‐consuming synthesis of preformed LLZO powders. In addition, performance‐optimized gradient microstructures can be produced by sequential casting of slurries with different compositions, resulting in dense and flat phase‐pure cathodes without unwanted ion interdiffusion or secondary phase formation. Freestanding cathodes with a thickness of 85 µm, a relative density of 95%, and an industrial relevant LCO loading of 15 mg show an initial capacity of 82 mAh g−1 (63% of the theoretical capacity of LCO) in a solid‐state cell with Li metal anodes, which is comparable to conventional LCO/LLZO cathodes and can be further improved in the future. [ABSTRACT FROM AUTHOR]

Solid-state batteries (SSBs) are promising next-generation batteries due to their potential for achieving high energy densities and improved safety compared to conventional lithium-ion batteries (LIBs) with a flammable liquid electrolyte. Despite their huge market potential, very few studies have investigated SSB recycling processes to recover and reuse critical raw metals for a circular economy. For conventional LIBs, hydrometallurgical recycling has been proven to be able to produce high-quality products, with leaching being the first unit operation. Therefore, it is essential to establish a fundamental understanding of the leaching behavior of solid electrolytes as the key component of SSBs with different lixiviants. This work investigates the leaching of the most promising Al- and Ta-substituted Li7La3Zr2O12 (LLZO) solid electrolytes in mineral acids (H2SO4 and HCl), organic acids (formic, acetic, oxalic, and citric acid), and water. The leaching experiments were conducted using actual LLZO production waste in 1 M of acid at 1:20 S/L ratio at 25 °C for 24 h. The results showed that strong acids, such as H2SO4, almost completely dissolved LLZO. Encouraging selective leaching properties were observed with oxalic acid and water. This fundamental knowledge of LLZO leaching behavior will provide the basis for future optimization studies to develop innovative hydrometallurgical SSB recycling processes. [ABSTRACT FROM AUTHOR]

Oxide-ceramic based electrolytes such as Li 7 La 3 Zr 2 O 12 (LLZO), are one of the most promising solid electrolytes for application in all-solid-state batteries. However, most of its constituents are listed as critical raw materials, highlighting the need to minimize waste during synthesis and processing. Therefore, we investigated the re-use of aged LLZO powder and aged LLZO green foils produced by tape-casting, an industrial processing route suitable for ASSBs. We established a new synthesis route to fully recovery Li-poor LLZO and pyrochlore phase La 2 Zr 2 O 7 by simply adding a Li source during firing. By using recycled LLZO powder in a <200 μm thick cast tape, we were able to prove a similar ionic conductivity of 2.1 × 10−4 S cm−1 at room temperature and a critical current density of 0.75 mA cm−2 at 60 °C compared to fresh powder. This simple and efficient re-synthesis strategy might hold the potential to minimize waste streams of critical raw materials in future industrial production processes of solid-state batteries. • Investigation of re-use of production waste of the solid electrolyte Li 7 La 3 Zr 2 O 12. • Waste powder and tape loses Li and thus forms a pyrochlore phases. • A new processing route was developed to re-introduce the waste directly. • The performance was shown to be almost identical to freshly synthesized powders. • This approach minimizes waste of critical raw materials in future ASB production. [ABSTRACT FROM AUTHOR]

The presence of a nonoptically active polymorph (yellow‐phase) competing with the optically active polymorph (black γ‐phase) at room temperature in cesium tin iodide (CsSnI3) and the susceptibility of Sn to oxidation represent two of the biggest obstacles for the exploitation of CsSnI3 in optoelectronic devices. Here room‐temperature single‐source in vacuum deposition of smooth black γ −CsSnI3 thin films is reported. This is done by fabricating a solid target by completely solvent‐free mixing of CsI and SnI2 powders and isostatic pressing. By controlled laser ablation of the solid target on an arbitrary substrate at room temperature, the formation of CsSnI3 thin films with optimal optical properties is demonstrated. The films present a bandgap of 1.32 eV, a sharp absorption edge, and near‐infrared photoluminescence emission. These properties and X‐ray diffraction of the thin films confirm the formation of the orthorhombic (B‐γ) perovskite phase. The thermal stability of the phase is ensured by applying in situ an Al2O3 capping layer. This work demonstrates the potential of pulsed laser deposition as a volatility‐insensitive single‐source growth technique of halide perovskites and represents a critical step forward in the development and future scalability of inorganic lead‐free halide perovskites. [ABSTRACT FROM AUTHOR]