Aqueous Processing of LiCoO2–Li6.6La3Zr1.6Ta0.4O12 Composite Cathode for High-Capacity Solid-State Lithium Batteries

Ye, Ruijie; Ihrig, Martin; Figgemeier, Egbert; Fattakhova‐Rohlfing, Dina; Finsterbusch, Martin

doi:10.1021/acssuschemeng.2c07556

Cited by 7 publications

(3 citation statements)

References 56 publications

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“…We suspect the reported self-discharge and/or poor Coulombic efficiency of LLZTO/LCO batteries at elevated temperatures are initiated by the spontaneous lithium migration discussed above. , Kim et al fabricated a Li/LLZO/LCO cell using two types of LLZO and measured the open circuit voltage after charging the cell to 4.05 V. Even with the improved electrochemical properties, the cell voltage continuously dropped for 2 h . Ye et al fabricated a LCO/LLZO composite cathode via a tape casting process and cycled the cell at 60 °C.…”

Section: Resultsmentioning

confidence: 99%

Trigger of the Highly Resistive Layer Formation at the Cathode–Electrolyte Interface in All-Solid-State Lithium Batteries Using a Garnet-Type Lithium-Ion Conductor

Onoue,

Nasu,

Matsumoto

et al. 2023

ACS Appl. Mater. Interfaces

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Interfacial materials design is critical in the development of all-solid-state lithium batteries. We must develop an electrode–electrolyte interface with low resistance and effectively utilize the energy stored in the battery system. Here, we investigated the highly resistive layer formation process at the interface of a layered cathode: LiCoO2, and a garnet-type solid-state electrolyte: Li6.4La3Zr1.4Ta0.6O12, during the cosintering process using in situ/ex situ high-temperature X-ray diffraction. The onset temperature of the reaction between a lithium-deficient Li x CoO2 and Li6.4La3Zr1.4Ta0.6O12 is 60 °C, while a stoichiometric LiCoO2 does not show any reaction up to 900 °C. The chemical potential gap of lithium first triggers the lithium migration from the garnet phase to the Li x CoO2 below 200 °C. The lithium-extracted garnet gradually decomposes around 200 °C and mostly disappears at 500 °C. Since the interdiffusion of the transition metal is not observed below 500 °C, the early-stage reaction product is the decomposed lithium-deficient garnet phase. Electrochemical impedance spectroscopy results showed that the highly resistive layer is formed even below 200 °C. The present work offers that the origin of the highly resistive layer formation is triggered by lithium migration at the solid–solid interface and decomposition of the lithium-deficient garnet phase. We must prevent spontaneous lithium migration at the cathode–electrolyte interface to avoid a highly resistive layer formation. Our results show that the lithium chemical potential gap should be the critical parameter for designing an ideal solid–solid interface for all-solid-state battery applications.

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Section: Resultsmentioning

confidence: 99%

Trigger of the Highly Resistive Layer Formation at the Cathode–Electrolyte Interface in All-Solid-State Lithium Batteries Using a Garnet-Type Lithium-Ion Conductor

Onoue,

Nasu,

Matsumoto

et al. 2023

ACS Appl. Mater. Interfaces

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“…This microstructure was observed experimentally for the ceramic LCO-LLZO composite cathodes fabricated by various methods, e.g., screen-printed cathodes 25 or tape-cast free-standing cathodes. 26,27 Similar to LCO, NCM is also a hexagonal layered oxide with comparable size and shape of the commercial powders, so replacing LCO with NCM powders should not signicantly affect the microstructure of composite cathodes. This was conrmed by a very similar microstructure of screen-printed NCM-LLZO cathodes, which have comparable relative density and porosity to the LCO-LZO cathodes.…”

Section: Microstructurementioning

confidence: 99%

Modelling electro-chemically induced stresses in all-solid-state batteries: screening electrolyte and cathode materials in composite cathodes

Mücke,

Yaqoob,

Finsterbusch

et al. 2023

J. Mater. Chem. A

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“…The use of LATP in various battery designs has been demonstrated by numerous groups, and the number of publications is steadily increasing. − LATP has been successfully used in hybrid systems in combination with polymers to produce separators , and as a solid electrolyte in solid-state cells in combination with inorganic cathode active materials (CAMs). , Even some fully inorganic LATP-based solid-state battery concepts have already been commercialized. , …”

Section: Introductionmentioning

confidence: 99%

Enabling High-Performance Hybrid Solid-State Batteries by Improving the Microstructure of Free-Standing LATP/LFP Composite Cathodes

Ihrig,

Dashjav,

Odenwald

et al. 2024

ACS Appl. Mater. Interfaces

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The phosphate lithium-ion conductor Li 1.5 Al 0.5 Ti 1.5 (PO 4 ) 3 (LATP) is an economically attractive solid electrolyte for the fabrication of safe and robust solid-state batteries, but high sintering temperatures pose a material engineering challenge for the fabrication of cell components. In particular, the high surface roughness of composite cathodes resulting from enhanced crystal growth is detrimental to their integration into cells with practical energy density. In this work, we demonstrate that efficient freestanding ceramic cathodes of LATP and LiFePO 4 (LFP) can be produced by using a scalable tape casting process. This is achieved by adding 5 wt % of Li 2 WO 4 (LWO) to the casting slurry and optimizing the fabrication process. LWO lowers the sintering temperature without affecting the phase composition of the materials, resulting in mechanically stable, electronically conductive, and free-standing cathodes with a smooth, homogeneous surface. The optimized cathode microstructure enables the deposition of a thin polymer separator attached to the Li metal anode to produce a cell with good volumetric and gravimetric energy densities of 289 Wh dm −3 and 180 Wh kg −1 , respectively, on the cell level and Coulombic efficiency above 99% after 30 cycles at 30 °C.

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Aqueous Processing of LiCoO₂–Li_6.6La₃Zr_1.6Ta_0.4O₁₂ Composite Cathode for High-Capacity Solid-State Lithium Batteries

Cited by 7 publications

References 56 publications

Trigger of the Highly Resistive Layer Formation at the Cathode–Electrolyte Interface in All-Solid-State Lithium Batteries Using a Garnet-Type Lithium-Ion Conductor

Trigger of the Highly Resistive Layer Formation at the Cathode–Electrolyte Interface in All-Solid-State Lithium Batteries Using a Garnet-Type Lithium-Ion Conductor

Modelling electro-chemically induced stresses in all-solid-state batteries: screening electrolyte and cathode materials in composite cathodes

Enabling High-Performance Hybrid Solid-State Batteries by Improving the Microstructure of Free-Standing LATP/LFP Composite Cathodes

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