Electrochemical Response of Cold-Sintered Cathode-Hybrid Electrolyte Bilayers: Deep Insights into the Determining Kinetic Mechanisms via Operando Electrochemical Impedance Characterization

[EN] This study reports the fabrication of solid-state bilayers combining LiFePO4 (LFP) cathodes with Li1.3Al0.3Ti1.7(PO4)3 (LATP)-based composite solid electrolytes using a cold sintering process. By optimizing sintering pressure, intimate cathode–electrolyte contact is achieved, resulting in impro...

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Detalhes bibliográficos
Autores: Ferrer-Nicomedes, Sergio, Vicente-Agut, Nuria, Barba-Juan, Antonio, Garcia-Belmonte, Germà, Mormeneo-Segarra, Andrés|||0000-0002-8827-3649
Formato: artículo
Fecha de publicación:2025
País:España
Recursos:Universitat Politècnica de València (UPV)
Repositorio:RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia
Idioma:inglés
OAI Identifier:oai:riunet.upv.es:10251/230868
Acesso em linha:https://riunet.upv.es/handle/10251/230868
Access Level:acceso abierto
Palavra-chave:Solid-state batteries
LiFePO4 cathode
LATP solid electrolyte
Cold Sintering Process
Ionic conductivity
Capacity fading
Descrição
Resumo:[EN] This study reports the fabrication of solid-state bilayers combining LiFePO4 (LFP) cathodes with Li1.3Al0.3Ti1.7(PO4)3 (LATP)-based composite solid electrolytes using a cold sintering process. By optimizing sintering pressure, intimate cathode–electrolyte contact is achieved, resulting in improved electrochemical performance. Bilayers cold-sintered at 300 MPa and 150 degrees C show high ionic conductivity (about 0.5 mS cm-1) and stable room-temperature capacities (160.1 mAh g-1 of LFP at C/10 and 75.8 mAh g-1 of LFP at 1 C). Operando electrochemical impedance spectroscopy is used to identify kinetic limitations and predict overall behavior. The results indicate that capacity fading may occur at higher pressures due to volume contraction of the LFP crystal cell. Overall, the work highlights cold sintering as a simple route to high-performance solid-state bilayers and demonstrates operando EIS as a non-destructive tool to understand and mitigate degradation in solid-state lithium batteries.