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Reimagining interface processing in solid-state batteries via electrochemical flash sintering
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DOI：10.1039/D6TA00082G.png)
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Abstract
En 中文
Electrochemical flash sintering (EFS) is a newly developed; solvent-free technique for ultrafast (∼2 s) densification of lithium-containing solid-state battery materials. Unlike conventional flash sintering—which relies on uncontrolled thermal runaway and requires high electronic conductivity—EFS couples electronic conduction in mixed conductors with Li+ transport across interfaces with pure ionic conductors in composite or multilayer architectures. Using spatially resolved synchrotron total scattering and pair distribution function analysis; we elucidate the mechanisms of EFS; contrasting them with conventional flash sintering of single-phase materials. Under conventional conditions; Li3V2(PO4)3 (LVP) undergoes localized decomposition and cracking at low frequencies and high currents; while Li1.3Al0.3Ti1.7(PO4)3 (LATP) requires high frequencies to overcome blocking behavior—resulting in electrode melting; infiltration; and vitreous extrusion at the pellet perimeter. In contrast; EFS enables densification of LVP–LATP composites at lower frequencies that fail for either phase alone; with reactions confined to localized hotspots. In an LVP–LATP|LATP|LVP–LATP multilayer; decomposition products are more broadly distributed; including vanadium migration into the electrolyte; nonetheless; no preferential cracking or new phases were observed at electrode–electrolyte interfaces. These findings establish EFS as a viable one-step processing strategy for integrating (electro)chemically distinct phases and lay the groundwork for its broader adoption in the dry fabrication of solid-state electrochemical energy storage systems.
Keywords:
Electrochemical flash sintering
Solid-state batteries
Interface processing
Lithium-containing materials
Densification
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