Ionic Percolation through Low-Temperature Densification of Glass-Ceramic LAGP Electrolytes for All-Solid-State Batteries
Marc Bertrand a, Steeve Rousselot a, Maxime Rioux a, David Aymé-Perrot b, Mickael Dolle a
a Université de Montréal, Avenue Thérèse-Lavoie-Roux, 1375, Montréal, Canada
b TotalEnergies OneTech SE, 2 Place Jean Millier, 92078 Paris La Défense Cedex, France
Proceedings of 24th International Conference on Solid State Ionics (SSI24)
Fundamentals: Experiment and simulation
London, United Kingdom, 2024 July 14th - 19th
Organizers: John Kilner and Stephen Skinner
Oral, Marc Bertrand, presentation 259
Publication date: 10th April 2024

In developing all-solid-state batteries with oxide-based materials, the densification of ceramic electrolytes (CE) is a key step to allow circulation of lithium ions. Traditional sintering techniques require high temperatures that often lead to unwanted interactions between the CE and active materials, undermining battery performance.

This research presents an alternative approach using the glass-forming abilities of certain CEs that can facilitate sintering at lower temperatures. When glass is heated above its glass transition temperature, it transforms into a viscous phase that allows for simultaneous densification and crystallization. If the glass transition temperature and crystallization temperature are lower than the sintering temperature, the resulting thermal treatment leads to a more conductive and denser CE compared to an already crystallized one subjected to the same treatment. We use a Nasicon-type ceramic electrolyte—specifically, Li1.5Al0.5Ge1.5(PO4)3 (LAGP)—to explore this method.

The study investigates the crystallization behavior of LAGP and its impact on ionic conductivity. Our results demonstrate an improvement in the density and conductive properties of the glass-ceramic electrolyte with a significatively lower temperature treatment. Moreover, X-ray diffraction techniques are employed to monitor the progression of crystallinity, revealing that an autocatalytic nucleation process allows for earlier lithium-ion pathway creation.

This finding provides meaningful insights into the production of ASSBs that could avoid the drawbacks of high-temperature assembly.

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