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Dissolution and Recrystallization Behavior of Li<sub>3</sub>PS<sub>4</sub> in Different Organic Solvents with a Focus on N-Methylformamide
Solid-state batteries can be built based on thiophosphate electrolytes such as β-Li3PS4. For the preparation of these solid electrolytes, various solvent-based routes have been reported. For recycling of end-of-life solid-state batteries based on such thiophosphates, we consider the development of dissolution and recrystallization strategies for the recovery of the model compound β-Li3PS4. We show that recrystallization can only be performed in polar, slightly protic solvents such as N-methylformamide (NMF). The recrystallization is comprehensively studied, showing that it proceeds via an intermediate phase with composition Li3PS4·2NMF, which is structurally characterized. This phase has a high resistivity for the transport of lithium ions and must be removed in order to obtain a recrystallized product with a conductivity similar to the pristine material. Moreover, the recrystallization from solution results in an increase of the amorphous phase fraction next to crystalline β-Li3PS4Green Open Access added to TU Delft Institutional Repository 'You share, we take care!' - Taverne project https://www.openaccess.nl/en/you-share-we-take-care Otherwise as indicated in the copyright section: the publisher is the copyright holder of this work and the author uses the Dutch legislation to make this work public.RST/Storage of Electrochemical Energ