Dissolution and Recrystallization Behavior of Li3PS4 in Different Organic Solvents with a Focus on N-Methylformamide
Kerstin Wissel (Technische Universität Darmstadt)
Luise M. Riegger (Justus Liebig University Giessen)
Christian Schneider (Max Planck Institute for Solid State Research)
Aamir I. Waidha (Technische Universität Darmstadt)
Theodosios Famprikis (TU Delft - RST/Storage of Electrochemical Energy)
Yuji Ikeda (University of Stuttgart)
Blazej Grabowski (University of Stuttgart)
Robert E. Dinnebier (Max Planck Institute for Solid State Research)
Bettina V. Lotsch (Ludwig Maximilians University, Max Planck Institute for Solid State Research)
Jürgen Janek (Justus Liebig University Giessen)
Wolfgang Ensinger (Technische Universität Darmstadt)
Oliver Clemens (University of Stuttgart)
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Abstract
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-Li3PS4