Dissolution and Recrystallization Behavior of Li<sub>3</sub>PS<sub>4</sub> in Different Organic Solvents with a Focus on N-Methylformamide

Journal article (2023)

Authors

Kerstin Wissel Technische Universität Darmstadt
Luise M. Riegger Justus Liebig University Giessen
Wolfgang Ensinger Technische Universität Darmstadt
Oliver Clemens University of Stuttgart
Christian Schneider Max Planck Institute for Solid State Research
Aamir Iqbal Waidha Technische Universität Darmstadt
T. Famprikis RST/Storage of Electrochemical Energy - AS
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
Research Group
RST/Storage of Electrochemical Energy (AS) (TU Delft)
Copyright: © 2023 Kerstin Wissel, Luise M. Riegger, Christian Schneider, Aamir I. Waidha, T. Famprikis, Yuji Ikeda, Blazej Grabowski, Robert E. Dinnebier, Bettina V. Lotsch, Jürgen Janek, Wolfgang Ensinger, Oliver Clemens
DOI
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https://doi.org/10.1021/acsaem.2c03278
Recycling Recrystallization N-methylformamide Solvent treatment Thiophosphate Β-LiPS
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Published Date

2023

Language

English

Reuse Rights

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Faculty

Applied Sciences

Department

RST/Radiation, Science and Technology

Research Group

RST/Storage of Electrochemical Energy

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

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