Dissolution and Recrystallization Behavior of Li3PS4 in Different Organic Solvents with a Focus on N-Methylformamide

Kerstin Wissel; Luise M. Riegger; Christian Schneider; Aamir I. Waidha; Theodosios Famprikis; Yuji Ikeda; Blazej Grabowski; Robert E. Dinnebier; Bettina V. Lotsch; Jürgen Janek; Wolfgang Ensinger; Oliver Clemens

doi:10.1021/acsaem.2c03278

Dissolution and Recrystallization Behavior of Li₃PS₄ in Different Organic Solvents with a Focus on N-Methylformamide

Kerstin Wissel^*
, Luise M. Riegger
, Christian Schneider
, Aamir I. Waidha
, Theodosios Famprikis
, Yuji Ikeda
, Blazej Grabowski
, Robert E. Dinnebier
, Bettina V. Lotsch
, Jürgen Janek
, Wolfgang Ensinger
, Oliver Clemens

^*Corresponding author for this work

RST/Storage of Electrochemical Energy

Research output: Contribution to journal › Article › Scientific › peer-review

25 Citations (Scopus)

182 Downloads (Pure)

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

Original language	English
Pages (from-to)	7790-7802
Journal	ACS Applied Energy Materials
Volume	6
Issue number	15
DOIs	https://doi.org/10.1021/acsaem.2c03278
Publication status	Published - 2023

Bibliographical note

Green 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.

Keywords

N-methylformamide
recrystallization
recycling
solvent treatment
thiophosphate
β-LiPS

Access to Document

10.1021/acsaem.2c03278

acsaem.2c03278Final published version, 4.84 MB

Cite this

Wissel, K., Riegger, L. M., Schneider, C., Waidha, A. I., Famprikis, T., Ikeda, Y., Grabowski, B., Dinnebier, R. E., Lotsch, B. V., Janek, J., Ensinger, W., & Clemens, O. (2023). Dissolution and Recrystallization Behavior of Li₃PS₄ in Different Organic Solvents with a Focus on N-Methylformamide. ACS Applied Energy Materials, 6(15), 7790-7802. https://doi.org/10.1021/acsaem.2c03278

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title = "Dissolution and Recrystallization Behavior of Li3PS4 in Different Organic Solvents with a Focus on N-Methylformamide",

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",

keywords = "N-methylformamide, recrystallization, recycling, solvent treatment, thiophosphate, β-LiPS",

author = "Kerstin Wissel and Riegger, \{Luise M.\} and Christian Schneider and Waidha, \{Aamir I.\} and Theodosios Famprikis and Yuji Ikeda and Blazej Grabowski and Dinnebier, \{Robert E.\} and Lotsch, \{Bettina V.\} and J{\"u}rgen Janek and Wolfgang Ensinger and Oliver Clemens",

note = "Green 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.",

year = "2023",

doi = "10.1021/acsaem.2c03278",

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Wissel, K, Riegger, LM, Schneider, C, Waidha, AI, Famprikis, T, Ikeda, Y, Grabowski, B, Dinnebier, RE, Lotsch, BV, Janek, J, Ensinger, W & Clemens, O 2023, 'Dissolution and Recrystallization Behavior of Li₃PS₄ in Different Organic Solvents with a Focus on N-Methylformamide', ACS Applied Energy Materials, vol. 6, no. 15, pp. 7790-7802. https://doi.org/10.1021/acsaem.2c03278

TY - JOUR

T1 - Dissolution and Recrystallization Behavior of Li3PS4 in Different Organic Solvents with a Focus on N-Methylformamide

AU - Wissel, Kerstin

AU - Riegger, Luise M.

AU - Schneider, Christian

AU - Waidha, Aamir I.

AU - Famprikis, Theodosios

AU - Ikeda, Yuji

AU - Grabowski, Blazej

AU - Dinnebier, Robert E.

AU - Lotsch, Bettina V.

AU - Janek, Jürgen

AU - Ensinger, Wolfgang

AU - Clemens, Oliver

N1 - Green 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.

PY - 2023

Y1 - 2023

N2 - 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

AB - 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

KW - N-methylformamide

KW - recrystallization

KW - recycling

KW - solvent treatment

KW - thiophosphate

KW - β-LiPS

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M3 - Article

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