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Elucidating the Role of Microstructure in Thiophosphate Electrolytes – a Combined Experimental and Theoretical Study of β ‐Li 3 PS 4

Ates, Tugce 1; Neumann, Anton ; Danner, Timo ; Latz, Arnulf ; Zarrabeitia, Maider 1; Stepien, Dominik 1; Varzi, Alberto ORCID iD icon 1; Passerini, Stefano 2
1 Karlsruher Institut für Technologie (KIT)
2 Helmholtz-Institut Ulm (HIU), Karlsruher Institut für Technologie (KIT)

Abstract:

Solid-state batteries (SSBs) are promising candidates to significantly exceed the energy densities of today's state-of-the-art technology, lithium-ion batteries (LIBs). To enable this advancement, optimizing the solid electrolyte (SE) is the key. β-Li$_{3}$PS$_{4}$ (β-LPS) is the most studied member of the Li$_{2}$S-P$_{2}$S$_{5}$ family, offering promising properties for implementation in electric vehicles. In this work, the microstructure of this SE and how it influences the electrochemical performance are systematically investigated. To figure this out, four batches of β-LPS electrolyte with different particle size, shape, and porosity are investigated in detail. It is found that differences in pellet porosities mostly originate from single-particle intrinsic features and less from interparticle voids. Surprisingly, the β-LPS electrolyte pellets with the highest porosity and larger particle size not only show the highest ionic conductivity (up to 0.049 mS cm$^{-1}$ at RT), but also the most stable cycling performance in symmetrical Li cells. This behavior is traced back to the grain boundary resistance. Larger SE particles seem to be more attractive, as their grain boundary contribution is lower than that of denser pellets prepared using smaller β-LPS particles.


Verlagsausgabe §
DOI: 10.5445/IR/1000146026
Originalveröffentlichung
DOI: 10.1002/advs.202105234
Scopus
Zitationen: 7
Web of Science
Zitationen: 8
Dimensions
Zitationen: 8
Cover der Publikation
Zugehörige Institution(en) am KIT Helmholtz-Institut Ulm (HIU)
Publikationstyp Zeitschriftenaufsatz
Publikationsdatum 23.06.2022
Sprache Englisch
Identifikator ISSN: 2198-3844
KITopen-ID: 1000146026
HGF-Programm 38.02.01 (POF IV, LK 01) Fundamentals and Materials
Erschienen in Advanced Science
Verlag Wiley Open Access
Band 9
Heft 18
Seiten Art.Nr. 2105234
Bemerkung zur Veröffentlichung Gefördert durch den KIT-Publikationsfonds
Vorab online veröffentlicht am 24.04.2022
Nachgewiesen in Web of Science
Dimensions
Scopus
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