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Synthetic Tailoring of Ionic Conductivity in Multicationic Substituted, High‐Entropy Lithium Argyrodite Solid Electrolytes

Lin, Jing 1; Schaller, Mareen 2; Cherkashinin, Gennady; Indris, Sylvio ORCID iD icon 2; Du, Jianxuan 1; Ritter, Clemens; Kondrakov, Aleksandr 1; Janek, Jürgen 1; Brezesinski, Torsten ORCID iD icon 1; Strauss, Florian 1
1 Institut für Nanotechnologie (INT), Karlsruher Institut für Technologie (KIT)
2 Institut für Angewandte Materialien – Energiespeichersysteme (IAM-ESS), Karlsruher Institut für Technologie (KIT)

Abstract:

Superionic conductors are key components of solid-state batteries (SSBs). Multicomponent or high-entropy materials, offering a vast compositional space for tailoring properties, have recently attracted attention as novel solid electrolytes (SEs). However, the influence of synthetic parameters on ionic conductivity in compositionally complex SEs has not yet been investigated. Herein, the effect of cooling rate after high-temperature annealing on charge transport in the multicationic substituted lithium argyrodite Li6.5[P0.25Si0.25Ge0.25Sb0.25]S5I is reported. It is demonstrated that a room-temperature ionic conductivity of ∼12 mS cm−1 can be achieved upon cooling at a moderate rate, superior to that of fast- and slow-cooled samples. To rationalize the findings, the material is probed using powder diffraction, nuclear magnetic resonance and X-ray photoelectron spectroscopy combined with electrochemical methods. In the case of moderate cooling rate, favorable structural (bulk) and compositional (surface) characteristics for lithium diffusion evolve. Li6.5[P0.25Si0.25Ge0.25Sb0.25]S5I is also electrochemically tested in pellet-type SSBs with a layered Ni-rich oxide cathode. ... mehr


Verlagsausgabe §
DOI: 10.5445/IR/1000165022
Veröffentlicht am 28.11.2023
Originalveröffentlichung
DOI: 10.1002/smll.202306832
Scopus
Zitationen: 9
Web of Science
Zitationen: 7
Dimensions
Zitationen: 11
Cover der Publikation
Zugehörige Institution(en) am KIT Institut für Angewandte Materialien – Energiespeichersysteme (IAM-ESS)
Institut für Nanotechnologie (INT)
Publikationstyp Zeitschriftenaufsatz
Publikationsjahr 2024
Sprache Englisch
Identifikator ISSN: 1613-6810, 1613-6829
KITopen-ID: 1000165022
HGF-Programm 38.02.01 (POF IV, LK 01) Fundamentals and Materials
Erschienen in Small
Verlag John Wiley and Sons
Band 20
Heft 15
Seiten Art.-Nr.: 2306832
Vorab online veröffentlicht am 27.11.2023
Nachgewiesen in Dimensions
Scopus
Web of Science
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