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High‐Entropy Lithium Argyrodite Solid Electrolytes Enabling Stable All‐Solid‐State Batteries

Li, Shenghao; Lin, Jing 1; Schaller, Mareen 2; Indris, Sylvio ORCID iD icon 2; Zhang, Xin; Brezesinski, Torsten ORCID iD icon 1; Nan, Ce-Wen; Wang, Shuo ; 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 solid electrolytes (SEs) are essential for bulk-type solid-state battery (SSB) applications. Multicomponent SEs are recently attracting attention for their favorable charge-transport properties, however a thorough understanding of how configurational entropy (ΔSconf) affects ionic conductivity is lacking. Here, we successfully synthesized a series of halogen-rich lithium argyrodites with the general formula Li5.5PS4.5ClxBr1.5-x (0≤x≤1.5). Using neutron powder diffraction and 31P magic-angle spinning nuclear magnetic resonance spectroscopy, the S2−/Cl−/Br− occupancy on the anion sublattice was quantitatively analyzed. We show that disorder positively affects Li-ion dynamics, leading to a room-temperature ionic conductivity of 22.7 mS cm−1 (9.6 mS cm−1 in cold-pressed state) for Li5.5PS4.5Cl0.8Br0.7 (ΔSconf=1.98R). To the best of our knowledge, this is the first experimental evidence that configurational entropy of the anion sublattice correlates with ion mobility. Our results indicate the possibility of improving ionic conductivity in ceramic ion conductors by tailoring the degree of compositional complexity. Moreover, the Li5.5PS4.5Cl0.8Br0.7 SE allowed for stable cycling of single-crystal LiNi0.9Co0.06Mn0.04O2 (s-NCM90) composite cathodes in SSB cells, emphasizing that dual-substituted lithium argyrodites hold great promise in enabling high-performance electrochemical energy storage.


Verlagsausgabe §
DOI: 10.5445/IR/1000164713
Veröffentlicht am 21.11.2023
Originalveröffentlichung
DOI: 10.1002/anie.202314155
Scopus
Zitationen: 31
Web of Science
Zitationen: 19
Dimensions
Zitationen: 33
Cover der Publikation
Zugehörige Institution(en) am KIT Institut für Angewandte Materialien – Energiespeichersysteme (IAM-ESS)
Institut für Nanotechnologie (INT)
Publikationstyp Zeitschriftenaufsatz
Publikationsjahr 2023
Sprache Englisch
Identifikator ISSN: 1433-7851, 1521-3773
KITopen-ID: 1000164713
HGF-Programm 38.02.01 (POF IV, LK 01) Fundamentals and Materials
Erschienen in Angewandte Chemie International Edition
Verlag John Wiley and Sons
Band 62
Heft 50
Seiten Art.Nr.: e202314155
Vorab online veröffentlicht am 30.10.2023
Nachgewiesen in Scopus
Dimensions
Web of Science
Globale Ziele für nachhaltige Entwicklung Ziel 7 – Bezahlbare und saubere Energie
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