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Solid Electrolytes: Extremely Fast Charge Carriers in Garnet‐Type Li 6 La 3 ZrTaO 12 Single Crystals
Author(s) -
Stanje Bernhard,
Rettenwander Daniel,
Breuer Stefan,
Uitz Marlena,
Berendts Stefan,
Lerch Martin,
Uecker Reinhard,
Redhammer Günther,
Hanzu Ilie,
Wilkening Martin
Publication year - 2017
Publication title -
annalen der physik
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.009
H-Index - 68
eISSN - 1521-3889
pISSN - 0003-3804
DOI - 10.1002/andp.201700140
Subject(s) - ionic conductivity , materials science , ion , diffusion , fast ion conductor , conductivity , relaxation (psychology) , electrolyte , ionic bonding , analytical chemistry (journal) , lithium (medication) , chemistry , thermodynamics , physics , electrode , medicine , psychology , social psychology , organic chemistry , chromatography , endocrinology
Abstract The development of all‐solid‐state electrochemical energy storage systems, such as lithium‐ion batteries with solid electrolytes, requires stable, electronically insulating compounds with exceptionally high ionic conductivities. Considering ceramic oxides, garnet‐type Li7 La3 Zr2 O12 and derivatives, see Zr‐exchanged Li6 La3 ZrTaO12 (LLZTO), have attracted great attention due to its high Li + ionic conductivity of 10− 3 S cm− 1at ambient temperature. Despite numerous studies focussing on conductivities of powder samples, only few use time‐domain NMR methods to probe Li ion diffusion parameters in single crystals. Here we report on temperature‐variable NMR relaxometry measurements using both laboratory and spin‐lock techniques to probe Li jump rates covering a dynamic time window spanning several decades. Both techniques revealed a consistent picture of correlated Li ion jump diffusion in the single crystal; the data perfectly mirror a modified BPP‐type relaxation response being based on a Lorentzian‐shaped relaxation function. The rates measured could be parameterized with a single set of diffusion parameters. Results from NMR are completely in line with ion transport parameters derived from conductivity spectroscopy.