TY - JOUR
T1 - Solid Electrolytes: Extremely Fast Charge Carriers in Garnet-Type Li6La3ZrTaO12 Single Crystals
AU - Stanje, Bernhard
AU - Rettenwander, Daniel
AU - Breuer, Stefan
AU - Uitz, Marlena
AU - Berendts, Stefan
AU - Lerch, Martin
AU - Uecker, Reinhard
AU - Redhammer, Günther J.
AU - Hanzu, Ilie
AU - Wilkening, Martin
PY - 2017/9
Y1 - 2017/9
N2 - 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 ionicconductivities. Considering ceramic oxides, garnet-type Li7La3Zr2O12andderivatives, see Zr-exchanged Li6La3ZrTaO12(LLZTO), have attracted greatattention due to its high Li+ionic conductivity of 10−3Scm−1at ambienttemperature. Despite numerous studies focussing on conductivities ofpowder samples, only few use time-domain NMR methods to probe Li iondiffusion parameters in single crystals. Here we report ontemperature-variable NMR relaxometry measurements using both laboratoryand spin-lock techniques to probe Li jump rates covering a dynamic timewindow spanning several decades. Both techniques revealed a consistentpicture of correlated Li ion jump diffusion in the single crystal; the dataperfectly mirror a modified BPP-type relaxation response being based on aLorentzian-shaped relaxation function. The rates measured could beparameterized with a single set of diffusion parameters. Results from NMRare completely in line with ion transport parameters derived from conductivityspectroscopy.
AB - 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 ionicconductivities. Considering ceramic oxides, garnet-type Li7La3Zr2O12andderivatives, see Zr-exchanged Li6La3ZrTaO12(LLZTO), have attracted greatattention due to its high Li+ionic conductivity of 10−3Scm−1at ambienttemperature. Despite numerous studies focussing on conductivities ofpowder samples, only few use time-domain NMR methods to probe Li iondiffusion parameters in single crystals. Here we report ontemperature-variable NMR relaxometry measurements using both laboratoryand spin-lock techniques to probe Li jump rates covering a dynamic timewindow spanning several decades. Both techniques revealed a consistentpicture of correlated Li ion jump diffusion in the single crystal; the dataperfectly mirror a modified BPP-type relaxation response being based on aLorentzian-shaped relaxation function. The rates measured could beparameterized with a single set of diffusion parameters. Results from NMRare completely in line with ion transport parameters derived from conductivityspectroscopy.
U2 - 10.1002/andp.201700140
DO - 10.1002/andp.201700140
M3 - Article
VL - 529
JO - Annalen der Physik
JF - Annalen der Physik
SN - 0003-3804
IS - 12
M1 - 1700140
ER -
