Li10GeP2S12 (LGPS) is a new solid electrolyte of the highest Li ionic conductivity reported by now. Anisotropic 3D Li ionic transport network consisting of ultrafast Li 1D diffusion tunnel and fast in-plane 2D pathways were previously predicted by molecular dynamics simulations. In this paper, we have studied in detail the Li ion dynamics in LGPS by multiple solid-state NMR methods. Two different Li motion processes, characterized by apparently different activation energies of 0.16 eV and 0. 26 eV, were unambiguously probed by both 7 Li and 31 P solid-state NMR and assigned to Li ion diffusions in 1D tunnel and in 2D plane respectively. 31 P spin-locking relaxation measurement further reveals that interstitial position Li(4) is active for in-plane Li migration.
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