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Ion-conducting garnets are important candidates for use in all-solid Li batteries and numerous materials have been synthesized with high ionic conductivities. For understanding ion conduction mechanisms, knowledge on Li + diffusion behaviour is essential. The proposed nano-scale lithium pathways are composed of tortuous and narrow Li + channels. The pulsed gradient spin-echo (PGSE) NMR method provides time-dependent 7 Li diffusion on the micrometre space. For powder samples, collision-diffraction echo-attenuation plots were observed in a short observation time, which had not been fully explained. The diffraction patterns were reduced or disappeared for single-crystal garnet samples of Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 (LLZO-Ta) and Li 6.5 La 3 Zr 1.5 Nb 0.5 O 12 (LLZO-Nb). The inner morphology and grain boundaries affect importantly the collision-diffraction behaviours which is inherent to powder samples. The 7 Li diffusion observed by PGSE-NMR depends on the observation time (Δ) and the pulsed field gradient (PFG) strength (g) in both powder and single-crystal samples, and the anomalous effects were reduced in the single-crystal samples. The scattered Li diffusion constants converged to a unique value (D Li ) with a long Δ and a large g, which is eventually the smallest value. The D Li activation energy was close to that of the ionic conductivity (σ). The D Li values are plotted versus the σ values measured for four powder and two single-crystal garnet samples. Assuming the Nernst-Einstein (NE) relation which was derived for isolated ions in solution, the carrier numbers (N NE ) were estimated from the experimental values of D Li and σ. The N NE values of metal-containing garnets were large (&lt;10 23 cm -3 ) and insensitive to temperature. They were larger than Li atomic numbers in cm 3 calculated from the density, molecular formula and Avogadro number for LLZOs except for cubic LLZO (Li 7 La 3 Zr 2 O 12 , N NE ∼ 10 20 cm -3 ).

physical chemistry chemical physics/pccp. physical chemistry chemical physics

Relationship between Li<sup>+</sup> diffusion and ion conduction for single-crystal and powder garnet-type electrolytes studied by <sup>7</sup>Li PGSE NMR spectroscopy

Relationship between Li+ diffusion and ion conduction for single-crystal and powder garnet-type electrolytes studied by 7Li PGSE NMR spectroscopy

Relationship between Li⁺ diffusion and ion conduction for single-crystal and powder garnet-type electrolytes studied by ⁷Li PGSE NMR spectroscopy