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Non-uniform lithium-ion migration in micrometre-space for garnet- and NASICON-type solid electrolytes studied by 7Li PGSE-NMR diffusion spectroscopy

Abstract

The Li+ migration behaviours in three garnet- and one NASICON-type solid oxide electrolytes were studied in micrometre-space by pulsed-gradient spin-echo (PGSE) 7Li NMR diffusion spectroscopy to clarify common and specific characteristics in each electrolyte. In these solid electrolytes clear evidences were not observed for grain-boundary effects in the Li+ diffusion. The Li+ diffusion constants were parameter-dependent such as the observation time (Δ) and pulsed field-gradient (PFG) strength (g) for all the inorganic solid electrolytes studied. For short Δ values, the Li+ ions undertake collisions and diffractions with the diffraction distance, Rdiffraction [μm]. The apparent Li+ diffusion constants (Dapparent [m2 s-1]) had wide range distributions. In this paper, we introduce the apparent diffusion radius, rradius [μm] and compared it with the Rdiffraction and mean square displacement (MSD) [μm]. The lengths of these distances were of micrometre order (10-6 m). The relations between the rradius, Rdiffraction and MSD suggest Li+ complicated migration behaviours in micrometre space. Using long Δ and large g, we obtained an equilibrated value of DLi. The temperature dependences of the number of carrier ions were estimated from the DLi and ionic conductivity in the four oxide solid electrolytes. For simple comparison and reference, the data of DLi. and ionic conductivity of LiPF6 in 1 M solution of propylene carbonate were added.

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Publication details

The article was accepted on 06 Jun 2018 and first published on 07 Jun 2018


Article type: Paper
DOI: 10.1039/C8CP02915F
Citation: Phys. Chem. Chem. Phys., 2018, Accepted Manuscript
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    Non-uniform lithium-ion migration in micrometre-space for garnet- and NASICON-type solid electrolytes studied by 7Li PGSE-NMR diffusion spectroscopy

    K. Hayamizu, S. Seki and T. Haishi, Phys. Chem. Chem. Phys., 2018, Accepted Manuscript , DOI: 10.1039/C8CP02915F

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