Abstract

The development of safe and long-lasting all-solid-state lithium-ion batteries needs electrolytes with exceptionally good transport properties. Here, we report on the combination of several solid-state nuclear magnetic resonance (NMR) techniques which have been used to precisely probe short-range as well as long-range Li+ dynamics in Li6PS5Br from an atomic-scale point of view. NMR data clearly reveal an extraordinary high Li diffusivity. This manifests in so-called diffusion-induced spin–lattice relaxation NMR rate peaks showing up at temperatures as low as 260 K. From a quantitative point of view, at ambient temperature the Li jump rate is of the order of 109 s–1 which corresponds to a Li+ conductivity in order of 10–3 to 10–2 S/cm, thus, indicating “liquid-like” Li+ diffusion behavior in Li6PS5Br.

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