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Elucidating lithium-ion and proton dynamics in anti-perovskite solid electrolytes
Ist Teil von
Energy & environmental science, 2018-01, Vol.11 (10), p.2993-3002
Ort / Verlag
Cambridge: Royal Society of Chemistry
Erscheinungsjahr
2018
Quelle
Alma/SFX Local Collection
Beschreibungen/Notizen
All-solid-state Li-ion batteries are currently attracting considerable research attention as they present a viable opportunity for increased energy density and safety when compared to conventional liquid electrolyte-based devices. The Li-rich anti-perovskite Li
3−x
OH
x
Cl has generated recent interest as a potential solid electrolyte material, but its lithium and proton transport capabilities as a function of composition are not fully characterised. In this work, we apply a combination of
ab initio
molecular dynamics and
1
H,
2
H and
7
Li solid-state NMR spectroscopy to study the mobility of lithium ions and protons in Li
3−x
OH
x
Cl. Our calculations predict a strongly exothermic hydration enthalpy for Li
3
OCl, which explains the ease with which this material absorbs moisture and the difficulty in synthesising moisture-free samples. We show that the activation energy for Li-ion conduction increases with increasing proton content. The atomistic simulations indicate fast Li-ion diffusion but rule out the contribution of long-range proton diffusion. These findings are supported by variable-temperature solid-state NMR experiments, which indicate localised proton motion and long-range Li-ion mobility that are intimately connected. Our findings confirm that Li
3−x
OH
x
Cl is a promising solid electrolyte material for all-solid-state Li-ion batteries.