Elucidating lithium-ion and proton dynamics in anti-perovskite solid electrolytes

James Dawson, Tavleen S. Attari, Hungru Chen, Steffen P. Emge, Karen E. Johnston, Muhammed Islam

Research output: Contribution to journalArticle

10 Citations (Scopus)

Abstract

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 Li3−xOHxCl 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 1H, 2H and 7Li solid-state NMR spectroscopy to study the mobility of lithium ions and protons in Li3−xOHxCl. Our calculations predict a strongly exothermic hydration enthalpy for Li3OCl, 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 Li3−xOHxCl is a promising solid electrolyte material for all-solid-state Li-ion batteries.
LanguageEnglish
Number of pages10
JournalEnergy & Environmental Science
Early online date30 Jul 2018
DOIs
StatusE-pub ahead of print - 30 Jul 2018

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Solid electrolytes
perovskite
lithium
Lithium
Perovskite
electrolyte
Protons
Ions
ion
Moisture
nuclear magnetic resonance
moisture
Hydration
Electrolytes
Nuclear magnetic resonance spectroscopy
Molecular dynamics
Enthalpy
enthalpy
hydration
activation energy

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Elucidating lithium-ion and proton dynamics in anti-perovskite solid electrolytes. / Dawson, James; Attari, Tavleen S.; Chen, Hungru; Emge, Steffen P.; Johnston, Karen E.; Islam, Muhammed.

In: Energy & Environmental Science, 30.07.2018.

Research output: Contribution to journalArticle

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