Issue 10, 2018

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


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.

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

Supplementary files

Article information

Article type
15 Mar 2018
30 Jul 2018
First published
30 Jul 2018
This article is Open Access
Creative Commons BY license

Energy Environ. Sci., 2018,11, 2993-3002

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

J. A. Dawson, T. S. Attari, H. Chen, S. P. Emge, K. E. Johnston and M. S. Islam, Energy Environ. Sci., 2018, 11, 2993 DOI: 10.1039/C8EE00779A

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