The accepted manuscript of our new paper on gallium doping in LLZrO battery materials is now available online:

• R. Jalem, M.J.D. Rushton, W. Manalastas Jr, M. Nakayama, T. Kasuga, J.A. Kilner, and Robin W. Grimes, "Effects of Gallium Doping in Garnet-Type Li₇La₃Zr2O₁₂ Solid Electrolytes ", Chemistry of Materials (2015). doi:10.1021/cm5045122

The paper is the result of an ongoing collaboration between the group and Dr. Randy Jalem. Randy originally spent several months with us at Imperial whilst visiting us as a PhD student from Nagoya Institute of Technology (Japan) and we would like to thank him and the other authors for all their hard work in bringing this to completion.

Research highlights:

• LLZrO is a candidate for use as solid electrolytes in battery applications.
• The effects of Ga doping on the structure are considered.
• Ga is found to stabilise the cubic phase.
• The connectivity of Li percolation networks in LLZrO are visualised.

Abstract

Garnet-type Li₇La₃Zr2O₁₂ (LLZrO) is a candidate solid electrolyte material that is now being intensively optimized for application in commercially competitive solid state Li⁺ ion batteries. In this study we investigate, by force-field-based simulations, the effects of Ga³⁺ doping in LLZrO. We confirm the stabilizing effect of Ga³⁺ on the cubic phase. We also determine that Ga³⁺ addition does not lead to any appreciable structural distortion. Li site connectivity is not significantly deteriorated by the Ga³⁺ addition (>90% connectivity retained up to x = 0.30 in Li^7–3xGa^xLa³Zr²O¹²). Interestingly, two compositional regions are predicted for bulk Li⁺ ion conductivity in the cubic phase: (i) a decreasing trend for 0 ≤ x ≤ 0.10 and (ii) a relatively flat trend for 0.10 < x ≤ 0.30. This conductivity behaviour is explained by combining analyses using percolation theory, van Hove space time correlation, the radial distribution function, and trajectory density.