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.
- 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.
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 Li7–3xGaxLa3Zr2O12). 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.