Print Email Facebook Twitter Investigation of Structure, Ionic Conductivity, and Electrochemical Stability of Halogen Substitution in Solid-State Ion Conductor Li3YBrxCl6- x Title Investigation of Structure, Ionic Conductivity, and Electrochemical Stability of Halogen Substitution in Solid-State Ion Conductor Li3YBrxCl6- x Author van der Maas, E.L. (TU Delft RST/Storage of Electrochemical Energy) Zhao, W. (TU Delft BN/Cees Dekker Lab) Cheng, Z. (TU Delft RST/Storage of Electrochemical Energy) Famprikis, T. (TU Delft RST/Storage of Electrochemical Energy) Thijs, M.A. (TU Delft RID/TS/Technici Pool) Parnell, S.R. (TU Delft RID/TS/Instrumenten groep) Ganapathy, S. (TU Delft RID/TS/Instrumenten groep) Wagemaker, M. (TU Delft RST/Storage of Electrochemical Energy) Date 2022 Abstract Li3YX6(X = Cl, Br) materials are Li-ion conductors that can be used as solid electrolytes in all solid-state batteries. Solid electrolytes ideally have high ionic conductivity and (electro)chemical compatibility with the electrodes. It was proven that introducing Br to Li3YCl6increases ionic conductivity but, according to thermodynamic calculations, should also reduce oxidative stability. In this paper, the trade-off between ionic conductivity and electrochemical stability in Li3YBrxCl6-xhalogen-substituted compounds is investigated. The compositions of Li3YBr1.5Cl4.5and Li3YBr4.5Cl1.5are reported for the first time, along with a consistent analysis of the whole Li3YBrxCl6-x(x = 0-6) tie-line. The results show that, while Br-rich materials are more conductive (5.36 × 10-3S/cm at 30 °C for x = 4.5), the oxidative stability is lower (∼ 3 V compared to ∼ 3.5 V). Small Br content (x = 1.5) does not affect oxidative stability but substantially increases ionic conductivity compared to pristine Li3YCl6(2.1 compared to 0.049 × 10-3S/cm at 30 °C). This work highlights that optimization of substitutions in the anion framework provide prolific and rational avenues for tailoring the properties of solid electrolytes. To reference this document use: http://resolver.tudelft.nl/uuid:5e9466db-c260-4b3a-a104-816671ec45f6 DOI https://doi.org/10.1021/acs.jpcc.2c07910 ISSN 1932-7447 Source The Journal of Physical Chemistry C, 127 (1), 125-132 Part of collection Institutional Repository Document type journal article Rights © 2022 E.L. van der Maas, W. Zhao, Z. Cheng, T. Famprikis, M.A. Thijs, S.R. Parnell, S. Ganapathy, M. Wagemaker Files PDF acs.jpcc.2c07910.pdf 3.15 MB Close viewer /islandora/object/uuid:5e9466db-c260-4b3a-a104-816671ec45f6/datastream/OBJ/view