Publication date: 10th April 2024
Among the different solid electrolytes, lithium halides show promising ionic conductivity and cathode compatibility. The complex composition-properties relationships makes rational design very challenging. In the first part of this work use the ionic potential, the ratio of charge number and ion radius, can effectively capture the key interactions within halide materials, making it possible to guide the design of especially complex halide compositions. This is demonstrated by the preparation of a family of complex layered halides that combine an enhanced conductivity with a favorable isometric morphology. In the second part we evaluate the the role of the Cl vs Br anion in the Li3YBrxCl6-x halide and investigate the trade-off between ionic conductivity and electrochemical stability. One of the main limitations of this material, and in general halide solid electrolytes, is the electrochemical instability at low working potentials, limiting its application. In this context we study the electrochemical and structural transformation and their (ir)reversibility, providing more insights into the stability limits of this material.