In a new publication in The Journal of Physical Chemistry C, we systematically investigate how the electronic, ionic, and mechanical properties of Li₆PS₅Cl (LPSCl) evolve with pressure and temperature, and how these factors shape its structural dynamics. By linking ion-transport behavior to particle rearrangement, plastic deformation, contact formation, and activation volume, we delve into how compression and decompression influence electrolyte performance.
High pelletizing pressures improved conductivity and electrical-contact uniformity, whereas low applied pressures caused poor interfacial contact. Under very high pressures (> 10 GPa), irreversible changes to the crystal structure occurred. At high pelletizing pressures, grain boundaries dominated ionic transport, while at lower applied pressure, the grain and grain-boundary contributions become comparable. Owing to a positive activation volume, the ionic conductivity exhibited a maximum (around 80 MPa), above which the ionic conduciivity decreased with pressure.
The open access publication is available here. This study was the outcome of a collaboration between rhd instruments and the University of Camerino within the Erasmus+ student exchange framework as well as project REFA (Referenz-Elektroden für Festkörper-Akkumulatoren, 03EI6055) financed by the Federal Ministry for Economic Affairs and Energy.
a) Nyquist plots of LPSCl powder during compression, and b) at 150 MPa before and after pelletizing. c) Pressure-dependent conductivity, and (d) equivalent capacitance. (CC-BY 4.0)