Publication date: 10th April 2024
To meet the global demand for high energy density batteries, research focuses on solid state batteries, which not only allow to enhance the ionic conductivity, but are also considered to be electrochemically more stable than their liquid counterpart.
In this study, the ion dynamics of different high-entropy solid electrolyte lithium argyrodites are investigated with several solid-state NMR techniques on different time and length-scales. This allows to correlate the structure with the local as well as long-range diffusion of the material. The motion of ions from one interstitial site to another site within the crystal lattice enables the fast ion conduction. Therefore, the detection of T1-relaxation times, which are sensitive to this “hopping” motion, is the ideal method to probe the local ion dynamics. Long-range diffusive motions over a few hundred nanometers are probed utilizing 7Li PFG-NMR.
We compare the effect of the multianionic and/or -cationic substitution on lithium argyrodites with the composition Li6+aP1−xMxS5I with M being an equimolar mixture of Si, Ge and Sb [1, 2, 3]. The long-range diffusion is characterized by fast ion diffusion and low activation energies of approximately 0.2 eV. T1-relaxometry allows to distinguish between intra- and intercage hopping. The activation energy of both motions agrees well with the long-range diffusion.
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