Publication date: 10th April 2024
The influence of microstructure on ionic conductivity and cell performance is a topic of broad scientific interest in solid-state batteries. The current understanding is that interfacial decomposition reactions during cycling induce local strain at the interfaces between solid electrolytes and anode/cathode, as well as within the electrode composites. Investigating the effects of internal strain on ion transport is particularly important given the significant local chemomechanical effects caused by volumetric changes of the active materials during cycling. Here, we characterize the induced strain in Li6PS5Br structure under applied pressure up to 10 GPa, with in-situ high pressure synchrotron diffraction and ex-situ powder diffraction. A permanent strain is observed in the material even after pressure release, indicating long-range strain fields typical for dislocations. Pair distribution function analysis reveals no change in the short-range local structure, but smaller coherence length for the more strained material is found, indicating that the origin of the long-range strain is caused by dislocations. With increasing strain, dislocation densities are also found. With increasing strain, an increase in the lithium ionic conductivity can be observed that extends into an improved ionic transport in solid-state battery electrode composites. This work shows the potential of strain engineering as an additional approach for tuning ion conductors in solid-state batteries without changing the composition of the material itself.
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