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High-entropy materials with tailorable properties are receiving increasing interest for energy applications. Among them, (disordered) rock-salt oxyfluorides hold promise as next-generation cathodes for use in secondary batteries. Here, we study the degradation behavior of a high-entropy oxyfluoride cathode material in lithium cells in situ via acoustic emission (AE) monitoring. The AE signals allow acoustic events to be correlated with different processes occurring during battery operation. The initial cycle proved to be the most acoustically active due to significant chemo-mechanical degradation and gas evolution, depending on the voltage window. Irrespective of the cutoff voltage on charge, the formation and propagation of cracks in the electrode was found to be the primary source of acoustic activity. Taken together, the findings help advance our understanding of the conditions that affect the cycling performance and provide a foundation for future investigations on the topic.

Acoustic Emission Monitoring of High-Entropy Oxyfluoride Rock-Salt Cathodes during Battery Operation