Linking Pressure to Electrochemical Evolution in Solid-State Conversion Cathode Composites
Conversion-type cathodes, such as sulfur, FeS2, and FeF3, offer high theoretical capacities in solid-state lithium batteries but are hindered by substantial volume changes during cycling, leading to interfacial contact loss, crack formation, and microstructural degradation. Here, we investigate the relationships between electrochemical, mechanical, and structural evolution in solid-state electrode composites with these three active materials. Using real-time stack-pressure monitoring, synchrotron X-ray absorption spectroscopy, and electrokinetic modeling, we elucidate how stress evolution is linked to reversible and irreversible redox reactions. Nonlinear stack pressure evolution in cells with sulfur, FeS2, and FeF3 electrode composites is found to arise from material-specific volume changes,more »