Operando X-ray Diffraction Computed Tomography Investigation of Morphological and Structural Changes Occurring During All-Solid-State Batter

In All-Solid-State batteries, halide electrolytes (HEs) like Li2ZrCl6 allows Li+ conduction in composite positive electrodes. Our discovery reveals HEs can serve as secondary redox-active centers along side primary redox material LiFePO4, boosting cell capacity by several tens of percent. Leveraging chloride redox chemistry, approximately 50% of electrons are extracted during charging, with 25% recoverable upon discharge which is therefore presumably due to bulk modifications like phase transformation. Oxidation sees a rise in cell impedance and irreversible pressure decrease, hinting at significant structural changes in positive electrodes influenced by nearby conductive surfaces. We ask for Operando XRD-CT to reveal local 3D crystallographic changes, aiding in understanding electrochemical mechanisms.