Abstract
Advancements in operando techniques have unraveled the complexities of the Electrode Electrolyte Interface (EEI) in electrochemical energy storage devices. However, each technique has inherent limitations, often necessitating adjustments to experimental conditions, which may compromise accuracy. To address this challenge, a novel battery cell design is introduced, integrating piezoelectric sensors with electrochemical analysis for surface‐sensitive operando measurements. This innovative approach aims to overcome conventional limitations by accommodating commercial‐grade battery electrodes within a single body, alongside a piezoelectric sensor. This enables operando electrogravimetric measurements to be realized, and the electrochemistry of a battery to be more faithfully reproduced at the sensor level. A proof of concept is carried out on both Li‐ion (LiFePO 4 //Graphite) and Na‐ion (Na 3 V 2 (PO 4 ) 2 F 3 //Hard carbon) systems, utilizing commercially available powder electrodes. In both cases, the results reveal rational mass variations at the sensor level during the cycling of commercial electrodes with mass loadings several orders of magnitude higher, while performing Galvanostatic Charge Discharge (GCD) tests across various C‐rates. This innovative design opens up possibilities for a broader application of operando electrogravimetry within the battery community, to enhance the understanding of EEI behavior and facilitate the development of more efficient energy storage solutions.