What type of study is this?

This is a In Vitro Study study (also classified as: Observational).

August 16, 2025Open Access

Analyses of Electrode–Electrolyte Interactions in Commercial Layered Oxide/Hard Carbon Na‐Ion Cells via Optical Sensors

CAClémence AlphenCentre National de la Recherche Scientifique JFJuan Forero‐SaboyaBoston College DFDominique FoixCentre National de la Recherche Scientifique

Key Points

Electrolyte decomposition is influenced by cathode composition, with O3 cathodes causing more decay than P2.
The addition of succinonitrile and prop-1-ene-1,3-sultone raises heat generation while reducing solvent decomposition.
Utilizing operando optical and mass spectrometry techniques, cell chemistry optimization is demonstrated across commercial sodium-ion cells.
These findings indicate the importance of combining calorimetric studies and optical sensing for advancing sodium-ion technology.

Abstract

Abstract Monitoring the chemical and physical processes during the initial charge of commercial‐type cells is crucial for accelerating their optimization. In this study, operando optical calorimetry, pressure sensing, and infrared fiber evanescent wave spectroscopy (IR‐FEWS) are harnessed as powerful diagnostic tools to investigate the first charge of the formation cycle of layered oxide‐based sodium‐ion cells composed of P2 or O3 cathode material and hard carbon (HC) anode. It is first revealed that the cathode composition significantly influences the initial charge behavior, showing that the O3 cathode triggers larger electrolyte decomposition than P2, which is associated with significant heat and gas generation at high states of charge. Then, the use of succinonitrile (SN) and prop‐1‐ene‐1,3‐sultone (PES) is explored as additives in the electrolyte, proving that while both additives raise the heat generation in P2/HC and O3/HC cells, they effectively suppress solvent and salt decomposition. These observations are further corroborated by online electrochemical mass spectrometry (OEMS) and X‐ray photoelectron spectroscopy (XPS) analyses. Overall, this work underlines the importance of combining operando calorimetric and chemical studies in optimizing the cell chemistry and highlights the effectiveness of optical sensing techniques for investigating the interphase formation in commercial‐type cells.

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