Topic: Unveiling Electrode–Electrolyte Interfaces in Advanced Batteries: In Situ/Operando Characterization and Mechanistic Insights

Electrode–electrolyte interfaces play a critical role in determining the electrochemical performance, cycling stability, and safety of rechargeable batteries. During operation, these interfaces undergo coupled structural and chemical transformations involving ion transport, charge transfer, interphase formation, and side reactions. Their dynamic and heterogeneous nature can obscure the mechanisms underlying capacity fading, interfacial instability, and battery degradation. Understanding how these processes evolve under working conditions is therefore essential for developing durable battery systems.

Recent advances in in situ/operando characterization, including synchrotron-based X-ray spectroscopy, advanced electron microscopy, Raman spectroscopy, nuclear magnetic resonance, and neutron-based techniques, have enabled more direct investigations of interfacial structures and chemical evolution under realistic electrochemical conditions. Integrating these experimental approaches with theoretical calculations and multiscale simulations can further elucidate interfacial reaction pathways, ion-transport kinetics, and degradation mechanisms. These developments offer new opportunities to establish fundamental relationships between interfacial chemistry and battery performance.

This Special Issue, “Unveiling Electrode–Electrolyte Interfaces in Advanced Batteries: In Situ/Operando Characterization and Mechanistic Insights,” highlights advances in characterization methods and mechanistic understanding of dynamic electrode–electrolyte interfaces. It provides a platform for original research, reviews, and perspectives that connect fundamental interfacial science with strategies for designing more efficient, durable, and safer rechargeable batteries.

This Special Issue welcomes original research articles, reviews, and perspectives on advanced characterization and mechanistic investigations of electrode–electrolyte interfaces in rechargeable batteries. Topics of interest include, but are not limited to:

● In situ/operando characterization of electrode–electrolyte interfaces;

● Synchrotron-based X-ray spectroscopy, diffraction, and imaging for battery interfaces;

● Advanced electron microscopy and spectroscopic techniques for interfacial analysis;

● Formation, evolution, and degradation mechanisms of solid–electrolyte and cathode–electrolyte interphases (SEI/CEI);

● Interfacial ion transport, charge transfer, and electrochemical reaction kinetics;

● Dynamic interfacial chemistry in lithium-, sodium-, potassium-, and zinc-based batteries;

● Interfacial evolution and reaction mechanisms in solid-state batteries;

● Operando investigation of electrode structural transformations and degradation processes;

● Multiscale characterization of interfacial heterogeneity and coupled chemo-mechanical phenomena;

● Theoretical modeling and simulations including AI on interfacial reactions and ion transport;

● Correlations among interfacial evolution, electrochemical performance, and battery failure mechanisms.