Eliminating Charge Transfer at Cathode-Electrolyte Interface for Ultrafast Kinetics in Na-Ion Batteries

Abstract

Sodium-ion batteries suffer from kinetic problems stemming from sluggish ion transport across the electrode-electrolyte interface, causing rapid energy decay during fast-charging or low-temperature operation. One exciting prospect to enhance kinetics is constructing neuron-like electrodes that emulate fast signal transmission in a nervous system. It has been considered that these bioinspired designs enhance electron/ion transport of the electrodes through carbon networks. However, whether they can avoid sluggish charge transfer at the electrode-electrolyte interface remains unknown. By connecting the openings of carbon nanotubes with the surface of carbon-coated Na₃V₂O₂(PO₄)₂F cathode nanoparticles, here we use carbon nanotubes to trap Na⁺ ions released from the nanoparticles during charge. Therefore, Na⁺ movement is confined only inside the neuron-like cathode, eliminating ion transport between the electrolyte and cathode, which has been scarcely achieved in conventional batteries. As a result, a 14-fold reduction in interfacial charge transfer resistance is achieved when compared to unmodified cathodes, leading to superior fast-charging performance and excellent cyclability up to 200C, and surprisingly, reversible operation at low temperatures down to -60 °C without electrolyte modification, surpassing other Na₃V₂O₂(PO₄)₂F-based batteries reported to date. As battery operation has relied on charge transfer at the electrode-electrolyte interface for over 200 years, our approach departs from this traditional ion transport paradigm, paving the way for building better batteries that work under harsh conditions.