Utilizing the full capacity of carbon black as anode for Na-ion batteries via solvent co-intercalation

Abstract

Carbonaceous materials have long been considered promising anode materials for Na-ion batteries. However, the electrochemical performance of conventional carbon anodes is generally poor because the sodium ion storage solely relies on the disordered region of the carbon materials in a carbonate-based electrolyte. The solvent co-intercalation mechanism for Na ions has been recently reported in natural graphite anodes for Na-ion batteries with ether-based electrolytes, but their capacities are still unsatisfactory. We show here for the first time that by combining regular Na ion storage in the disordered carbon layer and solvent co-intercalation mechanism in the graphitized layer of a commercial N330 carbon black as an anode material for Na-ion batteries in ether-based electrolyte, the reversible capacity could be fully realized and doubled in magnitude. This unique sodium intercalation process resulted in a significantly improved electrochemical performance for the N330 electrode with an initial reversible capacity of 234 mAh·g^–1 at 50 mA·g^–1 and a superior rate capability of 105 mAh·g^–1 at 3,200 mA·g^–1. When cycled at 3,200 mA·g^–1 over 2,000 cycles, the electrode still exhibited a highly reversible capacity of 72 mAh·g^–1 with a negligible capacity loss per cycle (0.0167%). Additionally, surface-sensitive C K-edge X-ray absorption spectroscopy, with the assistance of electrochemical and physicochemical characterizations, helped in identifying the controlled formation and evolution of a thin and robust solid electrolyte interphase film. This film not only reduced the resistance for sodium ion diffusion, but also maintained the structural stability of the electrode for extended cycle reversibility. The superior electrochemical performance of N330 carbon black strongly demonstrated the potential of applying ether-based electrolytes for a wide range of carbon anodes apart from natural graphite.