Extrinsic Surface-Driven Pseudocapacitive Contribution in Hard Carbon Anodes for Sodium-Ion Batteries Using a Chitosan-Derived Binder
摘要
Chitosan has attracted considerable interest as a sustainable, water-based electrode binder for sodium-ion batteries owing to its functional chemistry and favorable electrochemical properties. In this study, the electrochemical behavior of chitosan as a binder for hard carbon anodes is systematically investigated. The incorporation of chitosan significantly enhances the electrochemical performance of hard carbon anodes by introducing abundant amine and hydroxyl functional groups, which actively participate in interfacial charge storage. These functional groups modify the energy storage mechanism of hard carbon, leading to an increased contribution from surface-controlled capacitive kinetics. Quantitative analysis reveals that chitosan contributes approximately 26% extrinsic surface-driven pseudocapacitive contribution at a scan rate of 0.2 mV s−1, whereas conventional polyvinylidene fluoride (PVDF) binders predominantly promote diffusion-controlled sodium storage. Furthermore, chitosan effectively mitigates capacity degradation during continuous cycling. After 50 charge–discharge cycles, hard carbon anodes employing chitosan as the binder maintain a specific a capacity of 187 mAh g−1 (a capacity retention of 70%) , representing a substantial improvement compared with the 31 mAh g−1 (9.8% retention) observed for PVDF-based hard carbon anodes. This enhanced cycling stability is attributed to the strong interfacial interactions and improved charge-transfer kinetics induced by the amine and hydroxyl groups in chitosan, which increase extrinsic surface-driven pseudocapacitive contribution and maintain structural integrity during repeated cycling. Overall, chitosan demonstrates significant potential as an environmentally benign and high-performance binder for advanced sodium-ion battery anodes.
Graphical Abstract