Ultrathin (15 nm) Carbon Sheets with Surface Oxygen Functionalization for Efficient Pseudocapacitive Na‐ion Storage

Abstract Disordered carbon is the state of the art anode material for Na‐ion batteries due to their increased interlayer spacing and good electronic conductivity. However, its practical application is hindered by average specific capacity, poor rate performance, low coulombic efficiency and limited cycling stability. Herein, we report the superior pseudocapacitance enhanced Na‐ion storage of in situ surface functionalized carbon nanosheets. Anodes composed of ultrathin (~15 nm) carbon nanosheets demonstrated excellent reversible specific capacity (375 mAh/g at 25 mA/g), rate performance (150 mAh/g at 2 A/g), long‐term cycling performance (1000 cycles at 1 A/g) and coulombic efficiency (~100 %). Considerably higher pseudocapacitance (up to ~78 %) is also identified in this case compared to amorphous carbon particles. Spectroscopic and electrochemical studies proved Na‐ion intercalation in to the disordered carbon and pseudocapacitive storage driven by oxygen‐containing surface functional groups. Outstanding electrochemical performance is credited to the synergy between diffusion limited intercalation and pseudocapacitive surface Na‐ion storage. The demonstrated synthetic method of in situ functionalized carbon nanosheets is inexpensive and scalable. The strategy of functional group and morphology induced pseudocapacitive Na‐ion storage offer new prospects to design high‐performance Na‐ion battery electrodes.