Flexible Carbon Nanotube–Graphene/Sulfur Composite Film: Free-Standing Cathode for High-Performance Lithium/Sulfur Batteries

Abstract

Flexible lithium batteries with high energy density have recently received tremendous interest due to their potential applications in flexible electronic devices. Herein, we report a novel method to fabricate highly flexible and robust carbon nanotube–graphene/sulfur (CNTs–RGO/S) composite film as free-standing cathode for flexible Li/S batteries with increased capacity and significantly improved rate capability. The free-standing CNTs–RGO/S cathode was able to deliver a peak capacity of 911.5 mAh g–1sulfur (∼483 mAh g–1electrode) and maintain 771.8 mAh g–1sulfur after 100 charge–discharge cycles at 0.2C, indicating a capacity retention of 84.7%, which were both higher than the cathodes assembled without CNTs. Even after 100 cycles, the cathode showed a high tensile strength of 62.3 MPa. More importantly, the rate capability was improved by introducing CNTs. The CNTs–RGO/S cathode exhibited impressive capacities of 613.1 mAh g–1sulfur at 1C with a capacity recuperability of ∼94% as the current returned to 0.2C. These results demonstrate that the well-designed nanocomposites are of great potential as the cathode for flexible lithium sulfur (Li/S) batteries. Such improved electrochemical properties could be attributed to the unique coaxial architecture of the nanocomposite, in which the evenly dispersed CNTs enable electrodes with improved electrical conductivity and mechanical properties and better ability to avoid the aggregation and ensure the dispersive distribution of the sulfur species during the charge/discharge process.