Nitrogen, sulfur co-doped hierarchical carbon encapsulated in graphene with “sphere-in-layer” interconnection for high-performance supercapacitor

Rational design of electrode with hierarchical charge-transfer structure and good electronic conductivity is important to achieve high specific capacitance and energy density for supercapacitor, but it still remains a challenge. Herein, a nitrogen, sulfur co-doped pollen-derived carbon/graphene (PCG) composite with interconnected “sphere-in-layer” structure was fabricated, in which hierarchically pollen-derived carbon microspheres can serve as “porous spacers” to prevent the agglomeration of graphene nanosheets. The optimized PCG composite prepared with 0.5 wt% of graphene oxide (PCG-0.5) exhibited high specific capacitance (420 F g⁻¹ at 1 A g⁻¹), rate performance (280 F g⁻¹ at 20 A g⁻¹), and excellent cycling stability with 94% of capacitance retention after 10,000 cycles. The symmetrical device delivered a remarkable energy density of 31.3 Wh kg⁻¹ in neutral medium. Moreover, density functional theory calculation revealed that PCG electrode possessed the accelerated charge transfer and enhanced electronic conductivity, thus ensuring a remarkable electrochemical performance. This work may afford an effective strategy for the development of biomass-derived carbon electrodes with novel charge-transfer structure toward supercapacitor applications.