Synergistically Enhanced Interfacial Interaction to Polysulfide via N,O Dual-Doped Highly Porous Carbon Microrods for Advanced Lithium–Sulfur Batteries

Abstract

Lithium-sulfur (Li-S) batteries have received tremendous attention because of their extremely high theoretical capacity (1672 mA h g^-1) and energy density (2600 W h kg^-1). Nevertheless, the commercialization of Li-S batteries has been blocked by the shuttle effect of lithium polysulfide intermediates, the insulating nature of sulfur, and the volume expansion during cycling. Here, hierarchical porous N,O dual-doped carbon microrods (NOCMs) were developed as sulfur host materials with a large pore volume (1.5 cm³ g^-1) and a high surface area (1147 m² g^-1). The highly porous structure of the NOCMs can act as a physical barrier to lithium polysulfides, while N and O functional groups enhance the interfacial interaction to trap lithium polysulfides, permitting a high loading amount of sulfur (79-90 wt % in the composite). Benefiting from the physical and chemical anchoring effect to prevent shuttling of polysulfides, S@NOCMs composites successfully solve the problems of low sulfur utilization and fast capacity fade and exhibit a stable reversible capacity of 1071 mA h g^-1 after 160 cycles with nearly 100% Coulombic efficiency at 0.2 C. The N,O dual doping treatment to porous carbon microrods paves a way toward rational design of high-performance Li-S cathodes with high energy density.