Highly Efficient Retention of Polysulfides in “Sea Urchin”-Like Carbon Nanotube/Nanopolyhedra Superstructures as Cathode Material for Ultralong-Life Lithium–Sulfur Batteries

Despite high theoretical energy density, the practical deployment of lithium–sulfur (Li–S) batteries is still not implemented because of the severe capacity decay caused by polysulfide shuttling and the poor rate capability induced by low electrical conductivity of sulfur. Herein, we report a novel sulfur host material based on “sea urchin”-like cobalt nanoparticle embedded and nitrogen-doped carbon nanotube/nanopolyhedra (Co-NCNT/NP) superstructures for Li–S batteries. The hierarchical micromesopores in Co-NCNT/NP can allow efficient impregnation of sulfur and block diffusion of soluble polysulfides by physical confinement, and the incorporation of embedded Co nanoparticles and nitrogen doping (∼4.6 at. %) can synergistically improve the adsorption of polysulfides, as evidenced by beaker cell tests. Moreover, the conductive networks of Co-NCNT/NP interconnected by nitrogen-doped carbon nanotubes (NCNTs) can facilitate electron transport and electrolyte infiltration. Therefore, the specific capacity, rate capability, and cycle stability of Li–S batteries are significantly enhanced. As a result, the Co-NCNT/NP based cathode (loaded with 80 wt % sulfur) delivers a high discharge capacity of 1240 mAh g–1 after 100 cycles at 0.1 C (based on the weight of sulfur), high rate capacity (755 mAh g–1 at 2.0 C), and ultralong cycling life (a very low capacity decay of 0.026% per cycle over 1500 cycles at 1.0 C). Remarkably, the composite cathode with high areal sulfur loading of 3.2 mg cm–2 shows high rate capacities and stable cycling performance over 200 cycles.