Structural combination of polar hollow microspheres and hierarchical N-doped carbon nanotubes for high-performance Li-S batteries

Hierarchical structured materials constructed with conductive carbon materials have been extensively studied as S host materials for Li-S batteries. However, their outwardly developed hierarchical structures, which do not contain structures or materials to inhibit polysulfide dissolution, lead to the dissipation of dissolved polysulfides and poor dispersion properties during the slurry-making process, which results in non-uniformity in the cathodes. Herein, an assembly of polar materials (hollow structured SiO₂ microspheres) and electrically conductive hierarchical N-doped bamboo-like carbon nanotubes (b-NCNTs) is designed as an efficient S host material for minimizing the dissolution of polysulfides during Li-S battery operations. Highly aligned and packed b-NCNTs are grown in hollow structured SiO₂ microspheres. The SiO₂ layer coated on the surface of the hollow CoFe₂O₄ microspheres plays a key role in the synthesis of easily dispersible hierarchical b-NCNTs microspheres (b-NCNTs@SiO₂). The S-loaded b-NCNTs@SiO₂ electrodes show better cycling stability than S-loaded b-NCNTs electrodes. The polysulfide trapping of the polar SiO₂ layer and the well-developed b-NCNTs minimize the dissolution of polysulfides during cycling. In addition, the introduction of electronegative N atoms into the b-NCNTs lattice enhances their polysulfide trapping ability. The S-loaded b-NCNTs@SiO₂ electrodes exhibit stable discharge capacities of >771 mA h g^-1 over 195 cycles at a current density of 0.5 C and a high reversible capacity of 486 mA h g^-1 even at a high current density of 5.0 C.