Catalytic Self-Limited Assembly at Hard Templates: A Mesoscale Approach to Graphene Nanoshells for Lithium–Sulfur Batteries

Hollow nanostructures afford intriguing structural features ranging from large surface area and fully exposed active sites to kinetically favorable mass transportation and tunable surface permeability. The unique properties and potential applications of graphene nanoshells with well-defined small cavities and delicately designed graphene shells are strongly considered. Herein, a mesoscale approach to fabricate graphene nanoshells with a single or few graphene layers and quite small diameters through a catalytic self-limited assembly of nanographene on <i>in situ</i> formed nanoparticles was proposed. The graphene nanoshells with a diameter of ca. 10–30 nm and a pore volume of 1.98 cm³ g^–1 were employed as hosts to accommodate the sulfur for high-rate lithium–sulfur batteries. A very high initial discharge capacity of 1520 mAh g^–1, corresponding to 91% sulfur utilization rate at 0.1 C, was achieved on a graphene nanoshell/sulfur composite with 62 wt % loading. A very high retention of 70% was maintained when the current density increased from 0.1 C to 2.0 C, and an ultraslow decay rate of 0.06% per cycle during 1000 cycles was detected