Nano-sulfur confined in a 3D carbon nanotube/graphene network as a free-standing cathode for high-performance Li-S batteries

A free-standing nano-sulfur-based carbon nanotube/graphene (S/CNT/G) film with a conductive interlinked three-dimensional (3D) nanoarchitecture is fabricated via a facile solution-based method. This 3D multidimensional carbon-sulfur network combines three different nanoarchitectures, as follows: zero-dimensional sulfur nanoparticles, one-dimensional carbon nanotubes, and two-dimensional graphene. The CNTs with a one-dimensional structure act as a conductive matrix, and graphene with two-dimensional sheets is intercalated into the CNT scaffold to build a 3D structure, extending in an additional dimension to provide improved restriction for sulfur/polysulfides. Zero-dimensional sulfur nanoparticles are anchored uniformly on the interpenetrative 3D carbon framework to form a free-standing cathode. Moreover, this well-designed S/CNT/G film is flexible, highly conductive, binder free and current collector free. When directly used as a flexible cathode electrode, the synthesized S/CNT/G film delivers both excellent long-term cycling and high-rate performances. A high initial capacity of 948 mA h g(-1) is obtained, and subsequently, a reversible discharge capacity of 593 mA h g(-1) over 200 cycles is achieved at 0.5C. Even at a high rate of 3C, the S/CNT/G film with a 50 wt% sulfur content still exhibits a discharge capacity of 598 mA h g(-1). These results demonstrate the great potential of the S/CNT/G nanocomposite as a flexible and binder-free cathode for high performance Li-S batteries.