Membrane and electrode engineering of high-performance lithium-sulfur batteries modified by stereotaxically-constructed graphene

Abstract

Lithium-sulfur batteries have great potential as the next-generation clean energy storage systems due to their remarkable high-energy density and electrochemical capacity. Additionally, sulfur is used as a cathode material because of its characteristics of a low cost, environmental friendliness, and abundant nature. However, the polysulfide shuttle effect decreases the electrochemical performance of lithium-sulfur batteries. Here, a rational membrane/electrode design has been applied to lithium-sulfur batteries. A three-dimensional hierarchical nanoporous carbon material derived from cationic resins in a cost-effective process was synthesized at a high temperature and utilized as an intermediate layer to improve the rate capability and cycle stability of lithium-sulfur batteries. Furthermore, stereotaxically -constructed multiporous graphene with a high conductivity (1.6 × 10 3 S m −1 ), porosity and large specific surface area (824 m 2 g −1 ) has been applied in the cathode to increase the conductivity of sulfur, improve the transport of lithium-ions and increase the contact with the electrolyte. In particular, stereotaxically-constructed multiporous graphene was used as the sulfur carrier (sulfur loading 70 wt %). The electrochemical results revealed an initial discharge capacity of the hierarchical nanoporous carbon material intermediate layer-coated membrane of 1008 mAh g −1 at 0.5C, and the reversible capacity was 532 mAh g −1 at 1C after 300 cycles. Based on the experimental evidence and analyses, we concluded that the enhanced performance is due to the confinement of lithium polysulfides by the micropores and mesoporous structure of the hierarchical porous carbon material and the increased transportation of lithium ions and the improved wettability of membrane by electrolyte. • Hierarchical nanoporous carbon material (HNCM) has been synthesized at a high temperature by a cost-effective process. • The HNCM reduce the interfacial resistance and increase the wettability of membrane by electrolyte. • The stereotaxically-constructed multiporous graphene (SCMG) employed as sulfur host for Li–S batteries. • The resultant lithium-sulfur batteries exhibit a superior rate capacity and improved cycling capacity. • The multiple physical sorption of the modified layer greatly inhibit the shuttling of polysulfide.