An individual sandwich hybrid nanostructure of cobalt disulfide in-situ grown on N doped carbon layer wrapped on multi-walled carbon nanotubes for high-efficiency lithium sulfur batteries

Abstract

Binding and trapping of lithium polysulfide (LPS) are being conceived as the most effective strategies to improve lithium-sulfur (Li-S) battery performance. Therefore, exploiting a simple but cost-effective approach for the absorption and conversion of LPS and the transfer of electrons and Li⁺ ions is of paramount importance. Herein, sandwich structure MWCNTs@N-doped-C@CoS₂ integrated with multiple nanostructures of zero-dimensional (0D) CoS₂ nanoparticles, 1D carbon nanotubes (CNTs), and 2D N-doped amorphous carbon layer was obtained, where MWCNTs was firstly uniformly attached with a polydopamine (PDA) of excellent adhesion, followed by hydrothermal method, the Co²⁺ nanoparticles were in-situ grown on the PDA by the formation of complex compound of Co²⁺ and N atoms in PDA, and then the CoS₂ nanoparticles were in-situ grown on CNTs in a point-surface contact way by a bridging of N-doped amorphous carbon layer derived from the carbonization of attached PDA after the vulcanization at 500 °C under Ar atmosphere. The multifunction synergism of absorption, conductivity, and the kinetics of LPS redox is significantly improved, consequently effectively suppressing the shuttle effect and tremendously increasing the utilization rate of active substance. For the Li-S battery assembled with MWCNTs@N-doped-C@CoS₂-modified separator, its rate capacity and cycling performance can be greatly enhanced. It can exhibit a high initial discharge capacity of 1590 mAh g^-1 at 0.1 C, a stable long-term cycling performance with a relatively low capacity decay of 0.07% per cycle during 500 cycles at 1 C, and a reversible capacity of 772 mAh g^-1 and a capacity decay of 0.04% per cycle during 250 cycles at 2 C. Even at a large current density of 4 C, an initial specific discharge capacity of 634 mAh g^-1 can still be delivered. With a high sulfur loading of 5.0 mg cm^-2, additionally, an outstanding cycling stability can also be well maintained at 685 mAh g^-1 at 0.1 C after 50 cycles. This work provides a novel and simple but effective strategy to develop such sandwich hybrid materials comprised of polar metal sulfides and conductive networks via an effective bridging to help realize durable and stable Li-S battery.

Keywords: CoS(2); Lithium-sulfur battery; MWCNTs; Multifunctional separator; N-doped-carbon layer; Sandwich nanostructure integration; Synergistic effect.