Lithium-sulfur batteries have emerged as extraordinarily favorable energy storage devices due to their high specific capacity and energy density, safety and low cost. Unfortunately, the wide applications of lithium-sulfur batteries are hampered by several issues, such as the low electronic conductivity and slow redox kinetics, serious volumetric expansion and polysulfide "shuttle effect". To overcome these issues, in our work, we design and synthesize a composite sulfur host material of Co9S8 microspheres and N-doped carbon nanotubes, where the metallic sulfide Co9S8 with a good conductivity enables the immobilization of the polar lithium polysulfides owing to the strong polar chemisorptive capability, and the one dimensional N-doped carbon nanotubes can provide channels for fast electron and lithium-ion transport. As the lithium polysulfides are well confined, and the redox conversions are promoted, the Co9S8@N-CNTs/S-based lithium-sulfur battery possesses a superior energy storage performance, exhibiting a large specific capacity of 1233 mAh g -1 at 0.1 C and an outstanding cyclic performance, with a low decay of 0.045% per cycle and a Coulombic efficiency of more than 99% after 1000 cycles. Keywords: Metal sulfides; N-doped carbon nanotube; Cathode material; Lithium-sulfur battery. tightly attached to the N-CNTs is formed. In this composite, the polar metal sulfide Co9S8 enables a superior lithium polysulfide absorptivity via the polar chemical bond, which decreases polysulfide dissolution and the shuttle effect and increases the specific capacity and cyclic performance, while the N-doped carbon nanotubes can assist to increase the electronic conductivity and enlarge the interface between the electrode and electrolyte to further enhance the rate performance. Meanwhile, the N-CNTs/S composite and the Co9S8@N-CNTs/S composites with different contents of N-CNTs have been studied and compared. The unique Co9S8@N-CNTs composite-based sulfur cathode displays an outstanding overall electrochemical performance, making it promising for applications in 6 lithium-sulfur batteries.
Experimental
Preparation of Co9S8 and Co9S8@N-CNTsThe Co9S8@N-CNTs composite host was prepared using a solvothermal process. First, 27 mg of the N-CNTs was ultrasonically dispersed into 30 mL of ethylene glycol and 10 mL of distilled water to form a suspension. CoCl2· 6H2O (0.7138 g) and thiourea (0.4567 g) were added with stirring, and the ratio of CoCl2:thiourea was fixed as 60:40. The obtained solution was then subjected to a hydrothermal reaction for 12 h at 180 C. The product was filtered, adequately washed, and vacuum-dried for 24 h at 80 C. The obtained precursor was annealed for 3 h at 500 °C in H2/Ar (10%:90%). The obtained sample is denoted as Co9S8@N-CNTs. The pristine Co9S8 material was also prepared using the same processes but without adding the N-CNTs. The other Co9S8@N-CNTs composites with different contents of N-CNTs (13.5 mg and 40.5 mg) were prepared by a similar procedure. Hereafter, these obtained samples with different N...