A special core-shell ZnS-CNTs/S@NH cathode constructed to elevate electrochemical performances of lithium-sulfur...

Lithium-sulfur batteries (LSBs) are regarded as promising candidates for next-generation electrochemical energy storage systems due to their low cost and high energy density. However, the insulative sulfur, the volume expansion and high soluble polysulfides are three roots impeding their practical applications, and consequently bring challenges of low sulfur utilization, poor cyclic stability and sluggish redox kinetics. Herein, a special core-shell ZnS-CNTs/S@Ni(OH)₂ (labeled as ZnS-CNTs/S@NH) cathode has been designed to overcome above obstacles and elevate the electrochemical performance. The ZnS-CNTs/S@NH cathode is synthesized via a facile step-by-step strategy, in which ZnS-decorated CNTs was used as a framework to load sulfur and followed with a ultrathin Ni(OH)₂ (NH) layer encapsulation. The ZnS-CNT core combines merits of CNT network and polar ZnS quantum dots (QDs), accommodating the volume change, offering efficient pathways for fast electron/ion transport, and anchoring polysulfides through polar interactions. The outer Ni(OH)₂ shell physically confines the active material and meanwhile provides plenty of catalytic sites for effective polysulfide chemisorption. Benefiting from these merits, the ZnS-CNTs/S@NH cathode exhibits excellent cell performances in comparison with ZnS-CNTs/S and CNTs/S. Its discharge capacity at different C-rates is optimal in the three cathodes, which decreases from 1037.0 mAh g^-1 at 0.1 C to 646.1 mAh g^-1 at 2.0 C. Its cyclic capacity also manifests the slowest reduction from 861.1 to 760.1 mAh g^-1 after 150 cycles at 0.5 C, showing a high retention (88.3%) and a tiny average fading rate (0.078%). The strategy in this work provides a feasible approach to design and construct core-shell cathode materials for realizing practically usable Li-S batteries.