Single‐atomic tungsten‐doped Co₃O₄ nanosheets for enhanced electrochemical kinetics in lithium–sulfur batteries

Abstract The practical application of lithium–sulfur batteries (LSBs) is severely hindered by the undesirable shuttling of lithium polysulfides (LiPSs) and sluggish redox kinetics of sulfur species. Herein, a series of ultrathin single‐atomic tungsten‐doped Co₃O₄ (W_x‐Co₃O₄) nanosheets as catalytic additives in the sulfur cathode for LSBs are rationally designed and synthesized. Benefiting from the enhanced catalytic activity and optimized electronic structure by W doping, the W_x‐Co₃O₄ not only reduces the shuttling of LiPSs but also decreases the energy barrier of sulfur redox reactions of sulfur species, leading to accelerated electrode kinetic. As a result, LSB cathodes with the use of 5.0 wt% W_0.02‐Co₃O₄ as the electrocatalyst show the high reversible capacities of 1217.0 and 558.6 mAh g⁻¹ at 0.2 and 5.0 C, respectively, and maintain a high reversible capacity of 644.6 mAh g⁻¹ at 1.0 C (1.0 C = 1675 mA g⁻¹) after 500 cycles. With a high sulfur loading of 5.5 mg cm⁻² and electrolyte–electrode ratio of 8 μL_electrolyte mg_sulfur⁻¹, the 5.0 wt% W_0.02‐Co₃O₄‐based sulfur cathode also retains a high reversible areal capacity of 3.86 mAh cm⁻² at 0.1 C after 50 cycles with an initial capacity retention of 84.7%.