Universal design of three-dimensional porous graphene-iron based promotors for kinetically rationalized lithium-sulfur chemistry

Lithium-sulfur (Li-S) batteries are widely deemed to be one of the most potential candidates for future secondary batteries because of their remarkable energy density. Nevertheless, notorious polysulfide shuttling and retarded sulfur reaction kinetics pose significant obstacles to the further application of Li-S batteries. While rationally designed highly active electrocatalysts can facilitate polysulfide conversion, the universal and scalable synthesis strategies need to be developed. Herein, a universal synthetic strategy to construct a series of three-dimensional (3D) porous graphene-iron (3DGr-Fe) based electrocatalysts involving 3DGr-FeP, 3DGr-Fe₃C, and 3DGr-Fe₃Se₄ is exploited for manipulating the Li-S redox reactions. It has been observed that the implementation of a 3D porous Gr architecture leads to the well-designed conductive networks, while the uniformly dispersed iron nanoparticles introduce an abundance of active sites, fostering the lithium polysulfide conversion, thereby bolstering the overall electrochemical performance. The Li-S battery with the 3DGr-Fe based electrocatalyst exhibits remarkable capacity retention of 94.8% upon 100 times at 0.2 C. Moreover, the soft-packaged Li-S pouch cell based on such a 3DGr-Fe electrocatalyst delivers superior capacity of 1060.71 mA h g⁻¹ and guarantees for the continuous 30 min work of fan toy. This investigation gives comprehensive insights into the design, synthesis, and mechanism of 3DGr-Fe based electrocatalysts with high activity toward efficient and durable Li-S batteries.