LAUSR

Abstract Developing high energy density lithium-sulfur (Li–S) batteries mainly relies on the design of the electrode matrix which can accommodate high sulfur loading and still remain high utilization of active materials. Herein, a 3D hierarchical graphitic carbon foam supported graphene@Mo2C (GCF-G@Mo2C) heterostructure is introduced as a freestanding electrode for Li–S batteries with a facile and cost-effective method. The N-doped carbon foam wrapped by graphene sheets with agaric-like porous structure could promote fast electron and ion transport, meanwhile effectively anchor the polysulfides through physical confinement and chemical adsorption by strongly polar-polar interactions. More importantly, the Mo2C nanoparticles can act as the chemical anchoring center to provide strong polysulfide adsorption, as testified by experimental data and first-principle calculations. Moreover, the catalytic effect of Mo2C also accelerates the redox kinetics of polysulfide conversion, contributing to enhanced rate performance. As a result, the cell with GCF-G@Mo2C displays an initial capacity as high as 862 mAh g−1 and a retained capacity of 597 mAh g−1 after 600 cycles with only 0.051% capacity fade per cycle at 1C rate, presenting good cycling stability. In addition, the GCF-G@Mo2C substrate with high sulfur content (70 ​wt%) and sulfur loading (10.5 ​mg ​cm−2) achieves an ultra-high areal capacity of 12.6 mAh cm−2 at 0.1 ​C, offering a competitive cathode for high-performance Li–S batteries.