A Nickel‐Decorated Carbon Flower/Sulfur Cathode for Lean‐Electrolyte Lithium–Sulfur Batteries

Abstract Lithium–sulfur (Li–S) batteries involve a reversible conversion reaction between sulfur and lithium sulfide (Li 2 S) via a series of soluble lithium polysulfide intermediates (LiPSs), enabling a high theoretical specific capacity of 1675 mAh g –1 . However, this process exhibits large polarization and low sulfur utilization and suffers critical capacity fade. The primary approach to tackle the problem has so far been to infiltrate sulfur into nanostructured carbon. However, most studies using porous carbon as host materials have tested with high electrolyte to sulfur ratios (E/S) (generally > 15 µL mg −1 ) that compromise the cell‐level energy density. Here, a flower‐shaped porous carbon structure with nickel nanoparticles that can address the problems discussed above is designed. First, the 3D flower‐shaped carbon structure enables short ionic transport lengths. Second, the small pore diameters <10 nm and high specific surface areas > 3300 m 2 g −1 with sufficient pore volume are ideal for charging performance for low E/S ratios. Finally, Ni nanoparticles are employed onto the flower‐shaped network to improve the reaction kinetics. Collectively, it is successfully demonstrated that the batteries with a high mass loading of 5 mg cm −2 and a 5 µL mg −1 E/S ratio can retain cycle retention of 70% after 150 cycles.