Sulfurized Cyclopentadienyl Nanocomposites for Shuttle-Free Room-Temperature Sodium–Sulfur Batteries

A major challenge hindering the practical adoption of room-temperature sodium-sulfur batteries (NaSBs) is polysulfide dissolution and shuttling, which results in irreversible capacity decay and low Coulombic efficiencies. In this work, we demonstrate for the first time NaSBs using a ferrocene-derived amorphous sulfurized cyclopentadienyl composite (SCC) cathode. Polysulfide dissolution is eliminated via covalent bonding between the insoluble short-chain sulfur species and carbon backbone. Control experiments with a metal-free composite analogue determined that the iron species in the SCC does not have a significant role in polysulfide anchoring. Instead, the superior electrochemical performance is attributed to sulfur covalently bonded to carbon and the uniform nanoparticulate morphology of the SCC composite. In the carbonate-based electrolyte, a discharge capacity of 795 mAh g(S)-1 was achieved during early cycling at 0.2 C, and high Coulombic efficiencies close to 100% were maintained with capacity retention of 532 and 442 mAh g(S)-1 after 100 and 200 cycles, respectively.