Vanadium Dioxide-Graphene Composite with Ultrafast Anchoring Behavior of Polysulfides for Lithium–Sulfur Batteries

The lithium-sulfur (Li-S) battery has been deemed as one of the most promising energy-storage systems owing to its high energy density, low cost, and environmental benignancy. However, the capacity decay and kinetic sluggishness stemming from polysulfide shuttle effects have by far posed a great challenge to practical performance. We herein demonstrate the employment of low-cost, wet-chemistry-derived VO₂ nanobelts as the effective host additives for the graphene-based sulfur cathode. The VO₂ nanobelts displayed an ultrafast anchoring behavior of polysulfides, managing to completely decolor the polysulfide solution in 50 s. Such a fast and strong anchoring ability of VO₂ was further investigated and verified by experimental and theoretical investigations. Benefitting from the synergistic effect exerted by VO₂ in terms of chemical confinement and catalytic conversion of polysulfides, the Li-S batteries incorporating VO₂ and graphene manifested excellent cycling and rate performances. Notably, the batteries delivered an initial discharge capacity of 1405 mAh g^-1 when cycling at 0.2 C, showed an advanced rate performance of ∼830 mAh g^-1 at 2 C, and maintained a stable cycling performance at high current densities of 1, 2, and 5 C over 200 cycles, paving a practical route toward cost-effective and environmentally benign cathode design for high-energy Li-S batteries.