Porous-Shell Vanadium Nitride Nanobubbles with Ultrahigh Areal Sulfur Loading for High-Capacity and Long-Life Lithium–Sulfur Batteries

Lithium–sulfur (Li–S) batteries hold great promise for the applications of high energy density storage. However, the performances of Li–S batteries are restricted by the low electrical conductivity of sulfur and shuttle effect of intermediate polysulfides. Moreover, the areal loading weights of sulfur in previous studies are usually low (around 1–3 mg cm^–2) and thus cannot fulfill the requirement for practical deployment. Herein, we report that porous-shell vanadium nitride nanobubbles (VN-NBs) can serve as an efficient sulfur host in Li–S batteries, exhibiting remarkable electrochemical performances even with ultrahigh areal sulfur loading weights (5.4–6.8 mg cm^–2). The large inner space of VN-NBs can afford a high sulfur content and accommodate the volume expansion, and the high electrical conductivity of VN-NBs ensures the effective utilization and fast redox kinetics of polysulfides. Moreover, VN-NBs present strong chemical affinity/adsorption with polysulfides and thus can efficiently suppress the shuttle effect via both capillary confinement and chemical binding, and promote the fast conversion of polysulfides. Benefiting from the above merits, the Li–S batteries based on sulfur-filled VN-NBs cathodes with 5.4 mg cm^–2 sulfur exhibit impressively high areal/specific capacity (5.81 mAh cm^–2), superior rate capability (632 mAh g^–1 at 5.0 C), and long cycling stability.