Abstract
AbstractThe sluggish redox kinetics of sulfur electrode and the “shuttle effect” caused by soluble lithium polysulfides (LiPS) are critical challenges in the advancement of high‐energy lithium‐sulfur batteries. Here, a pioneering flexible self‐supporting composite scaffold that incorporates Janus V2O3/VN heterostructures embedded within multichannel nitrogen‐doped carbon nanofibers (MNCNF) is introduced. The MNCNF features a 3D hierarchical porous conductive network that facilitates rapid ion/electron transport while offering substantial space for high sulfur loading. Theoretical calculations demonstrate that the Janus V2O3/VN heterocatalyst, featuring a built‐in interfacial electric field, facilitates a smooth and rapid “capture‐diffusion‐conversion” of LiPS by leveraging the V2O3’s strong adsorption capacity, VN's high catalytic capability and promoted interfacial charge/ion transport, thereby accelerating bi‐directional sulfur conversion. The as‐designed sulfur electrode with a sulfur loading of 2.0 mg cm−2 showcases high rate capability of 618 mAh g⁻¹ at 5C with 68.1% capacity retention over 500 cycles. Notably, under harsh conditions of high sulfur loading (6.0 mg cm−2) and lean electrolyte (7.5 µL mg−1), it achieves a high initial areal capacity of 4.92 mAh cm−2 with 94.8% capacity retention over 150 cycles. This work offers valuable insights for the rational design of optimal vanadium‐based heterocatalysts aimed at facilitating rapid sulfur redox conversion.
Published Version
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