Nanofiber-Interlocked V₂CT_x Hosts Enriched with 3D Lithiophilic and Sulfophilic Sites for Long-Life and High-Rate Lithium–Sulfur Batteries

Lithium–sulfur batteries (LSBs) currently face challenges including lithium polysulfide shuttling, sluggish sulfur redox kinetics, severe lithium dendrite growth, and volume change. Herein, an advanced dual-functional host is designed by embedding 3D N-doped carbon fibers with abundant 2D V₂CT_x nanosheets (N/CF@V₂CT_x). The N-doped carbon fibers act as “thread” to connect the V₂CT_x nanosheets and form a unique open 3D macroporous structure. This structure effectively prevents the restacking of the V₂CT_x nanosheets and exposes their lithiophilic and sulfurophilic sites. Consequently, the N/CF@V₂CT_x host effectively suppresses the shuttling of LiPSs and improves the cathodic kinetics. Furthermore, the 3D-ordered porous skeleton integrated with abundant lithophilic sites enables uniform Li deposition and homogeneous Li-ion flux, thereby inhibiting dendrite growth and mitigating volume expansion. The as-assembled LSBs exhibit excellent rate capability (640 mAh g⁻¹ at 15 C) and outstanding cycling stability (0.019% capacity decay per cycle throughout 1200 cycles at 1 C). Moreover, the pouch cell assembled with the N/CF@V₂CT_x host demonstrates a high energy density of 350 Wh kg⁻¹ and good cycling stability. This research presents a promising approach to address the challenges of both the sulfur cathode and the lithium anode comprehensively and effectively in working LSBs.