Synergistic polysulfide regulation via nickel-based heterostructure anchored on self-supporting carbon cloth for high-performance lithium‑sulfur batteries

Lithium‑sulfur (Li S) batteries, despite their ultrahigh theoretical energy density and cost-effectiveness, face persistent challenges such as sluggish redox kinetics, severe polysulfide shuttling, and insufficient sulfur utilization. Herein, we propose a novel integrated Ni/V 2 O 3 heterostructure anchored on self-supporting carbon cloth (Ni/V 2 O 3 @CC) as a high-efficiency sulfur host to address these limitations. The three-dimensional conductive carbon cloth framework eliminates the need for binders while ensuring robust structural integrity and efficient electron transport. The rationally designed Ni/V 2 O 3 heterostructure synergistically combines metallic Ni, which offers catalytic active sites for accelerated sulfur conversion, with polar V 2 O 3 , enabling strong chemisorption of polysulfides. Experimental and theoretical analyses reveal that the abundant interfacial polar-catalytic centers in the heterostructure significantly suppress polysulfide shuttling and enhance redox kinetics. Consequently, the self-supporting Ni/V 2 O 3 @CC cathode demonstrates excellent cycling stability at 1.0C, delivering a high initial discharge capacity of 650 mAh g −1 even at 5.0C with 84% capacity retention after 100 cycles. Notably, it maintains a remarkable discharge capacity of 580 mAh g −1 even under a high mass loading of 4 mg cm −2 . This work establishes a new paradigm for integrating multifunctional heterostructures with freestanding substrates, paving the way toward practical high-energy-density Li S batteries with extended cycle life. A novel integrated Ni/V 2 O 3 heterostructure anchored on self-supporting carbon cloth (Ni/V 2 O 3 @CC) as a high-efficiency sulfur host. The three-dimensional conductive carbon cloth framework eliminates the need for binders while ensuring robust structural integrity and efficient electron transport. Moreover, the Ni/V 2 O 3 heterostructure synergistically combines Ni, which offers catalytic active sites for accelerated sulfur conversion, with polar V 2 O 3 , enabling strong chemisorption of polysulfides. Consequently, the self-supporting Ni/V 2 O 3 @CC cathode demonstrates superior electrochemical performance. • Ni/V 2 O 3 heterostructures on carbon cloth serve as high-efficiency, binder-free sulfur hosts for Li-S batteries. • Ni/V 2 O 3 provides polar-catalytic interfaces, combining strong chemisorption with accelerated sulfur conversion. • The design suppresses the polysulfide shuttle effect and enhances redox kinetics, verified by theory and experiments. • The self-supporting cathode delivers high-rate performance and maintains high capacity under high sulfur loading.