Oxygen-induced coordination reinforcement coupled with C–N structural regulation stabilizes VS2 for durable zinc-ion storage

The vanadium disulfide (VS 2 ) possesses great potential as an excellent zinc-ion energy storage material due to low diffusion barrier and reversible redox activity. However, its high-rate zinc-ion storage capability is limited by nanosheet restacking, structural fragility, and vanadium dissolution. Herein, a synergistic strategy integrating oxygen-induced coordination reinforcement with C–N structural and conductive network reinforcement is proposed to realize thermodynamic-kinetic stabilization of VS 2 cathodes. The incorporation of oxygen converts unstable V–S bonds into a stronger, more ordered V–O coordination, reconstructing the ligand field and stabilizing the vanadium valence state, which effectively inhibits dissolution. Concurrently, the polydopamine (PDA)-derived C–N provides stable anchoring sites to immobilize vanadium species, while CNT frameworks build efficient electron/ion transport pathways and buffer volume strain. The DFT calculations and synchrotron analyses verify the ligand-field reconstruction and vanadium stabilization mechanism. Consequently, the VS 2 /V 2 O 3 -NC/MWCNTs-C (denoted as VSO-NC/MWCNTs-C) delivers a high capacity of 358.89 mA h g −1 at 0.5 A g −1 , excellent rate capability of 242.22 mA h g −1 at 10 A g −1 , along with a high energy/power density of 388.64 Wh kg −1 /1000 W kg −1 , maintaining excellent stability over 6000 cycles at 10 A g −1 . This work offers an atomic-level coordination engineering strategy for advanced V-based cathodes for zinc-ion energy storage. The VSO-NC/MWCNTs-C cathode exhibits stable structural integrity, accelerated Zn 2+ transport, and significantly suppressed vanadium dissolution, delivering high capacity, fast kinetics, and long-life cycling for next-generation zinc-ion energy storage. Download: Download high-res image (301KB) Download: Download full-size image