Entropy-driven lattice reprogramming of vanadium oxide nanoribbons for coupled structural stabilization and fast Zn-ion transport in advanced aqueous zinc-ion batteries

Entropy engineering stabilizes V O frameworks via multi-cation co-doping. • DFT results show reduced Zn 2+ diffusion barriers through electronic tuning. • HE-VO cathodes achieve an ultra-low decay rate of 0.0034% per cycle. • High-mass-loading pouch cells demonstrate the practical scalability of HE-VO. Aqueous zinc-ion batteries (AZIBs) have emerged as promising candidates for safe and cost-effective energy storage. However, their practical deployment is constrained by sluggish Zn 2+ diffusion and structural degradation of cathode materials during cycling. Here, report an entropy-driven lattice reprogramming strategy that regulates layered vanadium oxide through multi-ion incorporation, enabling the construction of a high-entropy vanadium oxide (HE-VO) cathode. Beyond simple compositional modification, the introduced configurational entropy regulates the local coordination environment, simultaneously enhancing structural stability and Zn 2+ transport kinetics. As a result, HE-VO exhibits highly reversible Zn 2+ storage and outstanding electrochemical durability, delivering 300 mAh g −1 at 1 A g −1 and an ultralow capacity decay rate of only 0.0034% per cycle over 5000 cycles at 10 A g −1 . Moreover, a Zn||HE-VO pouch cell with a high-mass loading (∼8 mg cm −2 ) attains a specific capacity of 162 mAh g −1 at 2 A g −1 , highlighting the practical scalability of this strategy. This work provides a viable pathway toward the development of durable and high-rate electrode materials for advanced AZIBs. A HE-VO nanoribbon was synthesized through an entropy engineering strategy, which reprograms the V O lattice to enhance electronic structure, stabilize coordination, and facilitate ion diffusion via entropy-driven lattice expansion and charge redistribution. The tailored cathode consequently delivers exceptional electrochemical performance, while a high-loading pouch cell further demonstrates its practical viability, establishing entropy engineering as an effective strategy for achieving concurrently stable and fast-kinetic AZIBs. Download: Download high-res image (154KB) Download: Download full-size image