Discovery of D‐band Center Engineered Amorphous Cathode with Ultrahigh, Superfast, and Wide‐Temperature Zn ²⁺ Storage Capability

Developing high-performance cathodes for aqueous Zn-ion batteries (AZIBs) requires simultaneously achieving high capacity, fast kinetics, and wide-temperature stability. Herein, a paradigm-shifting approach rooted in d-band center engineering with a high-entropy amorphous structure (A-HE-VSe₂) host for Zn²⁺ storage. This synergistic design, achieved by incorporating multiple transition metal elements (V, Ti, Cr, Nb, Ta) and creating an amorphous structure, critically redistributes the d-band center. This electronic structure modulation fundamentally enhances intrinsic multi-metal redox activity and optimizes Zn²⁺ interactions. Simultaneously, the amorphous framework fortifies the host with abundant active sites and facilitates rapid ion transport. Consequently, the A-HE-VSe₂ cathode demonstrates a record-breaking performance, including an ultrahigh capacity (426 mAh g^-1 at 0.1 A g^-1), superfast rate capability (217 mAh g^-1 at 100 A g^-1), and exceptional durability over 25 000 cycles. Moreover, such an electrode exhibits robust wide-temperature adaptability. In-depth mechanistic studies and DFT calculations reveal that the high-entropy design not only promotes the zinc ion adsorption energy but also lowers the Zn²⁺ diffusion barrier, all of which are driven by the finely-tuned electronic structure. This work demonstrates that rationally engineering the electronic and atomic structure of amorphous hosts via high-entropy design unlocks superfast, ultrahigh, and thermally stable Zn²⁺ storage for next-generation energy storage applications.