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

Abstract 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‐VSe 2 ) host for Zn 2+ 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 Zn 2+ interactions. Simultaneously, the amorphous framework fortifies the host with abundant active sites and facilitates rapid ion transport. Consequently, the A‐HE‐VSe 2 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 Zn 2+ 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 Zn 2+ storage for next‐generation energy storage applications.