Asymmetrically Coordinated Dysprosium (Dy) Single Atoms/Clusters Synergistic Catalysts Promote High‐Performance Aqueous Zn–I 2 Batteries

ABSTRACT Aqueous zinc–iodine batteries have attracted considerable attention owing to their environmental friendliness and high theoretical capacity. However, the iodine cathode inevitably suffers from the formation of soluble polyiodides during charge/discharge processes, resulting in active material loss and heavy shuttle effects. In this manuscript, asymmetrically coordinated dysprosium (Dy‐N 3 O 5 ) single atoms and clusters (Dy SA+C –NC) were designed and synthesized through high‐temperature annealing of its ZIF precursor. The optimized Dy SA+C –NC contains highly dispersed Dy‐N/O single atom sites together with Dy cluster sites, which collectively strengthen polyiodide confinement and accelerate reversible iodine conversion. In addition, the nitrogen‐doped carbon host offers continuous electron transport pathways and pore‐confined spaces, contributing to electrolyte wetting, ion diffusion and iodine utilization. In situ Raman, in situ UV–vis and DFT calculation support that the Dy single atoms/clusters effectively confines iodine species and promotes rapid polyiodide conversion. Particularly, PDOS analysis reveals that the overlap between I‐5p and Dy‐5d states enhances interfacial electronic coupling for iodine activation, while the localized Dy‐4f states regulate the electronic environment of Dy centers. The Dy SA+C –NC@I 2 cathode delivers a high discharge capacity of 200.46 mAh g −1 at 5 A g −1 after 25 000 cycles. This work provides a strategy for the design of rare‐earth single atoms/cluster for long‐life aqueous zinc–iodine batteries.