Synergy of Multi‐Covalent Bonds Enabling High‐Performance Aqueous Zinc‐Ion Battery Cathodes Toward Industrial‐Grade Mass Loading and Broad‐Temperature Adaptability

The pursuit of high-performance cathode materials that are capable of operating reliably under industrially relevant conditions remains a formidable challenge for aqueous zinc-ion batteries (AZIBs). Here, we tackle this challenge by proposing a novel strategy-synergistic bond engineering-which represents a conceptual advance that departs from conventional approaches. This strategy is materialized in a vanadium oxide cathode, where the deliberate integration of multi-covalent bonds (O─N─O and N─V) triggers a powerful synergy, enabling efficient operation from baseline to demanding conditions. Through comprehensive simulations and in situ/ex situ characterizations, we elucidate the synergetic mechanism of these bonds: the O─N─O bonds accelerate Zn²⁺ diffusion via electrostatic shielding and provide abundant active sites via dynamic reconstruction, while the N─V bonds serve as structural pins that suppress vanadium dissolution and ensure structural integrity. Therefore, the cathode delivers an ultrahigh capacity of 624 mAh g⁻¹ at 0.1 A g⁻¹ and exceptional cycling stability (73% capacity retention after 10 000 cycles at 20 A g⁻¹). Crucially, it achieves a record-high capacity of 504 mAh g⁻¹ under a high mass loading of ≥7 mg cm⁻², along with substantial capacities of 117 and 308 mAh g⁻¹ at 0°C and 60°C, demonstrating the great promise of this "bond-level" design strategy.