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

Abstract

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.