Synergistic d‐π Coupling and Interfacial Catalysis Enable Electron‐Ion Dual Kinetics in Ah‐Level Zinc‐Ion Batteries

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ABSTRACT Aqueous zinc‐ion batteries (AZIBs) are constrained by mismatched electron and ion kinetics, where sluggish electronic transport in cathodes and high interfacial desolvation barriers of hydrated Zn 2+ jointly limit practical performance. Here, we report a molecular architectonic strategy that enables electron‐ion dual kinetics through synergistic d‐π coupling and interfacial catalysis. By in situ anchoring 1H‐imidazole‐4‐carboxylic acid (ICA) molecules onto tunnel‐structured VO 2 , an organic‐inorganic hybrid cathode (IVO 2 ) is constructed. The π ‐conjugated framework of ICA engages in strong d‐π orbital coupling with V 3d states, inducing p ‐type doping and enhancing electronic conductivity. Simultaneously, the abundant hydrogen‐bond donor/acceptor sites of ICA act as interfacial catalytic centers that lower the Zn 2+ desolvation energy barrier, thereby accelerating interfacial ion transfer. Benefiting from this coupled kinetic modulation, the optimized IVO 2 ‐1.5 cathode delivers a high specific capacity of 567.8 mAh g −1 and sustains over 10 000 cycles at ultrahigh rates. Importantly, this molecular‐scale kinetic advantage translates to practical devices, as an Ah‐level pouch cell with a mass loading of 21 mg cm −2 and a stringent N/P ratio of 9.1 achieves a discharge capacity of 1.01 Ah with over 100% capacity retention after 110 cycles. This work provides a viable strategy for bridging molecular‐scale kinetic engineering with practical aqueous batteries.

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Related topics: Advanced battery technologies research · Electrocatalysts for Energy Conversion · Advancements in Battery Materials