High-Performance Aqueous Zinc Batteries Based on Organic/Organic Cathodes Integrating Multiredox Centers

Organic cathode materials with redox-active sites and flexible structure are promising for developing aqueous zinc ion batteries with high capacity and large output power. However, the energy storage of most organic hosts relies on the coordination/incoordination reaction between Zn²⁺/H⁺ and a single functional group, which result in inferior capacity, low discharge platform, and structural instability. Here, the lead is taken in in situ electrodepositing stable poly(1,5-naphthalenediamine, 1,5-NAPD) as interlayer and excellent conductive poly(para-aminophenol, pAP) skin onto nanoporous carbon in sequence for the structural optimization of organic/organic cathodes, designated as C@multi-layer polymer. In situ analyses, electrochemical measurements, and theoretical calculation prove that both CO and CN active groups can act as a strong electron donor as well as Zn²⁺ host during the discharging process. Benefiting from the synergistic effect of the double organic layers, C@multi-layer polymer delivers high capacity, long lifespan, and excellent capacity reservation even at large discharge current and commercial mass loading (>10 mg cm⁻²). Introducing multiredox centers into one organic composites will provide new insights into designing advanced Zn–organic batteries.