Anhydride-Based Compound with Tunable Redox Properties as Advanced Organic Cathodes for High-Performance Aqueous Zinc-Ion Batteries

Organic materials with multiple active sites and flexible structural designs are becoming popular for use in aqueous zinc-ion batteries (AZIBs). However, their applicability is limited due to the low specific capacity and poor cycle stability originating from the introduction of inactive units and high solubility. Herein, three organic molecules with tunable redox properties were synthesized using anhydride (PMDA, 1,2,4,5-benzenetetracarboxylic anhydride-1,2-diaminoanthraquinone, NTCDA, 1,4,5,8-naphthalenetetracarboxylic dianhydride-1,2-diaminoanthraquinone, and PTCDA, 3,4,9,10-perylenetetracarboxylic dianhydride-1,2-diaminoanthraquinone, referred to as PM12, NT12, and PT12) in the solid-phase method. Density functional theory (DFT) simulations and experiments identified that NT12 exhibits superior electrochemical performance compared with PM12 and PT12 because of the low energy gap and large aromatic conjugated structure. They demonstrated specific capacities of 106.7, 192.9, and 124.9 mA h g-1 at 0.05 A g-1, respectively. Especially, NT12 displayed excellent initial specific capacity (85.4 mA h g-1 at 1 A g-1) and remarkable capacity retention (64.1% for 3000 cycles) due to dual active centers (C═N and C═O). The all-NT12 full-cell also had excellent performance (127.1 mA h g-1 under 1 A g-1 and 80.6% over 200 cycles). The organic compounds synthesized in this work have potential applications of AZIBs, highlighting the importance of molecular design to develop the next generation of advanced materials.