Tailored molecular architectures featuring synergistic multiple functional groups for ultrastable and high-rate...

The highly tunable structures and molecular designability of organic electrode materials (OEMs) make them attractive for advanced aqueous zinc-ion batteries (AZIBs). Nevertheless, the practical deployment of OEMs is hindered by several inherent drawbacks, such as high solubility in electrolytes, insufficient electrical conductivity, and underutilized active sites. These issues collectively contribute to unsatisfactory cycling life, mediocre rate capability, and limited specific capacity. To address these challenges, we present a rationally designed molecule with high Zn²⁺ affinity, oxidized indanthrone (O-IDT), which incorporates abundant electroactive sites (carbonyl (C=O) and imine (C=N)) within an expanded π-conjugated system. Enabled by a straightforward one-step synthesis, the tailored molecular structure of the chemically synthesized indanthrone (O-IDT-c) ensures high structural stability and enhanced π-electron delocalization. More importantly, in-situ analyses elucidate the synergistic effect between adjacent CO and CN groups, which collaboratively promote highly reversible Zn²⁺ coordination. As a result, the O-IDT-c delivers a high specific capacity of 297 mAh g^-1, remarkable rate performance (delivering 168 mAh g^-1 at an ultrahigh current density of 100 A g^-1, which represents 66% retention compared to its performance at 1 A g^-1), and outstanding long-term stability with 28,000 cycles at 50 A g^-1. This work offers valuable guidance for the molecular-level design of high-performance OEMs in advanced AZIBs.