π-Conjugated N-heterocyclic compound with redox-active quinone and pyrazine moieties as a high-capacity organic cathode for aqueous zinc-ion batteries

Abstract

Organic cathode materials have been widely used for aqueous zinc-ion batteries (ZIBs) due to their designable molecular structures and diverse redox groups. However, there are still many challenges that need to be overcome, such as limited specific capacity and utilization, inadequate electrical conductivity, unsatisfactory cycle durability and unclear charge storage mechanism. Herein, we report a π-conjugated N-heterocyclic compound containing dual-redox active groups (i.e. quinone and pyrazine), benzo[b]phenazine-6,11-dione (BPD), which are employed as a cathode material in aqueous ZIBs. The BPD cathode shows a high capacity of up to 429 mAh g−1 at 0.05 A g−1, 100 % capacity utilization and excellent cycling performance upon 10,000 cycles. The aqueous ZIB full cell with the BPD cathode delivers an energy density of 276 Wh kg−1, higher than the most previously reported organic cathode materials. Moreover, ex-situ characterizations, electrochemical experiments, and theoretical calculations, clearly illustrate that H+ and Zn2+ are co-inserted during the charge/discharge process. The high utilization and stability of BPD cathode is due to the high insolubility of both BPD and its discharge products. This work provides a reasonable strategy and unique perspective for the design and synthesis of novel high-performance organic cathode materials for aqueous ZIBs.