Novel Organic Cathode with Conjugated N-Heteroaromatic Structures for High-Performance Aqueous Zinc-Ion Batteries.

Abstract

Aqueous zinc-ion batteries (AZIBs) are being considered new choices of batteries not only because of their inherent safety but also because of their low price advantage. Nevertheless, it is still an important task to develop organic cathode materials with green sustainability and high performance. Hexaazatriphenylene (HAT)-based organic materials have shown great potential for use in AZIBs. Herein, 5,6,11,12,17,18-hexaazatrinaphthylene-2,8,14-tricarboxylic acid (HATTA) is designed and prepared as the AZIB cathode. Benefiting from the conjugative effect of -COOH, extended π-conjugated structure, and abundant active sites, the HATTA electrode exhibits a high capacity (225.8 mA h g-1 at 0.05 A g-1), an outstanding rate performance (136.1 mA h g-1 at 25 A g-1), and a long-term cycling lifespan (84.07% of the initial capacity after 10,000 cycles at 25 A g-1). Meanwhile, the characterization results of ex situ spectroscopic tests prove that the unsaturated bond (C═N) is the redox-active moiety of HATTA. In addition, the flexible Zn//HATTA battery also exhibits impressive long-term cycling stability and good flexibility, showing its promising application in wearable electronics. This work provides a strategy with rational designing for constructing high-performance AZIBs with organics.