Stable Hexaazatrinaphthalene-Based Planar Polymer Cathode Material for Organic Lithium-Ion Batteries

Abstract

Organic materials have garnered intensive focus as a new group of electrodes for lithium-ion batteries (LIBs). However, many reported organic electrodes so far still exhibit unsatisfying cycling stability because of the dissolution in the electrolytes. Herein, a novel azo-linked hexaazatrianphthalene (HATN)-based polymer (AZO-HATN-AQ) is designed and fabricated by the polymerization of trinitrodiquinoxalino[2,3-a:2',3'-c]phenazine (HATNTN) and 2,6-diaminoanthraquinone (DAAQ). The abundant redox-active sites, extended π-conjugated planar conformation, and low energy gap endow the AZO-HATN-AQ electrode with high theoretical capacity, excellent solubility resistance, and fast Li-ion transport. In particular, the fully lithiated AZO-HATN-AQ still keeps the planar structure, contributing to the excellent cycling stability. As a result, AZO-HATN-AQ cathodes show high specific capacity (240 mAh g^-1 at 0.05 A g^-1), prominent rate capability (98 mAh g^-1 at 8 A g^-1), and outstanding cycling stability (120 mAh g^-1 after 2000 cycles at 4 A g^-1 with 85.7% capacity retention) simultaneously. This study demonstrates that rational structure design of the polymer electrodes is an effective approach to achieving excellent comprehensive electrochemical performance.