Nanostructured organic electrode materials grown on graphene with covalent-bond interaction for high-rate and ultra-long-life lithium-ion batteries

Nanostructured organic tetralithium salts of 2,5-dihydroxyterephthalic acid (Li4C8H2O6) supported on graphene were prepared via a facile recrystallization method. The optimized composite with 75 wt.% Li4C8H2O6 was evaluated as an anode with redox couples of Li4C8H2O6/Li6C8H2O6 and as a cathode with redox couples of Li4C8H2O6/Li2C8H2O6 for Li-ion batteries, exhibiting a high-rate capability (10 C) and long cycling life (1,000 cycles). Moreover, in an all-organic symmetric Li-ion battery, this dual-function electrode retained capacities of 191 and 121 mA·h·g–1 after 100 and 500 cycles, respectively. Density functional theory calculations indicated the presence of covalent bonds between Li4C8H2O6 and graphene, which affected both the morphology and electronic structure of the composite. The special nanostructures, high electronic conductivity of graphene, and covalent-bond interaction between Li4C8H2O6 and graphene contributed to the superior electrochemical properties. Our results indicate that the combination of organic salt molecules with graphene is useful for obtaining high-performance organic batteries.