In situ synthesis of layered nickel organophosphonates for efficient aqueous nickel-zinc battery cathodes

Aqueous nickel-zinc (Ni-Zn) batteries have received increasing research interests because of their reliable safety and economical-friendliness. However, the retarded ionic diffusion, low capacity and limited stability of traditional Ni-based cathodes greatly impedes the practical application of Ni-Zn batteries. Herein, two metal organophosphonate materials of Ni methylphosphonate (Ni-MPA) and Ni phenylphosphonate (Ni-PPA) directly grown on Ni foam are constructed successfully through one step solvothermal technique. These two self supported Ni organophosphonates featured hybrid two-dimensional (2D) structures consisting of alternating inorganic and organic layers, where the inorganic layers are formed by six-coordinated Ni2+ bridged by oxygen atoms and capped by organophosphonate groups, availing to provide rich open redox reaction sites, rapid ion diffusion and structural flexibility. The research results reveal that the organic groups in phosphonic acid ligands have important influence on their electrochemical properties. Consequently, the Ni-MPA electrode exhibits a higher specific capacity of 2.27 mAh/cm2 compared to that of the Ni-PPA electrode (1.1 mAh/cm2) at 3.0 mA/ cm2; however, it demonstrates a more rapid transformation rate into Ni(OH)2 in an alkaline solution. Furthermore, the constructed Ni-MPA//Zn battery can deliver an impressive areal energy density of 2.95 mWh/cm2, good rate performance as well as a long-term cycling stability.