A High‐Capacity Negative Electrode for Asymmetric Supercapacitors Based on a PMo12 Coordination Polymer with Novel Water‐Assisted Proton Channels

The development of a negative electrode for supercapacitors is a critical challenge for the next-generation of energy-storage devices. Herein, two new electrodes formed by the coordination polymers Ni(itmb)4 (HPMo12 O40 )·2H2 O (1) and Zn(itmb)3 (H2 O)(HPMo12 O40 )·4H2 O (2) (itmb = 1-(imidazo-1-ly)-4-(1,2,4-triazol-1-ylmethyl)benzene), synthesized by a simple hydrothermal method, are described. Compounds 1 and 2 show high capacitances of 477.9 and 890.2 F g-1 , respectively. An asymmetric supercapacitor device assembled using 2 which has novel water-assisted proton channels as negative electrode and active carbon as positive electrode shows ultrahigh energy density and power density of 23.4 W h kg-1 and 3864.4 W kg-1 , respectively. Moreover, the ability to feed a red light emitting diode (LED) also demonstrates the feasibility for practical use. The results allow a better elucidation of the storage mechanism in polyoxometalate-based coordination polymers and provide a promising direction for exploring novel negative materials for new-generation high-performance supercapacitors.