Al-Based MOF-Derived Amorphous/Crystalline Heterophase Cobalt Sulfides as High-Performance Supercapacitor Materials

Transition metal sulfides (TMSs) are promising electrode materials due to their high theoretical specific capacitance, but sluggish charge transfer kinetics and an insufficient number of active sites hamper their applications in supercapacitors. In this work, a self-sacrificial template strategy was employed to construct Al-based MOF-derived metal sulfides with an amorphous/crystalline (a/c) heterophase, in which aluminum, nitrogen, and carbon species were evenly coordinated in the amorphous phase. The metal sulfides a/c-Co(Al)S-1 and a/c-Co(Al)S-2, originating from the CAU-1 and CoAl-MOF on NF as self-sacrificial templates, were investigated as electrode materials, respectively, in which the a/c-Co(Al)S-1 showed a more excellent electrochemical performance. Through acid etching CAU-1 using Co(NO₃)₂ followed by sulfuration, the a/c-Co(Al)S-1 with a unique 3D network structure was constructed, whose unique architecture expanded the interfacial contact with the electrolyte and provided vast active sites, accelerating the charge transportation and ion diffusion. Notably, the a/c-Co(Al)S-1 displayed a high specific charge of 1791.8 C g^-1 at 1 A g^-1, satisfactory cycle stability, and good rate capability. The corresponding assembled a/c-Co(Al)S-1//AC device delivered a high energy density of 77.1 Wh kg^-1 at 800 W kg^-1 and good durability (87.4% capacitance retention over 10 000 cycles).