Abstract

Incorporating metal compound nanoparticles into zeolitic imidazolate frameworks (ZIFs) has emerged as an effective way to solve the low conductivity issue of ZIFs, helping to boost their electrochemical performance. However, the resultant ZIFs/metal compound composites usually lack hierarchical pores, which causes the electrochemical performance to be far below expectations. Here, two rational post-treating strategies, namely, Ni2+/H2O etching and solvent-assisted etching, have been proposed to tailor the structure and composition of ZIF-67/Ni3S4 composite. Especially, Ni2+/H2O etching enables the self-transformation of ZIF-67 to CoNi layered double hydroxide (LDH), while solvent-assisted etching creates hierarchical pores in ZIF-67. After post-treatments, both resultant samples display significant improvements in energy storage capability and cycling lifespan as compared to untreated ZIF-67/Ni3S4 owing to their superior features including the hierarchical pore structure, enhanced pseudocapacitance property, and less internal and charge transfer resistance. The tailoring strategies together with mechanism studied here can provide perspectives and constructive designing knowledge to promote the widespread use of ZIFs or Ni3S4 based advanced electrodes toward high-performance supercapacitors.

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