Construction of NiCo-Layered Double Hydroxide Microspheres from Ni-MOFs for High-Performance Asymmetric Supercapacitors

Layered double hydroxide (LDH) materials, especially metal–organic framework (MOF)-derived LDHs, have attracted much attention in electrochemical capacitor applications. However, the construction of porous three-dimensional microsphere architectures with controlled morphology is highly demanded for high-performance supercapacitor electrodes. Thus, a simple and effective strategy is recommended to design and fabricate the well-defined layered structure of LDHs with high performance. In this study, we demonstrate the synthesis of nickel–cobalt-LDHs (NiCo-LDHs) by in-situ etching of the Ni-MOF template at different hydrolysis times. Based on the different characterization results of the sample, a formation mechanism has been proposed in terms of the proton production rate and etching process. As a result of the disparity in the layered structure and the surface area, the electrochemical behavior of the NiCo-LDHs has been altered. The sample NiCo-LDH/10 (prepared after the 10 h reaction) exhibited a high surface area and the large size of LDH sheets on microspheres, which promoted the rapid electrolyte ion transportation for supercapacitors and displayed a maximum specific capacity of 1272 C g–1 at 2 A g–1. In addition, the assembled asymmetric supercapacitor delivered a remarkable energy density of 36.1 Wh kg–1 with an outstanding cyclic stability (103.9% after 5000 cycles). This work establishes an effective strategy to synthesize a well-defined NiCo-LDH structure from the MOF template toward high-performance asymmetric supercapacitors, which could be extended to large-scale preparation of other transition metal-based LDHs from Ni-MOFs.