<p>Herein, ZIF-67 was used as a cobalt-based metal–organic framework precursor to obtain Co<sub>3</sub>O<sub>4</sub> nanosheets due to its uniform cobalt-imidazolate framework and its ability to form porous structures upon thermal decomposition. The ZIF-67-derived Co<sub>3</sub>O<sub>4</sub> nanosheets were synthesized by a hydrothermal method followed by a calcination process. The ZIF-67-derived Co<sub>3</sub>O<sub>4</sub> nanosheets presented pore sizes of 20&#xa0;nm, 28&#xa0;nm, and 139&#xa0;nm and a surface area of 315 m<sup>2</sup>&#xa0;g<sup>−1</sup>. The porous nanostructure resulted in a high specific capacitance of 350 F g<sup>−1</sup> at 5 A g<sup>−1</sup>. Cyclic voltammetry (CV) and galvanostatic charge–discharge (GCD) analysis confirmed the electrochemical activity and charge-storage behavior of the material. The charge-transfer resistance is negligible, as indicated by the very small semicircle in the electrochemical impedance spectroscopy plots, confirming high electrical conductivity before and after 5000 cycles. The Co<sub>3</sub>O<sub>4</sub> nanosheet-based electrode material exhibits 95% capacitance retention after 5000 cycles. The redox reactions in the Co<sub>3</sub>O<sub>4</sub> electrode material are dominated by ion diffusion because the b value is close to 0.5, as confirmed by power law calculations. The charge-storage process is dominated (92%) by diffusion, whereas only 8% of the charges are stored by surface processes when analyzed at 50&#xa0;mV&#xa0;s<sup>−1</sup>. The asymmetric device exhibits a capacitance of 156 F g<sup>−1</sup> at 1 A g<sup>−1</sup>, maximum energy density of 63 Wh kg<sup>−1</sup>, maximum power density of 12750 W kg<sup>−1</sup>, and 95% cyclic stability after 10,000 cycles. The diffusive and capacitive processes contribute significantly to maximizing charge storage in the Co<sub>3</sub>O<sub>4</sub> electrode material for battery-type supercapacitive devices.</p> Graphical Abstract <p></p>

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MOF-Assisted Synthesis of Hierarchically Porous ZIF-67-Derived Co3O4 Nanosheets Enabling High Specific Capacitance and Long-Cycle Stability for High-Current-Density Supercapacitors

  • M. B. S. Pravin,
  • Wajiah Mazhar,
  • Awatif Alshamari,
  • Zahra Bayhan,
  • Nithyadharseni Palaniyandy,
  • A. Raza,
  • R. Senthilkumar,
  • Aseel Smerat

摘要

Herein, ZIF-67 was used as a cobalt-based metal–organic framework precursor to obtain Co3O4 nanosheets due to its uniform cobalt-imidazolate framework and its ability to form porous structures upon thermal decomposition. The ZIF-67-derived Co3O4 nanosheets were synthesized by a hydrothermal method followed by a calcination process. The ZIF-67-derived Co3O4 nanosheets presented pore sizes of 20 nm, 28 nm, and 139 nm and a surface area of 315 m2 g−1. The porous nanostructure resulted in a high specific capacitance of 350 F g−1 at 5 A g−1. Cyclic voltammetry (CV) and galvanostatic charge–discharge (GCD) analysis confirmed the electrochemical activity and charge-storage behavior of the material. The charge-transfer resistance is negligible, as indicated by the very small semicircle in the electrochemical impedance spectroscopy plots, confirming high electrical conductivity before and after 5000 cycles. The Co3O4 nanosheet-based electrode material exhibits 95% capacitance retention after 5000 cycles. The redox reactions in the Co3O4 electrode material are dominated by ion diffusion because the b value is close to 0.5, as confirmed by power law calculations. The charge-storage process is dominated (92%) by diffusion, whereas only 8% of the charges are stored by surface processes when analyzed at 50 mV s−1. The asymmetric device exhibits a capacitance of 156 F g−1 at 1 A g−1, maximum energy density of 63 Wh kg−1, maximum power density of 12750 W kg−1, and 95% cyclic stability after 10,000 cycles. The diffusive and capacitive processes contribute significantly to maximizing charge storage in the Co3O4 electrode material for battery-type supercapacitive devices.

Graphical Abstract