Novel 2D/2D NiCo2O4/ZnCo2O4@rGO/CNTs self-supporting composite electrode with high hydroxyl ion adsorption capacity for asymmetric supercapacitor

doi:10.1016/j.jmst.2022.04.009

Abstract

Abstract:

The energy storage device has been urgently studied and developed to meet the increasing demand for energy and sustainable development. Due to the excellent conductivity of graphene and high performance of ZnCo₂O₄ and NiCo₂O₄, we design a self-supporting electrode based on vertically grown two-dimensional/two-dimensional (2D/2D) NiCo₂O₄/ZnCo₂O₄ hierarchical flakes on the carbon-based conductive substrate (NiCo₂O₄/ZnCo₂O₄@graphene/carbon nanotubes, NZ@GC). The density functional theory calculations indicate that the high OH⁻ adsorption capacity of the NiCo₂O₄/ZnCo₂O₄ nanosheets can significantly enhance the electrochemical reaction activity. NZ@GC shows a high capacitance of 1128.6 F g⁻¹ at 1 A g⁻¹. The capacitance retains 84.0% after 6000 cycles even at 10 A g⁻¹. A hybrid supercapacitor is fabricated using NZ@GC and activated carbon, exhibiting a large energy density of 50.8 W h kg⁻¹ at the power density of 800 W kg⁻¹. After 9000 charge/discharge cycles, the supercapacitor still has 86.1% capacitance retention. The NZ@GC film has showed the potential as promising electrodes in high efficiency electrochemical energy storage devices.

Key words: Supercapacitor, ZnCo₂O₄, NiCo₂O₄, Energy density, Excellent conductivity, High capacitance

Xiumei Chen, Na Xin, Yuxin Li, Cong Sun, Longhua Li, Yulong Ying, Weidong Shi, Yu Liu. Novel 2D/2D NiCo₂O₄/ZnCo₂O₄@rGO/CNTs self-supporting composite electrode with high hydroxyl ion adsorption capacity for asymmetric supercapacitor[J]. J. Mater. Sci. Technol., 2022, 127: 236-244.

Figures/Tables 8

Fig. 1. Fabrication process of NiCo2O4/ZnCo2O4@rGO/CNTs.

Fig. 2. Top view SEM images of (a) NiCo2O4@GO/CNTs and (b) NiCo2O4/ZnCo2O4@rGO/CNTs film. (c, d) TEM and (e) HRTEM images of the NiCo2O4/ZnCo2O4. (f) TEM and (g-j) corresponding elemental mapping images of O, Co, Zn, and Ni in NiCo2O4/ZnCo2O4.

Fig. 3. (a) XRD patterns of N@GC, NZ@GC and the standard patterns of NiCo2O4 and ZnCo2O4, (b) XPS spectrum of the survey, (c) Co 2p, (d) Ni 2p, (e) Zn 2p and (f) O 1s of NiCo2O4/ZnCo2O4@rGO/CNTs composites.

Fig. 4. (a) CV curves of GC, N@GC and NZ@GC at 2 mV s?1. (b) GCD curves of GC, N@GC and NZ@GC at 1 A g -1. (c, d) CV and GCD curves of the NZ@GC at various test conditions. (e) Cyclic performance of NZ@GC at 10 A g?1, inset is the SEM image of NiCo2O4/ZnCo2O4 after cycling test. (f) EIS spectra of N@GC and NZ@GC.

Fig. 5. Crystallographic models of (a) NiCo2O4 and NiCo2O4-OH; (b) ZnCo2O4 and ZnCo2O4-OH; (c) NiCo2O4/ZnCo2O4 and NiCo2O4/ZnCo2O4-OH; (d) calculated adsorption energies of OH? on the above three systems.

Fig. 6. (a) CV curves of the NZ@GC composite electrode at scan rates from 2 to 5 mV s?1; (b) relationship between logIp versus logv for the anodic peak and cathodic peak current of NZ@GC; Capacitance contribution rate of NZ@GC at a scan rate of (c) 2 mV s?1, (d) 3.5 mV s?1 and (e) 5 mV s?1, respectively; (f) Capacitive contribution percentage of the surface contribution at different scan rates.

Fig. 7. (a) Assembly illustration of the NZ@GC//AC hybrid supercapacitor; (b) Comparative CV curves of NZ@GC and AC at 2 mV s?1; (c) CV curves of NZ@GC//AC supercapacitor at 100 mV s?1; (d) CV and (e) GCD curves of the device; (f) Specific capacitance of NZ@GC//AC device.

Fig. 8. (a) Ragone plots of the NZ@GC//AC hybrid supercapacitor compared with other reported supercapacitors. Inset is the picture of the lighting up LEDs by the supercapacitor. (b) Cyclic tests of the as-assembled device at the current density of 10 A g?1 after 9000 cycles.

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Novel 2D/2D NiCo₂O₄/ZnCo₂O₄@rGO/CNTs self-supporting composite electrode with high hydroxyl ion adsorption capacity for asymmetric supercapacitor

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