Scalable fabrication of NiCo2O4/reduced graphene oxide composites by ultrasonic spray as binder-free electrodes for supercapacitors with ultralong lifetime

doi:10.1016/j.jmst.2021.05.040

Abstract

Abstract:

Durable and cost-effective electrode materials are essential for practical application of supercapacitors. Herein, large area NiCo₂O₄/reduced graphene oxide (NiCo₂O₄/rGO) composites with hierarchical structure were fabricated by a facile one-step ultrasonic spray on Ni foam and directly used as the binder-free electrodes for supercapacitors in aqueous KOH electrolyte. Owing to high electrical conductivity of rGO, hierarchical and layered structure of the electrode, as well as tight adhesion of active materials on the current collector, the as-obtained hybrid electrodes show a high specific capacitance of 871 F g^-1 at current density of 1 A g^-1, good rate performance and remarkable cycling stability with a capacitance retention of 134% after 30000 cycles. Besides, the assembled NiCo₂O₄/rGO//AC asymmetric supercapacitor (ASC) displays the maximum energy density of 29.3 Wh kg^-1 at a power density of 790.8 W kg^-1. Significantly, an ultralong cycling life of 102% capacitance retention is achieved for the ASC device after 30,000 charge/discharge cycles at 20 A g^-1. The scalable fabrication route and excellent electrochemical performance of the NiCo₂O₄/rGO composites open the door for making novel hybrid electrodes of advanced supercapacitors.

Key words: Ultrasonic spray, NiCo₂O₄/rGO, Binder-free electrode, Supercapacitor

Shi Zhongting, Sun Gan, Yuan Ruiwen, Chen Wenxiao, Wang Zhuo, Zhang Lu, Zhan Ke, Zhu Min, Yang Junhe, Zhao Bin. Scalable fabrication of NiCo₂O₄/reduced graphene oxide composites by ultrasonic spray as binder-free electrodes for supercapacitors with ultralong lifetime[J]. J. Mater. Sci. Technol., 2022, 99: 260-269.

Figures/Tables 9

Fig. 1. Schematic illustration for the fabrication of the NiCo2O4/rGO by ultrasonic spray.

Fig. 2. XRD patterns (a) and Raman spectra (b) of the NiCo2O4/rGO composites fabricated with different GO/metal precursor ratios.

Fig. 3. SEM (a, b) and TEM (c, d) images of the NiCo2O4/rGO fabricated with feedstock ratio of 1:15; (e) low-magnification SEM image and EDS elemental mapping.

Fig. 4. XPS spectra of the NiCo2O4/rGO composite fabricated with feedstock ratio of 1:15: (a) survey spectrum; high- resolution spectrum of C 1s (b), Ni 2p (c) and Co 2p (d).

Fig. 5. Electrochemical performance of the NiCo2O4/rGO fabricated with different GO/metal precursor ratios: (a) CV curves at 20 mV s-1; (b) GCD curves at 1 A g-1; (c) Specific capacitance as a function of current density; (d) Nyquist plots; (e) Cycling stability at 20 A g-1.

Table 1 The electrochemical supercapacitor performance in previous studies.

Electrode materials	Synthesis method	Specific capacitance (F g^-1)	Capacitance retention	Refs.
NiCo₂O₄/rGO	Ultrasonic spraying	871 (1 A g^-1)	134% (30000)	This work
Co₃O₄-NiO/GF	Immersion	766 (1 A g^-1)	86% (5000)	[36]
NiCo₂O₄@MnO₂	Electrodepositing	913.6 (0.5 A g^-1)	87.1% (3000)	[37]
CQD/NiCo₂O₄	Oil bath	856 (1 A g^-1)	98.7% (10000)	[38]
CNT/NiCo₂O₄	Electrochemical deposition	695 (1 A g^-1)	91% (1500)	[39]
C/NiCo₂O₄	Hydrothermal	404 (1 A g^-1)	87.1% (1000)	[40]
NiCo₂O₄@Ni foam	Combustion	646.6 (1 A g^-1)	96.5% (3000)	[41]
NiCo₂O₄-ECN	Hydrothermal	596.8 (2 A g^-1)	97% (3100)	[42]
CMK-3/Co₃O₄	Hydrothermal	1131.3 (0.5 A g^-1)	91% (3000)	[43]
Co₃O₄-NiO/GO	Hydrothermal	883 (1 A g^-1)	82% (3000)	[44]
MWCNT/GO/NiCo₂O₄	Hydrothermal	707 (2.5 A g^-1)	88% (5000)	[45]
Ni-Co-Mn hydroxide	Hydrothermal	1188 (1 A g^-1)	78.8% (50000)	[46]
NiCo₂O₄@rGO	Hydrothermal	1427 (8 A g^-1)	83.8% (10000)	[47]

Fig. 6. Illustration for structural advantage of the NiCo2O4/rGO composite.

Fig. 7. Quantitative capacitive analysis for the NiCo2O4/rGO composite with feedstock ratio of 1:15: (a) CV curves at various scan rates; (b) b-values acquired from the linear fitting of the logarithm of anodic peak current vs logarithm of scan rates; (c) CV curve with the shaded area showing surface capacitive contribution at 20 mV s-1; (d) contribution fractions of surface capacitive and diffusion-controlled components at various scan rates.

Fig. 8. Electrochemical performance of the NiCo2O4/rGO//AC ASC device in 2 M KOH electrolyte: (a) CV curves of the individual AC and NiCo2O4/rGO electrode at a scan rate 20 mV s-1; (b) CV curves in different potential windows at a scan rate of 20 mV s-1; (c) CV curves at various scan rates; (d) GCD curves at different current densities; (e) Ragone plot; (f) long-term cycling stability at 20 A g-1, and the inset showing a red LED-lighted by two ASCs.

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Scalable fabrication of NiCo₂O₄/reduced graphene oxide composites by ultrasonic spray as binder-free electrodes for supercapacitors with ultralong lifetime

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