Urea-assisted hydrothermal synthesis of MnMoO4/MnCO3 hybrid electrochemical electrode and fabrication of high-performance asymmetric supercapacitor

doi:10.1016/j.jmst.2021.05.025

Abstract

Abstract:

Transition metal molybdates/carbonates and hybrid nanomaterials have attracted great attention in energy storage applications because of their enriched redox activity, good electronic conductivity, and stable crystallinity. We synthesize a multicomponent MnMoO₄/MnCO₃ hybrid by a one-step hydrothermal method with urea as the reaction fuel. By controlling only the urea concentration in the initial precursor solution, the MnMoO₄/MnCO₃ molecular ratio is controlled effectively, which is found to have a profound effect on the electrochemical properties of the hybrid electrodes. The electrochemical measurements show that the specific capacitance of MnMoO₄/MnCO₃ hybrid is 1311 F/g, the energy density of 116.8 Wh/kg, and power density of 383 W/kg at a current density of 1 A/g with 79% capacitance retention over 5000 cycles. The fabricated asymmetric supercapacitor device exhibits good energy storage performance, including the specific capacitance of 97 F/g along with the energy density of 26.5 Wh/kg and the power density of 657 W/kg at a current density of 1 A/g and good reversibility with capacitance retention of 85% after 2000 cycles and 70% over 5000 cycles. The increase in the energy density of 900% with a mere 60% decrement in the energy density indicates its potential superior applications in high-power devices.

Key words: Asymmetric supercapacitors, Hydrothermal synthesis, MnMoO₄/MnCO₃ hybrid, Energy storage applications

Mohan Reddy Pallavolu, Arghya Narayan Banerjee, Ramesh Reddy Nallapureddy, Sang W. Joo. Urea-assisted hydrothermal synthesis of MnMoO₄/MnCO₃ hybrid electrochemical electrode and fabrication of high-performance asymmetric supercapacitor[J]. J. Mater. Sci. Technol., 2022, 96: 332-344.

Figures/Tables 9

Fig. 1. XRD patterns of MnMoO4/MnCO3 hybrids prepared at different urea concentrations.

Fig. 2. Raman spectra of MnMoO4, MnCO3, and the M0-M4 hybrids prepared at different urea concentrations.

Fig. 3. FESEM images (at two different magnifications) of (a)/(b) M0, (c)/(d) M1, (e)/(f) M2, (g)/(h) M3, and (i)/(j) M4 hybrids prepared at different urea concentrations.

Fig. 4. HRTEM images of (a) M1, (b) M2, (c) M3, and (d) M4 hybrids prepared at different urea concentrations.

Fig. 5. Core level XPS spectra for (a) Mo 3d, (b) Mn 2p, (c) C 1 s, and (d) O 1 s photoelectrons for all the hybrids.

Fig. 6. (a) CV curves of all the hybrid electrodes (in a three-electrode system), (b) Specific capacitance values calculated from CV data for all the hybrid electrodes, (c) GCD curves for all the hybrid electrodes (in a three-electrode system), (d) Specific capacitance values calculated from GCD data for all the hybrid electrodes.

Fig. 7. (a) Cyclic stability of the M3 hybrid electrode at 10 A/g current density. Inset: charge-discharge curves at 1st and 5000th cycles. (b) Ragone plots of all the hybrid electrodes. (c) Nyquist plots for all the hybrid electrodes from high-to-low frequency region (in a three-electrode system). Upper inset: Magnified version of the high-frequency region for M3 electrode showing the Warburg curve. Lower inset: Magnified version of the high-frequency intercept for all the hybrid electrodes. (d) Nyquist plots of all the hybrid electrodes at high-to-mid frequency region. Inset: Equivalent circuit.

Fig. 8. (a) CV curves of M3 hybrid and AC electrodes recorded by a three-electrode cell in 2 M NaOH electrolyte at a scan rate of 100 mV/s. (b) CV curves of ASC with M3 hybrid as positive electrode and AC as negative electrode (in a two-electrode system) at various scan rates. (c) GCD plot of ASC (in a two-electrode system) at various current densities. (d) Specific capacitance of ASC device at different current densities calculated from GCD curves. (e) Cyclic stability of the asymmetric supercapacitor over 5000 charge-discharge cycles. Inset: Charge-discharge curves for the last 15 cycles. (f) Nyquist plot of ASC device. Upper inset: Magnified version of the high-frequency region of the Nyquist plot showing the Warburg curve and high-frequency intercept. Lower inset: Ragone plot of the ASC device.

Table 1 Various electrochemical data of the hybrid electrodes.

Sample	Specific Capacitance (F/g)		Energy-Power performance		EIS data
Sample	From CV @10 mV/s	From GCD @1 A/g	Energy density (Wh/kg) @23.4 × 10³ W/kg	Energy density (Wh/kg) @23.4 × 10² W/kg	R_s (Ω)	R_ct (Ω)	CPE_DL (mF)	C_F (mF)
M0	227.6	560.0	58.4	163.6	0.8	20.8	0.7	0.4
M1	241.2	577.8	45.4	168.8	—-	—-	—-	—-
M2	262.6	753.3	64.9	220.0	—-	—-	—-	—-
M3	395.2	1311.1	116.8	383.0	0.7	10.5	0.3	1.9
M4	314.3	882.2	64.9	257.7	0.9	14.8	0.4	0.9

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Urea-assisted hydrothermal synthesis of MnMoO₄/MnCO₃ hybrid electrochemical electrode and fabrication of high-performance asymmetric supercapacitor

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