Microwave-assisted Synthesis of rGO/CeO2 Supercapacitor Electrode Materials with Excellent Electrochemical Properties

doi:10.6023/A21050216

Abstract

CeO₂ possesses excellent pseudocapacitance, nevertheless the electrochemical properties of carbon/CeO₂ composites need to be improved. In this paper, reduced graphene oxide (rGO)/CeO₂ composite is prepared via a simple microwave-assisted synthesis method. The typical synthesis process is as follows. Firstly, 60 mg of graphene oxide was dissolved into 50 mL of deionized water. Then 20 mL of 0.17 mol•L^-1 Ce(NO₃)₃•6H₂O solution was added under ultrasonic conditions. The electrostatic assembly led to the combination of the graphene oxide and Ce(NO₃)₃. Afterwards, 10 mL of 1.5 mol•L^-1 KOH was added dropwise into the mixed solution until the pH value up to 10. The rGO/CeO₂ was synthesized in the above-mentioned mixed solution by using the microwave heating method. The heating time was set for 45 s. Repeated the microwave heating process for five times after the solution cooled down to the room temperature. Finally, the rGO/CeO₂ was harvested by centrifugation, washing and freeze-drying. The CeO₂, in the form of particles, distributes uniformly and conformally on the surface of the corrugated rGO by the morphology observation. The existence of the tiny gaps is displayed between the nano-scaled CeO₂ particles. N₂ adsorption/desorption analysis suggests that the rGO/CeO₂ has large specific area and pores in the mesoporous size, which is helpful to the sufficient contact with the electrolyte. By the electrochemical measurements, the specific capacitance of the rGO/CeO₂ is as high as 468 F•g^-1 and the capacity retention is up to 107.3% after 10000 charge/discharge cycles. The excellent cycling stability is attributed to the good synergistic effect between the rGO with large specific area and the CeO₂ with uniform and thin layer, which decreases the resistance of ion transport, and the tiny gaps between CeO₂ particles, which mitigates the lattice expansion during the transformation from Ce⁴⁺ to Ce³⁺. The energy density of the assembled symmetrical supercapacitor rGO/CeO₂||rGO/CeO₂ reaches 18.16 Wh•kg^-1. As a supercapacitor electrode material, the rGO/CeO₂ has wide prospect.

Key words: microwave, graphene, cerium oxide, supercapacitor, electrochemistry

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Yao Zhai, Guoxiang Xin, Jiaqi Wang, Bangwen Zhang, Jinling Song, Xiaoxu Liu. Microwave-assisted Synthesis of rGO/CeO₂ Supercapacitor Electrode Materials with Excellent Electrochemical Properties[J]. Acta Chimica Sinica, 2021, 79(9): 1129-1137.

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Fig. & Tab. 14

Figure 1. TG curves of GO, rGO and rGO/CeO2

Figure 2. XRD patterns of rGO/CeO2 and CeO2

Figure 3. FESEM images of (a) rGO and (b, c) rGO/CeO2, (d) shows the energy spectra of (c)

Figure 4. TEM images of (a, b) low-magnification for CeO2, TEM images of (c, d) low-magnification and (e) of high-resolution for rGO/CeO2, (f) selected area electron diffraction pattern of rGO/CeO2

Figure 5. (a) N2 adsorption/desorption isotherm and (b) pore size distribution curve for rGO/CeO2

Figure 6. XPS spectra and fitting peaks for rGO/CeO2: (a) survey spectrum, (b) Ce 3d, (c) O 1s and (d) C 1s

Figure 7. (a) CV curves of rGO, CeO2 and rGO/CeO2 at a scan rate of 100 mV•s-1, (b) CV curves of rGO/CeO2 at a scan rate of 2~100 mV•s-1

材料	比电容/ (F•g^-1)	电流密度/扫速	电解液^a	参考文献
CeO₂/C	125	1 A•g^-1	6 M KOH	[12]
CeO₂/rGO	282	2 A•g^-1	3 M KOH	[13]
Graphene oxide/CeO₂	265	5 mV•s^-1	3 M KOH	[28]
CeO₂/activated carbon	162	10 mV•s^-1	1 M H₂SO₄	[31]
CeO₂/rGO	114	0.5 A•g^-1	6 M KOH	[33]
Hollow CeO₂ spheres/graphitic carbon	501	1 A•g^-1	6 M KOH	[34]
rGO/CeO₂	468	0.5 A•g^-1	3 M KOH	This work

Table 1. CeO2/carbon-based composites and their capacitance values

Figure 8. (a) GCD curves of rGO, CeO2 and rGO/CeO2 at a current density of 0.5 A•g-1, (b) GCD curve of rGO/CeO2 at 0.5~10 A•g-1 current density

Figure 9. EIS spectra of rGO, CeO2 and rGO/CeO2. Inset at the lower right shows magnified high frequency regions, and inset at the higher left shows electrical equivalent circuit

Figure 10. Capacitance retention of rGO, CeO2 and rGO/CeO2 for 10000 cycles

Figure 11. Electrochemical properties of the rGO/CeO2||rGO/CeO2: (a) Assembly diagram, (b) CV curves at different scan rates of 2~100 mV•s-1, (c) GCD curves at the current densities of 0.2~10A·g-1, (d) EIS spectrum, (inset shows the magnified high frequency region), (e) Capacity retention for 10000 cycles (inset shows the last eight curves of the GCD curves), (f) Ragone plot

Figure 12. Photographs of an LED light turned on by four rGO/CeO2||rGO/CeO2 connected in a series

Figure 13. Schematic illustration for the preparation process of rGO/CeO2 by microwave-assisted synthesis method

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微波辅助合成具有优异电化学性能的rGO/CeO₂超级电容器电极材料

Microwave-assisted Synthesis of rGO/CeO₂ Supercapacitor Electrode Materials with Excellent Electrochemical Properties

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微波辅助合成具有优异电化学性能的rGO/CeO2超级电容器电极材料