Mild fabrication of SiC/C nanosheets with prolonged cycling stability as supercapacitor

doi:10.1016/j.jmst.2021.09.012

Abstract

Abstract:

A facile and mild route to synthesize C-coated SiC nanosheets (SiC/C NSs) via wet-chemical etching in hydrofluoric acid (HF) at 60 °C for 48 h using carbon aluminum silicate (Al₄SiC₄) as raw materials is reported for the first time. HF molecule leads to the breaking of C-Al bonds in Al₄SiC₄, which eventually results in the formation of two-dimensional SiC nanosheets. A carbon layer with a thickness of approximately 1.5 nm is formed on the surface of SiC nanosheets due to the excess carbon. The prepared SiC/C NSs possess a smooth and rectangular sheet with a mean 150 nm in width, 500 nm in length and 10 nm in thickness, respectively. The crystallographic characterization indicates that 3C-SiC and 2H-SiC coexist and the parallel plane relationship of 3C/2H-SiC heterojunction is (111)_3C-SiC//(001)_2H-SiC. Due to the formed 3C-SiC/2H-SiC heterojunction and graphitic carbon, the fabricated electrode based on SiC/C NSs exhibits prolonged cycling stability and high specific areal capacitance as a promising supercapacitor candidate. It remains 91.2% retention even after 20,000 cycles and 734 μF/cm² at a scan rate of 10 mV/s.

Key words: SiC/C nanosheets, Al₄SiC₄, Etching, Supercapacitors, Stability

Shuang Liu, Enhui Wang, Shichun Liu, Chunyu Guo, Hailong Wang, Tao Yang, Xinmei Hou. Mild fabrication of SiC/C nanosheets with prolonged cycling stability as supercapacitor[J]. J. Mater. Sci. Technol., 2022, 110: 178-186.

Figures/Tables 8

Fig. 1. Schematic diagram of synthetic process of SiC/C NSs.

Fig. 2. (a) XRD patterns of the raw material Al4SiC4 and the synthesized SiC/C. (b) Rietveld refinement XRD patterns of the samples. (c) XPS survey spectrum of SiC/C NSs. (d-f) High-resolution XPS spectra of Si 2p (d), C 1 s (e) and O 1 s (f) of SiC/C NSs.

Fig. 3. Schematic diagram for the preparation of SiC/C NSs.

Fig. 4. (a) SEM image of Al4SiC4 under low magnification. (b) SEM image of the cross-section of Al4SiC4 under high magnification. (c-e) SEM images of SiC/C NSs under lower to higher magnification. (f) AFM topographic image of the nanosheet and the corresponding cross-sectional analysis along the red line.

Fig. 5. (a) TEM image of the obtained SiC/C NSs. (b) The structure schematic diagram of the interface of 3C/2H-SiC. (c) The lattice fringe image of 3C-SiC and related SAED pattern. (d) The lattice fringe image of 2H-SiC and related SAED pattern. (e) High-magnification TEM image of SiC nanosheet coated with graphite layer and corresponding SAED pattern.

Fig. 6. (a) CV curves obtained for SiC/C NSs at scan rates from 10 to 500 mV/s in a voltage range of 0-0.6 V. (b) The areal capacitance and the gravimetric capacitance at different scan rates. (c) Charge-discharge curves obtained for SiC/C NSs with the variation of current densities. (d) Cycling performance test of SiC/C NSs at a scan rate of 200 mV/s for 20,000 cycles.

Table 1. Comparison of the electrochemical performance of various SiC nanostructures applied for supercapacitor electrodes ever reported.

Electrode material	Electrolyte	Specific capacitance	Refs.
Nanocrystalline 3C-SiC films	0.1 mol/L H₂SO₄	70 μF/cm² at 10 mV/s	[13]
SiC nanowires	3.5 mol/L HCl	240 μF/cm² at 100 mV/s	[35]
N-doped polycrystalline 3C-SiC	1 mol/L H₂SO₄	743 μF/cm² at 50 mV/s	[36]
Graphene/SiC	1 mol/L Na₂SO₄	69 μF/cm² at 100 mV/s	[37]
Graphene/SiC/C	0.5 mol/L H₂SO₄	43 μF/cm² at 50 mV/s	[38]
3C-SiC/graphene hybrid nanolaminate	1 mol/L Na₂SO₄	321.4 μF/cm² at 10 mV/s	[14]
SiC nanocauliflowers	1 mol/L Na₂SO₄	188 F/g at 10 mV/s	[39]
SiC/N-MnO₂ composites	1 mol/L Na₂SO₄	273.2 F/g at 10 mV/s	[40]
Hollow SiC fibers	1 mol/L Na₂SO₄	22 F/g at 10 mV/s	[41]
Microsphere silicon carbide-MnO₂ nanoneedles	1 mol/L Na₂SO₄	52 F/g at 10 mV/s	[42]
SiC spheres	1 mol/L Na₂SO₄	72.4 F/g at 10 mV/s	[43]
SiC/C NSs	1 mol/L Na₂SO₄	734 μF/cm² at 10 mV/s 130 F/g at 10 mV/s	This work

Fig. 7. Schematic illustration of the mechanism for excellent electrochemical properties of SiC/C NSs.

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