SiO2@C hollow sphere anodes for lithium-ion batteries

Abstract

Abstract:

As anode materials for lithium-ion batteries, SiO₂ is of great interest because of its high capacity, low cost and environmental affinity. A facile approach has been developed to fabricate SiO₂@C hollow spheres by hydrolysis of tetraethyl orthosilicate (TEOS) to form SiO₂ shells on organic sphere templates followed by calcinations in air to remove the templates, and then the SiO₂ shells are covered by carbon layers. Electron microscopy investigations confirm hollow structure of the SiO₂@C. The SiO₂@C hollow spheres with different SiO₂ contents display gradual increase in specific capacity with discharge/charge cycling, among which the SiO₂@C with SiO₂ content of 67?wt% exhibits discharge/charge capacities of 653.4/649.6?mA?h?g^-1 over 160 cycles at current density of 0.11?mA?cm^-2. The impedance fitting of the electrochemical impedance spectroscopy shows that the SiO₂@C with SiO₂ content of 67?wt% has the lowest charge transfer resistance, which indicates that the SiO₂@C hollow spheres is promising anode candidate for lithium-ion batteries.

Key words: Silica, Hollow spheres, Carbon coating, Anode, Lithium-ion batteries

Liu Xuelian,Chen Yuxi,Liu Hongbo,Liu Zhi-Quan. SiO2@C hollow sphere anodes for lithium-ion batteries[J]. J. Mater. Sci. Technol., 2017, 33(3): 239-245.

Figures/Tables 13

Fig. 1. Schematic of fabrication process of the SiO2@C hollow spheres. SiO2 shell is formed on the PAA sphere template, and then carbon coating layer covers the shell after calcination of the template.

Fig.2. Schematic of fabrication process of the SiO2@C hollow spheres. SiO2 shell is formed on the PAA sphere template, and then carbon coating layer covers the shell after calcination of the template.

Fig. 3. SEM images of (a) SiO2@C-1.5, (b) SiO2@C-2 and (c) SiO2@C-2.5.

Fig. 4. TEM images of (a) SiO2@C-1.5, (b) SiO2@C-2 and (c) SiO2@C-2.5.

Fig. 5. (a) HAADF image of SiO2@C-2 and the corresponding element mapping images of (b) O, (c) Si and (d) C.

Fig. 6. CV profiles of (a) SiO2@C-1.5, (b) SiO2@C-2 and (c) SiO2@C-2.5 in the 0.001-3.0?V voltage window.

Fig. 7. Voltage profiles of (a) SiO2@C-1.5, (b) SiO2@C-2 and (c) SiO2@C-2.5 with current density of 0.11?mA?cm-2 and cutoff voltages of 0.001-3.0?V.

Fig. 8. Cyclic behavior and coulombic efficiencies of SiO2, SiO2@C-1.5, SiO2@C-2 and SiO2@C-2.5.

Fig. 9. (a) XPS survey spectrum of the SiO2@C-2 after 50 discharge/charge cycles; Enlarged (b) Si2p and (c) O1?s spectra of the SiO2@C-2 after 50 discharge/charge cycles.

Fig. 10. SEM image of the electrode of SiO2@C-2 after 160 lithiation-delithiation cycles.

Table 1 Electrochemical performance of SiO2 and SiO2-C composite anodes for lithium-ion batteries.

Materials	Content of SiO₂(wt%)	Current density	Initial discharge/charge specific capacity (mA?h?g^-1)	Reversible capacity (mA?h?g^-1)/cycle number (n)	Ref.
SiO₂ thin film	100	28?μA?cm^-2	539/388	510/100	[23]
SiO₂ nanocubes	100	100?mA?g^-1	3084/1457	919/30	[25]
Carbon-coated SiO₂nanopaticles	50.1	50?mA?g^-1	536/Ca.900	Above 500/50	[17]
Silicon oxide-carbon	95.8	70?mA?g^-1	1055/458	601/100	[20]
Carbon-coated silica macroparticles	—	0.2?mA?cm^-2	281/95	222/100	[26]
SiO2@graphene composite	—	500?mA?g^-1	—	Ca. 300/110	[19]
SiO₂@C hollow spheres	67	0.11?mA?cm^-2	318.7/153.6	649.6/160	This work

Fig. 11. The Nyquist plots of (a) SiO2, (b) SiO2@C-1.5, (c) SiO2@C-2 and (d) SiO2@C-2.5. The solid curves represent quantitative fitting data. (e) The equivalent circuit for quantitative simulation of the Nyquist plots.

Fig. 12. Plots of Rct as function of cycle number of SiO2, SiO2@C-1.5, SiO2@C-2 and SiO2@C-2.5.

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