Silicon/CNTs/Graphene Free-standing Anode Material for Lithium-ion Battery

doi:10.15541/jim20160520

Abstract

Abstract:

Porous 2D Silicon/CNTs/Graphene free-standing composites were prepared via a solution-based self-assembly process with vapor post-treatment and applied as anodes for lithium-ion batteries. Silicon nanoparticles (~50 nm) as active materials were uniformly embedded between graphene sheets without agglomeration. Graphene was used as electrical conductive carbon matrix to form a 2D conductive network for electrons. CNTs, with high electrical conductivity and mechanical strength, formed into a scaffold along with graphene to enhance the conductivity and mechanical properties of the carbon matrix. After vapor post-treatment, CNTs supported graphene film transferred from a tightly stacked film to a loose packed porous film. The porous structure of this free-standing composite anode provides large internal space to accommodate volumetric changes and provide abundant channels for diffusion of Li⁺, fast electron transport and easy penetration of electrolyte. The composites exhibite an outstanding rate performance and cyclic stability, delivering a capacity of 600 mAh/g at 4/A g and 1010 mAh/g after 100 cycles at 0.1 A/g. They also show high structure and mechanical stability after cycle test. It provides an exciting pathway to the rational design and fabrication of silicon anode and 2D graphene matrix for applications in lithium-ion batteries.

Key words: graphene, silicon, lithium-ion battery, free-standing, vapor post-treatment

CLC Number:

TM911
O613

BAI Xue-Jun, LIU Chan, HOU Min, WANG Biao, CAO Hui, FU Jun-Jie. Silicon/CNTs/Graphene Free-standing Anode Material for Lithium-ion Battery[J]. Journal of Inorganic Materials, 2017, 32(7): 705-712.

Figures/Tables 12

Fig. 1 Schematic illustration of synthesis of Si/CNTs/GP composites

Fig. 2 Zeta potential of GO and PDDA-GO at different pH

Fig. 3 XRD patterns of Si, CNTs, Si/GP, Si/CNTs/GO, and Si/CNTs/GP composite film

Fig. 4 Raman spectra of CNTs, Si/GP, Si/CNTs/GO and Si/CNTs/GP composite film

Fig. 5 XPS spectra of CNTs, Si/GP, Si/CNTs/GO, and Si/CNTs/GP composite(a) Survey spectra; (b) High resolution C1s spectra; (c) High resolution N1s spectra; (d) High resolution Si2p spectra

Fig. 6 TGA curves of Si, GP, Si/GP, and Si/CNTs/GP-(1, 2) composites in air

Fig. 7 Surface and cross-section FESEM images of (a,b,c) Si/GP, (d, e, f) Si/CNTs/GO, and (g, h, i) Si/CNTs/GP with digital photo inset

Fig. 8 CV curves of Si/CNTs/GP-1 composite

Fig. 9 Rate capacity of Si/GP and Si/CNTs/GP-(1, 2) at various rates as marked

Fig. 10 FESEM images of (a, b) Si/GP and (c, d) Si/CNTs/GP-1 anode after rate cycling test, with EDS inset

Fig. 11 Electrochemical impedance spectra of Si/GP and Si/CNTs/GP composites after rate cycling test The inset is the equivalent circuit

Table 1 EIS fitting results of Si/GP and Si/CNTs/GP-(1, 2) electrodes

Sample	R_s/Ω	R_SEI/Ω	R_ct/Ω
Si/GP	3.5	22.1	25.2
Si/CNTs/GP-1	2.5	8.7	19.9
Si/CNTs/GP-2	2.0	1.7	18.1

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