Construction of a core–double-shell structured Si@graphene@Al2O3 composite for a high-performance lithium-ion battery anode

Abstract

The vast volume expansion of the Si anode during the charging process leads to rapid cycling performance fading and limits its applications in lithium-ion batteries. In this study, a unique core–double-shell structured porous Si@graphene@glycerin-Al₂O₃ (p-Si@G@g-Al₂O₃) composite is successfully prepared by using a porous Si (p-Si) microsphere as the core and graphene(G)/Al₂O₃ as the double shell layer via an electrostatic self-assembly strategy and a glycerin-involved sol–gel process. The addition of glycerin can reduce the nucleation growth rate of Al(OH)₃ during the sol–gel process and enable more uniform deposition of an ultrathin Al₂O₃ layer on p-Si@G microspheres. Owing to the crucial role of the lithiated Al₂O₃ (LiAlO₂)/G double shell layer in shielding the inner p-Si microsphere from the electrolyte and consolidating the mechanical structure of the p-Si microsphere, the synthesized p-Si@G@g-Al₂O₃ shows good cycling stability with a high reversible capacity of 1804.5 mA h g⁻¹ at 0.2 A g⁻¹ and excellent rate capacity with a capacity of 439 mA h g⁻¹ at 8 A g⁻¹, superior to those of p-Si@G and p-Si electrodes. Moreover, the electrochemical performance of p-Si@G@g-Al₂O₃ can also be further improved by ∼10% by only adding 5 wt% of carbon nanotubes (CNTs) in a slurry, due to the good capability of CNTs in building the interconnecting network between p-Si@G@g-Al₂O₃ microspheres.