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The hollow Si nanospheres modified by the mechanically robust titanium dioxide (TiO 2 ) shell and the uniform carbon layer are intentionally designed and successfully prepared as the anode active material of high performance lithium-ion batteries. The effects of the robust TiO 2 shell and the uniform carbon layer on the structure and electrochemical performances for the Si@TiO 2 @C nanospheres are studied in detail by X-ray photoelectron spectroscopy, transmission electron microscopy, X-ray diffraction and charge/discharge tests. The results show that the hollow structure of the Si core can spontaneously absorb the huge volume expansion stress, the robust TiO 2 shell is used as a compact fence to promote the expansion towards the interior of the Si cavity instead of the exterior in the processes of charge/discharge, and the uniform carbon layer can effectively enhance the electrical conductivity and further control the integrity and stability of the well-wrapped core-shell-shell framework. Typically, the resultant hollow Si@TiO 2 @C nanospheres exhibit a high initial discharge capacity of 2557.1 mAh g −1 with coulombic efficiency of 86.06% as well as a large recuperative discharge capacity of 1270.3 mAh g −1 after 250 cycles at 1 A g −1 with a mean coulombic efficiency of 99.53%. Therefore, the hollow Si@TiO 2 @C nanospheres prepared by one-step sol-gel coating process show outstanding electrochemical properties and are considered as a prospective candidate to the adhibitions of the anode material for new generation power LIBs. [ABSTRACT FROM AUTHOR]

• Construct carbon protective shell to alleviate huge volume changes of Si. • Robust carbon framework can effectively maintains the structure integrity. • Carbon buffer layer can offer rich e-/ion channels to improve reaction kinetics. • The SCM electrode exhibited excellent electrochemical performance. Si-based anodes have revealed the potential as the next generation of lithium ion battery anode material, whereas the poor conductivity and huge volume changes during (de)lithiation process of silicon still limit their practical application. Herein, the Si/nitrogen doped carbon layer/carbon framework microspheres (SCM) are designed by nano-Si via electro-spray technology as anodes for lithium ion batteries. It has been found that the SCM consists of individual carbon-coated nano-Si primary particles linked by PAN framework, in which the carbon buffer layer can further absorb the stress of volume changes during charge/discharge process, and the carbon framework carbon framework not only provides fast diffusion path of electron, but also effectively reduces the consumption of electrolyte. Therefore, the initial columbic efficiency (ICE) of SCM anode can reach as high as 72%, and the SCM anode also shows a high specific capacity of 1192 mAh g−1 at 0.2 A g−1 and keeps a reversible capacity of 746 mAh g−1 after 200 cycles, demonstrating the as-designed SCM possesses an high ICE and a good electrochemical performance. This strategy provides a significant inspiration for fabricating high-performance Si/C anode materials of lithium-ion battery. [ABSTRACT FROM AUTHOR]