The world is facing an ever-growing global energy crisis with unprecedented depth and complexity. The sustainable development of high energy density lithium-ion batteries for electric vehicles and portable electric devices has become a feasible way to deal with this problem. Silicon suboxides (SiOx) have been deemed as one of the most promising anode materials because of their ultrahigh theoretical lithium storage capacity, proper working potential, natural abundance, and environmental friendliness. However, the mass utilization of SiOx-based anodes is severely obstructed by their low electrical conductivity and inevitable volume expansion. While lithium silicate and lithium oxide formed in the first lithiation process act as buffer layers to some extent, it is urgent to address the accompanying low initial Coulombic efficiency and unsatisfactory cycling stability. In this review, we summarized recent advances in the synthesis methods of SiOx-based materials. Besides, the benefits and shortcomings of the various methods are briefly concluded. Then, we discussed the effective combination of SiOx with carbon materials and designs of porous structure, which could considerably enhance the electrochemical performance in detail. Furthermore, progresses on the modified strategies, advanced characteristics and industrial applications for SiOx-based anodes are also mentioned. Finally, the remaining challenges encountered and future perspectives on SiOx-based anodes are highlighted.
Silicon anodes with a high theoretical capacity possess great potential applications in power batteries for electric vehicles, while their volume expansion always leads to crystal pulverization and electrode polarization. An ideal solution to alleviate such pulverization and polarization of silicon crystals is to simultaneously use nano-sized silicon crystals and introduce high viscosity and elasticity polymer binders. This work has achieved the adjustable introduction of hydroxyl groups to silicon nanocrystals under the optimal reaction temperature (e.g., 80 °C) and appropriate piranha solution composition (e.g., H2SO4/H2O2 = 3:1 v/v), ultimately forming an amorphous coating layer of ~1.3 nm on the silicon surface. The optimized silicon anode exhibits superior electrochemical performance (with an initial Coulombic efficiency of 85.5%; 1121.4 mA h g−1 at 1 A g−1 after 200 cycles) and improved hydrophilicity. The introduced hydroxyl groups significantly enhance the hydrophilicity of silicon in the electrolyte and the electrochemical activity of the silicon anodes. The hydroxyl groups achieve stronger bonding between silicon and polymer binders, ultimately improving the mechanical strength and stability of the electrode. The introduction of hydrophily functional groups on the surface of silicon crystals can be explored as an active strategy to solve the above issues. This surface engineering method could be extended to more fields of infiltrating silicon-based functional materials.