Microspheres of Si@Carbon-CNTs composites with a stable 3D interpenetrating structure applied in high-performance...

The huge volumetric expansion (>300 %) of Si that occurs during the charge-discharge process makes it to have poor cycling ability and weak stable structure. These factors are considered as critical obstacles to the further development of Si as anode for lithium-ion batteries (LIBs). Herein, novel 3D interpenetrating microspheres, i.e., Si@C-CNTs, which consist of silicon nanoparticles interpenetrated with carbon nanotubes (CNTs) and stuck with amorphous carbon (C) have been designed and prepared via a spray-drying assisted approach. As anode of LIBs, Si@C-CNTs microspheres can achieve high silicon loadings of around 86 % and a high initial coulomb efficiency of 80.8 %. The electrodes maintain a reversible specific capacity of 1585.9mAh/g at 500 mA g^-1 after 200 cycles, and deliver an excellent rate capability of 756.4 mAh/g at 5 A g^-1. The outstanding performance of Si@C-CNTs can be due to their 3D interpenetrating structure and the synergy effect between the CNTs network and amorphous carbon therein. They synergistically act as conductive matrices which significantly improve the conductivity of the composite; they also act binders and reinforcing skeleton which help the composite spheres to have stable structure. Especially, the latter (reinforcing skeleton) alleviates the volumetric effect induced by the expansion and shrinkage of silicon particles during lithiation. The unique architecture provides an ideal model that can be used to design Si-based composite anode for advanced LIBs.