Eco-Friendly Fabrication of Carbon Nanotubes-Reduced Graphene Oxide-Silicon for High Current Density Anode Materials of LIB

Silicon (Si) is considered a promising anode material for lithium-ion batteries (LIBs) due to its high performance. However, when Si is exposed to an electrolyte, it forms a solid electrolyte interphase (SEI) film and the following electrode decomposition results in poor performance of the LIB. Effective coverage of Si by carbon materials is an interesting potential solution to solve this problem. In this study, we prepared carbon nanotubes-reduced graphene oxide-silicon (CNTs-RGO-Si) composite materials by eco-friendly processes and showed that they can be used as a high-performance anode material for LIBs. Fabrication of the CNTs-RGO-Si composites was composed of three steps. The first step was the preparation of well dispersed CNTs-GO colloids by bead milling without any chemical treatment and then co-assembly of the CNT-GO-Si composites by spray drying the colloidal mixture. Finally, the CNT-RGO-Si was fabricated by thermal reduction of GO in the CNTs-GO-Si composite. The morphology of the as-fabricated CNTs-RGO-Si composites was generally the shape of a crumpled paper ball and the size of the composites showed a distribution of 1 to 5 µm. The highest capacitance of the CNT-RGO-Si composite after milling three times of CNTs-GO colloids was about 1634 mAh g ^− 1 during the 100-cycle charge and discharge test at 1 C high current density. The CNT-RGO-Si composites exhibited coulombic efficiency of over 96% with excellent stability.