Electrostatically Assembled Silicon–Carbon Composites Employing Amine-Functionalized Carbon Intra-interconnections for Lithium-Ion Battery Anodes

Recently, the development of silicon-based anodes for lithium-ion batteries has attracted tremendous attention for overcoming the disadvantages of commercial graphite-based anodes. In this work, we suggest a chemical methodology of synthesizing silicon–carbon composite anodes, with capacity values of 763 and 182 mAh/g at current densities of 0.1 and 5 A/g, respectively. An electrostatic assembly technique is designed to be triggered by a cationic polyelectrolyte, poly(ethylenimine), for negatively charged silicon nanoparticles and graphene oxides. Amine-functionalized carbon nanotubes are synthesized in a nondestructive fashion and incorporated additionally to provide intraconnected conductive pathways between neighboring composite materials. It is revealed that the electrochemical performance of intraconnected composite materials is determined by the chemical/physical factors of constituent compartments. The applicability toward all-solid-state batteries is also suggested with usage of a solid polymer electrolyte synthesized from a mixture of bisphenol A ethoxylate diacrylate, polyethylene glycol dimethyl ether, tert-butyl peroxypivalate, and bis(trifluoromethane)sulfonimide lithium salt.