Dispersant‐Free Colloidal and Interfacial Engineering of Si‐Nanocarbon Hybrid Anode Materials for High‐Performance Li‐Ion Batteries

Abstract Highly conducting nanomaterials have garnered significant attention owing to their potential application in Li‐ion batteries for stable electrodes. However, concerns persist regarding their dispersion and effective hybridization with active materials. This study reports a novel approach to enhance Si‐based anode materials using less defective graphene oxide (C‐GO) and highly oxidized single‐walled carbon nanotubes (C‐SWCNTs) fabricated using chlorate‐based oxidation. The method involves encapsulating Si alloy (SiA) particles with C‐GO and C‐SWCNTs, eliminating the need for additional additives. Composite structures with lithiophilic N‐doped SWCNTs and highly crystalline reduced C‐GO coatings on SiA surfaces are created through spray drying and subsequent chemical reduction. This unique combination yields high capacities, stable retention behaviors, and remarkable initial capacities (1224 mAh g⁻¹) with excellent retention rates (82.3% at 100 cycles, 0.1 C). A LIB full‐cell with a SiA/nanocarbon anode exhibited a high energy density of 350 Wh kg⁻¹, while maintaining 65% capacity retention after 200 cycles. The findings demonstrate the potential of this hybrid approach, which eliminates the need for other conducting additives while maintaining a minimal binder content (5 wt.%). This study presents a promising approach for enhancing Si‐based anode materials in lithium‐ion batteries, addressing the dispersion and hybridization challenges in nanomaterial‐enabled electrode design.