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Silicon is a good alternative to conventional graphite anode but it has bad cycling and rate performance. To overcome these severe problems, extensively interconnected silicon nanoparticles using carbon network derived from ultrathin cellulose nanofibers were synthesized. Ultrathin cellulose nanofibers, an abundant and sustainable material, entangle each silicon nanoparticle and become extensively interconnected carbon network after pyrolysis. This wide range interconnection provides an efficient electron path by decreasing the likelihood that electrons experience contact resistivity and also suppresses the volume expansion of silicon during lithiation. In addition, Ultrathin cellulose nanofibers are carboxylated and therefore adhesive to silicon nanoparticles through hydrogen bonding. This property makes ultrathin cellulose the perfect carbon source when making silicon composites. As a consequence, it exhibits 808 mAh g −1 of the reversible capacity after 500 cycles at high current density of 2 A g −1 with a coulombic efficiency of 99.8%. Even at high current density of 8 A g −1 , it shows a high reversible discharge capacity of 464 mAh g −1 . Moreover, extensively interconnected carbon network prevents the formation of a brittle electrode with a water-based binder. Therefore, this remarkable material has a huge potential for LIBs applications. [ABSTRACT FROM AUTHOR]

• TEMPO-oxidized cellulose nanofiber (TOCNF) is suitable for versatile additive. • The TOCNF can cat as both reinforcing fiber and assistant binder in silicon anode. • Its carboxylic groups can make intimate adhesion with silicon via hydrogen bonding. • The addition of a small amount (1 wt%) of TOCNF exhibits good cycling performance. • Enhanced mechanical properties and stress distribution are attributed to the TOCNF. Silicon (Si) has been considered the most promising anode material for next-generation lithium-ion batteries due to its high theoretical capacity and natural abundance. However, the Si anode suffers from massive volume change, which results in challenging cycling performance. Many researches demonstrated that polymeric binder plays an important role to sustain the structural integrity of Si anodes. While most studies about the binder material have been focused on enhancing distinctive properties such as adhesive strength and mechanical property, it has been recently shown that binder distribution can help to improve electrochemical performance. Herein, we introduce TEMPO-oxidized cellulose nanofiber (TOCNF) as a versatile additive for the binder of silicon anode. The one-dimensional morphology of TOCNF efficiently reinforces the mechanical properties of the electrode. The TOCNF additive also contains carboxylic groups with sufficient flexibility to induce intimate interaction with Si via hydrogen bonding. Based on all of these beneficial features of TOCNF, the addition of ~ 1 wt% of TOCNF of the whole weight of silicon anode slurry significantly improved cycling stability. With pre-mixing, the resulting Si-TOCNF allows efficient water-based binder solution penetration, thus improving uniform binder distribution of electrode. Furthermore, the well-distributed binder protects silicon surface and forms a stable SEI layer. The current study suggests that the TOCNF additive facilitates uniform binder distribution in the electrode with enhanced mechanical properties, leading to improved cycling performance. Image, graphical abstract [ABSTRACT FROM AUTHOR]