Solvent-Free Fabrication of Thick Electrodes in Thermoplastic Binders for High Energy Density Lithium-Ion Batteries.

The rapid development of electric vehicles has generated a recent demand for high energy density lithium-ion batteries (LIBs). One simple, effective way to enhance energy density of LIBs is to increase the thickness of electrodes. However, the conventional wet process used to fabricate thick electrodes involves the evaporation of large amounts of organic solvents, which causes an inhomogeneous distribution of conductive additives and binders. This weakens the mechanical and electrochemical network between active materials, resulting in poor electrochemical performance and structural degradation. Herein, we introduce a new strategy to produce homogeneous thick electrodes by using a dry, solvent-free process. Instead of using a conventional PVDF (polyvinylidene fluoride) binder, we employed a phenoxy resin as the binder in dry process for the first time. This thermoplastic binder exhibits better ductile properties than PVDF in the way that it generates a uniform network structure that connects the active materials during the hot press process. This enables the production electrochemically stable electrodes without using organic solvents, which record capacity retention rates of 73.5% over 50 cycles at a 40 mg/cm2 of thick electrodes. By contrast, thick electrodes produced with a PVDF binder via wet processing only have a capacity retention rate of 21.8% due to rapid structural degradation.

Synergetic Effect of Hybrid Conductive Additives for High-Capacity and Excellent Cyclability in Si Anodes.

Silicon is a promising anode material that can increase the theoretical capacity of lithium-ion batteries (LIBs). However, the volume expansion of silicon remains a challenge. In this study, we employed a novel combination of conductive additives to effectively suppress the volume expansion of Si during charging/discharging cycles. Rather than carbon black (CB), which is commonly used in SiO anodes, we introduced single-walled carbon nanotubes (SWCNTs) as a conductive additive. Owing to their high aspect ratio, CNTs enable effective connection of SiO particles, leading to stable electrochemical operation to prevent volume expansion. In addition, we explored a combination of CB and SWCNTs, with results showing a synergetic effect compared to a single-component of SWCNTs, as small-sized CB particles can enhance the interface contact between the conductive additive and SiO particles, whereas SWCNTs have limited contact points. With this hybrid conductive additive, we achieved a stable operation of full-cell LIBs for more than 200 cycles, with a retention rate of 91.1%, whereas conventional CB showed a 74.0% specific capacity retention rate.