Impact of binder content on particle fracture and microstructure of solvent-free electrodes for Li-ion batteries

Abstract

The fraction of polytetrafluoroethylene (PTFE) binder in solvent-free electrodes for Li-ion batteries, also known as dry-processed electrodes, is shown to have a dramatic impact on their processability, microstructural evolution and electrochemical performance. We show experimentally that increasing the binder fraction from 0.5 to 4 wt% transformed the electrode microstructure from an effective, open structure containing PTFE nano-fibrils to a compact morphology with fragmented active material and porosity blocked by PTFE agglomerates. The solvent-free electrodes showed a classic visco-elastic response during compression, comprising three distinct regions of deformation. The electrode stiffness and yield strength increased non-linearly with binder fraction such that for higher binder contents (>2 wt%), there was extensive LiNi_0.6Co_0.2Mn_0.2O₂ (NMC) particle fracture during the calendering process, with cracks propagating along the grains of polycrystalline NMC particles. Conversely at lower binder fraction (<2 wt%), PTFE readily fibrillated into highly textured (100) crystalline nano-fibrils and NMC particles remained largely intact. These electrodes showed superior electrochemical performance due to higher ionic mobility through the open nano-fibrillar microstructure and intact NMC particles.