The relatively low coulombic efficiency (CE), especially the high initial capacity loss (ICL), and short cycle life are two major obstacles limit the wide adoption of Si-based materials as anodes of commercial lithium-ion batteries (LIBs). In this work, we introduced an aqueous binary binder composed of polyacrylic acid (PAA) and a water-soluble polymer to a Si-based electrode. Used as anodes of LIBs, the Si-based electrodes with the binary binder exhibited lower ICL and longer cycle life than those with PAA binder. The improved battery performance is ascribed to the unique electrode structure with the binary binder. The analysis from Fourier-transform infrared spectroscopy (FTIR) reveals that the intermolecular hydrogen bonds has been formed between PAA and the new polymer. The formation of hydrogen bonds could affect the properties of slurry for electrode coating and the structure of dried electrodes. Compared to the PAA binder, the new binary binder increases the viscosity of aqueous slurries at low shear rates and prompts the shear thinning, which benefit the preparation of slurries with high stability. Observations from the electron microscopy reveal that a relative porous structure was generated in the electrodes with the binary binder, compared with those with PAA binder. The porous structure could not only facilitate the electrolyte transport, but also accommodate the large volume expansion of Si during the charge/discharge processes. In addition, a thin solid-electrolyte-interface (SEI) film was found at the surface of cycled electrodes with the binary binder.

Key words: aqueous binder coulombic efficiency Si-based anode lithium-ion battery