Capillary suspensions as beneficial formulation concept for high energy density Li-ion battery electrodes

We introduce a novel formulation concept to prepare high capacity graphite electrodes for lithium ion batteries. The concept is based on the capillary suspension phenomenon: graphite and conductive agent are dispersed in an aqueous binder solution and the organic solvent octanol is added as immiscible, secondary fluid providing the formation of a sample-spanning network resulting in unique stability and coating properties. No additional processing steps compared to conventional slurry preparation are required. The resulting ultra-thick electrodes comprise mass loadings of about 16.5 mg cm−2, uniform layer thickness, and superior edge contours. The adjustment of mechanical energy input ensures uniform distribution of the conductive agent and sufficient electronic conductivity of the final dry composite electrode. The resulting pore structure is due to the stable network provided by the secondary fluid which evaporates residue-free during drying. Constant current-constant potential (CC-CP) cycling clearly indicates that the corresponding microstructure significantly improves the kinetics of reversible Li+ (de-) intercalation. A double layer electrode combining a conventionally prepared layer coated directly onto the Cu current collector with an upper layer stabilized with octanol was prepared applying wet-on-wet coating. CC-CP cycling data confirms that staged porosity within the electrode cross section results in superior electrochemical performance.