Investigation of film solidification and binder migration during drying of Li-Ion battery anodes

• Insight into the property-determining drying and solidification of electrode films.
• Characteristic drying stages are revealed by a new experimental approach.
• High drying rates trigger binder gradients throughout electrode films.
• A top-down consolidation mechanism based on capillarity and diffusion is proposed.
• The impact of drying rate on electrochemical properties is revealed.

The property determining micro-structure of battery electrodes essentially evolves during drying, appointing it a paramount, yet insufficiently understood processing step in cell manufacturing. The distribution of functional additives such as binder or carbon black throughout the film strongly depends on the drying process. A representative state-of-the-art model system comprising graphite, polymeric binder, carbon black and solvent is investigated to gain an insight into the underlying processes. A new experimental approach is introduced that allows for revelation of the evolution of binder concentration gradients throughout the film during drying. Binder is detected by means of energy-dispersive x-ray spectroscopy (EDS) at the top and bottom surface. Drying kinetics is investigated and the impact of the drying process on electrochemical performance is disclosed. The enrichment of binder at the surface, which is observed while applying high drying rates, is shown to depend on two fundamental processes, namely capillary action and diffusion. The findings reveal characteristic drying stages that provide fundamental insights into film solidification. Based on that, a top-down consolidation mechanism capable of explaining the experimental findings is disclosed. Adhesion of the active layer to the substrate is shown to strongly depend on the local binder concentration in the vicinity of the substrate.

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