The optimisation of battery electrode architecture is a key aspect of improving battery performance, provided that precise characterisation of the complex battery microstructure is possible. In this work, X-ray nanotomography  was used at beamline ID16B  to obtain high-resolution images of the microstructure of graphite battery electrodes, providing 3D analysis and thorough quantification of the electrode/particle inner structure and porosity at the nanoscale.
A crucial step in the production of battery-grade natural graphite for lithium-ion batteries is the spheroidisation process: the morphological change that occurs in the electrode material during cycling or charging/discharging cycles. However, the low yield (30-50%) of this process results in a large quantity of wasted graphite fines that are not suitable for use in lithium-ion batteries due to their small particle size . A method was devised to recycle waste graphite fines via a re-agglomeration process followed by a petroleum pitch coating in order to obtain aggregated graphite particles with sound mechanical strength and battery-suitable size to be used for electrode preparation. A compression step called ‘calendering’ was applied to the electrode’s coating to reduce its thickness and consequently increase its volumetric capacity.
X-ray nanotomography measurements carried out at beamline ID16B provided important microstructural details of the electrode-representative volumes (128 × 128 × 108 µm3 with 50 nm voxel size), along with statistical analysis of ~500 particles imaged in a single measurement. Data acquired on non-calendered and calendered pristine electrodes show that higher electrode density could be reached by calendering the electrode, without considerably affecting the active material accessibility through diffusion in the pore network. Despite the considerable morphological changes, no clear agglomerate fractures were observed, and particle integrity was preserved as individual agglomerate particles could still be distinguished. This highlights the fact that structural integrity is maintained from the electrode scale down to the particle level, and that the calendering process does not compromise the electrochemical performance.
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Image: lectrode and particle porosity evolution with calendering in terms of (a) pore volume fraction and (b-e) microstructure. 3D rendering views of the (b) non-calendered and (c) calendered electrodes and (d,e) corresponding isolated graphite aggregated particles (with cross-section images).