Structural Change of Carbon Anode in a Lithium-ion Battery Product Associated with Charging Process Observed by Neutron Transmission Bragg-edge Imaging

Spectroscopic neutron Bragg-edge imaging was performed to study a lithium-ion battery (LIB) product. This non-destructive neutron imaging method is suitable for the evaluation of industrial products, but presents some difficulties for application to multicomponent products. The LIB includes a strong neutron scatterer and an absorber, and is thus a suitable test case for the use of neutron imaging in actual product measurement. In this study, we analyzed the variation of the graphite anode structure with changes in the battery charge level. The experiments were carried out using the compact neutron source at the Hokkaido University neutron source facility (HUNS). To eliminate the effect of scattered neutron contamination, we first determined the distance between the sample and detector required to reduce this effect to under 1%. Using this separation, the charge level dependence of the anode structure was measured. The graphite {002} Bragg-edge could be recognized on the neutron transmission spectra. The Bragg-edge was shifted and broadened with increasing battery charge. The edge was consistent with the existence of multiple graphite structural stages. The layer spacing distribution images for different charge levels showed the inhomogeneous fluctuation on the LIB lattice plane. Based on the images the fraction of the graphite structural stages were analyzed. The ratio of each stage varied with the charge level, and the ideal intercalation structure, in which the graphite layers are stuffed with Li-ions, was found to be minor in the final charging state.