In-situ observation of inhomogeneous degradation in large format Li-ion cells by neutron diffraction

This work presents a non-destructive in-situ method for probing degradation mechanisms in large format, operating, commercial lithium-ion batteries by neutron diffraction. A fresh battery (15 Ah capacity) was shown to have a uniform (homogeneous) local state of charge (SOC) at 4.0 V (9 Ah SOC) and 4.2 V (15 Ah SOC), with 1.33 C and 2.67 C charging rates, respectively. This battery was then aggressively cycled until it retained only a 9 Ah capacity, 60% of its original value. Inhomogeneous deterioration in the battery was observed: near the edges, both the graphite anode and the spinel-based cathode showed a significant loss of capacity, while near the central area, both electrodes functioned properly. An SOC mapping measurement of the degraded battery in the fully charged state (4.2 V) indicated that the loss of local capacity of the anode and cathode is coupled. ► In-situ probe degradation mechanisms in large format cells by neutron diffraction. ► The fresh cell has a spatially uniform (homogeneous) local state of charge. ► The degraded cell shows a spatially inhomogeneous deterioration. ► Capacity losses in the cathode and anode are coupled. ► Remediation strategies should focus on location-specific issues in the cell.