Volume and thickness change of NMC811|SiOx-graphite large-format lithium-ion cells: from pouch cell to active material level

In this study, the reversible thickness change of a large-format lithium-ion automotive pouch cell is investigated under precisely monitored cell pressure and temperature using an in-house built actively controlled pneumatic cell press. The quantitative and qualitative contribution of the state-of-the-art NMC811 cathode and the SiOx-graphite composite anode to the total pouch cell expansion is resolved by electrochemical dilatometry and validated. Results show that Ni-rich cathodes have a significant impact on the pouch cell expansion and exhibit highly nonlinear thickness change which is related to the change of the individual lattice parameters of the crystal structure. To resolve the contribution of both anode active materials to the total anode expansion, the capacities of SiOx and graphite are determined by differential voltage analysis and validated with half-cell measurements. Then, the volume expansion of SiOx and graphite as a function of the anode state of charge is calculated. By introducing fitting parameters and applying theories about the interaction of SiOx with the surrounding morphology the correlation between the volume expansion of the active materials and the thickness change of the SiOx-Gr composite anode is investigated. The findings suggest that there is significant nonlinear reduction of pore volume at low state of charge.