Low‐Temperature Charging and Aging Mechanisms of Si/C Composite Anodes in Li‐Ion Batteries: An Operando Neutron Scattering Study

The addition of Si compounds to graphite anodes has become an attractive way of increasing the practical specific energies in Li-ion cells. Previous studies involving Si/C anodes lacked direct insight into the processes occurring in full cells during low-temperature operation. In this study, a powerful combination of operando neutron diffraction, electrochemical tests, and post-mortem analysis is used for the investigation of Li-ion cells. 18650-type cylindrical cells in two different aging states are investigated by operando neutron diffraction. The experiments reveal deep insights and important trends in low-temperature charging mechanisms involving intercalation, alloying, Li metal deposition, and relaxation processes as a function of charging C-rates and temperatures. Additionally, the main aging mechanism caused by long-term cycling and interesting synergistic effects of Si and graphite are elucidated.