An Innovative Insight into Performance Degradation of NCM111 Cathode Induced by Suspension of Operation

The lifespan of lithium-ion batteries varies enormously from fundamental study to practical applications. This big difference has been typically ascribed to the high degree of uncertainty in unpredictable and complicated operation conditions in real-life applications. Here, we report that the pause of the charging−discharging process, which is frequently operated in practice but rarely studied in academics, is an important reason for the performance degradation of the NCM111 cathode. It is found that the pause during cycling could trigger a remarkable drop in capacity, giving rise to ∼30% more capacity decay compared with the continuously cycled sample. In situ synchrotron X-ray diffraction analysis reveals that the harmful H1−H2 phase transition, which typically appears in the initial cycle but disappears in subsequent cycles, is reactivated by the pausing process. The anisotropic lattice strains that occur during the H1−H2 transition result in mechanical fractures that terminate with an inert NiO-type rock-salt phase on the surface of particles. The present study indicates that the discontinuous usage of rechargeable batteries is also a key factor for cycle life, which might provide a distinct perspective on the performance decay in practical applications. © 2023 American Chemical Society.