Expanding the metrology of Coulombic efficiency using neutron depth profiling

The metrology of Coulombic efficiency (CE) is widely used for the qualification of rechargeable batteries particularly in assessing their state of health and the expected lifetime. The quantity of CE is conventionally defined as the ratio of the electric charge capacity in one round-trip cycle of discharge and charge of a battery. For better diagnosis of the health, failure and lifetime of rechargeable batteries, it is desirable to expand the traditional CE of the round-trip electric charge to including that of the round-trip CE of ionic charges as well as those of single trip CEs of ionic/electric charges for charging and electric/ionic charges for discharging. To enable such expansion, in operando ion metrology is needed. For the mainstream technology of lithium-containing batteries, neutron depth profiling is one of the techniques suited for Li ion metrology. In this report, we demonstrate the application of in situ neutron depth profiling to expanding the metrology of Coulombic efficiencies to include all four CEs. The methodology of expanded CE is exemplified using measurements and analyses on a model battery of LiFePO₄ vs. Li.