Direct Observation of Li-Ion Transport in Electrodes under Nonequilibrium Conditions Using Neutron Depth Profiling

One of the key challenges of Li-ion electrodes is enhancement of (dis)charge rates. This is severely hindered by the absence of a technique that allows direct and nondestructive observation of lithium ions in operating batteries. Direct observation of the Li-ion concentration profiles using operando neutron depth profiling reveals that the rate-limiting step is depended not only on the electrode morphology but also on the cycling rate itself. In the LiFePO4 electrodes phase nucleation limits the charge transport at the lowest cycling rates, whereas electronic conductivity is rate limiting at intermediate rates, and only at the highest rates ionic transport through the electrode is rate limiting. These novel insights into electrode kinetics are imperative for the improvement of Li-ion batteries and show the large value of in situ NDP in Li-ion battery research and development.