Modeling of lithium plating induced aging of lithium-ion batteries: Transition from linear to nonlinear aging

A physics-based Li-ion battery (LIB) aging model accounting for both lithium plating and solid electrolyte interphase (SEI) growth is presented, and is applied to study the aging behavior of a cell undergoing prolonged cycling at moderate operating conditions. Cell aging is found to be linear in the early stage of cycling but highly nonlinear in the end with rapid capacity drop and resistance rise. The linear aging stage is found to be dominated by SEI growth, while the transition from linear to nonlinear aging is attributed to the sharp rise of lithium plating rate. Lithium plating starts to occur in a narrow portion of the anode near the separator after a certain number of cycles. The onset of lithium plating is attributed to the drop of anode porosity associated with SEI growth, which aggravates the local electrolyte potential gradient in the anode. The presence of lithium metal accelerates the porosity reduction, further promoting lithium plating. This positive feedback leads to exponential increase of lithium plating rate in the late stage of cycling, as well as local pore clogging near the anode/separator interface which in turn leads to a sharp resistance rise.