Inhomogeneous degradation induced by lithium plating in a large-format lithium-ion battery

Abstract

With the demand for high-energy-density power sources for electric vehicles, large-format lithium-ion batteries are widely applied, considering their advantages in reducing the weight of inactive materials. However, large-format cells suffer from internal inhomogeneities, which become the bottleneck limiting their performance. Here, the inhomogeneous degradation in a large-format pouch cell is comprehensively investigated using a series of (non-)destructive techniques. Spatial-resolved deformation detection and ultrasonic diagnostics are utilized to study the evolution of inhomogeneity inside the large-format battery. Localized deformation and deposits are found to firstly appear at the tab-near regions and then propagate into central regions, which is identified by characterization tests to be induced by lithium plating. The inhomogeneous degradation mechanism inside the battery is summarized as an initiation-propagation process. During the process, lithium deposit is initiated by a local high current density, resulting in the local separator pore closure. Pore closure in the separator in return creates a high current density and overpotential in the adjacent area, leading to a continuous propagation of the lithium deposition area. Finally, an effective indicator—peak height in the differential voltage curve is proposed to detect the inhomogeneity in the battery, and thus offers guidance to the design and management of large-format cells.