Three dimensional studies of particle failure in silicon based composite electrodes for lithium ion batteries

Abstract

Silicon based composite electrodes for lithium ion batteries are of significant interest because of their potential to be high capacity alternatives to the commonly used graphitic carbon anodes. A drawback to their use, however, is the Si particle debonding and fracture that occurs as a result of the volumetric expansion by the lithium host particles upon lithiation of the anode electrode. We use X-ray micro computed tomography to visualize the evolution of the internal microstructure of a silicon-based electrode before and after four lithiation steps during the first half cycle of the cell. We develop a novel threshold edge detect method to perform 3D volumetric measurements of silicon particle expansion. According to our results, 100% lithiation of the composite anode resulted in up to 290% volume expansion of individual Si particles. Furthermore, the global and localized image intensity histogram profiles from 3D data were used to analyze the silicon particle X-ray attenuation effects as a function of lithiation: a decreasing attenuation with lithiation and the propagation of the reaction front through a core–shell process between the original state and 25% lithiation of the silicon-based electrode have been observed.