Title: Study of Structural Evolution of Silicon-Based Anodes in Lithium-Ion Batteries

The need for electrification across various sectors has led to increased demand for high-performance lithium-ion batteries (LIBs). Today’s commercial LIBs typically make use of a pure-graphite anode which offers long lifespans but a relatively meager capacity of 372 mAh/g. Silicon, by comparison, offers a theoretical capacity of 3600 mAh/g but generally suffers from short life spans due to numerous effects. Combining silicon and graphite active materials to form a composite anode can result in electrodes with improved capacities over pure-graphite systems and enhanced longevity over pure-silicon ones. However, introducing silicon to an otherwise stable graphite electrode can induce failure of the electrode partly due to the volumetric expansion/contraction that silicon experiences during lithiation/delithiation cycles. Understanding the morphological evolution of silicon particles in composite electrodes - particularly in a lithiated state - can yield a more comprehensive understanding of the interactions between the active materials which will contribute to the realization of anodes with improved capacities and lifespans. To date, characterizing lithiated silicon-containing anodes has been difficult owing to the reactivity of the lithiated materials and a lack of suitable methods to probe within an electrode’s bulk. In this work, we demonstrate recent successes in imaging lithiated silicon-composite and silicon oxide-composite electrodes via micro and nanoscale computed tomography (MicroCT, NanoCT) and electrochemical analysis to quantify (1) changes in particle size distributions over charge/discharge cycles, (2) lithium content in silicon particles as a function of depth from the electrode’s surface, (3) changes in particle morphology, and (4) electrode thickness. The development of this technique represents a significant step towards characterizing the physical behavior of silicon particles within electrodes without destroying the surrounding structures.