Visualization and Quantification of Electrochemical and Mechanical Degradation in Li Ion Batteries

TLDR

High‑energy‑density materials that undergo conversion and/or alloying reactions promise next‑generation lithium‑ion batteries, yet their substantial volume changes during electrochemical operation cause mechanical fracture and structural disintegration, leading to capacity loss. This study uses x‑ray tomography during battery operation to visualize and quantify the origins and evolution of electrochemical and mechanical degradation. Time‑resolved, three‑dimensional tomography provides chemical composition and morphology within individual particles and across the electrode during cycling. In tin(II) oxide, tomography reveals heterogeneous core‑shell lithiation, crack initiation and growth along preexisting defects, and irreversible electrode distortion, underscoring its utility for guiding durable material and strain‑tolerant electrode design.

Abstract

High-energy-density materials that undergo conversion and/or alloying reactions hold promise for next-generation lithium (Li) ion batteries. However, these materials experience substantial volume change during electrochemical operation, which causes mechanical fracture of the material and structural disintegration of the electrode, leading to capacity loss. In this work, we use x-ray tomography during battery operation to visualize and quantify the origins and evolution of electrochemical and mechanical degradation. Tomography provides the time-resolved, three-dimensional chemical composition and morphology within individual particles and throughout the electrode. In the model material tin(II) oxide, we witness distributions in onset and rate of core-shell lithiation, crack initiation and growth along preexisting defects, and irreversible distortion of the electrode, highlighting tomography as a tool to guide the development of durable materials and strain-tolerant electrodes.