Fracture of lithium-ion battery electrodes is found to contribute to capacity fade and reduce the lifespan of a battery. Traditional fracture models for batteries are restricted to consideration of a single, idealised particle; here, advanced X-ray computed tomography (CT) imaging, an electro-chemo-mechanical model and a phase field fracture framew. ••Realistic fracture predictions in an entire electrode microstructure.••Highly heterogeneous electrochemical and fracture response is predicted.••Prediction of elevated cracking due to enlarged cycling voltage windows.••Cracking shown to occur as a function of electrode thickness.••Increasing damage as the rate of discharge is increased.Lithium-ion batteryImage-based modelPhase fieldFractureElectrodeMicrostructureLithium-ion batteries (LIBs) are at the forefront of the effort to reduce global CO2 emissions. For example, the transition from the fossil fuel-based internal combustion engine to the electrical vehicle (EV) is growing at an increasingly rapid rate, a transition in which LIBs play a pivotal role. The lifespan of any technology is a crucial factor when sustainability is concerned, and for such a pivotal technology as the LIB, it is no exception. The lifespan of LIBs is known to be severely limited by cracking of the electrode components [1,2]. The electrodes within LIBs are a complex multi-material composite and their microstructure typically comprises active particles in which lithium is extracted or inserted, a binder that provides a conductive network for electronic conductivity, and a porous network that permits conduction of lithium-ions via an electrolyte. During charge or discharge, swelling or shrinking of the particles occurs due to insertion or extraction of lithium, giving a highly heterogeneous stress state. Consequently, pre-existing particle defects such as voids or cracks promote fracture, enabling disintegration of the particles and eventual loss of useable energy storage volume. The microstructural evolution of LIB electrodes is therefore central to overall battery performance and, in particular, the long-term degradation and lifespan.Mechanics plays a significant role in both solid-state lithium transport and the. Consider the schematic of a battery half-cell in Fig. 1a: we define a separator, electrode surface, current collector and a heterogeneous electrode domain comprising of active material, bound together by carbon additives, i.e. CBD, and micropores filled with electrolyte. Fig. 1b shows the image-based 3D domain to which the following theoretical fra.
