Soutenance de thèse : Abhilash VALISAMMAGARI

« Strain Evolution and Mechanical Failure in SiOx-Graphite Blend Electrodes for Li-Ion Batteries: An Experimental and Simulation Study »

Doctorant : Abhilash VALISAMMAGARI

Laboratoire INSA : MATEIS

École doctorale : ED34 : Matériaux de Lyon

Silicon is identified as a promising material for negative electrodes in next-generation lithium-ion batteries due to its high lithium storage capacity of 3579 mAh/g, which is nearly 10 times higher than the conventional graphite electrode capacity of 372 mAh/g. However, silicon's practical use faces critical challenges due to its volumetric expansion (up to 300%) during lithiation and delithiation cycles. This leads to mechanical degradation, such as electrode delamination and particle detachment, which diminishes performance and cycle life. To address these issues, researchers have turned to silicon oxides (SiOx), which offer a balance between high capacity and cycling stability by reducing volumetric expansion. Although SiOx has a lower capacity than pure silicon, it still outperforms graphite electrodes. However, the mechanical challenges like particle detachment are still existing, but, to a lesser extent than pure silicon. The objective of this thesis is to observe and understand the impact of particle swelling on the overall structural integrity of the electrode. Particularly, focussing on the loss of connectivity in the electrode and to extract possible information for optimizing SiOx-containing electrodes. For this puropose, experimental investigations, including synchrotron tomography and digital volume correlation, were used to gain high-resolution insights into both global and local strain field distribution within the electrode. Later, considering the granular structure of the electrodes, a particle-based method called Discrete Element Method (DEM) was employed to represent the microstructure of the electrode, and considering the insights from the experimental investigation such as the evolution of strains at the electrode scale, the coupling of particle swelling was performed to reproduce the global strain. Finally, the corresponding impact at the electrode scale swelling and the resulting detachement of the particles was assesed by conducting connectivity study on the assembly.