Investigation of the Influence of Silicon Oxide Content on Electrolyte Degradation, Gas Evolution, and Thickness Change in Silicon Oxide/Graphite Composite Anodes for Li-Ion Cells Using Operando Techniques

Abstract

This research paper investigates the influence of varying silicon oxide (SiOx) content on the performance and aging of lithium-ion cells. In-depth investigations encompass charge and discharge curves, thickness changes, electrolyte degradation, gas evolution, and chemical analysis of cells with different silicon oxide proportions in the anode and their associated cathodes. The results show that a higher silicon oxide content in the anode increases the voltage hysteresis between charge and discharge. Moreover, the first-cycle efficiencies decrease with a higher silicon oxide content, attributed to irreversible LixSiy formation and the subsequent loss of active lithium from the cathode during formation. The anodes experience higher thickness changes with increased silicon oxide content, and peaks in differential voltage curves can be correlated with specific anode active materials and their thickness change. A gas analysis reveals conductive salt and electrolyte intermediates as well as silicon-containing gaseous fragments, indicating continuous electrolyte decomposition and silicon oxide aging, respectively. Additionally, a chemical analysis confirms increased silicon-derived products and electrolyte degradation on electrode surfaces. These findings underscore the importance of a holistic aging investigation and help understand the complex chemical changes in electrode materials for designing efficient and durable lithium-ion cells.