Mass Spectral Molecular Mapping Shows Benefits of Thermal Evaporation in Prelithiated Silicon-Based Electrodes

Abstract

Silicon based composites have become increasingly popular as potential anodes for lithium-ion batteries due to their large storage capacity and potential ability to generate batteries with energy densities greater than 350 Wh/kg. These anodes often see reduced initial columbic efficiency (ICE) due to disruptive volume expansion up to 300% and continuous solid electrolyte interphase (SEI) layer formation. Prelithiation, where an excess reservoir of Li is added to the electrode to compensate for irreversible SEI formation losses during their sample preparation, has proven to solve the issue of immediate capacity loss. Thermal evaporation is a prelithiation technique with limited studies on its effectiveness. In this study, time-of-flight secondary ion mass spectrometry (ToF-SIMS) is used to highlight the benefits of prelithiation via thermal evaporation. ToF-SIMS provides chemical mapping and spatial information in 2D and 3D visualizing the deposition of lithium, identifying LixSiy alloy and LixSiyOz silicate formation, and the distribution of lithium passivation into the electrodes. Passivation under different atmospheric conditions, Ar and Ar/CO2 highlights the impact of the environment for the passivation effectiveness and formation of LixSiy alloy and LixSiyOz silicate. The ToF-SIMS molecular imaging and depth profiling results indicate that prelithiation via thermal evaporation effectively distributes lithium throughout the depth profile length and induces a greater degree of LixSiyOz silicate formation over LixSiy alloy. Our ToF-SIMS characterization results indicate the effectiveness of thermal evaporation in producing a more stable electrode and an electrode with an effective lithium reserve that can preserve its capacity.