Proceedings of MATSUS Fall 2024 Conference (MATSUSFall24)
DOI: https://doi.org/10.29363/nanoge.matsusfall.2024.208
Publication date: 28th August 2024
Amorphous silicon nitride (a-Si3N4) has emerged as a promising anode material for lithium-ion batteries due to its high theoretical capacity and improved stability compared to pure silicon anodes. However, the atomic-scale mechanisms of lithium (Li) incorporation and storage in a-Si3N4 remain elusive. In this work we employ first-principles calculations to investigate the initial stages of lithiation in a-Si3N4, to understand the various modes of Li incorporation that drive the transition from irreversible matrix formation to reversible Li storage. Our research identifies three distinct modes of Li incorporation, each associated with different local structural environments and Li concentrations. Notably, we uncover the crucial role intrinsic charge trapping plays in both the irreversible and reversible Li incorporation, firstly, driving the matrix formation and secondly, facilitating reversible Li storage and charge transport. These insights allow strategies for the optimisation of a-Si3N4-based anodes to be devised, with the potential to tune the balance between matrix formation and productive Li storage. These insights provide a fundamental understanding of the lithiation process in a-Si3N4 and pave the way for the design of next-generation anode materials with enhanced performance.
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