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The SiO x anode exhibits a high specific capacity and commendable durability for lithium-ion batteries (LIBs). However, its practical application is hindered by significant volumetric fluctuations during lithiation/delithiation, alongside a metastable nature, which induces mechanical instability and irreversible lithium consumption, ultimately impairing long-term capacity retention in full-battery cell configurations. In this study, we present a phase-engineering approach designed to improve the structural stability of SiO x anodes for LIB applications. By incorporating lithium fluoride, amorphous SiO x undergoes partial transformation into a quartz-like phase, which enhances mechanical integrity and mitigates irreversible lithium loss. This modified anode demonstrates significantly improved stability and prolonged cycle lifespan. Through a combination of multiscale simulations and in situ characterizations, we elucidate the stabilization mechanisms conferred by the quartz phase, providing critical insights into the role of SiO x ’s crystal structure in influencing degradation pathways. This work introduces an accessible and efficient method for controlling the crystallinity of SiO x, offering a practical solution to enhance the durability of high-energy-density LIBs.
Li et al. (Wed,) studied this question.