SiOx-Based Anode Materials with High Si Content Achieved Through Uniform Nano-Si Dispersion for Li-Ion Batteries

Abstract

Silicon alloy-based materials are widely studied as high-capacity anode materials to replace commercial graphite in lithium-ion batteries (LIBs). Among these, silicon suboxide (SiOx) offers superior cycling performance compared to pure Si-based materials. However, achieving a high initial Coulombic efficiency (ICE) remains a key challenge. To address this, previous studies have explored SixO composites (x ≈ 1, 2), where nano-Si is uniformly dispersed within a Si suboxide matrix to enhance ICE. While this approach improves reversible capacity and ICE compared to conventional SiO, it still falls short of the capacity achieved with pure Si. This study employs a high-energy mechanical milling approach with increased Si content to achieve higher reversible capacity and further enhance the ICE while also examining the effects of trace oxygen uniformly distributed within the Si suboxide matrix. Structural characterization via X-ray diffraction, Raman spectroscopy, and electron microscopy confirm that Si crystallites (<10 nm) are homogeneously embedded within the SiOx matrix, reducing crystalline Si size and inducing partial amorphization. Electrochemical analysis demonstrates an ICE of 89% and a reversible capacity of 2558 mAh g−1, indicating significant performance improvements. Furthermore, carbon incorporation enhances cycling stability, underscoring the material’s potential for commercial applications.