Passivating oxygen atoms in SiO through pre-treatment with Na₂CO₃ to increase its first cycle efficiency for lithium-ion batteries

Silicon monoxide (SiO) is a promising anode material for Li-ion batteries because of its high capacity. Though, its low first Coulombic efficiency (FCE) due to the formation of inactive Li–Si–O compounds during lithiation hinders its practical application. Herein, we report a facile pre-sodiation technique by annealing SiO with a small amount of Na₂CO₃ (≤ 5 wt%) under 850 °C, which improves FCE of pristine SiO from 61.4% to 86.0% without the use of lithium metal, solvent and disassembling and re-assembling of cells. Transmission electron microscopy, X-ray photoelectron spectroscopy, and nuclear magnetic resonance demonstrate that the incorporation of Na facilitates the disproportionation of SiO into crystalline Si and SiO₂ through nucleophilic substitution, and reduces the reactivity of the oxygen atoms with lithium and thereby suppresses the irreversible capacity during initial lithiation. The pre-sodiation process also improves thermal stability of SiO. Since the Na-containing SiO material is not sensitive to moisture in ambient condition, special handling of the material is not necessary. Combining with a LiFePO₄ cathode, the full cell shows a FCE of 85.8% with good cycle stability. The energy density of lithium-ion battery can even reach 900 Wh L⁻¹ based on a theoretical calculation with high-capacity Ni-based metal-oxide cathode.