Eco-friendly synthesis of SiO2 nanoparticles confined in hard carbon: A promising material with unexpected mechanism for Li-ion batteries

Abstract A fast, simple and environmentally friendly one-pot route to obtain carbon/SiO2 hybrid materials is reported in this work. This consists in simple mixture of carbon and silica precursors, followed by thermal annealing at different temperatures. An interpenetrating hybrid network composed of hard carbon and amorphous SiO2 nanoparticles (2–5 nm) homogeneously distributed was achieved. Increasing the annealing temperature from 600 °C up to 1200 °C, the material porosity and oxygen functional groups are gradually removed, while the amorphous nature of SiO2 is conserved. This allows to diminish the irreversible capacity during the first charge-discharge cycle and to increase the reversible capacity. An excellent cycling capability, with a reversible capacity up to 535 mA hg-1 at C/5 constant current rate was obtained for C/SiO2 materials used as anodes for Li-ion batteries. An atypical increase of the capacity during the first 50 cycles followed by a stable plateau up to 250 cycles was observed and related to electrolyte wettability limitation through the materials, particularly for those annealed at high temperatures which are more hydrophobic, less porous and the SiO2 nanoparticles less accessible. The SiO2 lithiation mechanism was evaluated by XRD, TEM and XPS post-mortem analyses and revealed the formation of reversible lithium silicate phases.