From silicon to silica: a green chemistry approach for hollow sphere nanoparticle formation

Herein we report on an environmentally friendly and scalable production route for hollow silica spheres (HSSs). The process is based on close to 100% conversion of non-crystalline solid Si nanoparticles (D̄ = 40 ± 9 nm) in mild alkaline solutions (pH ≤ 9.0) at ambient temperature. The Si nanoparticles are prepared using the centrifugal chemical vapor deposition (cCVD) method. Combining transmission electron microscopy (TEM) imaging and nanoparticle size analysis with hydrogen evolution data, elemental mapping, and nitrogen adsorption for surface area measurement, we show for the first time experimental data that document a Kirkendall type Si-to-HSS formation process. Our understanding is that the Si nanoparticles exposed to air form a SiO₂ film, which is stable in the mild alkaline environment. Silicon from the Si nanoparticles is transported through the thin SiO₂ film and is reacting with H₂O/OH^- species on the particle surface or in the already thickened SiO₂ shell to form silicic acid that in turn rapidly gets converted to a sol-gel to continue the growing of the silica shell. We foresee that this green chemistry approach can be utilized for HSS preparation for use in batteries, insulation materials and drug delivery.