Preparation of Mullite-Silica Composites Using Silica-Rich Monophasic Precursor Obtained as a Byproduct of Mineral Carbonation of Blast-Furnace Slag

Previously, mineral carbonation of blast-furnace slag was carried out to sequestrate CO2 and attain pure CaCO3 crystals. In this process, amorphous silica-alumina nanoparticles were obtained as a byproduct. In this study, the crystallization of these nanoparticles on calcination at various temperatures in air was examined using TGA-DTA, XRD, MAS-NMR spectroscopy, and FT-IR spectroscopy. The precursor nanoparticles (Si:Al = 78:22 mol %) were prepared using the solution extracted from blast-furnace slag (BFS) with acetic acid at room temperature. The XRD analysis showed that the initial amorphous state was retained up to 800 °C, and decomposition to amorphous silica and mullite started after calcination at 950 °C. At temperatures between 1150 °C and 1250 °C, amorphous silica crystalized to cristobalite, which eventually melted to glassy silica at 1500 °C. The mullite crystals initially adopted a metastable tetragonal phase and transformed to a stable, needle-like orthorhombic phase at higher temperatures. 27Al MAS-NMR spectroscopy revealed that octahedrally coordinated Al was favored up to a temperature of 800 °C as a result of the dehydration process and transformed into tetrahedrally coordinated Al at higher temperatures. A microstructural examination revealed that the initially randomly-oriented mullite developed into stable, needle-like grains owing to anisotropic grain growth in the presence of a glass phase at high temperatures. This study suggests that the recycling of BFS can be exploited for the procurement of a mullite-type ceramic material.