Aluminosilicate precursors were prepared by mechanochemical treatment of gibbsitesilica gel mixtures. The effect of grinding on their structure and thermal behavior has been examined by 27Al and 29Si MAS NMR, x-ray diffraction (XRD), differential thermal analysis-thermogravimetry (DTA-TG), and Fourier transform infrared (FTIR). After 8 h grinding, the hydrated alumina was completely changed to an amorphous phase which showed a new exothermic DTA peak at about 980 °C due to the formation of γ–Al2O3 or spinel phase. This behavior was related to changes in the Al and Si environments, as deduced from the MAS NMR spectra. With increased grinding time, some 4-coordinated Al appears, together with an Al resonance at about 30 ppm. Simultaneously, a new Si resonance appears at about −90 ppm, indicating a greater degree of homogeneity in the ground samples. Mullite crystallizes at 1200 °C from samples ground for 8–20 h, its XRD intensity increasing with increased milling times, in agreement with the NMR, DTA, and FTIR data. Changes in the Al and Si environments during heat treatment, as reflected by the NMR spectra, are also reported.
