Solid-state NMR characterisation of the thermal transformation of a Hungarian white illite

1H, 27Al, 29Si and 39K solid-state NMR are reported from a Hungarian illite 2:1 clay for samples heated up 1600 °C. This single-phase sample has a small amount of aluminium substitution in the silica layer and very low iron-content (∼0.4 wt%). Thermal analysis shows several events that can be related to features in the NMR spectra, and hence changes in the atomic scale structure. As dehydroxylation occurs there is increasing AlO 4 and AlO 5-contents. The silica and gibbsite layers become increasingly separated as the dehydroxylation progresses. Between 900 and 1000 °C the silica layer forms a potassium aluminosilicate glass. The gibbsite-layer forms spinel/ γ-Al 2O 3 and some aluminium-rich mullite. Then on heating to 1600 °C changes in the 29Si and 27Al MAS NMR spectra are consistent with the aluminosilicate glass increasing its aluminium-content, the amount of mullite increasing probably with its silicon-content also increasing, and some α-Al 2O 3 forming.