The grafting reaction between a trifunctional silylating agent and two kinds of 2:1 type layered silicates was studied using FTIR, XRD, TGA and 29Si CP/MAS NMR. XRD patterns clearly indicate the introduction of 3-aminopropyltriethoxysilane (γ-APS) into the clay interlayer. In the natural montmorillonite, γ-APS adopts a parallel-bilayer while it adopts a parallel-monolayer arrangement in the synthetic fluorohectorite. These different silane arrangements have a prominent effect on the mechanism of the condensation reaction within the clay gallery. In natural montmorillonite, the parallel-bilayer arrangement of γ-APS results in bidentate (T2) and tridendate (T3) molecular environment while the parallel-monolayer arrangement leads to monodentate (T1), as indicated by 29Si CP/MAS NMR spectra. This study demonstrates that the silylation reaction and the interlayer microstructure of the grafting products strongly depend on the original clay materials
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