Six new methyl silicon (IV) precursors of the type [MeSi{ON=C(R)Ar}
3
] [when R = Me, Ar = 2-C
5
H
4
N (1), 2-C
4
H
3
O (2) or 2-C
4
H
3
S (3); and when R = H, Ar = 2-C
5
H
4
N (4), 2-C
4
H
3
O (5) or 2-C
4
H
3
S (6)] were prepared and structurally characterized by various spectroscopic techniques. Molecular weight measurements and FAB (Fast Atomic Bombardment) mass spectral studies indicated their monomeric nature.
1
H and
13
C{
1
H} NMR spectral studies suggested the oximate ligands to be monodentate in solution, which was confirmed by
29
Si{
1
H} NMR signals in the region expected for tetra-coordinated methylsilicon (IV) derivatives. Thermogravimetric analysis of 1 revealed the complex to be thermally labile, decomposing to a hybrid material of definite composition. Two representative compounds (2 and 4) were studied as single source molecular precursor for low-temperature transformation to silica-based hybrid materials using sol-gel technique. Formation of homogenous methyl-bonded silica materials (MeSiO
3/2
) at low sintering temperature was observed. The thermogravimetric analysis of the methylsilica material indicated that silicon-methyl bond is thermally stable up to a temperature of 400 °C. Reaction of 2 and Al(OPr
i
)
3
in equimolar ratio in anhydrous toluene yielded a brown-colored viscous liquid of the composition [MeSi{ON=C(CH
3
)C
4
H
3
O}
3
.Al(OPr
i
)
3
]. Spectroscopic techniques
1
H,
13
C{
1
H},
27
Al{
1
H} and
29
Si{
1
H} NMR spectra of the viscous product indicated the presence of tetracoordination around both silicon and aluminum atoms. On hydrolysis it yielded methylated aluminosilicate material with high specific surface area (464 m
2
/g). Scanning electron micrography confirmed a regular porous structure with porosity in the nanometric range.