New layered hybrid organic–inorganic materials were obtained directly by hydrolysis and polycondensation of monosilylated precursors of type (EtO)3Si(CH2)3NH(C
O)NHCnH2n+1 (n = 3, 8, 12 and 16). These precursors were easily prepared by reaction between commercially available triethoxysilylpropylisocyanate and primary aminoalkanes. The obtained materials were characterized by combining elemental analysis, X-ray powder diffraction, 13C, 29Si NMR and FT-IR spectroscopies. They were found to be well condensed, and stable in water. We showed that their formation results from a cooperative effect between hydrogen bonding interactions originating from ureido groups and hydrophobic interactions between the long alkyl chains. There is no formation of material when n = 2, or from (EtO)3SiCnH2n+1 when n = 18, thus proving that both types of weak intermolecular interactions are required. The chelating property of these materials towards europium(III) ions was tested.
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