Issue 2, 2010

Insights into pore surface modification of mesoporous polymer–silica composites: introduction of reactive amines

Abstract

Pore surface engineering of mesoporous materials is fundamental for the development of highly selective sorbents, solid catalysts or drug delivery systems. In the present study, tailored mesoporous amine-functionalized polymersilica composites are synthesized using a two-step mesopore surface-confined polymerization technique. For this, a functional polymer, polychloromethylstyrene (PCMS), is first introduced as a uniform coating on the mesopore surface of mesoscopically ordered silica, e.g. SBA-15 or KIT-6 materials. In the second step, selected amines, as model functions, are attached to the polymer surface by nucleophilic substitution, generating a variety of nanoporous amino-polymersilica composites. In particular, it is shown that this approach allows for a tuning of surface concentration of the organic groups either by varying polymer loading or by copolymerization of the CMS monomers with non-reactive monomers (styrene). Moreover, this method is suitable for facile introduction of diverse types of amine groups, e.g. secondary amines, diamines, linear or branched polyamines. The pristine mesoporous silica hosts and the different functional mesoporous polymersilica composites are characterized in detail by nitrogen physisorption, powder X-ray diffraction, elemental analysis, thermogravimetrydifferential thermal analysis coupled with mass spectrometry (TG-DTA/MS), attenuated total reflection-IR spectroscopy (ATR-IR) and scanning electron microscopy. In addition, the obtained functionalized mesoporous composites are proven active as base catalysts in the Knoevenagel condensation. From these investigations, it appeared that the preparation method should be highly flexible and appropriate to enable modulation of location and distribution of various functional groups within mesopores.

Graphical abstract: Insights into pore surface modification of mesoporous polymer–silica composites: introduction of reactive amines

Supplementary files

Article information

Article type
Paper
Submitted
11 Sep 2009
Accepted
12 Nov 2009
First published
12 Jan 2010

New J. Chem., 2010,34, 355-366

Insights into pore surface modification of mesoporous polymersilica composites: introduction of reactive amines

R. Guillet-Nicolas, L. Marcoux and F. Kleitz, New J. Chem., 2010, 34, 355 DOI: 10.1039/B9NJ00478E

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