Hybrid CP-MS41 architectures ordered by covalently bound ionic species were synthesized via a template-directed, self-assembling process of tetraethoxysilane (TEOS) with 3-chloropropyltriethoxysilane (CIPTES). The solvent extracted CP-MS41 was activated by the consecutive immobilization of imidazole followed by alkylation with an alkyl halide resulting in the immobilized imidazole substituent CP-MS 41 (RIm(+)X(-)-MS41) or immobilized ionic liquid (IIL). A wide variety of CP-MS41 and RIm(+)X(-)-MS41 were synthesized and characterized using XRD, BET, FT-IR, EA, SEM, CP C-13-, Si-29-MAS-NMR, and TG/DTG, EA and FT-IR confirmed adduct formation of ionic-liquids with the host system. The effects of temperature. catalyst amount, influence of alkyl chain length, and variation of CO2 pressure were examined. (c) 2008 Elsevier B.V. All rights reserved.