Zebardasti Ali, Dekamin Mohammad G, Doustkhah Esmail, Assadi M Hussein N
Department of Chemistry, Iran University of Science and Technology, Tehran 1684613114, Iran.
International Center for Materials Nanoarchitechtonics, National Institute for Materials Science, 1-1 Namiki, Tsukuba, Ibaraki 305-0044, Japan.
Inorg Chem. 2020 Aug 17;59(16):11223-11227. doi: 10.1021/acs.inorgchem.0c01449. Epub 2020 Jul 31.
We synthesized a new organosiloxane bridge on the basis of an isocyanurate derivative through a simple melt-fusion approach by the reaction of 3-isocyanatopropyltriethoxysilane (IPTES) with 1,3,5-tris(2-hydroxyethyl)-1,3,5-triazinane-2,4,6(1,3,5)-trione (THEIC). The obtained carbamate-isocyanurate-based organosiloxane bridge precursor was used for the preparation of chemo- and thermostable periodic mesoporous organosilica (PMO-THEIC) on condensation with tetrathoxysilane silicon precursor through a soft-template approach. Furthermore, the synthesized PMO-THEIC with unique surface functionality was investigated for CO capture. The results show that the PMO-THEIC has higher activity than pure SBA-15 for CO capture due to the high affinity of carbamate functionalities embedded within the pore walls toward CO molecules. The affinity of organosiloxane bridge for CO molecules is mainly facilitated via the van der Waals force with carbamate functional groups rather than the isocyanurate ring, according to the density functional calculations.
我们通过3-异氰酸酯基丙基三乙氧基硅烷（IPTES）与1,3,5-三（2-羟乙基）-1,3,5-三嗪烷-2,4,6（1,3,5）-三酮（THEIC）反应，采用简单的熔融法，在异氰脲酸酯衍生物的基础上合成了一种新的有机硅氧烷桥。通过软模板法，将所得基于氨基甲酸酯-异氰脲酸酯的有机硅氧烷桥前体与四乙氧基硅烷硅前体缩合，用于制备化学稳定和热稳定的周期性介孔有机硅（PMO-THEIC）。此外，对合成的具有独特表面功能的PMO-THEIC进行了CO捕获研究。结果表明，由于孔壁内嵌入的氨基甲酸酯官能团对CO分子具有高亲和力，PMO-THEIC在CO捕获方面比纯SBA-15具有更高的活性。根据密度泛函计算，有机硅氧烷桥对CO分子的亲和力主要通过与氨基甲酸酯官能团的范德华力而不是异氰脲酸酯环来促进。
