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Cubic Pm3n mesoporous aluminosilicates assembled from zeolite seeds as strong acidic catalysts

机译:立方PM3N介孔铝硅硅酸盐从沸石种子组装为强酸性催化剂

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摘要

Cubic Pm3n mesoporous aluminosilicates isomorphous to SBA-1, with 3D interconnected pore structures, were assembled from Al-incorporating zeolite seeds at around pH 9 using cetyltriethylammonium bromide as a pore-directing agent. The resultant series of materials (termed Al-ZSBA-1) has the advantages of strong acidity from the zeolitic structure and good diffusivity of bulky reactants from the 3D interconnected mesopores. Al-ZSBA-1, with Al loading up to an Al/Si molar ratio of 0.057, still retains a cubic Pm3n structure and high surface area (ca. 600 m(2) g(-1)). The acidities were stronger than the counter materials prepared using sodium silicate as the silica source (referred to as Al-SBA-1-alk). Moreover, all the Al(III) ions in Al-ZSBA-1 retained their tetrahedral coordination after calcination at 823 K, while a portion of Al(III) in Al-SBA-1-alk became octahedrally coordinated. When tested for the catalytic alkylation of 2,4-di-tert-butylphenol with cinnamyl alcohol, Al-ZSBA-1 gave higher flavan selectivities and yields in comparison to Al-SBA-1-alk, ZSM-5, and beta zeolites.
机译:立方PM3N介孔铝硅酸盐与SBA-1同构(具有3D互连的孔结构),使用孔基于pH 9的藻类沸石种子组装,使用cetylthyltriylymonium溴化物作为孔隙杆菌作为孔隙 - 引导剂。所得的一系列材料(称为al-ZSBA-1)具有来自沸石结构的强酸的优势,并且是从3D相互连接的中孔中笨重的反应物的良好扩散性。 Al-ZSBA-1,Al加载高达0.057的Al/Si摩尔比仍然保留了立方PM3N结构和高表面积(约600 m(2)g(-1))。酸度比使用硅酸钠作为二氧化硅源(称为al-SBA-1-Alk)制备的反材料强。此外,Al-ZSBA-1中的所有Al(iii)离子在823 K处钙化后保留了四面体协调,而Al-SBA-1-Alk中的Al(iii)的一部分在Al-SBA-1-Alk中的一部分进行了协调。当测试2,4-DI-TERT叔丁醇与肉桂醇的催化烷基化时,Al-ZSBA-1与Al-SBA-1-Alk,ZSM-5和Beta沸石相比,flavan的选择性和产量更高。

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