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1.
Chemistry ; 20(52): 17616-23, 2014 Dec 22.
Artículo en Inglés | MEDLINE | ID: mdl-25348837

RESUMEN

Development of sustainable routes for synthesizing aluminophosphate-based zeolites are very important because of their wide applications. As a typical sustainable route, solvent-free synthesis of zeolites not only decreases polluted wastes but also increases product yields. Systematic solvent-free syntheses of hierarchically porous aluminophosphate-based zeolites with AEL and AFI structures is presented. XRD patterns and SEM images show that these samples have high crystallinity. N2 sorption isotherm tests show that these samples are hierarchically porous, and their surface areas are comparable with those of corresponding zeolites from hydrothermal route. Chosen as an example, catalytic oxidation of ethylbenzene with O2 shows that cobalt substituted APO-11 from the solvent-free route (S-CoAPO-11) is more active than conventional CoAPO-11 from hydrothermal route owing to the sample hierarchical porosity.

2.
Chem Commun (Camb) ; 50(80): 11844-7, 2014 Oct 14.
Artículo en Inglés | MEDLINE | ID: mdl-25147877

RESUMEN

We reported a universal route for synthesizing porous organic ligands (POLs) via solvothermal polymerization. The POLs were obtained quantitatively, showing high surface area, large pore volume, hierarchical porosity, and superior stability. The POL bearing a triphenylphosphine supported rhodium catalyst (Rh/POL-PPh3) exhibits high activity and excellent recyclability in 1-octene hydroformylation.

3.
J Am Chem Soc ; 136(6): 2503-10, 2014 Feb 12.
Artículo en Inglés | MEDLINE | ID: mdl-24450997

RESUMEN

Mesoporous zeolites are useful solid catalysts for conversion of bulky molecules because they offer fast mass transfer along with size and shape selectivity. We report here the successful synthesis of mesoporous aluminosilicate zeolite Beta from a commercial cationic polymer that acts as a dual-function template to generate zeolitic micropores and mesopores simultaneously. This is the first demonstration of a single nonsurfactant polymer acting as such a template. Using high-resolution electron microscopy and tomography, we discovered that the resulting material (Beta-MS) has abundant and highly interconnected mesopores. More importantly, we demonstrated using a three-dimensional electron diffraction technique that each Beta-MS particle is a single crystal, whereas most previously reported mesoporous zeolites are comprised of nanosized zeolitic grains with random orientations. The use of nonsurfactant templates is essential to gaining single-crystalline mesoporous zeolites. The single-crystalline nature endows Beta-MS with better hydrothermal stability compared with surfactant-derived mesoporous zeolite Beta. Beta-MS also exhibited remarkably higher catalytic activity than did conventional zeolite Beta in acid-catalyzed reactions involving large molecules.

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