化学工程
沸石
化学
纳米技术
材料科学
催化作用
有机化学
工程类
作者
Mariame Akouche,Jean‐Pierre Gilson,Nikolai Nesterenko,Simona Moldovan,Daniel Chateigner,Hussein El Siblani,Delphine Minoux,Jean‐Pierre Dath,Valentin Valtchev
标识
DOI:10.1021/acs.chemmater.9b05258
摘要
Colloidal zeolite precursors with sharp particle size distributions (ca. 3–5 nm) and identical chemical compositions, so called embryonic zeolites (EZs), are prepared by strict control of aluminosilicate precursor polymerization in zeolite-yielding systems. The organic structure-directing agent (OSDA) acts as a sacrificial template and is eliminated by high-temperature combustion after the synthesis. Physicochemical properties of the EZs, such as the pore size and volume and specific surface area, are determined by the size of the OSDA and synthesis conditions employed, that is, the larger the OSDA, the higher the microporous volume and the specific surface area of the derived EZs. The EZs belong to the family of extra-large microporous (1–2.5 nm) materials. Upon calcination, EZs retain their structure/porosity, and most of their aluminum remains in a tetrahedral coordination to provide Brønsted acidity. Pyridine adsorption shows a lower acidic strength for embryonic zeolites with respect to their crystalline counterparts (zeolites). An appropriate combination of extra-large micropores (1–2.5 nm) and Brønsted acid sites (∼25 μmol·g–1) leads to improved catalytic performances in the dealkylation of TiPBz, a proxy for bulky molecules reacting only on the external surface of crystalline zeolites. By varying the size of the OSDA for synthesizing the EZ, materials with controlled porosity, acidity, accessibility, and catalytic activity are prepared, and their properties extend to existing crystalline zeolites.
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