期刊
CATALYSIS SCIENCE & TECHNOLOGY
卷 12, 期 20, 页码 6098-6111出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d2cy00991a
关键词
-
资金
- National Key R&D Program of China [2021YFA1501401]
- National Natural Science Foundation of China [21872052, 21972044]
A novel and efficient strategy is developed to post-synthesize Ti-MSE catalysts by combining interzeolite transformation, dealumination, and isomorphous substitution of Ti. The resulting catalyst exhibits high catalytic activity and para-selectivity in anisole hydroxylation, possibly due to the strong interaction between the framework hydroxyls in Ti-MSE and the oxygen-containing substituent groups in aromatic substrates.
The practical application of MSE-type titanosilicate (Ti-MSE) catalysts in liquid-phase oxidation processes is facing the problem of inefficient and complex synthesis. A novel and efficient strategy is developed to post-synthesize Ti-MSE by the combination of interzeolite transformation, dealumination and isomorphous substitution of Ti. With the assistance of MCM-68 seeds and tetraethylammonium hydroxide (TEAOH) as an organic structure-directing agent, the MSE aluminosilicate was rapidly crystallized in only 1 day with a high solid yield of 88.3% via the dissolution-recrystallization of siliceous Beta zeolite. The structural similarity between the parent Beta and target MSE was revealed to play a vital role in realizing the efficient interzeolite transformation. After dealumination and solid-gas treatment with TiCl4 vapor, the Ti-MSE-trans catalyst was readily obtained, which exhibited high catalytic activity in anisole hydroxylation with a methoxyphenol yield of 54.9% and a particularly high para-selectivity of 96.2%. Electrostatic potential (ESP) and density functional theory (DFT) calculations revealed that the framework hydroxyls in Ti-MSE strongly interact with the oxygen-containing substituent groups in aromatic substrates, responsible for the high para-selectivity.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据