Stable single-unit-cell nanosheets of zeolite MFI as active and long-lived catalysts

微型多孔材料 沸石 催化作用 化学工程 材料科学 双功能 扩散 硅酸铝 纳米技术 化学 介孔材料 有机化学 复合材料 热力学 物理 工程类
作者
Minkee Choi,Kyungsu Na,Jeongnam Kim,Yasuhiro Sakamoto,Osamu Terasaki,Ryong Ryoo
出处
期刊:Nature [Nature Portfolio]
卷期号:461 (7261): 246-249 被引量:2185
标识
DOI:10.1038/nature08288
摘要

Zeolites-microporous crystalline aluminosilicates-are widely used in petrochemistry and fine-chemical synthesis because strong acid sites within their uniform micropores enable size- and shape-selective catalysis. But the very presence of the micropores, with aperture diameters below 1 nm, often goes hand-in-hand with diffusion limitations that adversely affect catalytic activity. The problem can be overcome by reducing the thickness of the zeolite crystals, which reduces diffusion path lengths and thus improves molecular diffusion. This has been realized by synthesizing zeolite nanocrystals, by exfoliating layered zeolites, and by introducing mesopores in the microporous material through templating strategies or demetallation processes. But except for the exfoliation, none of these strategies has produced 'ultrathin' zeolites with thicknesses below 5 nm. Here we show that appropriately designed bifunctional surfactants can direct the formation of zeolite structures on the mesoporous and microporous length scales simultaneously and thus yield MFI (ZSM-5, one of the most important catalysts in the petrochemical industry) zeolite nanosheets that are only 2 nm thick, which corresponds to the b-axis dimension of a single MFI unit cell. The large number of acid sites on the external surface of these zeolites renders them highly active for the catalytic conversion of large organic molecules, and the reduced crystal thickness facilitates diffusion and thereby dramatically suppresses catalyst deactivation through coke deposition during methanol-to-gasoline conversion. We expect that our synthesis approach could be applied to other zeolites to improve their performance in a range of important catalytic applications.
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