3 years ago

Highly Oriented Growth of Catalytically Active Zeolite ZSM-5 Films with a Broad Range of Si/Al Ratios

Highly Oriented Growth of Catalytically Active Zeolite ZSM-5 Films with a Broad Range of Si/Al Ratios
Zoran Ristanović, Joel E. Schmidt, Florian Meirer, Abhishek Dutta Chowdhury, Bert M. Weckhuysen, Donglong Fu
Highly b-oriented zeolite ZSM-5 films are critical for applications in catalysis and separations and may serve as models to study diffusion and catalytic properties in single zeolite channels. However, the introduction of catalytically active Al3+ usually disrupts the orientation of zeolite films. Herein, using structure-directing agents with hydroxy groups, we demonstrate a new method to prepare highly b-oriented zeolite ZSM-5 films with a broad range of Si/Al ratios (Si/Al=45 to ∞). Fluorescence micro-(spectro)scopy was used to monitor misoriented microstructures, which are invisible to X-ray diffraction, and show Al3+ framework incorporation and illustrate the differences between misoriented and b-oriented films. The methanol-to-hydrocarbons process was studied by operando UV/Vis diffuse reflectance micro-spectroscopy with on-line mass spectrometry, showing that the b-oriented zeolite ZSM-5 films are active and stable under realistic process conditions. Al asks for directions: The use of structure-directing organic reagents with hydroxy groups leads to highly b-oriented zeolite ZSM-5 films with a broad range of Al contents. Fluorescence micro-(spectro)scopy shows the effect of Al3+ on the zeolite film growth, and that the Al-tetrapropylammonium interactions lead to misorientation.

Publisher URL: http://onlinelibrary.wiley.com/resolve/doi

DOI: 10.1002/anie.201704846

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