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Utilizing operando catalyst regeneration to uncover insights in the methanol-to-hydrocarbons process
Chem Catalysis ( IF 11.5 ) Pub Date : 2024-10-15 , DOI: 10.1016/j.checat.2024.101134
Sophie H. van Vreeswijk, Luke A. Parker, Arnaud T. Sanderse, Ramon Oord, Florian Meirer, Bert M. Weckhuysen

The methanol-to-hydrocarbons (MTH) catalyst deactivation is reversible, and deactivating coke molecules can be removed via regeneration experiments. Regeneration of small-pore zeolite SSZ-13 first leads to the elimination of polyaromatic deactivating compounds, leaving the active aromatic intermediates intact. Partial regeneration experiments can provide an alternative approach to study small-pore zeolites by mimicking co-feeding of aromatic intermediates. Catalyst properties and reaction intermediates were followed with operando UV-visible spectroscopy and X-ray diffraction. It was shown that all the coke is formed within the zeolite cages and that the lattice expansion is due to the formation of hydrocarbon molecules. Additionally, indications for separate reaction mechanisms to produce ethylene and propylene were established. With confocal fluorescence microscopy (CFM), it was determined that upon regeneration, the hydrocarbons were less conjugated and more homogeneously distributed. A full hydrocarbon pool mechanism was established for the MTH reaction over zeolite SSZ-13.

中文翻译:


利用原位催化剂再生来揭示甲醇制碳氢化合物工艺的见解



甲醇制碳氢化合物 (MTH) 催化剂的失活是可逆的,并且可以通过再生实验去除失活的焦炭分子。小孔径沸石 SSZ-13 的再生首先导致多环芳烃失活化合物的消除,保持活性芳香族中间体完好无损。部分再生实验可以通过模拟芳香族中间体的共喂养来提供一种替代方法来研究小孔沸石。催化剂性质和反应中间体之后进行原位紫外-可见光谱和 X 射线衍射。结果表明,所有焦炭都是在沸石笼内形成的,晶格膨胀是由于碳氢化合物分子的形成。此外,还建立了产生乙烯和丙烯的单独反应机制的指示。使用共聚焦荧光显微镜 (CFM) 确定,在再生时,碳氢化合物的共轭较少且分布更均匀。为沸石 SSZ-13 上的 MTH 反应建立了全烃池机制。
更新日期:2024-10-15
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