inGAP Centre for Research Based Innovation and Department of Chemistry, University of Oslo, Postboks 1033, Blindern, Oslo, Norway.
Phys Chem Chem Phys. 2013 Jun 14;15(22):8662-71. doi: 10.1039/c3cp44343d. Epub 2013 Apr 11.
The methanol to gasoline process over the zeolite catalyst ZSM-5 in a lab-sized reactor bed (4 mm diameter) has been studied in operando with high energy synchrotron X-ray diffraction. The fast z-scan method was used, scanning the reactor repeatedly and at speed through the X-ray beam. The X-ray diffraction data were processed using high throughput parametric Rietveld refinement to obtain real structural parameters. The diffraction data show only very subtle changes during the process and this allows us to demonstrate the combination of very large data volumes with parametric Rietveld methods to study weak features of the data. The different possible data treatment methodologies are discussed in detail and their effects on the results obtained are demonstrated. The trends in unit cell volume, zeolite channel occupancy and crystallite strain indicate that more or larger reaction intermediates are present close to the reactor outlet.
在实验室规模的反应器床(4 毫米直径)中,使用沸石催化剂 ZSM-5 将甲醇转化为汽油的过程已经通过高能量同步加速器 X 射线衍射进行了原位研究。使用快速 z 扫描方法,以速度穿过 X 射线束重复扫描反应器。使用高通量参数 Rietveld 精修处理 X 射线衍射数据,以获得真实的结构参数。衍射数据在过程中仅显示出非常细微的变化,这使我们能够将非常大数据量与参数 Rietveld 方法相结合,以研究数据的微弱特征。详细讨论了不同的可能数据处理方法,并展示了它们对所得到的结果的影响。单元晶胞体积、沸石通道占有率和微晶应变的趋势表明,在靠近反应器出口处存在更多或更大的反应中间体。