Transformation of Propane over ZnSnPt Modified Defective HZSM-5 Zeolites: The Crucial Role of Hydroxyl Nests Concentration

oleh: Wei Zhou, Jiaxu Liu, Jilei Wang, Long Lin, Ning He, Xiaotong Zhang, Hongchen Guo

Format: Article
Diterbitkan: MDPI AG 2019-06-01

Deskripsi

A series of ZnSnPt supported defective MFI zeolites with different SiO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> ratios (30, 110, 700, and &#8734;) and hydroxyl nests concentration were prepared and characterized by multiple techniques including scanning electron microscopy (SEM), nitrogen physisorption, NH<sub>3</sub>-TPD, transmission electron microscopy (TEM), hydrogen temperature programmed reduction (H<sub>2</sub>-TPR), and Fourier transform infrared spectrometer (FT-IR). It was found that Br&#248;nsted acid sites (Si(OH)Al) with strong acid strength and the hydroxyl nests with weak acid strength coexisted over the defective ZSM-5 zeolites and ZnSnPt Lewis acid sites preferentially located on the hydroxyl nests. The increase in the concentration of hydroxyl nests and SiO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> ratios apparently improved the distribution of ZnSnPt Lewis acid sites. The hydroxyl nest incorporated ZnSnPt Lewis acid sites showed extraordinary dehydrogenation ability. Specially, <i>operando</i> dual beam Fourier transform infrared spectrometer (DB-FTIR) was applied to characterize the propane transformation under reaction conditions. At low SiO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> ratios, the propane efficiently transforms into propene and aromatics (total selectivity of 93.37%) by the cooperation of Br&#248;nsted acid sites and ZnSnPt Lewis acid sites. While at high SiO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> ratios, the propane mainly transforms into propene (selectivity of above 95%) and hydrogen. This study provides guidance for the preparation of highly efficient propane dehydrogenative transformation catalyst.