期刊
RESEARCH ON CHEMICAL INTERMEDIATES
卷 47, 期 1, 页码 249-268出版社
SPRINGER
DOI: 10.1007/s11164-020-04340-3
关键词
ZSM-5; One-step acid treatment; Hierarchical structure; Acidity; MTP
资金
- National Natural Science Foundation of China [21661031, 21766026]
- discipline project of Ningxia [NXYLXK2017A04]
- doctor scientific research starting foundation of Yanbian University [602020073]
A one-step acid treatment method was developed for synthesizing hierarchical HZSM-5, while hierarchical Mg/ZSM-5 was obtained by the incipient impregnation method to increase propylene yield in the methanol-to-propylene reaction. The samples were characterized by various techniques, showing improved SiO2/Al2O3 molar ratio and well-distributed acid sites. The hierarchical Mg/ZSM-5 exhibited high propylene selectivity and resistance to carbon deposition in the MTP reaction.
One-step acid treatment for template- and solvent-free synthesized NaZSM-5 was developed to obtain hierarchical HZSM-5. Hierarchical Mg/ZSM-5 was obtained by the incipient impregnation method, which further increased the propylene yield of the methanol-to-propylene (MTP) reaction. The physicochemical properties of the samples were characterized by X-ray fluorescence (XRF), X-ray diffraction (XRD), scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDS), N-2 adsorption-desorption, pyridine adsorption-IR (Py-IR) and NH3 temperature-programmed desorption (NH3-TPD). The results indicated that one-step acid treatment (250 degrees C, 12 h) could increase the SiO2/Al2O3 molar ratio from 29.43 to 53.33 and maintain the well-distributed state of acid sites. The blocked pore structure was opened to introduce additional mesoporosity. Additionally, NaZSM-5 was synchronously converted to HZSM-5, thereby avoiding ion-exchange procedures. Synchronization of dealumination, desodiation and introduction of the mesoporous structure was achieved in one step, providing a good matrix for further impregnation with Mg species. The obtained hierarchical Mg/ZSM-5 (0.3 M-MgO) showed low diffusion hindrance and reduction in external surface acid sites (especially Bronsted acid sites), affording high propylene selectivity (53.34%) and good resistance to carbon deposition (similar to 0.77%) in the MTP reaction. [GRAPHICS] .
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