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In-situ synthesis of ultrafine Fe-ZSM-5 zeolite for methanol to propylene (MTP) reaction
WANG Youhe1, LI Chencan1,2, DAI Chang1, ZANG Jinlong1, DU Ningning1, MAO Yuxin1, YAN Zifeng1
(1.State Key Laboratory for Heavy Oil Processing in China University of Petroleum(East China), Qingdao 266580, China;2.Shandong High-End Chemical Research Institute, Heze 274002, China)
Abstract:
Ultrafine Fe-ZSM-5 zeolite containing framework heteroatoms with around 50-120 nm in diameter was successfully in-situ synthesized via a dry gel conversion method. The fabricated samples were characterized by means of XRD, SEM, TEM, UV-Vis, NH3-TPD, Py-FT-IR and N2 adsorption-desorption isotherms. The results indicate that Fe source added in-situ can not only reduce the size of zeolite particles, but also reduce the acid strength of zeolite. Ultrafine Fe-ZSM-5 zeolite prepared by in-situ synthesis method contains three kinds of Fe species, and most of Fe attributes to isolated framework Fe3+ species in tetrahedral coordination and the rest exists as oligomerized FeOx and Fe2O3 particles. But Fe/ZSM-5 zeolite prepared by impregnation method mainly contains latter two forms of Fe species with a little of Fe3+ in the framework of the zeolite. The acid properties of ZSM-5 zeolite were modified by Fe modification, which improved the selectivity of propylene in MTP reaction. Compared to the Fe/ZSM-5 zeolite fabricated by traditional impregnation method, the in-situ synthesized ultrafine Fe-ZSM-5 zeolite containing framework heteroatoms presents higher propylene selectivity in the MTP process due to smaller grain size and more suitable acid properties.
Key words:  ultrafine Fe-ZSM-5 zeolite  dry gel conversion  in-situ synthesis  methanol to propylene