Citation:
HU Si, ZHANG Qing, XIA Zhi, NG Yan-Jun, XU Jun, DENG Feng, DOU Tao. Catalytic Conversion of Methanol to Propylene over (NH4)2SiF6-Modified Nanosized HZSM-5 Zeolite[J]. Acta Physico-Chimica Sinica,
;2012, 28(11): 2705-2712.
doi:
10.3866/PKU.WHXB201207171
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(NH4)2SiF6-modified nanosized HZSM-5 zeolite was prepared and investigated as a catalyst formethanol to propylene conversion. The effects of this modification on the framework, textural propertiesand acidity of both the parent and the modified HZSM-5 zeolite were investigated by powder X-raydiffraction (XRD), 27Al magic angle spinning nuclear magnetic resonance (27Al MAS NMR), X-rayfluorescence (XRF), X-ray photoelectron spectroscopy (XPS), N2 adsorption, transmission electronmicroscopy (TEM), temperature-programmed desorption of ammonia (NH3-TPD), and infraredspectroscopy of adsorbed pyridine (Py-IR). The catalytic performance of these materials on the methanolto propylene (MTP) conversion process was tested under operating conditions of T=450℃, p=0.1 MPa(pMeOH=50 KPa) and WHSV=1 h-1. The results showed that surface aluminum on the nanosized ZSM-5zeolite could be selectively removed by the (NH4)2SiF6 solution and that the number of acidic sites on theHZSM-5 zeolite gradually decreased with increasing (NH4)2SiF6 concentration. Moreover, after modification with an optimally concentrated (NH4)2SiF6 solution, an obvious increase in specific surface area as well asmesopore volume was observed for the nanosized HZSM-5 with a resulting dramatic improvement in thecatalytic performance of this material for the MTP reaction. Both the propylene selectivity and propylene/ethylene (P/E) mass ratio resulting from use of the modified HZSM-5 increased significantly to 45.1% and8.0, as compared to results of 28.8% and 2.6 obtained with the original material. In addition, the catalyticlifespan of the modified zeolite was double that of the original.
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