氟硅酸铵改性纳米HZSM-5分子筛催化甲醇制丙烯

doi:10.3866/PKU.WHXB201207171

Abstract

Abstract:

(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(p_MeOH=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.

Key words: Nanosized ZSM-5, Dealumination, Pore structure, Acidity, Propylene selectivity, Catalytic lifetime

MSC2000:

O643.3

Click here to download Supporting Info material in PDF type

HU Si, ZHANG Qing, XIA Zhi, GONG Yan-Jun, XU Jun, DENG Feng, DOU Tao. Catalytic Conversion of Methanol to Propylene over (NH₄)₂SiF₆-Modified Nanosized HZSM-5 Zeolite[J].Acta Phys. -Chim. Sin., 2012, 28(11): 2705-2712.

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Catalytic Conversion of Methanol to Propylene over (NH₄)₂SiF₆-Modified Nanosized HZSM-5 Zeolite

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Catalytic Conversion of Methanol to Propylene over (NH₄)₂SiF₆-Modified Nanosized HZSM-5 Zeolite