期刊
JOURNAL OF CATALYSIS
卷 230, 期 1, 页码 140-149出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2004.12.007
关键词
syngas; dimethyl ether; hybrid catalyst; dehydration of methanol; HZSM-5 zeolite; magnesium oxide modification
A series of HZSM-5 zeolites modified with various contents of magnesium oxide (0-10 wt%) were prepared with an incipient impregnation technique and characterized by X-ray diffraction, N-2 adsorption, temperature-programmed desorption of NH3 and CO2, Al-27 MAS NMR., and FT-IR. The modified HZSM-5 zeolites were mixed physically with methanol synthesis components (CuO-ZnO-Al2O3) to perform the direct synthesis of dimethyl ether (DME) from syngas under pressurized fixed-bed continuous-flow conditions. The results indicated that modification of HZSM-5 with a suitable amount of MgO significantly decreased the selectivities for undesired by-products like hydrocarbons and CO2 from 9.3 and 37.1% to less than 0.4 and 31%, respectively, through the removal of unselective strong Bronsted acid sites and hence enhanced the selectivity for DME from 49% to more than 64%, whereas the conversion of carbon monoxide was scarcely affected. However, when the MgO contents were equal to or higher than 5 wt%, both the conversion of CO and selectivity for DME decreased markedly because of the decreased activity for methanol dehydration. A mechanism for methanol dehydration to DME involving both acidic and basic sites on the HZSM-5 zeolites modified with MgO has been proposed based on the results obtained. (C) 2004 Elsevier Inc. All rights reserved.
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