Role of dehydration catalyst acid properties on one-step DME synthesis over physical mixtures

被引:181
作者
Ramos, FS
de Farias, AMD
Borges, LEP
Monteiro, JL
Fraga, MA
Sousa-Aguiar, EF
Appel, LG
机构
[1] MCT, Inst Nacl Tecnol, Lab Catalise, BR-22081312 Rio De Janeiro, Brazil
[2] Inst Mil Engn, Praca Gen Tiburcio, BR-22290270 Rio De Janeiro, Brazil
[3] Univ Fed Rio de Janeiro, COPPE, NUCAT, BR-21941 Rio De Janeiro, Brazil
[4] Petrobras SA, CENPES, BR-21949900 Rio De Janeiro, Brazil
关键词
dimethyl ether; methanol; natural gas; synthesis gas; solid-acid catalysts;
D O I
10.1016/j.cattod.2004.12.007
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
The direct synthesis of dimethyl ether (DME) was studied in a continuous high-pressure unit composed basically of a Berty reactor and online gas chromatograph. A commercial methanol synthesis catalyst and some solid-acid catalysts (alumina, HZSM-5, tungsten-zirconia and sulfated-zirconia) were used as physical mixtures. The dehydration catalysts were characterised by pyridine adsorption followed by IR spectroscopy and tested in the methanol dehydration reaction itself. All samples were active regardless of the differences in their acidity and a relationship between catalytic activity for methanol-to-DME and acidity could be envisaged; the activity of a solid acid on this reaction was found to be determined mainly by the number of its more acidic sites. On the one-step DME synthesis from syngas the addition of an acid catalyst to the catalytic system strongly shifted the methanol synthesis reaction, increasing significantly the pass conversion of CO. As a general rule, it could be concluded that the determining rate of DME direct synthesis is determined by the acid properties of the dehydrating catalyst, i.e., its acid strength and number of acid sites. (c) 2004 Elsevier B.V. All rights reserved.
引用
收藏
页码:39 / 44
页数:6
相关论文
共 19 条
[1]   Effective utilization of remote coal through dimethyl ether synthesis [J].
Adachi, Y ;
Komoto, M ;
Watanabe, I ;
Ohno, Y ;
Fujimoto, K .
FUEL, 2000, 79 (3-4) :229-234
[2]   Isotopic and chemical titration of acid sites in tungsten oxide domains supported on zirconia [J].
Baertsch, CD ;
Soled, SL ;
Iglesia, E .
JOURNAL OF PHYSICAL CHEMISTRY B, 2001, 105 (07) :1320-1330
[3]   Solid acid catalysts based on supported tungsten oxides [J].
Barton, DG ;
Soled, SL ;
Iglesia, E .
TOPICS IN CATALYSIS, 1998, 6 (1-4) :87-99
[4]   Spectroscopic characterization of the acid properties of metal oxide catalysts [J].
Busca, G .
CATALYSIS TODAY, 1998, 41 (1-3) :191-206
[5]   Boria modified alumina probed by methanol dehydration and IR spectroscopy [J].
de Farias, AMD ;
Esteves, AML ;
Ziarelli, F ;
Caldarelli, S ;
Fraga, MA ;
Appel, LG .
APPLIED SURFACE SCIENCE, 2004, 227 (1-4) :132-138
[6]  
Fujimoto K., 2000, US Patent, Patent No. 6147125
[7]   Bifunctional catalysts for conversion of synthesis gas to dimethyl ether [J].
Ge, QJ ;
Huang, YM ;
Qiu, FY ;
Li, SB .
APPLIED CATALYSIS A-GENERAL, 1998, 167 (01) :23-30
[8]   KINETICS OF BIMOLECULAR ETHER FORMATION FROM ALCOHOLS OVER ALUMINA [J].
KNOZINGER, H ;
KOCHLOEFT, K ;
MEYE, W .
JOURNAL OF CATALYSIS, 1973, 28 (01) :69-75
[9]  
Knozinger H., 1974, J CATAL, V3, P142
[10]   Catalytic conversion of methane to more useful chemicals and fuels: a challenge for the 21st century [J].
Lunsford, JH .
CATALYSIS TODAY, 2000, 63 (2-4) :165-174