Generating hydrogen-rich fuel-cell feeds from dimethyl ether (DME) using physical mixtures of a commercial Cu/Zn/Al2O3 catalyst and several solid-acid catalysts

被引:102
|
作者
Semelsberger, Troy A.
Ott, Kevin C.
Borup, Rodney L.
Greene, Howard L.
机构
[1] Los Alamos Natl Lab, Div Mat Sci & Technol, Los Alamos, NM 87545 USA
[2] Los Alamos Natl Lab, Div Chem, Los Alamos, NM 87545 USA
[3] Case Western Reserve Univ, Dept Chem Engn, Cleveland, OH 44106 USA
关键词
dimethyl ether; hydrolysis; zeolites; methanol; alumina; zirconia; acidity; ZSM-5; Y; steam reforming; hydrogen; fuel cells;
D O I
10.1016/j.apcatb.2006.02.015
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Homogeneous physical mixtures containing a commercial Cu/ZnO/Al2O3 catalyst and a solid-acid catalyst were used to examine the acidity effects on dimethyl ether hydrolysis and their subsequent effects on dimethyl ether steam reforming (DME-SR). The acid catalysts used were zeolites Y [Si/Al = 2.5 and 15: denoted Y(Si/Al)], ZSM-5 [Si/Al = 15, 25, 40, and 140: denoted Z(Si/Al)] and other conventional catalyst supports (ZrO2, and gamma-Al2O3). The homogeneous physical mixtures contained equal amounts, by volume, of the solid-acid catalyst and the commercial Cu/ZnO/Al2O3 catalyst (BASF K3-110, denoted as K3). The steam reforming of dimethyl ether was carried out in an isothermal packed-bed reactor at ambient pressure. The most promising physical mixtures for the low-temperature production of hydrogen from DME contained ZSM-5 as the solid-acid catalyst, with hydrogen yields exceeding 90% (T = 275 degrees C, SIC = 1.5, tau = 1.0 s and P = 0.78 atm) and hydrogen selectivities exceeding 94%, comparable to those observed for methanol steam reforming (MeOH-SR) over BASF K3-110, with values equaling 95% and 99%, respectively (T = 225 degrees C, S/ C = 1.0, tau = 1.0 s and P = 0.78 atm). Large production rates of hydrogen were directly related to the type of acid catalyst used. The hydrogen production activity trend as a function of physical mixture was [GRAPHICS] (c) 2006 Elsevier B.V. All rights reserved.
引用
收藏
页码:291 / 300
页数:10
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