Vapour phase dehydration of crude methanol to dimethyl ether over Na-modified H-ZSM-5 catalysts

被引:211
作者
Vishwanathan, V [1 ]
Jun, KW [1 ]
Kim, JW [1 ]
Roh, HS [1 ]
机构
[1] Korea Res Inst Chem Technol, Div Chem Technol, Taejon 305600, South Korea
关键词
dehydration; crude methanol; dimethyl ether (DME); surface acidity;
D O I
10.1016/j.apcata.2004.08.011
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
A series of Na-modified H-ZSM-5 catalysts, with Na content varying from 0 to 80 mol%, were prepared by an impregnation method, characterized by TPD of ammonia and FT-IR pyridine methods, and tested for the dehydration of crude methanol (i.e. pure/anhydrous methanol containing 20 mol% of H2O) in a fixed-bed micro-reactor under normal atmospheric pressure. Though the unmodified H-ZSM-5 catalyst was more active and stable in the presence of water than the commercial gamma-Al2O3, the Na-modified H-ZSM-5 catalysts showed the optimum activity (C-MeOH > 80%) and 100% selectivity for DME in a wide range of temperatures: 230-340 degreesC. The catalysts were tested for the time-on-stream (TOS) and remained least sensitive towards water for a total reaction period of 65 h. The superior performance of Na-modified H-ZSM-5 catalyst is attributed mainly to the elimination of strong surface acid-sites by partial substitution of Na in H-ZSM-5, resulting in the prevention of coke and/or hydrocarbon formation. (C) 2004 Elsevier B.V. All rights reserved.
引用
收藏
页码:251 / 255
页数:5
相关论文
共 24 条
[1]   Spectroscopic and XRD characterisation of zeolite catalysts active for the oxidative methylation of benzene with methane [J].
Adebajo, MO ;
Long, MA ;
Frost, RL .
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY, 2004, 60 (04) :791-799
[2]   LIGHT ALKENES FROM SYNGAS VIA DIMETHYL ETHER [J].
CAI, GY ;
LIU, ZM ;
SHI, RM ;
HE, CQ ;
YANG, LX ;
SUN, CL ;
CHANG, YJ .
APPLIED CATALYSIS A-GENERAL, 1995, 125 (01) :29-38
[3]   Surface acidity of MCM-41 by in situ IR studies of pyridine adsorption [J].
Chakraborty, B ;
Viswanathan, B .
CATALYSIS TODAY, 1999, 49 (1-3) :253-260
[4]   HYDROCARBONS FROM METHANOL [J].
CHANG, CD .
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 1983, 25 (01) :1-118
[5]   POISONING AND NATURE OF ALUMINA SURFACE IN DEHYDRATION OF METHANOL [J].
FIGOLI, NS ;
HILLAR, SA ;
PARERA, JM .
JOURNAL OF CATALYSIS, 1971, 20 (02) :230-&
[6]   HEATS OF ADSORPTION OF WATER ON ALPHA-ALUMINA AND GAMMA-ALUMINA [J].
HENDRIKS.BA ;
RUDHAM, R ;
PEARCE, DR .
JOURNAL OF CATALYSIS, 1972, 24 (01) :82-&
[7]  
Ihm SK, 2003, ACS SYM SER, V852, P183
[8]  
Joo OS, 2002, B KOR CHEM SOC, V23, P1103
[9]  
Jun KW, 2003, B KOR CHEM SOC, V24, P106
[10]  
Jun KW, 2002, B KOR CHEM SOC, V23, P803