An Oft-studied reaction that may never have been: Direct catalytic conversion of methanol or dimethyl ether to hydrocarbons on the solid acids HZSM-5 or HSAPO-34

被引:246
作者
Song, WG
Marcus, DM
Fu, H
Ehresmann, JO
Haw, JF
机构
[1] Univ So Calif, Loker Hydrocarbon Res Inst, Los Angeles, CA 90089 USA
[2] Univ So Calif, Dept Chem, Los Angeles, CA 90089 USA
关键词
D O I
10.1021/ja016499u
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Using highly purified reagents and careful tests, we show that methanol and dimethyl ether are apparently unreactive on the two most important methanol-to-hydrocarbon catalysts, HZSM-5 and HSAPO-34. Thus, none of the "direct" mechanisms involving two to four carbon atoms in intermediates such as oxonium ylides, carbenes, carbocations, and free radicals are applicable. Only the "indirect" route (hydrocarbon pool) is an established mechanism for this chemistry. An active catalyst requires a hydrocarbon pool that typically begins with products from organic impurities in the feed, carrier gas, or the solid acid itself. Impurities may also play important roles in other reactions catalyzed by solid acids. Copyright © 2002 American Chemical Society.
引用
收藏
页码:3844 / 3845
页数:2
相关论文
共 16 条
[1]   HYDROCARBONS FROM METHANOL [J].
CHANG, CD .
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 1983, 25 (01) :1-118
[2]   CONVERSION OF METHANOL AND OTHER O-COMPOUNDS TO HYDROCARBONS OVER ZEOLITE CATALYSTS [J].
CHANG, CD ;
SILVESTRI, AJ .
JOURNAL OF CATALYSIS, 1977, 47 (02) :249-259
[3]   EVIDENCE OF AUTO-CATALYSIS IN METHANOL TO HYDROCARBON REACTIONS OVER ZEOLITE CATALYSTS [J].
CHEN, NY ;
REAGAN, WJ .
JOURNAL OF CATALYSIS, 1979, 59 (01) :123-129
[4]   On the reaction mechanism for hydrocarbon formation from methanol over SAPO-34 .2. Isotopic labeling studies of the co-reaction of propene and methanol [J].
Dahl, IM ;
Kolboe, S .
JOURNAL OF CATALYSIS, 1996, 161 (01) :304-309
[5]   ON THE REACTION-MECHANISM FOR HYDROCARBON FORMATION FROM METHANOL OVER SAPO-34 .1. ISOTOPIC LABELING STUDIES OF THE CO-REACTION OF ETHENE AND METHANOL [J].
DAHL, IM ;
KOLBOE, S .
JOURNAL OF CATALYSIS, 1994, 149 (02) :458-464
[6]   Pulse-quench catalytic reactor studies reveal a carbon-pool mechanism in methanol-to-gasoline chemistry on zeolite HZSM-5 [J].
Goguen, PW ;
Xu, T ;
Barich, DH ;
Skloss, TW ;
Song, WG ;
Wang, ZK ;
Nicholas, JB ;
Haw, JF .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1998, 120 (11) :2650-2651
[7]   Roles for cyclopentenyl cations in the synthesis of hydrocarbons from methanol on zeolite catalyst HZSM-5 [J].
Haw, JF ;
Nicholas, JB ;
Song, WG ;
Deng, F ;
Wang, ZK ;
Xu, T ;
Heneghan, CS .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2000, 122 (19) :4763-4775
[8]   Methanol-to-hydrocarbons: process technology [J].
Keil, FJ .
MICROPOROUS AND MESOPOROUS MATERIALS, 1999, 29 (1-2) :49-66
[9]  
Lok B. M., 1984, US Patent, Patent No. 4440871
[10]  
MIALE JN, 1966, Patent No. 3280212