A comparative study of methanol to olefin over CHA and MTF zeolites

被引:92
作者
Zhu, Qingjun
Kondo, Junko N.
Tatsumi, Takashi
Inagaki, Satoshi
Ohnuma, Ryosuke
Kubota, Yoshihiro
Shimodaira, Yoshiki
Kobayashi, Hisayoshi
Domen, Kazunari
机构
[1] Tokyo Inst Technol, Chem Resources Lab, Midori Ku, Yokohama, Kanagawa 2268503, Japan
[2] Yokohama Natl Univ, Div Mat Sci & Chem Engn, Hodogaya Ku, Yokohama, Kanagawa 2408501, Japan
[3] Univ Tokyo, Fac Sci, Dept Appl Chem, Shinjuku Ku, Tokyo 1628601, Japan
[4] Kyoto Inst Technol, Dept Chem Mat Technol, Sakyo Ku, Kyoto 6068585, Japan
[5] Univ Tokyo, Dept Chem Syst Engn, Bunkyo Ku, Tokyo 1138656, Japan
关键词
D O I
10.1021/jp063172c
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
H-SSZ-13 (CHA) and H-UTM-1 (MTF) zeolites have been synthesized, characterized, and employed as catalysts for the methanol-to-olefin (MTO) reaction. Both zeolites have eight-membered rings, and their structures and acidities are characterized by Al-27 magic-angle spinning (MAS) NMR, NH3-TPD (temperature-programmed desorption), and in-situ IR spectroscopy. In-situ IR spectroscopy indicates that methanol is efficiently activated on the Bronsted acid sites of both zeolites. At 673 K, the methanol is quantitatively converted to hydrocarbons, mainly ethene and propene, over H-SSZ-13, whereas H-UTM-1 only initially gives a small amount of alkenes, the main product being dimethyl ether. It is proposed that the limited space in the cages of the MTF zeolite prevents formation of intermediate polymethylbenzenes and thereby also formation of hydrocarbons, whereas the cage size in the CHA type zeolite, which is active, is large enough to accommodate polymethylbenzenes.
引用
收藏
页码:5409 / 5415
页数:7
相关论文
共 38 条
[1]   Theoretical study of the methylbenzene side-chain hydrocarbon pool mechanism in methanol to olefin catalysis [J].
Arstad, B ;
Nicholas, JB ;
Haw, JF .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2004, 126 (09) :2991-3001
[2]   The reactivity of molecules trapped within the SAPO-34 cavities in the methanol-to-hydrocarbons reaction [J].
Arstad, B ;
Kolboe, S .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2001, 123 (33) :8137-8138
[3]   Crystal structure of zeolite MCM-35 (MTF) [J].
Barrett, PA ;
Díaz-Cabañas, MJ ;
Camblor, MA .
CHEMISTRY OF MATERIALS, 1999, 11 (10) :2919-2927
[4]   Coke precursor formation and zeolite deactivation: mechanistic insights from hexamethylbenzene conversion [J].
Bjorgen, M ;
Olsbye, U ;
Kolboe, S .
JOURNAL OF CATALYSIS, 2003, 215 (01) :30-44
[5]   FTIR adsorption studies of H2O and CH3OH in the isostructural H-SSZ-13 and H-SAPO-34:: Formation of H-bonded adducts and protonated clusters [J].
Bordiga, S ;
Regli, L ;
Lamberti, C ;
Zecchina, A ;
Bjorgen, M ;
Lillerud, KP .
JOURNAL OF PHYSICAL CHEMISTRY B, 2005, 109 (16) :7724-7732
[6]   Methanol to hydrocarbons: spectroscopic studies and the significance of extra-framework aluminium [J].
Campbell, SM ;
Jiang, XZ ;
Howe, RF .
MICROPOROUS AND MESOPOROUS MATERIALS, 1999, 29 (1-2) :91-108
[7]   HYDROCARBONS FROM METHANOL [J].
CHANG, CD .
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 1983, 25 (01) :1-118
[8]   Recent advancements in ethylene and propylene production using the UOP/Hydro MTO process [J].
Chen, JQ ;
Bozzano, A ;
Glover, B ;
Fuglerud, T ;
Kvisle, S .
CATALYSIS TODAY, 2005, 106 (1-4) :103-107
[9]   Computational elucidation of the transition state shape selectivity phenomenon [J].
Clark, LA ;
Sierka, M ;
Sauer, J .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2004, 126 (03) :936-947
[10]   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