CATALYTIC CONVERSION OF OXYGEN-CONTAINING CYCLIC-COMPOUNDS .1. CYCLOHEXANOL CONVERSION OVER H[AL]ZSM-5 AND H[B]ZSM-5

被引:21
作者
BRABEC, L
NOVAKOVA, J
KUBELKOVA, L
机构
[1] J. Heyrovský Institute of Physical Chemistry, Academy of Sciences of the Czech Republic, 182 23 Prague 8
来源
JOURNAL OF MOLECULAR CATALYSIS | 1994年 / 94卷 / 01期
关键词
ACIDITY EFFECTS; CYCLOHEXANOL; CYCLOHEXENE; METALLOSILICATES;
D O I
10.1016/0304-5102(94)87033-0
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
Cyclohexanol (CHL) conversion was measured under low-pressure on-stream conditions on HZSM-5 zeolites and on H-boralite using small amounts of catalysts. Catalytic runs were followed by TPD of the surface species, which also were studied using FTIR spectroscopy. It was found that the individual reaction steps, low-temperature dehydration (yielding cyclohexene), skeletal isomerization (ring contraction to methylcyclopentene) and reactions involving H-transfer (formation of methylcyclopentane, substituted aromatics and simple olefins) were conditioned by the presence of strong acid sites whose number needed for these reactions increased from the dehydration to the H-transfer reactions. The CHL reaction was compared with the reactions of cyclohexene, and the effect of Lewis acid sites present in some cases together with the Bronsted sites was discussed. Ammonia was found to block the active centers, reduce the isomerization and especially the reactions involving H-transfer. Contrary to ammonia, methanol reacted with the CHL surface complexes yielding more substituted aromatics and more olefins than CHL or methanol alone (and/or simple sum of CHL and methanol products).
引用
收藏
页码:117 / 130
页数:14
相关论文
共 25 条
[1]   AN INFRARED-SPECTROSCOPY STUDY OF SIMPLE ALCOHOLS ADSORBED ON H-ZSM-5 [J].
ARONSON, MT ;
GORTE, RJ ;
FARNETH, WE .
JOURNAL OF CATALYSIS, 1987, 105 (02) :455-468
[2]   THE INFLUENCE OF OXONIUM ION AND CARBENIUM ION STABILITIES ON THE ALCOHOL/H-ZSM-5 INTERACTION [J].
ARONSON, MT ;
GORTE, RJ ;
FARNETH, WE .
JOURNAL OF CATALYSIS, 1986, 98 (02) :434-443
[3]   C-13 NMR IDENTIFICATION OF INTERMEDIATES FORMED BY 2-METHYL-2-PROPANOL ADSORPTION IN H-ZSM-5 [J].
ARONSON, MT ;
GORTE, RJ ;
FARNETH, WE ;
WHITE, D .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1989, 111 (03) :840-846
[4]  
BERANEK L, 1960, COLLECT CZECH CHEM C, V25, P2513
[5]   INFRARED STUDY OF CYCLOHEXANOL CHEMISORPTION IN SAPO MOLECULAR-SIEVES [J].
BEZOUHANOVA, C ;
KALVACHEV, Y ;
LECHERT, H .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1991, 87 (19) :3315-3317
[6]   TEMPERATURE-PROGRAMMED DESORPTION STUDIES OF ALCOHOL DECOMPOSITION ON ZNO - 1-PROPANOL, 1-BUTANOL, AND 2-BUTANOL [J].
BOWKER, M ;
PETTS, RW ;
WAUGH, KC .
JOURNAL OF CATALYSIS, 1986, 99 (01) :53-61
[7]   THE EFFECT OF THE FLUORIDE-ION ON THE CATALYTIC ACTIVITY OF ALPO4 IN THE CYCLOHEXENE SKELETAL ISOMERIZATION [J].
CAMPELO, JM ;
GARCIA, A ;
LUNA, D ;
MARINAS, JM .
JOURNAL OF CATALYSIS, 1986, 102 (02) :299-308
[8]   EFFECT OF SULFATE ION ON CATALYTIC ACTIVITY OF ALPO4 IN THE SKELETAL ISOMERIZATION OF CYCLOHEXENE [J].
CAMPELO, JM ;
GARCIA, A ;
LUNA, D ;
MARINAS, JM .
JOURNAL OF CATALYSIS, 1986, 102 (02) :447-451
[9]   HYDROCARBONS FROM METHANOL [J].
CHANG, CD .
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 1983, 25 (01) :1-118
[10]   CONVERSION OF CYCLOHEXENE OVER Y-ZEOLITES - A MODEL REACTION FOR HYDROGEN TRANSFER [J].
CHENG, WC ;
RAJAGOPALAN, K .
JOURNAL OF CATALYSIS, 1989, 119 (02) :354-358