Insight into the Dual Cycle Mechanism of Methanol-to-Olefins Reaction over SAPO-34 Molecular Sieve by Isotopic Tracer Studies

被引:6
作者
Yu, Bowen [1 ,2 ]
Lou, Caiyi [1 ,2 ]
Zhang, Wenna [1 ]
Xu, Shutao [1 ]
Han, Jingfeng [1 ]
Yu, Zhengxi [1 ]
Wei, Yingxu [1 ]
Liu, Zhongmin [1 ]
机构
[1] Chinese Acad Sci, iChEM Collaborat Innovat Ctr Chem Energy Mat, Natl Engn Lab Methanol Olefins, Dalian Natl Lab Clean Energy,Dalian Inst Chem Phy, Dalian 116023, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100039, Peoples R China
基金
中国国家自然科学基金; 国家重点研发计划;
关键词
SAPO-34; Methanol-to-olefin(MTO); Polymethylbenzene; Dual-cycle mechanism; Isotopic tracer; CARBON-CARBON BOND; MTO REACTION; HEPTAMETHYLBENZENIUM CATION; HYDROCARBON FORMATION; CO-REACTION; CONVERSION; ZEOLITE; SELECTIVITY; CATALYSIS; H-ZSM-5;
D O I
10.1007/s40242-020-0216-x
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Methanol-to-olefins(MTO) reaction is one of the important non-petroleum routes to produce light olefins over acidic molecular sieves. In this study, the complete reaction course of MTO on SAPO-34 molecular sieve with retained organics evolution from induction period to deactivation period was investigated systematically at different weight hourly space velocities(WHSV) of methanol. By the aid of(12)C/C-13-methanol isotopic switch experiment, the dual cycle mechanism involving aromatics-based cycle and alkenes-based cycle was evaluated during the whole reaction process. The detailed reaction route varied with the evolution of the retained organics in the catalyst at different reaction stages. The aromatics-based cycle and alkenes-based cycle alternately dominate the reaction process. In the efficient reaction period, aromatics-based cycle is the main reaction mechanism, while in the induction and deactivation periods, the contribution of alkenes-based cycle mechanism will become more important.
引用
收藏
页码:1203 / 1208
页数:6
相关论文
共 45 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]   Conversion of methanol to hydrocarbons over zeolite H-ZSM-5: On the origin of the olefinic species [J].
Bjorgen, Morten ;
Svelle, Stian ;
Joensen, Finn ;
Nerlov, Jesper ;
Kolboe, Stein ;
Bonino, Francesca ;
Palumbo, Luisa ;
Bordiga, Silvia ;
Olsbye, Unni .
JOURNAL OF CATALYSIS, 2007, 249 (02) :195-207
[3]   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
[4]   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
[5]   Initial Carbon-Carbon Bond Formation during the Early Stages of the Methanol-to-Olefin Process Proven by Zeolite-Trapped Acetate and Methyl Acetate [J].
Chowdhury, Abhishek Dutta ;
Houben, Klaartje ;
Whiting, Gareth T. ;
Mokhtar, Mohamed ;
Asiri, Abdullah M. ;
Al-Thabaiti, Shaeel A. ;
Basahel, Suliman N. ;
Baldus, Marc ;
Weckhuysen, Bert M. .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2016, 55 (51) :15840-15845
[6]   FREE-RADICALS IN DIMETHYL ETHER ON H-ZSM-5 ZEOLITE - A NOVEL DIMENSION OF HETEROGENEOUS CATALYSIS [J].
CLARKE, JKA ;
DARCY, R ;
HEGARTY, BF ;
ODONOGHUE, E ;
AMIREBRAHIMI, V ;
ROONEY, JJ .
JOURNAL OF THE CHEMICAL SOCIETY-CHEMICAL COMMUNICATIONS, 1986, (05) :425-426
[7]   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
[8]   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
[9]   Understanding the Early Stages of the Methanol-to-Olefin Conversion on H-SAPO-34 [J].
Dai, Weili ;
Wang, Chuanming ;
Dyballa, Michael ;
Wu, Guangjun ;
Guan, Naijia ;
Li, Landong ;
Xie, Zaiku ;
Hunger, Michael .
ACS CATALYSIS, 2015, 5 (01) :317-326
[10]   ON THE MECHANISM OF METHANOL CONVERSION TO HYDROCARBONS OVER HZSM-5 [J].
DESSAU, RM ;
LAPIERRE, RB .
JOURNAL OF CATALYSIS, 1982, 78 (01) :136-141