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题名: Reaction Behaviors and Kinetics during Induction Period of Methanol Conversion on HZSM-5 Zeolite
作者: Qi, Liang1, 2;  Wei, Yingxu1;  Xu, Lei1;  Liu, Zhongmin1
关键词: methanol ;  induction period ;  kinetics ;  activation energy ;  HZSM-5
刊名: ACS CATALYSIS
发表日期: 2015-07-01
DOI: 10.1021/acscatal.5b00654
卷: 5, 期:7, 页:3973-3982
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Physical
研究领域[WOS]: Chemistry
英文摘要: The reaction behavior in the induction period of the methanol to hydrocarbon (MTH) reaction over HZSM-5 (Si/Al = 19) zeolite has been investigated in a fixed-bed reactor. It is found that the induction period could be more than 2 h when the reaction was performed at a temperature of 255 degrees C and below. Meanwhile, three reaction stages can be clearly distinguished in the induction period: i.e., the initial C-C bond formation stage, the hydrocarbon pool (HCP) species formation stage, and the autocatalysis reaction stage. For each reaction stage, the kinetic parameters as well as the apparent activation energies have been evaluated. The HCP species formation stage is shown to be the rate-determining step. Addition of a ppm amount (molar) of benzene, toluene, or p-xylene to the methanol feed leads to a shortened induction period due to a lower energy barrier for both the HCP species formation and the autocatalysis reaction. A critical value of HCP species, [HCP](c), that is required for starting the autocatalysis reaction (the third stage) has been proposed. This critical value was measured to be 1 toluene molecule per 276 unit cells for HZSM-5 zeolite when toluene is cofed with methanol.
关键词[WOS]: SURFACE METHOXY GROUPS ;  TO-OLEFIN PROCESS ;  FUNCTIONAL THEORY CALCULATIONS ;  DIMETHYL ETHER FORMATION ;  CARBON-CARBON BOND ;  IN-SITU ;  HYDROCARBON FORMATION ;  REACTION-MECHANISM ;  ZSM-5 ZEOLITE ;  AROMATIC-HYDROCARBONS
语种: 英语
WOS记录号: WOS:000357626800009
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/146397
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Chinese Acad Sci, Dalian Inst Chem Phys, iChEM Collaborat Innovat Ctr Chem Energy Mat, Natl Engn Lab Methanol Olefins,Dalian Natl Lab Cl, Dalian 116023, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China

Recommended Citation:
Qi, Liang,Wei, Yingxu,Xu, Lei,et al. Reaction Behaviors and Kinetics during Induction Period of Methanol Conversion on HZSM-5 Zeolite[J]. ACS CATALYSIS,2015,5(7):3973-3982.
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