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Reaction Behaviors and Kinetics during Induction Period of Methanol Conversion on HZSM-5 Zeolite
Qi, Liang1,2; Wei, Yingxu1; Xu, Lei1; Liu, Zhongmin1
关键词Methanol Induction Period Kinetics Activation Energy Hzsm-5
刊名ACS CATALYSIS
2015-07-01
DOI10.1021/acscatal.5b00654
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
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
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.
语种英语
WOS记录号WOS:000357626800009
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被引频次:24[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://cas-ir.dicp.ac.cn/handle/321008/146397
专题中国科学院大连化学物理研究所
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
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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.
APA Qi, Liang,Wei, Yingxu,Xu, Lei,&Liu, Zhongmin.(2015).Reaction Behaviors and Kinetics during Induction Period of Methanol Conversion on HZSM-5 Zeolite.ACS CATALYSIS,5(7),3973-3982.
MLA Qi, Liang,et al."Reaction Behaviors and Kinetics during Induction Period of Methanol Conversion on HZSM-5 Zeolite".ACS CATALYSIS 5.7(2015):3973-3982.
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