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Investigating the Coke Formation Mechanism of H-ZSM-5 during Methanol Dehydration Using Operando UV-Raman Spectroscopy

文献类型：期刊论文

作者Fan, Fengtao1; An, Hongyu1,2; Zhang, Fei1,2; Guan, Zaihong3; Liu, Xuebin3; Li, Can1
刊名ACS CATALYSIS
出版日期2018-10-01
卷号8期号:10页码:9207-9215
关键词operando Raman spectroscopy coke H-ZSM-5 methanol dehydration
ISSN号2155-5435
DOI10.1021/acscatal.8b00928
通讯作者Fan, Fengtao(ftfan@dicp.ac.cn) ; Li, Can(canli@dicp.ac.cn)
英文摘要Methanol dehydration on solid acid catalysts is a fundamental step in many industrial chemical processes, such as methanol to dimethyl ether (MTD) and methanol to olefin (MTO). The performance of catalysts often encounters the detrimental effect of coke deposition. However, the heterogeneous distribution of feedstock and product in a fixed-bed reactor usually brings in difficulties in the study of the coking mechanism. In this work, the coking progress of H-ZSM-5 in a fixed-bed reactor under MTD conditions is investigated using operando UV-Raman spectroscopy. Methylbenzenium carbenium ions (MB+), a key precursor for coke formation, was identified by UV resonance Raman spectroscopy and isotope exchange experiments. At higher temperature (473 K), MB+ rapidly transforms into "hard coke" at the beginning of the catalyst bed. The relative intensity of the 1605 cm(-1) peak can serve as an indicator for the catalyst deactivation. Moreover, water formed during MTD can suppress the transformation of MB+ into "hard coke" at the later parts of the bed. These results provide important information for the key steps and intermediates about coke formation on solid acid catalysts during methanol conversion, and the findings will contribute to improved catalytic performance in the related catalytic reaction.
WOS关键词POLYCYCLIC AROMATIC-HYDROCARBONS ; TO-OLEFINS CONVERSION ; ZEOLITE H-MFI ; DIMETHYL ETHER ; CATALYST DEACTIVATION ; ZEOTYPE CATALYSTS ; ACID CATALYSTS ; MTH REACTION ; HZSM-5 ; ZSM-5
资助项目National Natural Science Foundation of China[21373212] ; Strategic Priority Research Program of the Chinese Academy of Sciences[XDB06040400] ; Strategic Priority Research Program of the Chinese Academy of Sciences[XDB17020000] ; DMTO project of the Dalian Institute of Chemical Physics[DICP DMTO201407]
WOS研究方向Chemistry
语种英语
WOS记录号WOS:000447224100024
出版者AMER CHEMICAL SOC
资助机构National Natural Science Foundation of China ; National Natural Science Foundation of China ; Strategic Priority Research Program of the Chinese Academy of Sciences ; Strategic Priority Research Program of the Chinese Academy of Sciences ; DMTO project of the Dalian Institute of Chemical Physics ; DMTO project of the Dalian Institute of Chemical Physics ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Strategic Priority Research Program of the Chinese Academy of Sciences ; Strategic Priority Research Program of the Chinese Academy of Sciences ; DMTO project of the Dalian Institute of Chemical Physics ; DMTO project of the Dalian Institute of Chemical Physics ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Strategic Priority Research Program of the Chinese Academy of Sciences ; Strategic Priority Research Program of the Chinese Academy of Sciences ; DMTO project of the Dalian Institute of Chemical Physics ; DMTO project of the Dalian Institute of Chemical Physics ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Strategic Priority Research Program of the Chinese Academy of Sciences ; Strategic Priority Research Program of the Chinese Academy of Sciences ; DMTO project of the Dalian Institute of Chemical Physics ; DMTO project of the Dalian Institute of Chemical Physics
源URL[http://cas-ir.dicp.ac.cn/handle/321008/166826]  
专题大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者Fan, Fengtao; Li, Can
作者单位1.Chinese Acad Sci, Dalian Inst Chem Phys, Collaborat Innovat Ctr Chem Energy Mat iChEM, State Key Lab Catalysis,Dalian Natl Lab Clean Ene, Zhongshan Rd 457, Dalian 116023, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
3.BP Dalian Branch, Energy Innovat Lab, Dalian, Peoples R China
推荐引用方式
GB/T 7714		 Fan, Fengtao,An, Hongyu,Zhang, Fei,et al. Investigating the Coke Formation Mechanism of H-ZSM-5 during Methanol Dehydration Using Operando UV-Raman Spectroscopy[J]. ACS CATALYSIS,2018,8(10):9207-9215.
APA Fan, Fengtao,An, Hongyu,Zhang, Fei,Guan, Zaihong,Liu, Xuebin,&Li, Can.(2018).Investigating the Coke Formation Mechanism of H-ZSM-5 during Methanol Dehydration Using Operando UV-Raman Spectroscopy.ACS CATALYSIS,8(10),9207-9215.
MLA Fan, Fengtao,et al."Investigating the Coke Formation Mechanism of H-ZSM-5 during Methanol Dehydration Using Operando UV-Raman Spectroscopy".ACS CATALYSIS 8.10(2018):9207-9215.

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来源：大连化学物理研究所

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