中国科学院机构知识库网格
Chinese Academy of Sciences Institutional Repositories Grid
Verifying the olefin formation mechanism of the methanol-to-hydrocarbons reaction over H-ZSM-48

文献类型:期刊论文

作者Zhang, Jie1,2; Huang, Zhihua1,2; Xu, Lanjian1,2; Zhang, Xiaomin2; Zhang, Xinzhi2; Yuan, Yangyang2; Xu, Lei2
刊名CATALYSIS SCIENCE & TECHNOLOGY
出版日期2019-05-07
卷号9期号:9页码:2132-2143
ISSN号2044-4753
DOI10.1039/c8cy02621a
通讯作者Yuan, Yangyang(yuanyangyang@dicp.ac.cn) ; Xu, Lei(leixu@dicp.ac.cn)
英文摘要The methanol to hydrocarbons reaction over a unidimensional 10-membered-ring zeolite, H-ZSM-48, was investigated in the temperature range of 723-973 K. C3-5 olefins were the dominant products of reaction at 723 K. Multiple approaches (constant, transient, co-feed and isotope labelling experiments) have been adopted to clarify the underlying reaction pathway. The results indicate that both of the olefin-and aromatics-based cycles contribute to light olefin formation, and the aromatics-based cycle can be significantly enhanced with increasing reaction temperature. Ethene is formed predominantly from the aromatics-based cycle while propene and higher olefins are mainly derived from the olefin-based cycle. The C-12/C-13-methanol isotopic switching experiments manifest that hexamethylbenzene is the most active aromatic intermediate. Co-feeding of C-13-methanol and C-12-benzene at 543 K reveals that the paring mechanism is the dominant mechanism for aromatic dealkylation. More importantly, the first experimental evidence that the two carbons of ethene are derived from aromatic ring carbons is obtained based on the isotopic pattern. Furthermore, the investigation on coke-covered H-ZSM-48 reveals that the reaction of methylbenzenes occurs mainly inside the channels. This work will shed new light on the reaction pathway of the MTH reaction over unidimensional zeolites.
WOS关键词CATALYTIC PERFORMANCE ; REACTION PATHWAY ; METHYLCYCLOPENTENYL CATIONS ; HEPTAMETHYLBENZENIUM CATION ; PROPYLENE PRODUCTION ; FRAMEWORK TOPOLOGY ; SHAPE SELECTIVITY ; ZEOLITE H-ZSM-5 ; MTO CONVERSION ; CO-REACTION
资助项目National Natural Science Foundation of China[21576252] ; National Natural Science Foundation of China[21506202]
WOS研究方向Chemistry
语种英语
WOS记录号WOS:000468630500008
出版者ROYAL SOC CHEMISTRY
资助机构National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China
源URL[http://cas-ir.dicp.ac.cn/handle/321008/171855]  
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Yuan, Yangyang; Xu, Lei
作者单位1.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
2.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
推荐引用方式
GB/T 7714
Zhang, Jie,Huang, Zhihua,Xu, Lanjian,et al. Verifying the olefin formation mechanism of the methanol-to-hydrocarbons reaction over H-ZSM-48[J]. CATALYSIS SCIENCE & TECHNOLOGY,2019,9(9):2132-2143.
APA Zhang, Jie.,Huang, Zhihua.,Xu, Lanjian.,Zhang, Xiaomin.,Zhang, Xinzhi.,...&Xu, Lei.(2019).Verifying the olefin formation mechanism of the methanol-to-hydrocarbons reaction over H-ZSM-48.CATALYSIS SCIENCE & TECHNOLOGY,9(9),2132-2143.
MLA Zhang, Jie,et al."Verifying the olefin formation mechanism of the methanol-to-hydrocarbons reaction over H-ZSM-48".CATALYSIS SCIENCE & TECHNOLOGY 9.9(2019):2132-2143.

入库方式: OAI收割

来源:大连化学物理研究所

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