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Verifying the olefin formation mechanism of the methanol-to-hydrocarbons reaction over H-ZSM-48
Zhang, Jie1,2; Huang, Zhihua1,2; Xu, Lanjian1,2; Zhang, Xiaomin1; Zhang, Xinzhi1; Yuan, Yangyang1; Xu, Lei1
Corresponding AuthorYuan, Yangyang(yuanyangyang@dicp.ac.cn) ; Xu, Lei(leixu@dicp.ac.cn)
Source PublicationCATALYSIS SCIENCE & TECHNOLOGY
2019-05-07
ISSN2044-4753
DOI10.1039/c8cy02621a
Volume9Issue:9Pages:2132-2143
Funding ProjectNational Natural Science Foundation of China[21576252] ; National Natural Science Foundation of China[21506202]
Funding OrganizationNational 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
WOS SubjectChemistry, Physical
WOS Research AreaChemistry
WOS KeywordCATALYTIC PERFORMANCE ; REACTION PATHWAY ; METHYLCYCLOPENTENYL CATIONS ; HEPTAMETHYLBENZENIUM CATION ; PROPYLENE PRODUCTION ; FRAMEWORK TOPOLOGY ; SHAPE SELECTIVITY ; ZEOLITE H-ZSM-5 ; MTO CONVERSION ; CO-REACTION
AbstractThe 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.
Language英语
Funding OrganizationNational 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
WOS IDWOS:000468630500008
PublisherROYAL SOC CHEMISTRY
Citation statistics
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/171856
Collection中国科学院大连化学物理研究所
Corresponding AuthorYuan, Yangyang; Xu, Lei
Affiliation1.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
Recommended Citation
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.
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