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A Mechanistic Study of Methanol-to-Aromatics Reaction over Ga-Modified ZSM-5 Zeolites: Understanding the Dehydrogenation Process
Gao, Pan1,2; Xu, Jun1; Qi, Guodong1; Wang, Chao1; Wang, Qiang1; Zhao, Yanxi3,4; Zhang, Yuhua3,4; Feng, Ningdong1; Zhao, Xingling1,2; Li, Jinlin3,4; Deng, Feng1
2018-10-01
Source PublicationACS CATALYSIS
ISSN2155-5435
Volume8Issue:10Pages:9809-9820
AbstractThe methanol-to-aromatics (MTA) reaction was investigated on Ga-modified ZSM-5 zeolites (Ga/ZSM-5). As revealed by Ga-71 and H-1 solid-state NMR and FT-IR of pyridine adsorption measurements, cationic Ga species are formed as Lewis acid sites by substitution of Bronsted acid sites on H-ZSM-5. Further experimental studies show that C-5- and C-6-cycloalkenes are generated during the MTA reaction, which lead to the formation of cyclic carbocations as precursors to aromatics. Isotope exchange experiments demonstrate that the reactivity of the cyclic carbocations on Ga/ZSM-5 is much higher than that on H-ZSM-5 and they play an intermediate role in the formation of aromatics. In addition to the traditional bimolecular hydrogen transfer (HT) reaction, the dehydrogenation of alkenes with the release of H-2 (DeaH(2) process) was identified to significantly contribute to the formation of aromatics. The transformation of cycloalkenes to aromatics is favored by promotion of the DeaH(2) process and competes with the HT route on Ga/ZSM-5, while these cycloalkenes tend to crack back to alkenes, and the dominating HT route results in lower aromatic selectivity on H-ZSM-5. A DeaH(2)-aromatization route mediated by the cooperation of cationic Ga species and Bronsted acid sites was proposed for the enhanced formation of aromatics on Ga/ZSM-5 zeolite.
Keywordmethanol-to-aromatics dehydrogenation process mechanism metal-modified zeolite solid-state NMR spectroscopy
Funding OrganizationNational Natural Science Foundation of China ; National Natural Science Foundation of China ; key program for frontier science of the Chinese Academy of Sciences ; key program for frontier science of the Chinese Academy of Sciences ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; key program for frontier science of the Chinese Academy of Sciences ; key program for frontier science of the Chinese Academy of Sciences ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; key program for frontier science of the Chinese Academy of Sciences ; key program for frontier science of the Chinese Academy of Sciences ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; key program for frontier science of the Chinese Academy of Sciences ; key program for frontier science of the Chinese Academy of Sciences
DOI10.1021/acscatal.8b03076
WOS KeywordSTATE NMR-SPECTROSCOPY ; CATALYZED METHYLATION REACTIONS ; BRONSTED/LEWIS ACID SYNERGY ; CHEMICAL-VAPOR-DEPOSITION ; PROPANE AROMATIZATION ; SELECTIVE CONVERSION ; OLEFINS CONVERSION ; HYDROGEN-TRANSFER ; HYDROCARBON-POOL ; HZSM-5 CATALYSTS
Language英语
Funding ProjectNational Natural Science Foundation of China[21622311] ; National Natural Science Foundation of China[21473245] ; National Natural Science Foundation of China[21603265] ; National Natural Science Foundation of China[21733013] ; key program for frontier science of the Chinese Academy of Sciences[QYZDB-SSW-SLH027]
Funding OrganizationNational Natural Science Foundation of China ; National Natural Science Foundation of China ; key program for frontier science of the Chinese Academy of Sciences ; key program for frontier science of the Chinese Academy of Sciences ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; key program for frontier science of the Chinese Academy of Sciences ; key program for frontier science of the Chinese Academy of Sciences ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; key program for frontier science of the Chinese Academy of Sciences ; key program for frontier science of the Chinese Academy of Sciences ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; key program for frontier science of the Chinese Academy of Sciences ; key program for frontier science of the Chinese Academy of Sciences
WOS Research AreaChemistry
WOS SubjectChemistry, Physical
WOS IDWOS:000447224100089
PublisherAMER CHEMICAL SOC
Citation statistics
Cited Times:18[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.apm.ac.cn/handle/112942/13330
Collection磁共振应用研究部
Corresponding AuthorXu, Jun; Deng, Feng
Affiliation1.Chinese Acad Sci, State Key Lab Magnet Resonance & Atom & Mol Phys, Natl Ctr Magnet Resonance Wuhan, Wuhan Inst Phys & Math,Key Lab Magnet Resonance B, Wuhan 430071, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
3.South Cent Univ Nationalities, Key Lab Catalysis & Mat Sci, State Ethn Affairs Commiss, Wuhan 430074, Peoples R China
4.South Cent Univ Nationalities, Minist Educ, Wuhan 430074, Peoples R China
Recommended Citation
GB/T 7714
Gao, Pan,Xu, Jun,Qi, Guodong,et al. A Mechanistic Study of Methanol-to-Aromatics Reaction over Ga-Modified ZSM-5 Zeolites: Understanding the Dehydrogenation Process[J]. ACS CATALYSIS,2018,8(10):9809-9820.
APA Gao, Pan.,Xu, Jun.,Qi, Guodong.,Wang, Chao.,Wang, Qiang.,...&Deng, Feng.(2018).A Mechanistic Study of Methanol-to-Aromatics Reaction over Ga-Modified ZSM-5 Zeolites: Understanding the Dehydrogenation Process.ACS CATALYSIS,8(10),9809-9820.
MLA Gao, Pan,et al."A Mechanistic Study of Methanol-to-Aromatics Reaction over Ga-Modified ZSM-5 Zeolites: Understanding the Dehydrogenation Process".ACS CATALYSIS 8.10(2018):9809-9820.
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