DICP OpenIR
Methanol to Olefins Reaction Route Based on Methylcyclopentadienes as Critical Intermediates
Zhang, Wenna1,3; Zhi, Yuchun1; Huang, Jindou1; Wu, Xinqiang1; Zeng, Shu1,3; Xu, Shutao1; Zheng, Anmin2,4; Wei, Yingxu1; Liu, Zhongmin1
Corresponding AuthorZheng, Anmin(zhenganm@wipm.ac.cn) ; Wei, Yingxu(weiyx@dicp.ac.cn) ; Liu, Zhongmin(liuzm@dicp.ac.cn)
Keywordmethanol-to-olefins H-SAPO-34 indirect mechanism methylcyclopentadiene cyclopentadienes-based cycle
Source PublicationACS CATALYSIS
2019-08-01
ISSN2155-5435
DOI10.1021/acscatal.9b02487
Volume9Issue:8Pages:7373-7379
Funding ProjectNational Natural Science Foundation of China[91745109] ; National Natural Science Foundation of China[21703239] ; National Natural Science Foundation of China[91545104] ; National Natural Science Foundation of China[21473182] ; Youth Innovation Promotion Association of the Chinese Academy of Sciences[2014165] ; LiaoNing Revitalization Talents Program[XLYC1807227] ; Key Research Program of Frontier Sciences, CAS[QYZDY-SSW-JSC024]
Funding OrganizationNational Natural Science Foundation of China ; National Natural Science Foundation of China ; Youth Innovation Promotion Association of the Chinese Academy of Sciences ; Youth Innovation Promotion Association of the Chinese Academy of Sciences ; LiaoNing Revitalization Talents Program ; LiaoNing Revitalization Talents Program ; Key Research Program of Frontier Sciences, CAS ; Key Research Program of Frontier Sciences, CAS ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Youth Innovation Promotion Association of the Chinese Academy of Sciences ; Youth Innovation Promotion Association of the Chinese Academy of Sciences ; LiaoNing Revitalization Talents Program ; LiaoNing Revitalization Talents Program ; Key Research Program of Frontier Sciences, CAS ; Key Research Program of Frontier Sciences, CAS ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Youth Innovation Promotion Association of the Chinese Academy of Sciences ; Youth Innovation Promotion Association of the Chinese Academy of Sciences ; LiaoNing Revitalization Talents Program ; LiaoNing Revitalization Talents Program ; Key Research Program of Frontier Sciences, CAS ; Key Research Program of Frontier Sciences, CAS ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Youth Innovation Promotion Association of the Chinese Academy of Sciences ; Youth Innovation Promotion Association of the Chinese Academy of Sciences ; LiaoNing Revitalization Talents Program ; LiaoNing Revitalization Talents Program ; Key Research Program of Frontier Sciences, CAS ; Key Research Program of Frontier Sciences, CAS
WOS SubjectChemistry, Physical
WOS Research AreaChemistry
WOS KeywordHYDROCARBON-POOL ; REACTION-MECHANISM ; ZEOLITE H-ZSM-5 ; CO-REACTION ; CONVERSION ; INSIGHTS ; HSAPO-34 ; ETHENE ; CYCLE ; IONS
AbstractStarting from C1 raw material, methanol conversion to hydrocarbons has been realized via a rather complicated pathway. In this contribution, we proposed an alternative methanol reaction route and provided a general understanding of such complex indirect mechanism. The methylcyclopentenyl cations and their deprotonated counterparts (methylcyclopentadienes) were validated to appear on the working H-SAPO-34 catalyst by in situ C-13 MAS NMR spectroscopy and the GC-MS technique, and their catalytic reactivity was revealed by the C-12/C-13-CH3OH isotopic switch experiment. In this context, a cyclopentadienes-based cycle was established, in which light olefins were formed with methylcyclopentadienes as critical intermediates. The feasibility of this alternative route was confirmed by density functional theory calculations. Notably, the cyclopentadienes-based cycle runs in parallel with the traditional alkenes-based and aromatics-based cycles; these three mechanistic cycles are interrelated through interconversion of the involved intermediates, including alkene, cyclopentadiene, and aromatic species. All these three cycles work together for the C-C bond assembly in the methanol-to-olefins reaction system. These findings help to build a more complete methanol conversion network and advance the in-depth understanding of indirect mechanism of methanol conversion.
Language英语
Funding OrganizationNational Natural Science Foundation of China ; National Natural Science Foundation of China ; Youth Innovation Promotion Association of the Chinese Academy of Sciences ; Youth Innovation Promotion Association of the Chinese Academy of Sciences ; LiaoNing Revitalization Talents Program ; LiaoNing Revitalization Talents Program ; Key Research Program of Frontier Sciences, CAS ; Key Research Program of Frontier Sciences, CAS ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Youth Innovation Promotion Association of the Chinese Academy of Sciences ; Youth Innovation Promotion Association of the Chinese Academy of Sciences ; LiaoNing Revitalization Talents Program ; LiaoNing Revitalization Talents Program ; Key Research Program of Frontier Sciences, CAS ; Key Research Program of Frontier Sciences, CAS ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Youth Innovation Promotion Association of the Chinese Academy of Sciences ; Youth Innovation Promotion Association of the Chinese Academy of Sciences ; LiaoNing Revitalization Talents Program ; LiaoNing Revitalization Talents Program ; Key Research Program of Frontier Sciences, CAS ; Key Research Program of Frontier Sciences, CAS ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Youth Innovation Promotion Association of the Chinese Academy of Sciences ; Youth Innovation Promotion Association of the Chinese Academy of Sciences ; LiaoNing Revitalization Talents Program ; LiaoNing Revitalization Talents Program ; Key Research Program of Frontier Sciences, CAS ; Key Research Program of Frontier Sciences, CAS
WOS IDWOS:000480503700080
PublisherAMER CHEMICAL SOC
Citation statistics
Cited Times:3[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/173428
Collection中国科学院大连化学物理研究所
Corresponding AuthorZheng, Anmin; Wei, Yingxu; Liu, Zhongmin
Affiliation1.Chinese Acad Sci, Natl Engn Lab Methanol Olefins, iChEM Collaborat Innovat Ctr Chem Energy Mat, Dalian Inst Chem Phys,Dalian Natl Lab Clean Energ, Dalian 116023, Peoples R China
2.Chinese Acad Sci, Inst Phys & Math, Natl Ctr Magnet Resonance Wuhan, State Key Lab Magnet Resonance & Atom Mol Phys, Wuhan 430071, Hubei, Peoples R China
3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
4.Zhengzhou Univ, Sch Mat Sci & Engn, Zhengzhou 450052, Henan, Peoples R China
Recommended Citation
GB/T 7714
Zhang, Wenna,Zhi, Yuchun,Huang, Jindou,et al. Methanol to Olefins Reaction Route Based on Methylcyclopentadienes as Critical Intermediates[J]. ACS CATALYSIS,2019,9(8):7373-7379.
APA Zhang, Wenna.,Zhi, Yuchun.,Huang, Jindou.,Wu, Xinqiang.,Zeng, Shu.,...&Liu, Zhongmin.(2019).Methanol to Olefins Reaction Route Based on Methylcyclopentadienes as Critical Intermediates.ACS CATALYSIS,9(8),7373-7379.
MLA Zhang, Wenna,et al."Methanol to Olefins Reaction Route Based on Methylcyclopentadienes as Critical Intermediates".ACS CATALYSIS 9.8(2019):7373-7379.
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