New Insight into the Hydrocarbon-Pool Chemistry of the Methanol-to-Olefins Conversion over Zeolite H-ZSM-5 from GC-MS, Solid-State NMR Spectroscopy, and DFT Calculations
文献类型：期刊论文
| 作者 | Wang, Chao1; Chu, Yueying1; Zheng, Anmin1; Xu, Jun1; Wang, Qiang1; Gao, Pan1; Qi, Guodong1; Gong, Yanjun2; Deng, Feng1 |
| 刊名 | CHEMISTRY-A EUROPEAN JOURNAL
 |
| 出版日期 | 2014-09-22 |
| 卷号 | 20期号:39页码:12432-12443 |
| 关键词 | carbocations olefins reaction mechanisms solid-state NMR spectroscopy zeolites |
| 英文摘要 | Over zeolite H-ZSM-5, the aromatics-based hydrocarbon-pool mechanism of methanol-to-olefins (MTO) reaction was studied by GC-MS, solid-state NMR spectroscopy, and theoretical calculations. Isotopic-labeling experimental results demonstrated that polymethylbenzenes (MBs) are intimately correlated with the formation of olefin products in the initial stage. More importantly, three types of cyclopentenyl cations (1,3-dimethylcyclopentenyl, 1,2,3-trimethylcyclopentenyl, and 1,3,4-trimethylcyclopentenyl cations) and a pentamethylbenzenium ion were for the first time identified by solid-state NMR spectroscopy and DFT calculations under both co-feeding ([C-13(6)]benzene and methanol) conditions and typical MTO working (feeding [C-13]methanol alone) conditions. The comparable reactivity of the MBs (from xylene to tetramethylbenzene) and the carbocations (trimethylcyclopentenyl and pentamethylbenzium ions) in the MTO reaction was revealed by C-13-labeling experiments, evidencing that they work together through a paring mechanism to produce propene. The paring route in a full aromatics-based catalytic cycle was also supported by theoretical DFT calculations. |
| WOS标题词 | Science & Technology ; Physical Sciences |
| 类目[WOS] | Chemistry, Multidisciplinary |
| 研究领域[WOS] | Chemistry |
| 关键词[WOS] | SURFACE METHOXY GROUPS ; REACTION-MECHANISM ; H-BETA ; HEPTAMETHYLBENZENIUM CATION ; AROMATIC-HYDROCARBONS ; CATALYTIC CONVERSION ; REACTION CENTERS ; DIMETHYL ETHER ; MTO REACTION ; CO-REACTION |
| 收录类别 | SCI |
| 语种 | 英语 |
| WOS记录号 | WOS:000342626200015 |
| 公开日期 | 2015-07-14 |
| 源URL | [http://ir.wipm.ac.cn/handle/112942/1424]  |
| 专题 | 武汉物理与数学研究所_磁共振应用研究部 |
| 作者单位 | 1.Chinese Acad Sci, Wuhan Inst Phys & Math, Wuhan Ctr Magnet Resonance, State Key Lab Magnet Resonance & Atom Mol Phys, Wuhan 430071, Peoples R China 2.China Univ Petr, CNPC Key Lab Catalysis, State Key Lab Heavy Oil Proc, Beijing 102249, Peoples R China |
| 推荐引用方式 GB/T 7714 | Wang, Chao,Chu, Yueying,Zheng, Anmin,et al. New Insight into the Hydrocarbon-Pool Chemistry of the Methanol-to-Olefins Conversion over Zeolite H-ZSM-5 from GC-MS, Solid-State NMR Spectroscopy, and DFT Calculations[J]. CHEMISTRY-A EUROPEAN JOURNAL,2014,20(39):12432-12443. |
| APA | Wang, Chao.,Chu, Yueying.,Zheng, Anmin.,Xu, Jun.,Wang, Qiang.,...&Deng, Feng.(2014).New Insight into the Hydrocarbon-Pool Chemistry of the Methanol-to-Olefins Conversion over Zeolite H-ZSM-5 from GC-MS, Solid-State NMR Spectroscopy, and DFT Calculations.CHEMISTRY-A EUROPEAN JOURNAL,20(39),12432-12443. |
| MLA | Wang, Chao,et al."New Insight into the Hydrocarbon-Pool Chemistry of the Methanol-to-Olefins Conversion over Zeolite H-ZSM-5 from GC-MS, Solid-State NMR Spectroscopy, and DFT Calculations".CHEMISTRY-A EUROPEAN JOURNAL 20.39(2014):12432-12443. |
入库方式： OAI收割
来源：武汉物理与数学研究所
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