Methylbenzene hydrocarbon pool in methanol-to-olefins conversion over zeolite H-ZSM-5
文献类型：期刊论文
| 作者 | Wang, Chao1; Xu, Jun1; Qi, Guodong1; Gong, Yanjun2; Wang, Weiyu1; Gao, Pan1; Wang, Qiang1; Feng, Ningdong1; Liu, Xiaolong1; Deng, Feng1 |
| 刊名 | JOURNAL OF CATALYSIS
 |
| 出版日期 | 2015-12-01 |
| 卷号 | 332页码:127-137 |
| 关键词 | Olefins Zeolites Mechanism Carbocations NMR spectroscopy |
| 英文摘要 | The formation and reactivity of a methylbenzenes (MBs) hydrocarbon pool in the induction period of the methanol-to-olefins (MTO) reaction over zeolite H-ZSM-5 was investigated and the mechanistic link of MBs to ethene and propene was revealed. Time evolution analysis of the formed MBs and C-12/C-13 methanol-switching experiments indicate that in the induction period bulkier compounds such as tetraMB and pentaMB have higher reactivity than their lighter counterparts such as p/m-diMB and triMB. By correlating the distribution of MBs trapped on H-ZSM-5 with ethene and propene, we found that tetraMB and pentaMB favor the formation of propene, while p/m-diMB and triMB mainly contribute to the formation of ethene. On the basis of this relationship, the olefin (ethene and propene) selectivity can be controlled by regulating the distribution of trapped MBs by varying the silicon-to-aluminum ratio of ZSM-5, reaction temperature, and space velocity. The reactivity of MBs and the correlation of MBs with olefins were also verified under steady-state conditions. By observation of key cyclopentenyl and pentamethylbenzenium cation intermediates using in situ solid-state NMR spectroscopy, a paring mechanism was proposed to link MBs with ethene and propene. P/M-diMB and triMB produce ethylcyclopentenyl cations followed by splitting off of ethene, while tetraMB and pentaMB generate propyl-attached intermediates, which eventually produce propene. This work provides new insight into the MBs hydrocarbon pool in MTO chemistry. (C) 2015 Elsevier Inc. All rights reserved. |
| WOS标题词 | Science & Technology ; Physical Sciences ; Technology |
| 类目[WOS] | Chemistry, Physical ; Engineering, Chemical |
| 研究领域[WOS] | Chemistry ; Engineering |
| 关键词[WOS] | H-BETA ; REACTION-MECHANISM ; AROMATIC-HYDROCARBONS ; PRODUCT SELECTIVITY ; HEPTAMETHYLBENZENIUM CATION ; CATALYTIC CYCLE ; CO-REACTION ; HZSM-5 ; SAPO-34 ; CHEMISTRY |
| 收录类别 | SCI |
| 语种 | 英语 |
| WOS记录号 | WOS:000366073500015 |
| 公开日期 | 2016-01-19 |
| 源URL | [http://ir.wipm.ac.cn/handle/112942/9076]  |
| 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, Natl Ctr Magnet Resonance Wuhan, 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,Xu, Jun,Qi, Guodong,et al. Methylbenzene hydrocarbon pool in methanol-to-olefins conversion over zeolite H-ZSM-5[J]. JOURNAL OF CATALYSIS,2015,332:127-137. |
| APA | Wang, Chao.,Xu, Jun.,Qi, Guodong.,Gong, Yanjun.,Wang, Weiyu.,...&Deng, Feng.(2015).Methylbenzene hydrocarbon pool in methanol-to-olefins conversion over zeolite H-ZSM-5.JOURNAL OF CATALYSIS,332,127-137. |
| MLA | Wang, Chao,et al."Methylbenzene hydrocarbon pool in methanol-to-olefins conversion over zeolite H-ZSM-5".JOURNAL OF CATALYSIS 332(2015):127-137. |
入库方式： OAI收割
来源：武汉物理与数学研究所
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