Mechanism of alkane H/D exchange over zeolite H-ZSM-5 at low temperature: a combined computational and experimental study
文献类型：期刊论文
| 作者 | Xue, Nianhua3; Xu, Bolian3; Ding, Qian1,4; Feng, Zhaochi1; Chu, Yueying2; Zheng, Anmin2; Deng, Feng2 |
| 刊名 | CATALYSIS SCIENCE & TECHNOLOGY
 |
| 出版日期 | 2016 |
| 卷号 | 6期号:14页码:5350-5363 |
| ISSN号 | 2044-4753 |
| DOI | 10.1039/c6cy00467a |
| 文献子类 | Article |
| 英文摘要 | Theoretical calculations have provided fundamental insights into the possible pathways for the H/D exchange of isobutane with H-ZSM-5 zeolite at room temperature. It is theoretically demonstrated that neither the direct exchange mechanism nor the indirect bimolecular hydride transfer mechanism is an efficient route for isobutane activation due to high activation barriers, which possibly prohibit H/D exchange at low temperatures. It is revealed that a trace of olefin impurities can considerably accelerate the formation of an alkoxyl intermediate which is involved in the bimolecular hydride transfer mechanism. Once the alkoxyl intermediate is generated from the olefin impurities, the catalytic cycle is self-sustaining. On the other hand, the theoretical calculations also illustrate that the extra-framework aluminum (EFAl) species in the dealuminated zeolite has no obvious promotional effect on the H/D exchange. Furthermore, our calculations are also consistent with the experimental results. |
| WOS关键词 | EXTRA-FRAMEWORK ALUMINUM ; SOLID-STATE NMR ; DENSITY-FUNCTIONAL THEORY ; H BOND ACTIVATION ; HYDRIDE TRANSFER ; EXTRAFRAMEWORK ALUMINUM ; THEORETICAL CALCULATION ; SULFATED ZIRCONIA ; ZSM-5 ZEOLITE ; HIGH-FIELD |
| WOS研究方向 | Chemistry |
| 语种 | 英语 |
| WOS记录号 | WOS:000379438000011 |
| 出版者 | ROYAL SOC CHEMISTRY |
| 源URL | [http://cas-ir.dicp.ac.cn/handle/321008/170358]  |
| 专题 | 大连化学物理研究所_中国科学院大连化学物理研究所 |
| 通讯作者 | Zheng, Anmin; Deng, Feng |
| 作者单位 | 1.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China 2.Chinese Acad Sci, State Key Lab Magnet Resonance & Atom & Mol Phys, Natl Ctr Magnet Resonance Wuhan, Wuhan Inst Phys & Math, Wuhan 430071, Peoples R China 3.Nanjing Univ, Key Lab Mesoscop Chem, Sch Chem & Chem Engn, Nanjing 210093, Jiangsu, Peoples R China 4.Chinese Acad Sci, Grad Univ, Beijing 100864, Peoples R China |
| 推荐引用方式 GB/T 7714 | Xue, Nianhua,Xu, Bolian,Ding, Qian,et al. Mechanism of alkane H/D exchange over zeolite H-ZSM-5 at low temperature: a combined computational and experimental study[J]. CATALYSIS SCIENCE & TECHNOLOGY,2016,6(14):5350-5363. |
| APA | Xue, Nianhua.,Xu, Bolian.,Ding, Qian.,Feng, Zhaochi.,Chu, Yueying.,...&Deng, Feng.(2016).Mechanism of alkane H/D exchange over zeolite H-ZSM-5 at low temperature: a combined computational and experimental study.CATALYSIS SCIENCE & TECHNOLOGY,6(14),5350-5363. |
| MLA | Xue, Nianhua,et al."Mechanism of alkane H/D exchange over zeolite H-ZSM-5 at low temperature: a combined computational and experimental study".CATALYSIS SCIENCE & TECHNOLOGY 6.14(2016):5350-5363. |
入库方式： OAI收割
来源：大连化学物理研究所
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