C-C Bond Formation in Syngas Conversion over Zinc Sites Grafted on ZSM-5 Zeolite | |
Chen, YX; Gong, K; Jiao, F; Pan, XL; Hou, GJ; Si, R; Bao, XH | |
刊名 | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION |
2020 | |
卷号 | 59期号:16页码:6529-6534 |
关键词 | PROPANE AROMATIZATION SELECTIVE CONVERSION REDUCING CATALYST LIGHT OLEFINS SYNTHESIS GAS ACTIVE-SITES PARA-XYLENE SOLID ACID HIGH-FIELD METHANOL |
ISSN号 | 1433-7851 |
DOI | 10.1002/anie.201912869 |
文献子类 | 期刊论文 |
英文摘要 | Despite significant progress achieved in Fischer-Tropsch synthesis (FTS) technology, control of product selectivity remains a challenge in syngas conversion. Herein, we demonstrate that Zn2+-ion exchanged ZSM-5 zeolite steers syngas conversion selectively to ethane with its selectivity reaching as high as 86 % among hydrocarbons (excluding CO2) at 20 % CO conversion. NMR spectroscopy, X-ray absorption spectroscopy, and X-ray fluorescence indicate that this is likely attributed to the highly dispersed Zn sites grafted on ZSM-5. Quasi-in-situ solid-state NMR, obtained by quenching the reaction in liquid N-2, detects C-2 species such as acetyl (-COCH3) bonding with an oxygen, ethyl (-CH2CH3) bonding with a Zn site, and epoxyethane molecules adsorbing on a Zn site and a Bronsted acid site of the catalyst, respectively. These species could provide insight into C-C bond formation during ethane formation. Interestingly, this selective reaction pathway toward ethane appears to be general because a series of other Zn2+-ion exchanged aluminosilicate zeolites with different topologies (for example, SSZ-13, MCM-22, and ZSM-12) all give ethane predominantly. By contrast, a physical mixture of ZnO-ZSM-5 favors formation of hydrocarbons beyond C3+. These results provide an important guide for tuning the product selectivity in syngas conversion. |
语种 | 英语 |
内容类型 | 期刊论文 |
源URL | [http://ir.sinap.ac.cn/handle/331007/32741] |
专题 | 上海应用物理研究所_中科院上海应用物理研究所2011-2017年 |
作者单位 | 1.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai, Peoples R China 2.Chinese Acad Sci, Dalian Inst Chem Phys, Collaborat Innovat Ctr Chem Energy Mat 2011, State Key Lab Catalysis,Natl Lab Clean Energy, 457 Zhongshan Rd, Dalian 116023, Peoples R China 3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China |
推荐引用方式 GB/T 7714 | Chen, YX,Gong, K,Jiao, F,et al. C-C Bond Formation in Syngas Conversion over Zinc Sites Grafted on ZSM-5 Zeolite[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2020,59(16):6529-6534. |
APA | Chen, YX.,Gong, K.,Jiao, F.,Pan, XL.,Hou, GJ.,...&Bao, XH.(2020).C-C Bond Formation in Syngas Conversion over Zinc Sites Grafted on ZSM-5 Zeolite.ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,59(16),6529-6534. |
MLA | Chen, YX,et al."C-C Bond Formation in Syngas Conversion over Zinc Sites Grafted on ZSM-5 Zeolite".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 59.16(2020):6529-6534. |
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