Fast detection and structural identification of carbocations on zeolites by dynamic nuclear polarization enhanced solid-state nmr
文献类型：期刊论文
| 作者 | Xiao, Dong1,2,3; Xu, Shutao4; Brownbill, Nick J.3; Paul, Subhradip5; Chen, Li-Hua6; Pawsey, Shane7; Aussenac, Fabien8; Su, Bao-Lian6,9; Han, Xiuwen1; Bao, Xinhe1 |
| 刊名 | Chemical science
 |
| 出版日期 | 2018-11-21 |
| 卷号 | 9期号:43页码:11 |
| ISSN号 | 2041-6520 |
| DOI | 10.1039/c8sc03848a |
| 通讯作者 | Blanc, frederic(frederic.blanc@liverpool.ac.uk) |
| 英文摘要 | Acidic zeolites are porous aluminosilicates used in a wide range of industrial processes such as adsorption and catalysis. the formation of carbocation intermediates plays a key role in reactivity, selectivity and deactivation in heterogeneous catalytic processes. however, the observation and determination of carbocations remain a significant challenge in heterogeneous catalysis due to the lack of selective techniques of sufficient sensitivity to detect their low concentrations. here, we combine c-13 isotopic enrichment and efficient dynamic nuclear polarization magic angle spinning nuclear magnetic resonance spectroscopy to detect carbocations in zeolites. we use two dimensional c-13-c-13 through-bond correlations to establish their structures and si-29-c-13 through-space experiments to quantitatively probe the interaction between multiple surface sites of the zeolites and the confined hydrocarbon pool species. we show that a range of various membered ring carbocations are intermediates in the methanol to hydrocarbons reaction catalysed by different microstructural -zeolites and highlight that different reaction routes for the formation of both targeted hydrocarbon products and coke exist. these species have strong van der waals interaction with the zeolite framework demonstrating that their accumulation in the channels of the zeolites leads to deactivation. these results enable understanding of deactivation pathways and open up opportunities for the design of catalysts with improved performances. |
| WOS关键词 | IN-SITU NMR ; DOUBLE-RESONANCE NMR ; TO-OLEFIN CATALYSIS ; SN-BETA ZEOLITE ; CARBENIUM IONS ; REACTION-MECHANISM ; HEPTAMETHYLBENZENIUM CATION ; H-BETA ; HETEROGENEOUS CATALYSIS ; HYDROCARBONS REACTION |
| WOS研究方向 | Chemistry |
| WOS类目 | Chemistry, Multidisciplinary |
| 语种 | 英语 |
| WOS记录号 | WOS:000449701000003 |
| 出版者 | ROYAL SOC CHEMISTRY |
| URI标识 | http://www.irgrid.ac.cn/handle/1471x/2373096 |
| 专题 | 大连化学物理研究所 |
| 通讯作者 | Blanc, Frederic |
| 作者单位 | 1.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, 457 Zhongshan Rd, Dalian 116023, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 3.Univ Liverpool, Dept Chem, Crown St, Liverpool L69 7ZD, Merseyside, England 4.Chinese Acad Sci, Dalian Inst Chem Phys, Natl Engn Lab Methanol Olefins, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China 5.Univ Nottingham, Sir Peter Mansfield Imaging Ctr, DNP MAS NMR Facil, Nottingham NG7 2RD, England 6.Wuhan Univ Technol, State Key Lab Adv Technol Mat Synth & Proc, 122 Luoshi Rd, Wuhan 430070, Hubei, Peoples R China 7.Bruker BioSpin Corp, 15 Fortune Dr, Billerica, MA 01821 USA 8.Bruker BioSpin, 34 Rue Ind BP 10002, F-67166 Wissembourg, France 9.Univ Namur, CMI, Lab Inorgan Mat Chem, 61 Rue Bruxelles, B-5000 Namur, Belgium 10.Univ Liverpool, Stephenson Inst Renewable Energy, Crown St, Liverpool L69 7ZD, Merseyside, England |
| 推荐引用方式 GB/T 7714 | Xiao, Dong,Xu, Shutao,Brownbill, Nick J.,et al. Fast detection and structural identification of carbocations on zeolites by dynamic nuclear polarization enhanced solid-state nmr[J]. Chemical science,2018,9(43):11. |
| APA | Xiao, Dong.,Xu, Shutao.,Brownbill, Nick J..,Paul, Subhradip.,Chen, Li-Hua.,...&Blanc, Frederic.(2018).Fast detection and structural identification of carbocations on zeolites by dynamic nuclear polarization enhanced solid-state nmr.Chemical science,9(43),11. |
| MLA | Xiao, Dong,et al."Fast detection and structural identification of carbocations on zeolites by dynamic nuclear polarization enhanced solid-state nmr".Chemical science 9.43(2018):11. |
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来源：大连化学物理研究所
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