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DOI | 10.1038/s41467-017-00083-9 |
Gas reactions under intrapore condensation regime within tailored metal-organic framework catalysts | |
Agirrezabal-Telleria, Iker1; Luz, Ignacio2; Ortuno, Manuel A.3; Oregui-Bengoechea, Mikel1; Gandarias, Inaki1; Lopez, Nuria3; Lail, Marty A.2; Soukri, Mustapha2 | |
2019-05-06 | |
发表期刊 | NATURE COMMUNICATIONS
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ISSN | 2041-1723 |
出版年 | 2019 |
卷号 | 10 |
文章类型 | Article |
语种 | 英语 |
国家 | Spain; USA |
英文摘要 | Production of 1-butene, a major monomer in polymer industry, is dominated by homogeneous protocols via ethylene dimerization. Homogeneous catalysts can achieve high selectivity but require large amounts of activators and solvents, and exhibit poor recyclability; in turn, heterogeneous systems are robust but lack selectivity. Here we show how the precise engineering of metal-organic frameworks (MOFs) holds promise for a sustainable process. The key to the (Ru)HKUST-1 MOF activity is the intrapore reactant condensation that enhances ethylene dimerization with high selectivity (> 99% 1-butene) and high stability (>120 h) in the absence of activators and solvents. According to spectroscopy, kinetics, and modeling, the engineering of defective nodes via controlled thermal approaches rules the activity, while intrapore ethylene condensation accounts for selectivity and stability. The combination of well-defined actives sites with the concentration effect arising from condensation regimes paves the way toward the development of robust MOF catalysts for diverse gas-phase reactions. |
领域 | 资源环境 |
收录类别 | SCI-E |
WOS记录号 | WOS:000466872000004 |
WOS关键词 | TOTAL-ENERGY CALCULATIONS ; SINGLE-SITE CATALYSTS ; ETHYLENE DIMERIZATION ; SELECTIVE HYDROGENATION ; HETEROGENEOUS CATALYSIS ; CHEMISTRY ; OLIGOMERIZATION ; TRANSFORMATION ; SORPTION ; DEFECTS |
WOS类目 | Multidisciplinary Sciences |
WOS研究方向 | Science & Technology - Other Topics |
URL | 查看原文 |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/203397 |
专题 | 资源环境科学 |
作者单位 | 1.Univ Basque Country, UPV EHU, Engn Sch, Dept Chem & Environm Engn, Plaza Torres Quevedo 1, Bilbao 48013, Spain; 2.RTI Int, 3040 E Cornwallis Rd, Res Triangle Pk, NC 27709 USA; 3.Barcelona Inst Sci & Technol, Inst Chem Res Catalonia ICIQ, Av Paisos Catalans 16, Tarragona 43007, Spain |
推荐引用方式 GB/T 7714 | Agirrezabal-Telleria, Iker,Luz, Ignacio,Ortuno, Manuel A.,et al. Gas reactions under intrapore condensation regime within tailored metal-organic framework catalysts[J]. NATURE COMMUNICATIONS,2019,10. |
APA | Agirrezabal-Telleria, Iker.,Luz, Ignacio.,Ortuno, Manuel A..,Oregui-Bengoechea, Mikel.,Gandarias, Inaki.,...&Soukri, Mustapha.(2019).Gas reactions under intrapore condensation regime within tailored metal-organic framework catalysts.NATURE COMMUNICATIONS,10. |
MLA | Agirrezabal-Telleria, Iker,et al."Gas reactions under intrapore condensation regime within tailored metal-organic framework catalysts".NATURE COMMUNICATIONS 10(2019). |
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