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Metal-organic Framework-based Composite Ni@MOF asHeterogenous Catalyst for Ethylene Trimerization
Applied Catalysis A: General ( IF 5.5 ) Pub Date : 2020-02-06 , DOI: 10.1016/j.apcata.2020.117457
Liduo Chen , Yan Jiang , Hongliang Huo , Jinyi Liu , Yuying Li , Cuiqin Li , Na Zhang , Jun Wang

MIL-125(Ti)-NH2 has been post-synthetically modified by reaction of pyridine with the terephthalate amino groups to form pyridine-imine that act as ligands of nickel(II). [email protected] showed moderate catalytic activity and high selectivity to low carbon olefins C4 and C6. Upon activation with MAO, the catalytic activity could achieve 1.81 × 105 g/mol Ni h, and the selectivity toward C6 was about 76.7%, of which the 1-C6= occupied 91.5% under the reaction condition of 50 °C, 1.0 MPa, Al/Ni = 800. Compared with homogenous pyridine-imine nickel complex, the selectivity toward C6 of [email protected] composite was greatly enhanced, which could be attributed to confinement effect of pore wall of MOF structure. Moreover, the [email protected] could be reused for at least two more catalytic runs without significant loss of activity or selectivity, indicating [email protected] had good catalytic stability and recyclability. A possible ethylene oligomerization mechanistic pathway involving reaction intermediates is proposed based on the Cossee mechanism.



中文翻译:

基于金属-金属骨架的Ni @ MOF复合材料作为乙烯三聚反应的均相催化剂

MIL-125(Ti)-NH 2已通过吡啶与对苯二甲酸酯氨基的反应进行合成后修饰,以形成吡啶-亚胺,该吡啶-亚胺充当镍(II)的配体。[受电子邮件保护]对低碳烯烃C 4和C 6表现出中等的催化活性和高选择性。经MAO活化后,催化活性可达到1.81×10 5 g / mol Ni h,对C 6的选择性为76.7%,其中在50°C反应条件下1-C 6 =占91.5%。 ,1.0 MPa,Al / Ni =800。与均相吡啶-亚胺镍配合物相比,[电子邮件保护]对C 6的选择性增强了复合材料的性能,这归因于MOF结构孔壁的约束作用。而且,[受电子邮件保护]可以再使用至少两次,而不会显着降低活性或选择性,这表明[受电子邮件保护]具有良好的催化稳定性和可回收性。基于Cossee机理,提出了一种可能的涉及反应中间体的乙烯低聚机理。

更新日期:2020-02-06
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