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Regulating the physical properties of silica immobilized Fe(II), Ni(II) and Co(II) catalysts towards ethylene oligomerization reactions
Molecular Catalysis ( IF 3.9 ) Pub Date : 2023-08-16 , DOI: 10.1016/j.mcat.2023.113465
Makhosonke Ngcobo , Alina Ouissa , Wolfgang Kleist , Werner R. Thiel , Stephen O. Ojwach

Immobilization of the phenol((triethoxysilyl)propylimino) ligand (LH) on SBA15 and MCM41 afforded the ligands LH-SBA15 and LH-MCM41 respectively. The reactions of LH-SBA15 and LH-MCM41 with NiCl2, CoCl2 and FeCl2 salts produced the respective materials [Ni(LH-SBA15)2Cl2], (Ni-SBA15), [Co(LHSBA15)2Cl2], (Co-SBA15), [Fe(LH-SBA15)2Cl2], (Fe-SBA15) and [Ni(LH-MCM41)2Cl2], (Ni-MCM41) in good yields. The functional group determination, morphology, physical and surfaced properties of the materials containing immobilized ligands and complexes were established from FT-IR, TGA, TEM, SEM-EDX, PXRD, ICP-AES, and nitrogen physisorption measurement techniques. Activation of the complexes on the surface with EtAlCl2 as co-catalyst formed active catalysts for the oligomerization of ethylene affording mainly C6 oligomers. The SBA-15 immobilized catalysts were more active than the corresponding MCM-41 materials, while Ni(II) catalysts performed better than the corresponding Co(II) and Fe(II) systems. The immobilized catalysts could be used in three cycles without significant loss of catalytic activity and selectivity.



中文翻译:

调节二氧化硅固定 Fe(II)、Ni(II) 和 Co(II) 催化剂对乙烯低聚反应的物理性质

将苯酚((三乙氧基甲硅烷基)丙基亚氨基)配体( LH )固定在SBA15和MCM41上分别提供配体LH-SBA15LH-MCM41 。LH-SBA15LH-MCM41与NiCl 2、CoCl 2和FeCl 2盐的反应产生各自的材料[Ni( LH-SBA15 ) 2 Cl 2 ]、( Ni-SBA15 )、[Co( LHSBA15 ) 2 Cl 2 ], ( Co-SBA15 ), [Fe( LH-SBA15 ) 2 Cl 2 ], (Fe-SBA15 ) 和 [Ni( LH-MCM41 ) 2 Cl 2 ], ( Ni-MCM41 ) 产率良好。通过 FT-IR、TGA、TEM、SEM-EDX、PXRD、ICP-AES 和氮物理吸附测量技术,确定了含有固定配体和配合物的材料的官能团测定、形态、物理和表面性质。以EtAlCl 2作为助催化剂活化表面络合物,形成主要提供C 6的乙烯低聚活性催化剂低聚物。SBA-15固定化催化剂比相应的MCM-41材料更具活性,而Ni(II)催化剂的性能优于相应的Co(II)和Fe(II)体系。固定化催化剂可以循环使用三个循环,而催化活性和选择性没有明显损失。

更新日期:2023-08-17
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