树枝状吡啶亚胺铬催化剂的合成及其催化性能研究
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摘要
以1. 0代聚酰胺-胺树枝状大分子为配体骨架、吡啶二甲醛为原料,合成了一种新型树枝状吡啶亚胺(DPI)配体,再以CrCl_3·6H_2O为络合试剂,制备DPI-Cr催化剂。采用IR、UV-Vis、MS、元素分析等确证了产物结构。考察溶剂种类、助催化剂种类、反应温度、乙烯压力以及Al/Cr摩尔比对DPI-Cr催化乙烯齐聚性能的影响。结果表明,DPI-Cr催化剂表现出良好的催化活性和烯烃选择性,优化反应条件下,催化效率可达4. 91×10~4g/mol Cr·h,C_6和C_8选择性为73. 90%。
A novel dendritic pyridineimine ligand DPI was synthesized using 1. 0 G dendritic polyamide-amine and pyridine dialdehyde as the raw materials,and the dendritic pyridineimine chromium( DPI-Cr) catalyst was synthesized with chromium chloride hexahydrate complex as reagent. The structure of the DPI-Cr catalyst was fully characterized by FT-IR,UV-Vis,MS and element analysis. The effect of solvent type,co-catalyst type,reaction temperature,reaction pressure and Al/Cr molar ratio on the catalytic performance in ethylene oligomerization was detected in detail. The results showed that the DPI-Cr catalyst displays better catalytic activity and olefine selectivity.Under the optimal reaction conditions,the catalytic activity could reach up to 4. 91 × 10~4 g/( mol Cr·h),and the selectivity of C_6 and C_8 was 73. 90%.
A novel dendritic pyridineimine ligand DPI was synthesized using 1. 0 G dendritic polyamide-amine and pyridine dialdehyde as the raw materials,and the dendritic pyridineimine chromium( DPI-Cr) catalyst was synthesized with chromium chloride hexahydrate complex as reagent. The structure of the DPI-Cr catalyst was fully characterized by FT-IR,UV-Vis,MS and element analysis. The effect of solvent type,co-catalyst type,reaction temperature,reaction pressure and Al/Cr molar ratio on the catalytic performance in ethylene oligomerization was detected in detail. The results showed that the DPI-Cr catalyst displays better catalytic activity and olefine selectivity.Under the optimal reaction conditions,the catalytic activity could reach up to 4. 91 × 10~4 g/( mol Cr·h),and the selectivity of C_6 and C_8 was 73. 90%.
引文
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[6] Y Shen,M Kuang,Z Shen et al. Angew. Chem. Int. Ed.,2008,47(12):2227~2230.
[7] R Malgas,S F Mapolie,S O Ojwach et al. Catal. Commun.,2008,9(7):1612~1617.
[8] T V Laine,U Piironen,K Lappalainen et al. J. Organomet.Chem.,2000,606(2):112~124.
[9] R Malgas,S F Mapolie,S O Ojwach et al. Catal. Commun.,2008,9(7):1612~1617.
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[14] J Wang,P Zang,S Chen et al. J. Macromol. Sci. A,2013,50(2):163~167.
[15] A Aid,R D Andrei,S Amokrane et al. Appl. Clay Sci.,2017,146:432~438.
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[22]李桂英,张其震,李爱香.生物医学工程研究,2003,22(1):57~59.