取代水杨醛类镍配合物的合成及催化丙烯齐聚的研究

论文编号:CL062  论文字数:9534,页数:23

摘 要： 本文以l-甲酰基-2-萘酚为原料合成二（1-甲酰基-2-萘酚）镍（Ⅱ）络合物，以此为丙烯齐聚催化剂。用红外图谱表征配合物的结构，用DSC测试了配合物的热性能。将配合物二（2-羟基-1-萘甲醛亚胺）镍负载在硅胶上。以二（1-甲酰基-2-萘酚）镍（Ⅱ），均相及负载的二（2-羟基-1-萘甲醛亚胺）镍为主催化剂，以三乙基三氯化二铝为助催化剂，进行丙烯齐聚反应。用气相色谱对丙烯齐聚反应的产物进行分析。通过紫外光谱研究了配合物/三苯基膦溶液体系的性质，推测催化活性中心形成的可能机理。
 
关键词：l-甲酰基-2-萘酚; 负载催化剂;镍配合物;丙烯齐聚。

Abstract:  In this paper, bis(1 - formyl -2 -naphthol)Ni(Ⅱ) complex was synthesized from 1- formyl -2-naphthol, this complex can be used as catalyst for propylene oligomerization. The complex was characterized by IR and UV spectrum. The thermal property of complex was determined by DSC. The complex bis(2 - hydroxyl -1 - naphthaldehyde imine) nickel was supported on SiO2. Prepylene oligomerization was performed by three types catalysts, bis(1-formyl-2-naphthol) Nickel (Ⅱ) , bis (2 - hydroxy -1 - naphthaldehyde imine)Ni(Ⅱ) and it’s heterogeneous with co-catalyst Et3Al2Cl3. The oligomeric products were analysised by GC. The properties of complexe/triphenylphosphine solution system were investigated by UV method, and    the plausible formation mechanism of catalytic active site was deduced.
Keywords：l-formyl-2–naphthol; Supporting catalysts; Ni(Ⅱ) complex; Propylene oligomerization.

目  录
中文摘要 I
英文摘要 II
目录 III
1  绪论 1
1.1概述 1
1.2  丙烯二聚催化体系 1
1.2.1  镍(Ni)系丙烯二聚催化体系 2
1.2.2.非镍系丙烯二聚催化体系 3
1.3 丙烯二聚的反应机理 4
1.4 席夫碱及其性能 5
1.5 配合物负载 7
1.6 丙烯二聚物的应用 7
1.7 论文的研究意义 7
2 实验部分 9
2.1  原料和仪器 9
2.2  实验步骤 10
2.2.1  二（1-甲酰基-2-萘酚）镍（Ⅱ）的合成 10
2.2.2 二（2-羟基-1-萘甲醛亚胺）镍硅胶负载 10
2.2.3 丙烯齐聚反应 11
2.3.4 气相色谱 11
3.结果与讨论 12
3.1  分析与表征 12
3.1.1  红外图谱 12
3.1.2 DSC图谱 13
3.1.3 紫外图谱 13
3.3 丙烯齐聚的研究 14
3.2.1 不同配体对丙烯齐聚的影响 14
3.2.2 配合物负载对丙烯齐聚的影响 14
3.2.3 三苯基膦对丙烯齐聚的影响 14
4、总结和展望  16
致谢 17
参考文献 18